Recent Advances in The Chemistry and Properties of Atmospheric Nucleants - A Review

171
Recent Advances in the Chemistry and Properties of Atmospheric

Nucleants: a Review
By ALBERTO C. MONTEFINALE,TrIo MONTEFINALEand HENRY M. PAPI~E1)
Summary.- A survey is carried out of recent progress in the investigation of weather-active

atmospheric nucleants. Emphasis is placed on the work done during the last decade, and some resulting implications are discussed.
Introduction
The last few years have witnessed a considerable expansion of the experimental
work which has to do with the atmospheric nucleants in general, and in particular
with the types of nuclei involved directly in cloud formation and precipitation phenomena. This expansion appears to be largely due to an increased interest in atmospheric sciences, environmental problems, and also to an increasing need for fresh
water. Much insight was thus gained into the chemistry and nature of both, naturallyoccurring atmospheric aerosol and of the particulate matter which originates from
human activities. Progress was also made in the development and study of artificial
ways of production of suitable nucleants and in their application to weather-control.
Scientific and engineering aspects of artificial rain stimulation, hail prevention and
clearing of fog, are thus now in an advanced stage of development and testing [1-3] 2)
and concern arises, on the other hand, about the effects of air pollution and inadvertent weather-modification [4] by human activities.
It would, therefore, appear to be of interest to survey, briefly, the progress made
during the last few years and since the time when a number of monographs was written
on the subject [5-7]. Owing to the impossibility of mentioning, let alone describing in
this short review, the detailed fundamentals of both aerosol behaviour, physical
action and of its role in weather phenomena, no such attempt will be made here.
Those aspects were already extensively discussed by MASON [8], BYERS [9], ZETTLEMOYER [10] and others; quotation of work antecedent to references [5-9] will hence
be made only for the sake of comprehension.
1) Center for Aerosol Nucleation; National Research Council of Italy; Via Vettore 4 (Monte
Sacro), 1-00141 Roma.
8) Numbers in brackets refer to References, page 201.
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A.C. Montefinale, T. Montefinale and H. M. Pap&
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1. Condensation nuclei
Those are known to consist, essentially, of a hygroscopic or wettable substance
which promotes the growth of a water cluster or droplet at suitable vapor saturations
in the air. In the absence of coagulation, agglomeration and coalescence, and at
conditions of constant temperature and humidity, the rate of growth and the size of
the resulting droplet will obviously depend on the chemical nature and on the dimensions of the primary nucleus which, if very small, was so far detected and studied
alone by inducing its growth in a supersaturated atmosphere (expansion technique)
and, also, by electrostatic charging and evaluations of its mobility. Condensation
nuclei are thus semi-arbitrarily divided into three classes which will hereafter be
separately discussed in terms of recent work thereon carried out. No comments will
be attempted on the role of the small ions (radius less than 5 x 10-2 micron) in nucleation processes, because of the lack of information on the primary chemical nature of
those tropospheric ions and hence on their modes of action other than electrostatic.
To all practical effects those ions may be excluded from the population of active
condensation nuclei, because of the high water supersaturations necessary for their
action. However, since they are known to electrostrict conspicuous amounts of water
molecules [11-12], the study of a possible component of the vertical transport of
water, caused by electric gradients and due to those clusters, could with time become
of more than academic interest.
a. Aitken nuclei (radius between 5 x 10-2-2 x 10 -1 micron)
Those smallest particles of the condensation nuclei spectrum are commonly
detected and their concentrations evaluated using instruments of the AITKEN, POLLAK
or Rich type, which operate on the principle of expansion and optical (or photoelectric) means of counting [8]. Because of their small size it is generally believed that
they mostly consist of hygroscopic gases and of products of their interaction and
photooxidation [14]. Photolytic transformation, into hygroscopic material, of originally sparsely-soluble organic products, is also possible. The chemical nature of those
nuclei has hence, so far and with a few exceptions only, largely been estimated by
tentative deduction. Concentrations of up to about 10 7 cm -3 are known to exist in
air-polluted cities at low altitudes, and to decrease to about 103 cm- 3 either with
elevation (at about 2.5 km over unpolluted areas) or over the ocean, under conditions
of normal vertical mixing and in the absence of inversions or extensive stratified
clouds [8]. It is now accepted that processes which occur overland are the main source,
per unit area, of those nuclei which derive from combustions (fires), volcanic eruptions, air pollution and biological activity. Bubble-film disruptions and RAYLEIGH
jets do not seem to account for the production of large amounts of sea-salt nuclei of
that size; halogen gases may, however, separate from marine nuclei aloft and may
thus also be expected to react, either directly or photochemically, with otherwise
Vol. 91, 1971/VIII)
Chemistryand Properties of AtmosphericNucleants
173
inactive particulates, yielding small condensation nuclei. Halogens are also known to
react with water yielding acid, hygroscopic and oxidizing products.
A recent paper by WENT [15] points to processes of natural generation of AIT~CEN
nuclei in artificially-unpolluted areas, via photochemical reactions which involve
plant-emanations of both terrestrial and marine origin (mainly terpenes) and NO~
gas. NO~ is here to be regarded as NO, NO2, N203 or a mixture thereof and their
products of hydration, with possible traces of NO; transients photochemically generated when nitrate-containing substance is present in the aerosol. A number of earlier
contributions supports the hypothesis of the effect of natural and artificial short-wave
radiation on the production (or 'activation') of those condensation nuclei in humid
air which contains traces of impurities [16-23]. Pre-activation effects by sunlight have
recently also been reported [24], and may be due to a photoproduction of oxidants in
the irradiated air and their subsequent reactions [25] thus contributing to the persistence of the An'KEN particulates during nighttime [26]. On the other hand ammonia,
and hence also the salts of ammonium, are known to be a common constituent of the
atmospheric aerosol, as they originate from human and animal activities [7, 27].
Photooxidation or ionization in moist air, of ammonia which by itself is hygroscopic,
yields even more hygroscopic NO~ [28] which is known to promote further photooxidation of some aerosol components through a number of chemical steps [29-31],
where pernitrite transients [32], organic peroxides [14], and/or higher oxides of
nitrogen are probably involved. Strong nucleation effects of water vapor due to NO~
were, in fact, observed by several investigators [28, 33-35]. Similar considerations
may be applied, on a much larger scale, to artificially polluted areas [36-38] where
concentrations of photoreactive [3940] aerosol systems, which contain oxides of
nitrogen and sulfur compounds, are notoriously high [41-42]. NO~ generation is
there, per unit area, substantially above its natural rates of production by the oxidation of biological NH3, auroras [43], thunderstorms (see comments by VI~MHSTER
with this regard, Ref. [44]), and upper-atmospheric reactions ([45] and others).
The above discussion is meant to provide a general qualitative idea about the
chemical processes which may account for the generation of AIT~ZENparticulates and
for their changes of concentration according to geography and timing. The importance of
those nuclei, briefly, consists in providing plentiful centers of condensation which have
negligible sedimentation rates and which require low supersaturations of water vapor
(about 2~ at the most) to promote a 'smooth" vapor-liquid transition of phase.
Supersaturations required are considerably higher in the case of small ions [8-10] or
for homogeneous nucleation [8-10], and the practical occurrence of those last two
processes, in the free atmosphere, thus appears to be very unlikely.
Chemical methodsfor the analysis of soluble components of the atmospheric aerosol
[46], and hence a quest for their hygroscopicity, may, necessarily be applied only to
the range of size-spectrum investigated, because of considerable changes of chemical
composition along this spectrum. Inasmuch this presents experimental difficulties in
the case of AITI~ENnuclei, much progress was recently also achieved in this area of
174
A.C. Montefinale,T. Montefinaleand H. M. Pap6e
(Pageoph,
research. It was thus found that a large part of those nuclei often consists, in polluted
areas, of ammonium sulfate [47-48] whose concentration influences the visibility
values [49-50] depending on humidity. There is clearly much need for more measurements of this type, and for their extension to various parts of the world, before the
chemistry and distribution of those nuclei is fully understood. Because of the size of
some economically important, naturally fog-bound areas [51 ] those investigations also
appear to be of more than academic interest. For the same reason there is also much
need for further work on mechanisms by which AITKEN nuclei become inactivated,
coagulate [7], or disappear by rainout or washout [52]. Most available information
on those particulates is merely based on measurements of their mobilities when electrically charged. The upper limit of their diameter range coincides, in fact, with the
limit of this technique.
b. Large nuclei (radius between 0.2-1.0 micron)

Because of relatively low water-vapor saturations in the air and necessary for their
action as centers of condensation, because of their large concentrations in the atmosphere and their low sedimentation rates [53], those nuclei are known to play an
important role in the processes of natural cloud-droplet formation. There exists a
variety of devices and methods of collection whereby the particles captured may be
examined under high-resolution microscopes, or at least counted. Impactor collectors,
spider-thread meshes, conimeters, thermal precipitators, sorting devices (conifuges),
flame counters, millipore filters and other field techniques developed before 1957 are
extensively described and commented on by MASON [8]. More elaborate instruments
based on principles of centrifugal [54] or electric [13] separation, have recently also
been developed. Automatic systems which operate on principles of acoustic counting
[55] or light-scattering [56-57] are, likewise, available. Since the large condensation
nuclei are plentiful (about 102 x cm -3, depending on locations and altitudes) the
determination of their chemical nature is comparatively easiel then in the case of the
much smaller AITKEN aerosol which also sometimes seems to contain similar chemical
ingredients [7, 48].
Direct chemical analyses of large, hygroscopic nuclei show that NH+j and SO2
predominate in those particles [7, 41, 47, 48, 49, 58, 59] together with some C1[7, 48, 49, 58, 59], phosphates [60], smaller amounts of Na +, Mg + +, Ca + +, NO3
[49, 60], fluoride [61] and other trace constituents. Sulfate, chloride and ammonium
components also compare in Antarctic-atmosphere aerosols [62] together with excesses
over O H - of hydrogen cations which seem to be associated with products of sulfur
oxidation [63]. Despite a general belief that chloride is of marine origin, there is
evidence that some of it may originate from industrial and vehicular emission overland [60], vice-versa, despite an offhand thought that ammonia and hence the ammonium constituent of the aerosol may almost entirely be of terrestrial nature, much
of it is generated by the oceans [64].
Vol. 91, 1971/VIII)
Chemistryand Properties of Atmospheric Nucleants
175
With some analogy to AITKEN nuclei the large, hygroscopic, particulates are
believed to generate overland from smoke, pollution, and also from coagulation of
smaller aerosol formed by gaseous reactions and photolytic processes. Over the sea
they are mostly produced by disruption [8, 65] of bubble films on the surface. Their
concentration in the atmosphere hence depends on the wind force, as found by
WOODCOCK (see Ref. [8]). As previously mentioned, the ocean-generated nuclei also
include some organic material [15, 66] or products of its photoalteration [15, 67] and,
likewise, some salts of ammonium. Since photolytic reactions seem to play a large
part in the chemical changes of those airborne solids and liquids, it is not surprising
that relative concentrations of the chemical ingredients of the sea aerosol differ from
those in sea-water [7, 68-73]. This difference [74-75] also appears to depend on the
ion radii involved and on the valence and atom weight of the components [76].
Consistent, large-scale projects on analyses of chemicals dissolved in precipitation
were carried out by JUNGE over the United States [7]. Those results are supplemented
by data of the Scandinavian sampling network [77] and by data obtained from the
North, Western European area [78]. JUNGE'S maps of distribution illustrate the influence of the sea on the balance of chlorine and sodium in the atmosphere. They also
show that there is a fairly uniform distribution of potassium over the USA, an increase
of calcium and sulfate with the distance inland, and that the sulfate in the air is probably of anthropogenic origin. Both, nitrate and ammonia, are associated with higher
latitudes there, possibly either due to densities of vegetation coverage, auroral production [43], industrial activities, and the photolytic depletion of ammonium nitrate
at lower latitudes [32]. It is of interest to note at this point and with regard to this last
statement that, according to JUNGE'S analyses carried out at Round Hill and in Florida
[7], only very small amounts of nitrate appear to coexist with ammonium in the large
nuclei; this same lack of coexistence is also apparent from more recent data obtained
by EGGLETON [49]. It thus appears that besides a natural photolytic depletion of ammonium nitrate [32, 79], the ammonium nitrate-NO x systems scavenge eachother
irreversibly with a concurrent defixation of biologically assimilable atmospheric
compounds of nitrogen [80], and through steps which involve the spontaneous decomposition of ammonium nitrite.
A number of up to date contributions is further illustrative of the geographic
extension of large nuclei [58, 81]. Continental air masses usually contain more of
those particles than oceanic atmospheres do and size distributions do not appear to
vary greatly from continent to continent [82]. The lifetime of cloud nuclei generally
seems to be of about three days; this notwithstanding those particulates are known to
reach areas which are uninfluenced by air pollution [83] and are remote from natural
and artificial sources of dusts, sulfates, halides, sodium, ammonia etc. [7, 70, 84-87].
The annual fluctuations of the water-soluble component of the terrestrial aerosol
strongly depends on human activities and on biological processes. Thus, in the United
States [7], NH3 and NO~ generally attain concentration maxima during the springsummer period in unpolluted areas and in accordance with the cycle of soil biology.
176
(Pageoph,
This situation is reversed in urban areas, because of combustion processes. Similar

considerations may be applied to SO2 and SO2; very high negative correlation
between annual SO 2 concentrations in the air and temperature were, in fact, recently
found by KNAU~R [42] in the atmosphere of a big city. Median diameters of sulfate
particulates, and their concentrations in urban areas, generally also depend on humidity values there [88]; humidity also appears to favor the oxidation process of SOz
to SO3 [89-90] thus indicating that this reaction largely occurs in solution. Overall
concentrations of CI-, both in precipitation and in the air overland, are generally
higher in winter than in summer [78, 91] although it is yet not clear whether this is
predominantly due to increased circulation patterns or to processes of combustion.
Many references so far quoted in this paper also contain results on size distributions and concentrations of large nuclei in the air, as a function of altitude. According
to recent findings [92], a marked discontinuity occurs in the well known logarithmic
distribution of large condensation nuclei, with elevation. This is explained in terms
of rainout and washout phenomena. Distributions of those nuclei are known to
change with the geographic position (which determines the origin of their bulk) and
hence, also with the time of the year, the latitude [93] and meteorological factors.
Large nuclei, hence, normally consist of a mixture of chemical compounds. The
components of this mixture are either hygroscopic or are of a mineral, insoluble but
wettable nature, or both, with a possibility of organic contamination from emanations
of vegetation and other biological phenomena. Chemical analyses and investigations
of the large nuclei were therefore carried out, until recently, with the aim of a qualitative straightforward assessment of the inorganic anionic and cationic groups which
compare in those particulates and little attention was often paid as to whether the
particles captured were 'wet' or 'dry'. Much of the so called atmospheric chemistry
also consisted, essentially, of rainwater analyses for those species. It appears to be
somewhat unfortunate that interest in the chemical composition of those nuclei took
so much time to arise. Before about 1950, and with a few exceptions only, most investigators were largely concerned with determinations of size spectra of those particles, their concentrations in the air, and with the relative humidities necessary for
their 'activation' i.e. their growth to an instrumentally detectable size, by deliquescence or adsorption of water films on the surface. Deductions, on the role of those
chemical species in cloud-nucleation, are complicated in that particles captured in the
vicinity of the earth's surface may be expected to have different relative compositions
[94] from the effective nuclei of cloud formation and that the analysis of precipitation is, on the other hand, likewise not quite representative of the chemical nature of
cloud nuclei [95].
Advances in the use of formvar for making replicas of liquid and solid aerosols [96]
recently enabled the development of continuous particle samplers [97] suitable for
mounting on airplanes and hence for extensive investigations of their geographic
distributions. This, together with modern techniques in applications of electron microscopy [48] enabled better evaluations of the physical aspects of large nuclei to be
Vol. 91, 1971/VIII)
177
carried out. It also enabled to differentiate between solid nucleating substances and
their solutions. Much progress was also done in the application of various methods of
analytic chemistry to the investigation of large aerosols [98] and, aside of conventional
wet and chromatographic methods [46] the use of modern standardized instrumental
techniques enables the once tedious microanalyses to be performed promptly and
efficiently. Selective electrodes, neutron activation, absorption spectroscopy, flame
and emission spectroscopy and fluorescence methods are now routinely used by qualified chemists and may shortly supplant some other laborious semi-qualitative ways of
small-particle detection and evaluation such as, for example, the use of gelatins and
Liesegang ring formation thereon. Although this latter method is still applied [99] and
useful for adaptation in rocket-borne sensors [100], it is subject to systematic errors
due to both, traces of 'impurities' invariably coexistent with the aerosol component
for which the gelatin has been designed and to temperature variations [101-102]. This
method is, therefore, to be used with utmost caution in cases where chemical compositions of particles to be detected or analyzed are not exactly known and, hence, the
gelatins not suitably calibrated for the particular purpose.
Because of difficulties encountered in the past, in evaluating the chemical nature of
large nuclei, not much fundamental work seems to have been done on the chemical
reactions of the inorganic particles in the atmosphere. A large exception consists of
the work of several investigators whose interest in air pollution has recently contributed to the large part of the present knowledge on the reactions in which those nuclei
participate. Much of this work has already been quoted in this paper. More fundamental research includes the effect of moist atmospheres on sodium chloride particulates
[103] whereby OH- impurities appear to replace CI-, and the photochemistry of
halide ion solutions with the release of halide atoms and solvated electrons whose
capture (and subsequent reactions) depends on scavenger impurities [104]. On the
other hand, following a paper by ROBBINSet al. [105], work from this laboratory has
indicated that natural oxidative photolysis may be expected to induce alterations in
nitrate-bearing aerosol and may lead to the destruction of its NH4NO 3 component
[32] and also to the release of hygroscopic oxides of nitrogen from nitrate-bearing
particulates. There is little doubt that photolysis of the NO; anion in solution also
contributes to the release of halides from sea aerosol. This type of chemical reaction
does not require extreme conditions which were proposed by some earlier workers
and were recently discussed by DtJc~ [106]. As previously mentioned, nitrate is
plentiful in the atmosphere and large natural deposits thereof (whose origin is still
under discussion) are known to exist in several parts of the world [107]. More work
on processes which involve sodium chloride particulates will be discussed in the next
section.
Particles of diameters corresponding to the size of large nuclei were first detected
in the stratosphere by JUNGE [7] and the present knowledge about their chemical
composition stems from the work of FRIEND et al. [108], MossoP [109-110] and
FRIEND [111] who found, at altitudes between 12-18 km, concentrations of about
12 PAGEOPI-I 9l (t971]vnI)
178
A. C, Montefinale,T. Montefinaleand H. M. Papee
(Pageoph,
3 x 104 particles x m- 3. This material largely consists of ammonium sulfate and persulfate, and is of terrestrial origin. Since ammonium nitrate readily decomposes
under ultraviolet radiation and since co-dissolved sulfate is partly oxidized to persulfate under those conditions [32] this part of the aerosol may primarily originate
from the inter-reaction and oxidative photolysis of NH~ and SOz - bearing solution
droplets of the Aitken type size [112] and from their subsequent coagulation into
larger particulates. It has previously been mentioned that a large part of the Aitken
nuclei consists of hygroscopic and deliquescent (NH4)2SO 4 which obviously initially
carried NH 3 and NOx contamination. It would, therefore, appear difficult to view an
'in situ' formation of those stratospheric compounds from anhydrous SO2 and NH a
[l 13] and the photolytic mechanism, previously mentioned, offhand appears more
plausible. More discussion on those stratospheric particulates is given by CADLE [61.
A feature of interest in the behavior of both, soluble and insoluble solid aerosol
substance, is their property of electrification during humidification and desiccation
cycles. This obviously influences the activity of those nuclei, since it enhances their
power of coalescence with cloud droplets [114]; it also contributes to the balance of
atmospheric electricity and ion formation, because of the electric charge ejection by
those nuclei. A large amount of pioneering work on this subject is due to MOHLEISEN
[115-1171; the effect was independently confirmed by other workers who used pure
chemicals [118]. It is possible that this effect partly determines the charge-separation
phenomena which accompany the contact of volcanic lava with the sea [119], with
subsequent condensation of electrically-charged droplets and their disruptive evaporation [120]. Charging effects of a qualitatively similar nature, but occurring on insoluble, porous particulates during the release of gases therein adsorbed were, also,
more recently observed [121-124]. It was possible to establish, in this latter case, a
relationship between the rates of desorption and rates of electrical charging of those
particulates. It appears to be of added interest that the sign depended in this case on
the chemical nature and acidity of the adsorbing substance investigated, with most
interesting implications towards the generation of atmospheric electricity.
The above summary deals with some aspects of the present knowledge on the
nature, distribution and chemistry of large condensation nuclei. It also shows that
many problems thereon yet remain to be solved and that the information on their
nature, distribution, origin and chemistry needs much supplementing. The role of
those particulates in everydays occurrences is, however, better assessed, because of
their importance in cloud-formation processes. Growing clouds absorb (and probably
generate) large amounts of those nuclei; they release them upon their dissipation or
they reduce their concentration during precipitation [125]. Changes of cloud-nucleus
content of the air primarily determine the cloud-droplet concentrations and stability
[1261. Also, the number of cloud droplets is now known to agree with the number of
large, airborne cloud nuclei [127]. Those observations certainty warrant a further
extensive experimental effort aimed at investigating and understanding the chemistry
of this aerosol.
Vol. 91, 1971/VIII)
179
c. The giant condensation nuclei (radius > 1 micron).

Owing to their large size and fast sedimentation rates, concentrations of those
nuclei, in the atmosphere, are much smaller than those of the 'large' particulates. The
usual ranges are from 1-100 particles per liter over the oceans (depending on size,
altitude and wind force), to 102-104 over the continents [8]. Their concentrations in
the air and their chemical compositions also depend, primarily, on the geographic
position and on the meteorological conditions; concentrations are known to change
according to those parameters and from day to day, by up to 2-3 orders of magnitude.
As far as the nature of those nuclei is concerned chances are, for example, that a giant
particle may consist of spores or pollen at a suitable time of the year and over areas
of extensive vegetation. It may just as well be silica or clay advected from a desert, or
a particle of sea-salt over the ocean. It may also be a piece of soil or rock either dry or
coated with a hygroscopic substance (NaC1, NH4C1, H2SO 4 etc.). The transition
from one chemical type of nuclei to another may, in a sense, be continuous, the relative compositions being dependent on the intermixing of the original components and
hence on the environment which generates them [128]. Thus MESZAROS [129] gives
spans of pH ranges between 3.5 and 9 units for precipitation in Budapest, depending
on concentrations of calcium therein. Those pH limits may, of course, also be expected to vary with the geographic position and time, according to the source of
acidity and changes of human and biological activities [130]. Since such large changes
of pH do occur in precipitation it is obvious that individual nuclei, which often consist
of concentrated solutions, will be subject to much wider fluctuations of their hydrogen
ion concentration [63]. Also, since atmospheric nuclei are made of mixtures of various
chemical substances, the use of instrumental analyses (glass microelectrodes) is here
preferable to titration methods for purposes of acidity determinations~ because of
possible buffering influences of various aerosol constituents [63].
A recent paper by NELSON and GOKHALE [131] describes a series of samplings
taken in flight over the New York State. The Authors obtained counts which averaged,
below one km of flight altitude, in clear air and without turbulence, about one nucleus
of 20-50 micron diameter size, per liter. No nuclei of diameters above 50 micron
were detected. Average corresponding concentrations on a moderately disturbed day,
were 1.5 nuclei per liter of air, and there were also about 80 nuclei per cubic meter, of
diameters above 50 micron. Those particles consisted, apparently, of soil or rock
fragments whose surface was possibly coated and/or reacted with man-made materials.
No sodium chloride was detected in this case. The nuclei were of a mixed type, as
substantiated by hygroscopic patches thereon; water films hence formed on those
particles at relative humidities of 100 K. Two recent papers by RAMANA MURTY et al.
[132-133] are illustrative of proportions: (non hygroscopic)/(hygroscopic) particulates in this type of nuclei and in the area of Delhi. Reference [133] gives, in particular,
details on nuclei collected in flights at elevations between 300 and 3000 meters. The
Authors generally found averages of about 500 hygroscopic particles per cubic meter,
180
A.C. Montefinale, T. Montefinale and H. M. Pap6e
(Pageoph,
with the exception of turbulent monsoon periods when this number was thrice as
much. At the same time, non hygroscopic particles were about 5 104 m -3 in summer and 2 x 104 x m -3 both during winter and the monsoon. Chloride averages were
of the order of 70-250 per cubic meter, with maximum values during the monsoon
and at 1500 meters of elevation; other soluble particles prevalently consisted of nitrates and sulfates. Mixed particles of non marine and possibly partly stratospheric
origin, whose soluble part contained sulfates, persulfates, ammonium and H +
components, were also recently found in the air of Antarctica [62]. Further information on the geographic distribution of those giant aerosols of land origin may be
inferred from some of the references previously quoted in this paper, especially from
the work of JtllqGE [7] and his maps of distribution of atmospheric chemicals in precipitation. Generally speaking, it still, unfortunately, appears to be fashionable to
measure concentrations of those nuclei and to speak about their 'activity' without
paying much attention to their' chemical nature and, hence, to their potential action
and reactions aloft. It is, indeed, also surprising to see how little fundamental work
on compositions and reactions of compounded chemical systems, such as may be
expected to occur in those nuclei, was done in the past and is being done at present,
under controlled laboratory conditions.
Inasmuch the chloride component of the large nuclei may partly originate overland, the giant aerosols which were collected over the oceans, or in their vicinity, largely
consist of sea-salt. Although they also contain some material which offhand might not
be thought to be associated with this salt [134-135], their composition appears to be
less complex and variable than that of the giant nuclei of land origin. The giant marine
nuclei are produced, according to WOODCOCK and Associates [7, 8], over the oceans
by the action of air bubbles entrained by whitecaps; those bubbles, upon bursting,
produce Rayleigh jets of sea water and hence project tiny droplets into the air [65,
136, 137]. A similar process occurs, on a very large scale, when molten lava encounters
sea-water [138]. As shown by WOODCOCK,the concentration of those particles in the
air is thus also dependent on the altitude and the force of the wind which carries the
ejected droplets aloft [7, 8].
A large amount of our knowledge about the geographic distribution of marine
aerosols over the area of the United States, derives from the work of JUNGE [7].
European distributions are based on data gathered by the Scandinavian network and
the stations of North-Western Europe [78]. Distributions on a global scale and production rates of those particles over the oceans were recently evaluated by TOBA
[139-140]. Those rates are found to change with the seasons of the years since they
depend primarily on the distributions of surface winds and are also influenced by
humidities over the surface of the sea. Estimates thus depend on local conditions, the
usual orders of magnitude being between 10 -2 and 10~ particles cm -2 sec -1.
Much of the work done on this subject was summarized by JtlNGE [7] and further
developed by TOBA [141-142]. It is, of course, also to be expected that vertical distributions will depend on surface winds and humidities. Pioneering contributions on
Vol. 91, 1971/VIII)
181
this subject are due to WOODCOCK, LODGE and others, and are summarized in References [7, 8]. The general lines of those logarithmic distributions were also recently
discussed by TOBA [141]; the particle numbers are found to decrease with altitude, the
population of smaller particles being probably reduced by coagulation and washout,
and that of the larger ones by rainout, washout and sedimentation. Although seasonal
effects and local meteorological and circulation conditions are determining factors in
this case, decreases of about an order of magnitude may generally be expected to
occur between those concentrations within the first ten meters from the surface of the
sea and the elevation of about 3 kilometers. In terms of magnitude orders the same
approximate difference passes, up to 3 km of elevation, between categories of particles
of diameters >__10 tl, 6-10 g, 3-6 Ix, and below 3 g where average concentrations, at
sea level, are roughly of about 5 x 10z, 104, 105 and 106 per cubic meter, respectively.
Current techniques applied to the detection and capture of giant nuclei were also
extensively reviewed by MASON; they range from a straightforward use of suitablycoated glass slides [8, 96], to konimeters, cascade impactors and automatic flame
counters. More elaborate instruments [54, 97] are also available. A recent paper by
LEE and PATTERSON[60] shows that the use of appropriate impactors [143] now permits
both size distributions and chemical analyses of giant aerosols to be carried out with
precision, on a routine basis. The techniques quoted above are generally adapted, by
workers involved, to the particular pre-requisites of their projects and to their experimental conditions [144]. Chemical analysis is subsequently performed by adapting a
suitable technique according to circumstances; those methods were already previously
mentioned under 'large nuclei'.
The abundance of marine salt aerosols, the apparent simplicity of their chemical
nature at the point of origin, and the vast amount of work carried out on alkaline
halides, by workers in several disciplines of science, enables to make a number of
considerations on the behaviour of those substances and on related mechanisms of
water nucleation thereby. It offhand appears to be obvious that marine aerosol,
which essentially consists of very impure sodium chloride, will act here differently
than chemically pure NaC1. This has recently also been commented on by PUESCHEL
et al. [145] whose research emphasizes differences in rates of droplet growth on nuclei
of pure NaC1 and marine salt, at various values of relative humidity. This research is
indicative of conditions which involve relatively 'fresh' sea-spray nuclei where the role
of organic films adsorbed may be substantial since organic impurities are known to
affect both, growth and evaporation of droplets [146-148]. The situation becomes,
however, much more complex and interesting when possible environmental effects on
marine particles, which find themselves at higher altitudes and for prolonged periods
of time, are considered. The surface of those solid particles may in fact be expected to
assume, under these circumstances, completely different properties from those of the
original product, be it reagent-purity NaC1 [103] or sea-salt. Some work on such
changes related to pure sodium chloride, dates back to several years ago [149-151];
NaC1 particulates which were treated with plasma or in electrical discharges, are known
182
(Pageoph,
to eject photoelectrons upon illumination with visible light [152] and since they thus
acquire, during their fall in the air, a conspicuous electric charge which favors coalescence, they were used in tests on warm-cloud dissipation [153-154]. The emission of
exo or photo-electrons from solid surfaces which were suitably suitably pre-stressed,
is today widely known to occur on a number of materials (cf. [153] for further references and reviews on the subject). Those include appropriately pre-irradiated
sodium chloride [155-156] and they may also include cases of pre-stressing [157] as
may occur in desiccation processes. More of the earlier References on this subject were
pooled by one of us in 1962 [158]. Even the chemically pure chloride of sodium is now
known to be affected by ultraviolet light [159] and also to be tribochemically affected
by mechanical friction in air, with generation of nitrates [160]. Aside, therefore, of the
'impurities' which a sodium chloride particle of marine origin initially contains when
it is ejected from the sea, and besides the contamination which it may subsequently
acquire in the air, it can hardly be expected that a solid nucleus of marine salt will
remain aloft unaltered for long periods of time. Considerations of this nature are also
thought to be of help in understanding the M~HLEISENeffect [115-119]; the cycles of
hydration and dehydration mentioned, if accompanied by electric effects, are of
added interest in that they could lead to a multiplication of nuclei by the evaporative
ejection of small droplets from an electrically-charged, deliquescent particulate [120],
with the consequent formation of smaller nuclei.
A liquid particle of marine aerosol may also be expected to undergo chemical
change during its residence time in the air [104]. Some of those changes may lead to
the separation of chlorine from the drops. The more concentrated the solutions in
those drops, the more this separation would offhand appear to be favored. Various
hypotheses on the possible chemical aspects of this change were recently summarized
by DUCE [106]. It is known, however [7], that giant marine nuclei contain substantial
amounts of nitrate. This is found to decompose under ultraviolet radiation through a
process which involves the formation of highly-oxidizing transients [161-163] capable
at suitable conditions, of liberating halogens from their solutions. Rates of liberation
will here obviously be I>Br>C1; the process of nitrate-photolysis has also been
found to proceed under natural sunlight illumination [164-165] and its kinetics to
depend on co-dissolved inorganic substance [166, 29]. Ammonium nitrate is also
affected, with the consequent defixation of biologically assimilable nitrogen [32]; since
the process is enhanced by chlorides this may explain the absence of ammonium from
JUN6E'S giant marine aerosol at Round Hill and in Florida [7]. Being this photolytic
reaction of a highly oxidizing nature, processes of consequent nitration and chlorination of organic matter contained in those systems are also to be expected to occur and
it is hoped that this discussion will stimulate more work along the line.
The few giant nuclei that normally [167-168] compare in the stratosphere are,
probably, of extraterrestrial origin, as substantiated by their high velocities of sedimentation. Most available information about their chemical nature is, again, given
by JUN6E [7] and Associates. Elaborate methods of X-ray spectroscopy and fluore-
Vol. 91, 1971/VIII)
183
scence were used for the analysis of those particulates which were found to contain,
primarily, Si, Ca, Fe, A1 and K, with minor quantities of other elements. As previously
mentioned in this paper, most of the stratospheric aerosol consists, however, of 'large'
hygroscopic ammonium sulfate and persulfate nuclei, hence the existence of mixed
particulates is also possible in this case.
d. The role of condensation nuclei in nature

Although the numerous Aitken nuclei provide excellent centers of water vapor
condensation in instruments designed for their study, it is now believed that the large
nuclei, which require lesser saturations of water vapor for their 'activation', are largely
responsible for the formation of cloud droplets [9, 10]. A close agreement between
numbers of cloud droplets in a cloud, and of those nuclei outside the cloud and per
unit volume was, in fact, recently observed by TWOMEY and WARNER [127]. Those
large, mostly hygroscopic, particles are thus thought to be of primary importance in
processes of natural cloud formation while the giant particles appear to play a large
role in the precipitation of warm (above 0~ clouds, at otherwise suitable circumstances. It is generally agreed that the warm-cloud type of precipitation occurs through
coalescence processes which normally require droplets of diameters larger than about
20 micron for an efficient capture of smaller droplets [1, 10]. Hence the practical
importance, in the atmosphere, of the giant nuclei on which those droplets grow. In
this area of research classic work includes, therefore, computations by B~ST [169] and
KEITH and ARONS [170] which deal with the growth of drops of salt solutions, and the
pioneering work of WOODCOCKand Associates [171-173] and of TURNER [174] on the
role of sea salt in precipitation. The importance of giant nuclei and, consequently, of
the large drops in precipitation mechanisms from warm clouds, has been demonstrated
in a series of contributions by BOWENand by LUDLAM[1, 8] which thus integrated the
well known 'chain reaction' mechanism of warm rain formation, proposed by LANGMUm [175], whereby an individual large drop which falls through a cloud, upon
reaching a radius of a few mm by coagulation and coalescence, disintegrates into
smaller drops which, in turn, behave likewise and so on. It is evident that in the case
of electrically-charged drops (or nuclei), the coalescence mechanism will be greatly
enhanced, as briefly reviewed by PRUVVACHER [176] and experimentally confirmed,
during the last decade, by a number of other workers [177-184]. Collision efficiencies
between those droplets are found to increase by a few thousand percent, according to
diameters, electric fields and charges involved. It would thus appear that the use of
giant, electrically charged, nuclei, could lead to successful experiments on the modification of 'warm' clouds, and it could also be expected to yield encouraging results in
projects on hail suppression, since quantities relatively small (about one particle per
liter of air), in comparison to the possibilities of modern technology, here appear to
be needed [185] for a partial suppression of damage on the soil.
There is yet another effect to consider. A number of recent contributions is in-
184
A.C. Montefinale, T. Montefinale and H. M. Pap6e
(Pageoph,
dicative of lowerings of water supercooling by small amounts of some dissolved

electrolytes [186-t87]. Although some previous work (see Ref. [186]) indicates that
concentrated solutions behave differently, this effect, if real, could have influence on
overall glaciation processes in supercooled clouds which contain large amounts of
inorganic salts, and be expected to apply in areas of high inorganic aerosol concentration. Also, since small amounts of some dissolved salts provoke increases of the
rates of dendritic ice-growth [188], formation of spongy [189] - and hence less damaging hail - could here also possibly be favored.
2. The nuclei of ice formation

Since pure liquid water may undercool up to about - 40~ (sometimes referred to
as SClJAEFER'Spoint [9]), and since water contained in a cloud often reaches temperatures of - 10~ and sometimes of - 35~ [8], large amounts of energy may be expected
to be released from those supercooled clouds during their incipient return to equilibrium and according to their size. The heat of fusion which is released upon glaciation,
from those hydrometeors, increases the buoyancy of the glaciating cloud mass and it
hence increases its vertical development; glaciation, once initiated, is favored by the
temperature dependent differences between water vapor pressures on ice and on
supercooled water, and the transfer of water onto the ice phase sets practically in as
soon as glaciation begins within the cloud. This is followed by a fast growth of the ice
embryos into snow crystals, by the size increase of the latter and, consequently, by
the increase of their velocities of sedimentation, their accretion with water droplets
and their ultimate melting and fallout as liquid, at suitable temperatures. The process,
which is widely known as the BZRGZRONmechanism of precipitation [190, 8] obviously
therefore requires the presence of ice particulates within the cloud and, as the homogeneous transition of phase necessitates considerable undercoolings [8, 10] a large
effort was understandably directed, since 1946, towards the finding of suitable
artificial inductors of this phase transition, and towards the individuation of the
natural ones.
The best ice nucleants available in nature are the ice crystals themselves (of which,
for example, cirrus clouds are made). They obviously do not require lag times for
their 'activation' [191-192] since the initial ice-embryo is already formed. A method
of producing large amounts of these nuclei in a supercooled cloud, by still larger,
local, undercoolings, was first developed and tested by SCHAZFZR [193] and is still
widely used today for cloud-seeding purposes. The method consists in dropping solid
CO 2 into those clouds, whereby enormous amounts of ice crystals are formed in the
wake of the falling dry-ice pellets. Qualitatively similar results were also, more recently, achieved by means of spraying of some highly-volatile liquids [194] and the subsequent production of very low temperatures, upon their evaporation.
Earlier ideas which first led VONNEGUTto the discovery of silver-iodide as a practical, ice-forming compound [195], were based on the principle ofepitaxy (lattice para-
Vol. 91, 1971/VIII)
185
meter similarity) between ice and the nucleator. Thus arose the concept of 'sublimation'
(here to be regarded as the opposite of what this term usually means) which implied a
direct transfer of water vapor onto the solid, epitaxially favored, nucleator substance.
This attractive criterion now appears to be but one of the many mechanisms by which
nucleation may take place and the earlier widespread acceptance of its exclusivity
seems to have delayed the progress of this branch of science for some years. On the
other hand, the concept of 'freezing' (an earlier-postulated mechanism involving the
spontaneous freezing of minute drops) was subsequently also found to be incomplete.
More recent research [196-198] emphasizes the predominance of the 'contact nucleation' mechanism (mechanical contact between a supercooled drop and ice, or a suitable catalyzing substance) and nucleating materials are hence now more broadly
termed 'ice-forming nuclei'.
The mechanisms at which a substance may nucleate ice at a given temperature
depend on a variety of physical factors and they also depend on the structure and
shape of the nucleator. A brief review by S~NGER [199] provides an early discussion
and it also raises the point that the surface of an efficient, pure, solid nucleator should
primarily be insoluble. This surface (and also the water to be nucleated) should,
moreover, be uncontaminated by specific poisons [200-201], both of the above
prerequisites befitting any catalyzing solid surface which is used in chemical
processes.
Ice-nucleating properties of a solid hence also depend on its surface area [202-203]
and shape [204], since the amount of active sites on a nucleus may be expected to be a
function of those parameters [205]. On the other hand, recent investigations on the
freezing of supercooled water in clean and relatively large glass capillaries appears to
show the absence of capillary effects alone on the temperature of phase transition [206].
This notwithstanding, capillary effects seem to determine the so-called 'pre-activation'
towards ice-nucleation, which some particulates possess and which, essentially, consists of increasing temperature thresholds of ice-formation after a particle has already
acted as an ice-nucleus and, normally, in the absence of intermediate thawing [207208]. There is also evidence, however, that in some cases 'memory' effects may be
expected to persist even after the nuclei were heated up to as much as 6.5~ [209].
More recent work points, at the same time, to the importance of crystalline monolayer forms of water adsorbed on suitable substrates [210-211] as an explanation of
those memory effects.
Necessary prerequisites for the initiation of the phase transition of water, on a
suitable solid, were also found to include the molecular structure of the nucleator
material [212] and the surface dislocations contained on its surface ([213] and B. J.
MAsoN, as described in Ref. [214]). Those are well known to promote chemical reactivity [215-217]. Added to this are the effects of hydrophilic impurity sites on essentially hydrophobic substances [214, 218-219] with consequent formation of large
water clusters and their subsequent freezing at suitable conditions [220-221]. Another
factor is electrofreezing [222-223] which may be expected to be favored by photo-
186
A.C. Montefinale,T. Montefinaleand H. M. Papde
(Pageoph,
sensitive, heterogeneous and largely hydrophobic surfaces, such as those of impure

silver iodide. Lastly, but not to the least extent, nucleability depends on ambiental
conditions such as vapor supersaturations and rates of cooling [224].
a. Natural ice-forming nuclei
It is to be expected that natural ice-forming nuclei of mineral origin will not be
made of chemically-pure particulates but that they will often carry soluble, hygroscopic contaminations, thus also entering the bracket of condensation nuclei. Correlations between concentrations of large condensation nuclei, and ice-forming particulates in the air are, in fact, well known [225]. It is also known that the presence oficenucleants at ground level is often associated with precipitation [225-227], that they
frequently show well-defined geographic bands of concentration [226] and that the
so-called 'ice-nucleus storms' tend to occur during unstable meteorological situations
[227-230]. Investigations of the nature of inorganic, ice-forming substances in the
atmosphere have, understandably, been the object of extensive work. Earlier studies
by SCHAEFER [see Ref. (8)] who established that some clay, soil and sand particles
were active at temperatures above -20~
were followed by more detailed work of
several investigators [8] including MASON and MAYBANK [231] and MASON [232].
Ice-forming properties of clays and stony meteorites were thus investigated in detail
and more recently, FUKUTA [233] and SANO, FUJITANI and MAENA [203] also tested
various inorganic chemicals for their ice-nucleating properties. Field work by KUMAI
[234] and KUMAIand FRANCIS[235] has later shown that clay mineral particles account
for a large percentage of natural nucleators in the atmosphere, in some areas of the
world. The search for natural ice-nucleants still appears to continue and was also
recently extended to organic substances, following the discovery of those activities in
some of these materials [236-237].
Inasmuch KUMAIwent to great pains to evaluate the chemical nature of his nuclei,
much of the individuation of those particles, in nature, is still carried out by searching
for the effect and disregarding the composition of those substances. Thus there seems
here to be some analogy with the approach which leads to the evaluation of condensation nuclei concentrations in the air. Briefly, the particulates are detected by their ability
to form ice, at suitable saturations, and the ice-particles grown are then counted.
Various methods to achieve this were recently reviewed by BOUCHER [10] and, according to the principle of operation involved, use is made of cloud chambers of the
mixing, diffusion or expansion types. Briefly, a suitable volume of adequately moist
air which contains nuclei, is introduced into the chamber where temperature and
humidity are preadjusted according to requirements. The number of nuclei is then
evaluated either by direct observation of ice crystals thereon formed and easily
detectable visually by their characteristic glitter, or by the counting of centers of
crystal growth induced by those falling ice crystals in a saturated sucrose solution
situated at the bottom of the chamber. Parameters measured by those methods
Vol. 91, 1971/VIII)
187
usually include the nucleations threshold (the maximum temperature at which a substance induces the change of phase of supercooled water drops) and the activity (the
fraction of nuclei active) at a specific temperature. Other methods which are essentially based on visual or optical examination, at constant temperatures, of phase
transition in water droplets [192, 224, 238] or supercooled films [191] condensed on
hydrophobic surfaces, were also extensively used by a number of Authors. Handy,
standardized methods of ice-forming-nuclei-capture by millipore filters, followed by
their development and counting using sucrose or sodium silicate solutions [239-242],
were also more recently brought forth and efficient, modern, automated system [243]
now offer several advantages over the older methods.
Despite observations which corroborate the existence of a close relationship, in
some types of clouds, between fall-out rates of snow or graupel, and the concentrations of those atmospheric ice-nuclei [244] which are active at cloud top temperatures,
it would appear that the number of those particles is not a simple function of the total
number of ice crystals contained in some other types of clouds. The reason for this
apparent discrepancy seems to be due to naturalprocesses of ice-multiplication, with a
consequent increase of the number of ice particles over the nuclei. Several mechanisms
were proposed and tested in the labratory to explain this phenomenon which sometimes shows up in excesses, by several orders of magnitude, of ice-crystals over icenuclei within and around the cloud respectively, and according to its supercooling
[245-248]. Implications and possible causes were recently discussed by Mossop [249]
on the basis of past experimental evidence. Possible mechanisms include fragmentation and shattering of large freezing drops during their fall [250-251], evaporative
ice-filament formation on available ice particles and their subsequent shattering
[252-253], ice-whisker formation in electric fields [254] and their shattering [255-258],
riming and shattering and ice-crystal generation in electric fields [259]. It is, therefore,
of added interest to recall at this point some of REITER'Swork [260-261 ] on the electrical effects which accompany the freezing of NOx-contaminated water and also his
implication on the multiplication of ice crystals which could thus both partly be due
to, and further generate, in a freezing hydrometeor, oxides of nitrogen which are well
known for their electricity,carrying properties. While there seems to be little doubt
that processes such as those described may occur in nature, there is also evidence to
the effect that those phenomena require the presence of primacy nuclei for their initiation. Their presence seems also to be necessary for the production of ice particulates
by mechanical shock [262-264] such as, for example, thunderclaps in a thundercloud
[265], though the elucidation of this mechanism offhand appears to be still the object
of some controversy [266].
Despite a number of reviews on the subject [8-10, 267] there still is a variety of
opinion on the source of natural, atmospheric ice-forming nuclei. It is unfortunate
th at, because of the continuing increase of air pollution all over the world and because
of its effect on the concentration of those nuclei in the air [268-269], this situation
may hardly be expected to improve. The counts often increase during rain showers
188
(Pageoph,
and during fog dissipation indicating, as they do, their well known dependence on the
vertical exchange of air masses as well as the preactivation memory effects which
depend on the state of the surface of those particles and on their contamination. The
scientific literature is indicative of a predominantly land-origin [270-271] of those
particulates, although there are also some hints to the contrary [272]. Despite the
presence of clay in a large percentage of snow crystals collected in unpolluted atmospheres [234-235] there would appear to be no offhand association of ice-forming
nuclei with terrestrial or volcanic dust over Australia (226, 273]. Some papers appear,
in fact, to be indicative [228, 274] of a requirement by a nucleator particle, of a
residence time in the cleaner, upper strata of the atmosphere, possibly since this may
cause its surface to decontaminate sufficiently by radiolysis, photolysis and outgassing,
to re-activate it for purposes of ice-formation.
b. The extra-terrestrial nuclei of ice formation

There being an influx rate of about 104 tons [275] of interplanetary dust, per day,
on Earth, it would seem to be evident that the search for ice-forming particulates
should not be confined to earthly sources alone. Thus, on the basis of rainfall-peak
distributions over a number of years, BOWEN [276] put forward the hypothesis of icenucleating effects due to meteor showers, with a time lag of about 30 days which aie
necessary for the small particulates, thus generated in the upper atmosphere, to reach
the levels of the clouds. Earlier arguments for and against this hypothesis, as well as
BOWEN's subsequent work were extensively commented on by FLETCHER [277-278],
Mossov [267] and others, and were followed by further research which dealt with the
lunar influence on both, the ice-nucleus concentration [226, 279-280] and the widespread precipitation phenomena [281-283]. The interest which arose because of
BowEN's theory has until recently yielded interesting discussions on the subject
[284-286] although the controversy still appears to persist.
Several previously-quoted studies [7, 108-111, 144] bear evidence that the stratospheric aerosol layer contains large amounts of insoluble material which prevalently
appears to be of extraterrestrial origin. It was pointed out that the stratospheric
sulfate layer [7] may poison the ice-nucleating activity of those solid particulates of
extraterrestrial origin [226], unless the meteoritic material traversed this region very
quickly. Despite a number of recent papers which suggest but a low ice-forming
activity of the meteoritic material, and of dusts found at higher altitudes in some
places of the world [287-288], there is evidence that nucleating properties depend on
the chemical composition of those meteorites [289] and that samples collected at high
elevations at other locations may exhibit larger ice-forming activities [290-293]. Also,
particles obtained from meteorites which were boiled under partial vacuum in a solar
furnace [294] were shown to be active at -15~ the discrepancies mentioned above
evidently arising from the treatment which the surface of those particles underwent.
It is clear that a preheated, outgassed and hence uncontaminated and prequenched
Vol. 91, 1971/VIII)
189
surface of a meteoritic particle, as it appears in nature, and also of suitable chemical

composition and size, will behave differently towards the catalysis of ice-formation,
than the same material would after a prolonged contamination and/or hydration. It
is also clear that conditions towards both activation and poisoning of those surfaces
do seem to exist in the upper regions of the atmosphere and that consequently the
apparent discrepancies of the results obtained by various workers are here due to
differences in environmental influences to which those particles were subjected during
their history.
c. On some commonly-used artificial nuclei of ice-formation and on
the resulting implications
Notwithstanding the large number of 'artificial' inorganic solid substances which
have, until now, been investigated in the laboratory for their ice-forming properties,
the study of silver iodide, the first-discovered [295-296] and tested ice nucleator for
weather modification [195], continues to yield information, in this area of research,
towards the nature of processes which occur on solid surfaces, and towards their
prerequisites for ice-embryo formation. Thus, although the concept of the epitaxial
fit first stimulated VONNECUTto carry out his pioneering work, and although the importance of this fit, between the ice-lattice and that of a nucleator [297], was observed
to favor, under some circumstances [298], the transition of supercooled water to
ice, it has also been shown that pure, unheated and unquenched silver iodide substance,
which does not contain hygroscopic impurities, is a very poor ice-forming agent
[299-300]. The compound may, however, be activated by light (see observations by
MASON, Ref. [230] and [191,301]), probably following the formation of surface inhomogeneities which are known to promote the nucleability of ice on AgI [302]. Also,
and aside of surface contamination and irregularities, AgI normally used for purposes
of ice-nucleation may always be expected to be intrinsically impure, due to the presence of more than one phase, therein generated by thermal dispersion [303-307] and
the fast quenching which follows its introduction into the air. It was pointed out,
moreover, that silver iodide is essentially hydrophobic [308, 218] and that its icenucleating properties depend on the number of hydrophilic sites, due to impurities.
Those sites favor the formation of primary water clusters [204,309] which subsequently
extend into ice, at suitable conditions. Since silver iodide is photochemically sensitive
[310-311] and since it yields photogalvanic effects in the presence of soluble contaminations [312-313] it is be expected that those factors may also contribute to the formation of those separated polar sites at which water clusters will develop. Some of the
above mentioned properties also apply to the case of lead iodide [314-318] which is
known to be an excellent ice-forming substance [319, 213] and whose surface, for the
purpose of its ice-forming effects, probably consists of a mixture of mono and diiodides, and of the basic iodide.
Despite its extensive use in cloud physics and weather-control research, silver
190
(Pageoph,
iodide is expensive and its use is therefore limited to very small (submicron) particles.
Although this yields large surface areas per unit weight, it also exposes the material
to faster photodeterioration [320-322] and hydrodecay [323-325]. The first factor induces a collapse of the surface structure because of a primary photodissociation into
elements and their subsequent reactions, the second provokes the leaching of active
sites and a decrease of the overall surface area, especially in presence of complexing
KI or NaI [326] salts. The cumulative decay of the activity, due to both of those factors, may reach up to about three orders of magnitude per hour.
Instruments designed with the purpose of dispersion, from the ground or from
aircraft, of silver iodide aerosol, range from burners of various design - where a
suitably complexed (with NaI, amines, ammonia etc.) solution (in acetone, amines etc.)
undergoes combustion in a supporting fuel (propane etc.) [327] - to the use of AgIimpregnated charcoal or gunpowder [8] and of detonating fuses named 'Weathercord'
which incorporate this iodide [328]. 'Pyrotechnic' devices which operate on the principle of alumino or magnesiothermic reduction of silver iodate and other oxidants, or
which contain adequate self-sustaining combustible chemical mixtures and include AgI
to be dispersed, were also, more recently developed in the United States [329-332]
following similar general ideas which were elsewhere previously brought forth [333-336].
Inasmuch the use of generators, which burn complexed AgI solutions, would
readily imply that silver iodide particulates thus produced will be strongly contaminated by other hygroscopic products [337], interest in the role of those contaminations seems to have arisen only very recently [338-341]. The reason for this is that the
aerosol thus prepared 'worked' in most of the cases anyway, although with different
yields and according to the method used. Also, concern about the chemistry of AgI
surface action took several years to materialize mainly because of the happy coincidence that, as previously mentioned, AgI should indeed be contaminated in order to
be active as an ice nucleator.
As a result of an increasing interest in the surface properties of inorganic icenucleator materials, and following the elaboration of more precise techniques for
their investigation [342-343], the field of study of those substances understandably
extended, during the last decade, to an impressive array of organic compounds. This
trend was started in 1957 by BASHKIROVAand KRASIKOV[344] with their report on
phloroglucinol's ice-forming activity at about - 6 ~ and with its subsequent testing
in the field [345]. Added impulse was provided by the work of HEAD [346-348] who
investigated a variety of steroids and other polycyclic compounds and found that the
ice-forming activity of some of them depended both on the freshness of the surface
exposed by grinding and on its hydrogen-bonding properties [349]. Parallel investigations which pointed to similar conclusions are due to KOMABAYASIand IKEBE [350];
other work on arninoacids, some of which were found to be active at about - 4 ~ is
due to POWERand POWER [351]. Several of the most important points raised by those
investigations were subsequently confirmed by FUKUTAand MASON[236]. The finding
that aminoacids nucleate ice assumes importance because of more recent work by
Vol. 91, 1971/VIII)
191
SIDLE who confirmed, experimentally, the presence of some of those compounds in

the atmosphere [352]. More investigation and discussion along this line is due to
others [353]; indication was thus obtained of a correlation between the chemical
properties of a substance and this type of surface action [354-355], and the influence
of both, the age of a sample [356] and of the experimental or environmental conditions
involved [357], on its ice-forming nucleability. As things are today it would also
appear to be of interest to investigate some of those organic materials for their susceptibility to activation [358] or inactivation by chemical reaction or surface poisoning
due to products of atmospheric natural and artificial air pollution. It would also be of
interest to test their activities after having them adsorbed on suitable mineral substrates, such as occur in natural aerosols. Work of this kind would add to the knowledge about the role of these nucleators in nature, as the activity of many of them is
known to be strongly dependent on the mode of their preparation [359-360].
Despite a widespread use of silver iodide in weather modification experiments,
some other recently-found 'artificial' nucleators (and the methods of their dispersion)
merit attention because of their simplicity, versatility and low cost. One of them is
solid metaldehyde [361] which, when freshly ground, was found to nucleate ice at
about -0.4~ Suitable generators of metaldehyde smokes were therefore developed
[362] and tested in the field for its action on supercooled clouds [363]. The substance
probably acts on the basis of the principle of epitaxy; its drawback consists of the
high rates of evaporation of the microcrystals dispersed and of their possible deterioration by exposure to humidity and light. Like silver iodide, it should therefore be
directly introduced into seedable clouds. The other substance is dry urea [364] which,
though very hygroscopic and readily soluble, acts on a supercooled cloud by local
undercooling due to its enormously endothermic heat of solution. This provokes a
rapid freezing of a water film formed on a particle of this material. Suitable dispersing
units of this compound were hence also developed [365] and the substance tested in
the atmosphere [364, 366]. Because of its hygroscopicity urea also offers, when
dispersed as a powder of adequate size, the advantage of acting as condensation nuclei.
Paradoxially, its drawback lies in its high solubility and hygroscopicity, both preventing
its regenerability in the atmosphere, for ice-forming purposes, by desiccation. It is also
known to be affected by NOx and its properties of acting as a condensation nucleus
could therefore be affected by air pollution. In order to explete its ice-forming properties
it should hence also be introduced directly into a supercooled cloud to be seeded.
The third versatile product is the sulfide of aluminum. The ice-forming activity of
this substance, when freshly prepared from the elements, starts at about -3.5~ This
property ofA12S a was discovered in 1962 and patents covering its use first appeared in
1965. Giant nuclei of aluminum sulfide are used, as recently described [367], in a form
encapsulated in spherules of alumina and sodium aluminate. They have also been
tested, as of late, for purposes of weather modification [368-369] and although
alumininum sulfide, alike AgI, has also a hexagonal crystalline form, its action is
primarily thought to be due to the creation, during its slow reaction with water, of
192
(Pageoph,
a mosaic structure which involves polar sulfidic forms intermixed with sparsely
soluble and insoluble material. The use of bulky apparatuses is unnecessary for the
dispersion of AlzS3-containing smoke, since monodisperse particulates (about 1.5
micron of diameter) are generated by the combustion of suitable self-sustaining solid
chemical mixtures. Those mixtures covert themselves almost quantitatively into the
aerosol which is driven out of the flame by a current of simultaneously-generated
nitrogen gas. Since those nuclei also possess some hygroscopicity due to the presence
of both, sodium aluminate and A12S3 which is known to react slowly with water yielding hydrogen sulfide and the hydroxide of aluminum, this type of aerosol also
belongs to the class of condensation nuclei. It hence is also an example of what is
commonly termed 'mixed nucleator'.
Some of the analytical chemistry methods which were previously mentioned in
connection with the analyses of condensation nuclei, may also be used to analyze the
ice-forming particulates. The obvious difficulty consists however here both, in the individuation of the ice-forming particle at the center of the snow crystal, and in the
subsequent evaluation of its chemical nature. This task calls for high-precision,
tedious and time-consuming work, and for the use of expensive and complicated instrumentation; it is thus not surprising that not many contributions are available
along this line. Outstanding research includes the use of electron-microscopic techniques and electron-diffraction patterns [234, 235, 370]; those enabled the identification
of natural clay minerals in crystals of snow.
Since silver iodide continues to be regarded by many workers as a very fashionable
ice-forming agent, much effort was, understandably, devoted to the search for traces
of this material both in ice-crystals and in the precipitation collected on the ground,
following cloud-seeding experiments. Techniques based on the use of electron microscopy on suitably pre-treated samples [371-372] were hence also applied to this case.
Methods based essentially on the extraction of silver iodide from water samples, and
on its subsequent re-use as ice-forming substance, in adequately calibrated cloud
chambers, are also available [373-376]. Those advances were later followed by the
development of techniques which involve neutron activation procedures [377-378]
thus leading to the increase of both, precision and consistence of the results. Finally,
atomic absorption spectroscopy [379] and techniques of inducing crystal growth in KI
solutions supersaturated with respect to AgI [380] have very recently also been used
as a tool for the quantitative analysis of silver in seeded snow.
It would appear to be somewhat unfortunate that a much larger effort was thus
devoted, in the past, to the development of methods applied to the monitoring of silver
iodide submicron particles in precipitation, than to the search for the nature and
modes of action of natural, ice-forming, nucleators.
3. The induction, inhibition and alteration of natural hydrometeor processes

Natural, weather-active, condensation and ice-forming nuclei in the air are thought
Vol. 91, 1971/VIII)
193
to exert a large influence on everydays life of a large fraction of the population of the
world. The emerging art of artificial cloud-modification hence stimulates the hopes
of being able to increase the natural precipitation in arid areas, of relieving drought
and also of avoiding excessive and damaging downpours and consequent floods. Airline authorities and inhabitants of chronically fog-bound territories await the day
when efficient fog-dispersal procedures will become operational, and modern progresses in hail-suppression warrant optimism towards an economical application,
on a large scale, of the results of a number of field tests, now under experimental study
in several parts of the world. Most experimentation carried out in these three branches
of weather control involves the use of suitable nucleator particulates, and of devices
designed for their economical and efficient production.
a. The action by condensation nuclei
As previously mentioned, the principle of operation consists here of dispersing

adequate hygroscopic chemicals, in conditions which favor their penetration within
or above the cloud mass or fog to be seeded. The particles should be essentially monodisperse and of a diameter which classifies them among the giant nucleators.
Their action on warm (above 0~
consists of removing the stagnant droplets
because of the hygroscopicity [381-383] of the nucleant and by subsequent coalescence.
Pioneering work on the subject dates back to 1938 [384]; concentrated solutions of
calcium chloride were then used in field-tests and in amounts of about 2.5 gins per
cubic meter of fog. A more rigorous experimentation, based on the use of monodisperse (about 1-4 micron in diameter) sodium chloride was recently performed by
JIUSTO and Associates [385] in cloud chambers where conditions were pre-set according to natural requirements. Since the object of this research was to increase visibilities, estimates were computed from the well known laws which govern this palameter
in a cloud of particulates [386-387]. Following the development of efficient generators
of monodisperse (diameter about 1.5 micron) and electroactive condensation nuclei
[335-336] experiments were also recently carried out in the Po-Valley which is known
to be chronically-infested by shallow fogs [51] during the cold season. The results
obtained yielded overall average increases of ground visibility of about 300 meters
over a vast area [368]. There seems, therefore, to be no doubt that successful operations of fog-clearing, by the use of giant nuclei, are now only a matter of proper
logistics.
As mentioned earlier in this paper, seeding of clouds with giant condensation nuclei
has, as its object, the induction of coalescence processes and the consequent increase
of precipitation on the ground at a predetermined place. Seeding may be carried out
from a plane, or from the ground, but in this latter case under conditions which favor
the formation of suitable updrafts, whereby nuclei may penetrate into the available
or prospective hydrometeors. Earlier results obtained by the use of this technique are
quoted in Reference [1]; the procedure was, more recently, used in Puerto Rico [388],
13 PAGEOPIt91 (1971]vnI)
194
A.C. Montefinale, T. Montefmale and H. M. Pap6e
(Pageoph,
India [389] and Italy [369] with consequent increases in precipitation values up to
about 50~.
Since no appreciable growth of electrically-uncharged water drops, which are
smaller than 10-20 micron in diameter, appeals to occur under natural conditions,
and since hail may be due to the freezing of a few large droplets which are available
in a congested cloud, it has been proposed in the past that the introduction of large
amounts ( > 102 x m -3) [185] of giant condensation nuclei into the base of a cloud,
could lead to the formation of sufficient excesses of those potential hail embryos, to
reduce their individual average size and thus prevent their reaching the ground in
solid form. This very important study was strenghtened by the work of APPLEMAN
[390] who pointed out to the possibility of existence of a natural hail suppression
mechanism in the coastal regions of the United States. This, obviously, is a region
where sea-salt giant condensation nuclei abound. Also, an added point of interest
consists, in the case of hail-formation, as related to nuclei, of the suggestion that since
small amounts of some dissolved salts favor dendritic growth of ice, less damaging
spongy hail [189] could fall from a cloud treated with a suitable amount of efficient
nuclei of condensation, than it would from an untreated cloud and at the same
conditions. The amount of particles required to fulfill the requirements of any of
those processes is by no means prohibitive and it would indeed appear to be of large
interest to test this double query with one field experimentation to be carried out in an
area where hailstorms regularly recur, and where the perishable produce is sufficiently
dense and important to warrant the disponibility of reliable data on past, pre-experimental losses, and also on the contemporaneous losses of some suitable adjacent control areas.
b. The action by nuclei of ice-formation

The artificial stimulation of rain from supercooled clouds is normally based on the
assumption that the number of natural ice-nuclei is insufficient, in those clouds, to
induce their precipitation at temperatures within prevailing. Organized attempts at the
induction of precipitation by seeding with adequate ice-forming nucleants, are being
therefore carried out in various places of the world, since a number of years. The
arising difficulties are mostly due to the necessity of calculating the significance of the
success achieved, if any; significant results were obtained by a number of workers in
the past despite the fact that, on the other hand, the use of very similar methods yielded
in other cases results which were either non significant or, sometimes, even negative
(significant decreases of precipitation). Nuclei used for the purpose still usually consist of silver iodide which is either dispersed, at suitable meteorological conditions,
from ground,based burners or from aircraft. Some of those techniques are known to
have produced increases of precipitation of up to 20~, especially in mountainous
areas and usually during normally rainy seasons. The results obtained are evaluated
either on the basis of a historical period, or a reference area adjacent to the target
Vol. 91, 1971/viii)
195
territory, or both. Better still, use is often made of randomly chosen no-seeding,
periods on the target area itself.
The possibility of decreasingprecipitation by overseeding has also been discussed
in the past [8]. An experimental investigation of this possibility would offhand
appear to be attractive if carried out in some maritime areas where large, seasonal
and localized precipitations are known to occur. Briefly, and for example, a transformation of a supercooled liquid cloud into an iced form, by a very large excess
of suitably-introduced nuclei may result in an absence of precipitation on the
ground and an almost quantitative transformation of that cloud mass into small
ice particles.
On the basis of principles mentioned earlier in this paper dissipation of supercooled
fogs was carried out in the past by many workers, using either solid CO2 or AgI or
volatile hydrocarbons. The aim was, as usual, to provoke a transition of phase either
by the use of nuclei or by local undercoolings, to avail oneself of their growth at the
expense of the remaining liquid, and to induce their subsequent fallout. Results obtained by the use of ice-forming nuclei (and/or supercooling) in fog-clearing and artificial stimulation of rain were, in the past, the object of a multitude of technical reports
and also of several scientific papers. A large amount of the most up-to-date reliable
work on this subject is either directly described in three recent volumes on weather
modification problems [3-4, 391] or is therein contained as references.
Principles of overseeding, using ice-forming nuclei in amounts larger than about
10-102 per cubic meter of air [392-393] were also applied to hail suppression. Clear-cut,
successful and outstanding work includes recent operations carried out in Kenya
where silver iodide was directly introduced from aircraft into developing thundercells
(T. J. HENDERSON, Ref. [4] p. 474). It also includes the use of AgI and PbI 2 which is
delivered into selected spots of a gathering hailstorm by means of properly aimed
missiles and at a suitable time of the development of the storm [394-396]. Significantly,
operations based on the use of mixed giant nuclei of quite straightforward composition, such as white clay and portland cement, are also known to have induced changes
and dissipation of thunderstorms when adequate amounts (about 40 kg) of those
powdered substances were therein dropped from aircraft [397].
4. The inadvertent modification of weather

The recent spread of automobiles, industries and urban developments has led to an
impressive increase of miscellaneous particulate matter in the air on a global scale
[398]. Inasmuch most of this material may, from the human and ecological point of
view, be merely classified as offensive and disturbing dirt, its role with regard to
weather is now known to raise concern of the meteorological profession. A classic
paper on the subject was written by SCnAEFBR in 1968 and was accompanied by a
number of parallel contributions on a scale of one full scientific session [4]. Briefly,
the pollution of air introduces enormous amounts of both, ice forming and condensa-
196
A.C. Montefinale, T. Montefinale and H. M. PapOe
(Pageoph,
tion nuclei, into the atmosphere, and the consequences of this, though offhand alarming, are now still difficult to foretell.
Aside of some offenders well-known since many years, such as the smoke from
extensive natural fires and industrial activities, which may be expected to change clouddroplet populations [399-400], distributions, ice-nuclei contents in the air [401] and
precipitation patterns [402], and besides the ammonia in the atmosphere [27] which
could yield Aitken nuclei but also noxious transients [403] by chemical photooxidation, lead metal from vehicular emissions is now thought to influence weather phenomena to some extent. Modern, large cities are known to generate this assimilable [404]
poison in submicron-sized [405-410] particulates, at rates of some hundred weight
per day, and steady-state amounts of lead which floats in the atmosphere of an unventilated city of a few million people, may be estimated in terms of tons. Since leadiodide is known to be an excellent ice-nucleator material, it is not surprising that
mixtures of automobile exhausts and gasoline vapors, with iodine vapor, were also
found to nucleate ice [411-414]. Large amounts of 'natural' ice-forming nuclei are
thought to be due to this reaction [415], depending also on the availability of iodine in
the air and hence on the geographic location of a city. The kinetics of photo and
hydrodecay of those nuclei, which probably consist of large lead particulates whose
surface contains sites reacted with iodine, were not yet fully determined. There is no
doubt, however, that atmospheric lead may thus not only represent a direct hazard to
health but that it may also influence humans because of its interconnection with
weather phenomena.
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Recent Advances in The Chemistry and Properties of Atmospheric Nucleants - A Review

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Recent Advances in The Chemistry and Properties of Atmospheric Nucleants - A Review

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171

Recent Advances in the Chemistry and Properties of Atmospheric

Summary.- A survey is carried out of recent progress in the investigation of weather-active

A.C. Montefinale, T. Montefinale and H. M. Pap&

Vol. 91, 1971/VIII)

Chemistryand Properties of AtmosphericNucleants

A.C. Montefinale,T. Montefinaleand H. M. Pap6e

b. Large nuclei (radius between 0.2-1.0 micron)

Vol. 91, 1971/VIII)

Chemistryand Properties of Atmospheric Nucleants

A.C. Montefinale,T. Montefinaleand H. M. Pap6e

This situation is reversed in urban areas, because of combustion processes. Similar

Vol. 91, 1971/VIII)

Chemistryand Properties of AtmosphericNucleants

A. C, Montefinale,T. Montefinaleand H. M. Papee

Vol. 91, 1971/VIII)

Chemistryand Properties of Atmospheric Nucleants

c. The giant condensation nuclei (radius > 1 micron).

A.C. Montefinale, T. Montefinale and H. M. Pap6e

Vol. 91, 1971/VIII)

Chemistryand Properties of Atmospheric Nucleants

A.C. Montefinale,T. Montefinaleand H. M. Pap6e

Vol. 91, 1971/VIII)

Chemistryand Properties of AtmosphericNucleants

d. The role of condensation nuclei in nature

A.C. Montefinale, T. Montefinale and H. M. Pap6e

dicative of lowerings of water supercooling by small amounts of some dissolved

2. The nuclei of ice formation

Vol. 91, 1971/VIII)

Chemistryand Properties of Atmospheric Nucleants

A.C. Montefinale,T. Montefinaleand H. M. Papde

sensitive, heterogeneous and largely hydrophobic surfaces, such as those of impure

Vol. 91, 1971/VIII)

Chemistryand Properties of Atmospheric Nucleants

A.C. Montefinale,T. Montefinaleand H. M. Pap6e

b. The extra-terrestrial nuclei of ice formation

Vol. 91, 1971/VIII)

Chemistryand Properties of AtmosphericNucleants

surface of a meteoritic particle, as it appears in nature, and also of suitable chemical

A.C. Montefinale,T. Montefinaleand H. M. Pap6e

Vol. 91, 1971/VIII)

Chemistryand Properties of Atmospheric Nucleants

SIDLE who confirmed, experimentally, the presence of some of those compounds in

A.C. Montefinale,T. Montefinaleand H. M. Pap6e

3. The induction, inhibition and alteration of natural hydrometeor processes

Vol. 91, 1971/VIII)

Chemistryand Properties of Atmospheric Nucleants

As previously mentioned, the principle of operation consists here of dispersing

A.C. Montefinale, T. Montefmale and H. M. Pap6e

b. The action by nuclei of ice-formation

Vol. 91, 1971/viii)

Chemistryand Properties of Atmospheric Nucleants

4. The inadvertent modification of weather

A.C. Montefinale, T. Montefinale and H. M. PapOe

Vol. 91, 1971/VIII)

Chemistry and Properties of Atmospheric Nucleants

A . C . Montefinale, T. Montefinale and H. M. Pap&

[46] P. CHOVIN,Pollution Atmosph~riqueetChimieAnalytique, Bull. Soc. Chim. France. 5 (1968),

Vol. 91, 1971/VIII)

Chemistry and Properties of Atmospheric Nucleants

[73] R. H. LOUCKS and J. W. WINCHESTER,Some Features of Chlorine and Bromine in Aerosols,

A . C . Montefinale, T. Montefinale and H. M. Pap6e

[101] P. J. HILSSON, Liesgang Phenomenon - the Importance of lmpurities in Periodic Precipitation,