www.aspbs.

com/enn
Encyclopedia of
Nanoscience and
Nanotechnology
Photoconductivity of Carbon Nanotubes
Akihiko Fujiwara
Japan Advanced Institute of Science and Technology, Tatsunokuchi, Ishikawa, Japan,
and Japan Science and Technology Corporation, Kawaguchi, Saitama, Japan
CONTENTS
1. Introduction
2. Physical Properties of Carbon Nanotubes
3. Photoconductivity of Carbon Nanotubes
4. Related Phenomena
5. Summary
Glossary
References
1. INTRODUCTION
Since the discovery of carbon nanotubes (CNTs) by Iijima
in 1991 [1], they have attracted great attention as potential
electronic materials because of the one-dimensional tubu-
lar network structure on a nanometer scale. The variety
of band structures of the CNTs, being either semiconduct-
ing or metallic, depending on the chirality and diameter
of the CNT, is also a novel feature. For this reason, it is
expected that CNTs become model samples for an ideal one-
dimensional metal and an ideal one-dimensional semicon-
ductor. In addition, CNTs are also expected to be one of
the greatest candidates for nanotechnology materials, such
as nanometer scale wirings and nanometer scale devices
[24].
A CNT can be described as a single graphite (graphene)
sheet rolled into a cylindrical shape. A concentric tubu-
lar structure can be made of two or more nanotubes with
different diameters. The former and the latter are called
single-wall carbon nanotubes (SWCNTs) and multiwall car-
bon nanotubes (MWCNTs), respectively. The thinnest CNTs
are found in a most inner CNT of MWCNTs and SWCNTs
grown in zeolite AlPO
4
-5 (AFI) single crystals; the diam-
eter is about 0.4 nm [5, 6]. The diameter of thick CNTs
is at most a few 10 nanometers. In most cases, CNTs with
large diameters are MWCNTs; in the case of SWCNTs,
a cross-section will not be able to maintain circular struc-
ture but it will be distorted. Moreover, in MWCNTs with
large diameters, structure strongly depends on production
conditions and can be not only concentric, but also the
structure in which a graphene is scrolled upa polyhedral
graphite tube with defects at the vertex and mixtures of them
[710].
For the theoretical approach and the interpretation of
experimental results, SWCNTs are suited, because interac-
tion between layers and the effect of defects must be taken
into consideration in the case of MWCNTs. Most of the
experimental observation had been on MWCNTs in the
beginning of research on CNTs. After the establishment of
a synthesis method for high-quality SWCNTs [1113], exten-
sive research on SWCNTs, as well as MWCNTs, is per-
formed. Since researches eld of photoconductivity of CNTs
reviewed in this article have a short history, only the research
for two kinds of SWCNT samples are reported [1419].
Photoconductivity has not been observed in MWCNT sam-
ples. Therefore, if there is no notice, there will be a discus-
sion about the SWCNT in this article.
This chapter is organized as follows. The physical prop-
erties needed for discussion about the photoconductivity of
CNTs are presented in Section 2. In Section 3, the pho-
toconductive properties observed in two kinds of SWCNTs
are shown. Here, experimental methods are also described,
because introduction of this is important because it has been
succeeded only with a few groups in spite of many trials.
As related phenomena, two types of photo-induced current
modulations are presented in Section 4. Section 5 summa-
rizes the chapter.
2. PHYSICAL PROPERTIES
OF CARBON NANOTUBES
A number of excellent books and review articles have sum-
marized the physical and chemical properties of CNTs [24,
20, 21]. In this section, properties related to photoconduc-
tivity are briey described.
2.1. Molecular Structure
A SWCNT can be made by rolling a graphene sheet into a
cylindrical shape [24, 2023]. Although the tubular struc-
ture with any diameter and direction can be made when
ISBN: 1-58883-064-0/$35.00
Copyright 2004 by American Scientic Publishers
All rights of reproduction in any form reserved.
Encyclopedia of Nanoscience and Nanotechnology
Edited by H. S. Nalwa
Volume 8: Pages (569574)
570 Photoconductivity of Carbon Nanotubes
we make it from papers without a pattern on the surface,
the network structure of carbon has to be take into account
for CNTs. In a graphene sheet, carbon atoms form a two-
dimensional network of a six-membered ring, namely, a
hexagonal (or honeycomb) lattice by connecting their three
sp
2
hybrid orbitals. There are two sites, A- and B-site, in
the graphene: one carbon is bonded to three carbons of
another site. When graphene is rolled into cylindrical shape
and one carbon is put on any other carbon in the same
site, a CNT can be formed in principle. Relation between
these two overlapped carbon atoms on the graphene can be
described by chiral vector C
|
= na
1
+ na
2
, where n, n are
integers and a
1
, a
2
are the unit vectors of the graphene. The
direction of the chiral vector C
|
is perpendicular to the CNT
axis and its length, 1 C
|
= a(n
2
+n
2
+nn)
1,2
is equal
to that of circumference of the CNT, where a is the length
of a
1
and a
2
. In actuality, because a sp
2
hybrid orbital cannot
be maintained for small diameters and the tubular structure
is distorted for large diameters, the diameter of SWCNTs is
considered to be about 0.42.0 nm.
2.2. Electronic Structure
It is intelligible when the electronic structure of a SWCNT,
as well as molecular structure, is considered on the basis
of a graphene sheet [2025]. It is necessary to consider the
periodic boundary conditions along the circumference of
the CNT to the electronic structure of the graphene. Since
the graphene sheet has a hexagonal lattice, the rst Brillouin
zone becomes a right hexagon. In energy-dispersion rela-
tions, the =

(conduction) band and the = (valence) band

are degenerate only at the six corners of the hexagonal rst
Brillouin zone, K and K

points, which the Fermi energy

passes. Since the density of states at the Fermi energy is
zero, the graphene is a zero-gap semiconductor. Although
all the points in the rst Brillouin zone are allowed for the
graphene sheet, in the case of CNTs, allowed points are
only on the line prolonged in the direction of the CNT axis
through the ! point (the center of the rst Brillouin zone)
and the parallel lines that separated 2k=/1 (k: integer) from
this line. Therefore, when these straight lines pass through K
(K

) points, since energy dispersion will pass Fermi energy,

CNTs become metallic. The distance between K (K

) points
and the allowed line through the ! point is 2= (2n+n)/31.
As a result, when 2n+n, that is, nn, is the multiple of 3,
CNTs become metallic. In other cases, CNTs become semi-
conducting. In the energy dependence of density of states
in CNTs, van Hove singularity (VHS) appears to be reect-
ing one-dimensional nature. Moreover, because =

(conduc-
tion) and = (valence) bands are almost symmetrical, the
density of state near the Fermi energy shows the symmetri-
cal energy dependence in respect to the Fermi energy.
2.3. Optical Absorption
Theoretical prediction shows the optical transition takes
place only between symmetrical bands, under the congura-
tion that the polarization vector E is parallel to the nanotube
axis by taking into account the depolarization effect [26].
Corresponding to high transition probability between the
symmetric VHSs, three characteristic absorption bands in
an optical absorption spectrum are observed in the energy
range from an infrared region to a visible region [13, 27].
Two absorption bands in the lower energy and one at the
highest energy originate from semiconducting and metallic
SWCNTs, respectively.
It is well known that the exciton binding energy becomes
innite in the limit of an ideal one-dimensional electron-
hole system [2830]. Therefore, the effect of exciton plays an
important role in optical absorption for the one-dimensional
system of SWCNTs. This effect is considered to mainly
modify the lowest band of the optical absorption spectrum,
which was predicted theoretically [31]. Experimental results
of optical absorption are consistent with this prediction
[13, 27].
2.4. Electronic Transport Properties
Although there are many ndings of novel properties and
functions, such as single electron transport [32, 33], spin
transport [34], rectication [35, 36], switching function [37],
tunable electronic structure by magnetic elds [38, 39], sin-
gle molecule CNT transistors [4042], and superconductiv-
ity [43, 44] in electron transport properties, we focus on
the electron scatteringballistic or diffusive. The ballis-
tic conduction in CNTs even at room temperature (RT)
was pointed out by observation of quantized conduction in
MWCNTs at rst [45]. Ballistic conduction of SWCNTs was
proposed by the detailed analysis of the coulomb blockade
behavior of SWCNTs which act as a quantum dot [32]. From
the subsequent research for semiconducting SWCNTs, the
mean-free path is estimated to be about 100 nm which is
about one-tenth of the CNT length, and the result suggests
diffusive conduction in semiconducting SWCNTs in spite of
ballistic conduction in metallic SWCNTs [46]. This is con-
sidered to be due to the electron scattering at defects and
the bending parts of CNTs.
3. PHOTOCONDUCTIVITY
OF CARBON NANOTUBES
The research on photoconductivity for two kinds of
SWCNTs has been reported. One is observed in the
SWCNTs with a diameter of about 1.4 nm, being closed-
packed into bundles and forming a two-dimensional tri-
angular lattice [1417]. Another is in the SWCNTs, with
a diameter of about 0.4 nm grown in zeolite AlPO
4
-5
(AFI) single crystals, which are one type of the thinnest
SWCNTs [18, 19]. In MWCNTs, photoconductivity has not
been observed thus far.
3.1. Single-Wall Carbon Nanotube Bundles
Photoconductivity of CNTs has been discovered in the lm
sample of SWCNT bundles, and the most detailed research
has been performed for this sample [1417]. In this sec-
tion, detailed experimental methods for the observation,
photoconductive properties, and possible mechanisms are
presented.
Photoconductivity of Carbon Nanotubes 571
3.1.1. Experimental Technique
The samples of SWCNT bundles were synthesized by evap-
oration of composite rods of nickel (Ni), yttrium (Y), and
graphite in helium atmosphere by arc discharge [12, 13] or
ablating a graphite target containing Ni and cobalt (Co) cat-
alysts at 1250

C in an argon atmosphere by using a pulsed
Nd:YAG laser [11]. Observations by transmission electron
microscopy (TEM) revealed that soot is mainly composed of
SWCNTs and also amorphous carbons and metal particles.
The diameter of the SWCNTs is determined to be about
1.4 0.2 nm by the Raman frequency of a breathing mode
and TEM observation. The typical length of SWCNT bun-
dles estimated by scanning electron microscopy (SEM) is a
few micrometers.
To prepare lm samples, soot-containing SWCNTs were
dispersed in methyl alcohol by an ultrasonic vibrator and
suspension of SWCNTs was dropped on a glass substrate.
The typical lm sample size is about 100 m 100 m and
the thickness of the lm is between 300 and 500 nm. The
samples were annealed in vacuum at 10
6
Torr and 673 K
for 2 hours to remove the absorbed gases and methyl alco-
hol from samples. A pair of gold electrodes separated by a
10-m gap was evaporated in vacuum onto the surface of
the lm samples and connected to a DC regulated power
supply (100 mV). In order to reduce the number of junc-
tions between SWCNTs in the current pass, the narrow gap
of 10 m was chosen because the resistance of the junctions
dominates the total resistance of the sample and obscures
the intrinsic transport properties of SWCNTs.
The samples were mounted in a continuous-ow cryostat
and cooled by owing the vapor of liquid He and liquid N
2
in the temperature range from 10 K to RT and from 100 K
to RT, respectively. As a light source, an optical paramet-
ric oscillator (OPO), excited by a pulsed Nd:YAG laser, was
used. The photon energy was in the range of 0.5 to 2.8 eV
and the pulse duration was 5 ns. The light intensity is from a
few tens nJ/pulse to 1500 nJ/pulse. The temporal proles of
the laser pulse and the photocurrent were monitored with
a digitizing oscilloscope. In order to avoid spurious ringing
in the fast pulse detection, we were obliged to use the input
impedance of the oscilloscope (50 H) as the reference resis-
tor, despite the obvious disadvantage of lower sensitivity.
The resistance of samples in the dark is ca. 100 H at RT and
800 H at around 10 K.
3.1.2. Observed Behaviors
The temporal evolution of photocurrent shows a Gaussian-
like peak with a 5 ns width corresponding to the pulse
duration of the laser. Photocurrent increases with increas-
ing incident light intensity. When photocurrent is less than
10 A, the photocurrent intensity responds linearly to inci-
dent light intensity. On the other hand, it shows a satura-
tion behavior above 10 A; this saturation is often observed
under intense light intensity and might be due to the lack
of replenishment of carriers [47]. In photoconductivity exci-
tation spectra estimated from the slope of the linear part in
light intensity dependence of photocurrent, two clear peaks
in photoconductivity excitation spectra at RT are observed
around 0.7 and 1.2 eV. These energies are very close to
the energy difference of rst and second symmetrical pairs
of VHSs of semiconducting SWCNTs with a diameter of
1.4 nm. In addition, these spectra are very similar to the
optical absorption spectra of SWCNTs prepared by the same
method [13, 27].
The photoconductive response at 13.2 K is much higher
than that at RT, whereas the optical absorption is hardly
enhanced even at a low temperature [48]. Moreover, the
enhancement strongly depends on the photon energy; the
intensities of the peak in photoconductivity excitation spec-
tra at 0.7 and 1.2 eV were enhanced by about two and one
orders of magnitude, respectively. The observed photocon-
ductive response monotonically increases with a decrease in
temperature between 10 K and RT, and shows the saturation
around 10 K.
3.1.3. Mechanism
From the correspondence between the optical absorp-
tion spectra of semiconducting carbon nanotubes and pho-
toconductivity spectra, it is clear that the photocurrent
originates from photoexcitation of electrons in semiconduct-
ing SWCNTs. Temperature dependence of photoconductiv-
ity Au(T ) can be represented by Au(T ) =An(T )e(T ) =
An(T )(e
2
,n

) {l(T )/:(T )}, where An(T ), e, (T ), n

,
l(T ), and :(T ) are carrier numbers increased by light irra-
diation, carrier charge, mobility of charge carrier, effec-
tive mass of charge carrier, mean-free path, and thermal
velocity [47]. Therefore, the temperature dependence of
Au(T ) should be attributed to that of An(T ) and/or (T )
l(T )/:(T ). T
3,2
dependence of (T ) is expected in con-
ventional semiconductors with the regime of the diffusive
transport due to electronphonon interactions, because l(T )
and :(T ), respectively, follow T
1
and T
1,2
. On the other
hand, by assuming the ballistic conduction, l(T ) is expected
to be limited to the nanotube length and to become inde-
pendent of temperature. In this case, (T ) is expected to
follow T
1,2
. Therefore, Au(T ) is expected to follow T
3,2
or T
1,2
for the interband transition, because An(T ) hardly
depends on temperature. In this way, photoconductivity
increases with a decrease in temperature for the interband
transition, although temperature dependence of photocon-
ductivity changes owing to the type of transportballistic or
diffusive.
If exciton absorption is dominant in the semiconduct-
ing SWCNTs, as pointed out by the theoretical and exper-
imental approach on optical absorption [13, 27, 31], free
carriers contributing to the photoconductivity An(T ) are
created through thermal dissociation of excitons. In this
case, An(T ) will decrease with a decrease in tempera-
ture, and then, Au(T ) will decrease, which is contrary to
the experiment result. Experimental results naively support
the theory that the photocarriers originate from the usual
interband transition. Very recently, photoconductivity was
observed in SWCNTs with the diameter of 0.4 nm [18, 19] as
described in the next subsection. Since these samples have a
stronger one-dimensional structure, binding energy of exci-
ton is expected to be much larger than our samples. It is
expected that the comparison of the photoconductive prop-
erties between these samples gives valuable information to
solve this contradiction.
572 Photoconductivity of Carbon Nanotubes
3.2. Single-Wall Carbon Nanotubes
in Zeolite Single Crystals
Another example of observation of photoconductivity is
shown in this section [18, 19]. Novel features of this type
of sample are the smallest diameter and the almost perfect
alignment of SWCNTs in the zeolite single crystals. For these
reasons, this sample is very suitable for estimation of the
effect of the one dimensionality and the optical anisotropy.
3.2.1. Experimental Technique
The samples of SWCNTs in one-dimensional channels of
zeolite AFI single crystals were synthesized by thermal treat-
ment of paralyzed carbon encapsulated in the AFI crys-
tal at 500800

C [6, 49]. Single-wall carbon nonotubes
are grown in one-dimensional channels along the c-axis of
AFI. Observations by TEM revealed that after dissolving the
AFI framework residual materials are SWCNTs and raft-
like graphite; the diameter of the SWCNTs is determined to
be about 0.42 0.2 nm. Three possible structures, (n, n) =
(5, 0), (3, 3), (4, 2), are proposed for this type of nanotube.
Typical dimensions of an AFI single crystal containing SWC-
NTs are 75160 m in a cross-section diameter of a hexag-
onal face and ca. 300 m in length along the c-axis of AFI.
The gold wires of 100150 mm in diameter were attached
to both hexagonal faces of the AFI single crystal. Bias volt-
age was applied between these two wires by a DC regulated
power supply up to 1.5 V. Current ows along the c-axis of
AFI, namely, the CNT axis. Linearly polarized light from
a CW-Ar
+
-ion laser or a CW-Ti/sapphire laser pumped by
an Ar
+
-ion laser was focused onto the central part of one
surface of the AFI crystal. The direction of incident light is
perpendicular to the CNT axis. The size of the illuminated
spot was set about 100 m in diameter. The resistance of
samples in the dark is around 100 MH at RT.
3.2.2. Observed Behaviors
Conductance increases during the photo irradiation with
the period of about 10 s. The response time is less than
50 ms. Photocurrent is proportional to the incident light
intensity at low intensities. Although neither photon energy
dependence (photoconductivity excitation spectra) nor tem-
perature dependence have been investigated in detail, the
information about optical anisotropy have been presented
in this sample. By using this sample, it is conrmed that
three absorption bands characteristic of CNTs are observed
when a polarization vector is parallel to the c-axis of the
AFI crystal (E c), that is, the CNT axis, whereas opti-
cal absorption has hardly been detected for the case that
the polarization vector is perpendicular to the nanotube axis
(E c) [19, 50, 51], which is consistent with the theoretical
prediction as described in Section 23 [26]. Corresponding
to this, photoconductive response strongly depends on the
angle between the polarization vector and the CNT axis;
photocurrent for E c is about twice as large as that for
E c.
Intrinsic resistance of the SWCNT sample in the dark
increases to more than twice the values by irradiating an
intense light of about 10 mW. During the process of an
increase in the resistance, the increases in photoconductive
response and in optical anisotropy are also observed. This
result suggests that the intense light irradiation results not in
the collapse of CNTs but in the increase in an effective semi-
conductor SWCNT, namely, the rearrangement of the nano-
tube structure within zeolitefor example, the connection
of a divided semiconductor nanotubes and the structure con-
version from the metallic SWCNTs to semiconducting ones.
4. RELATED PHENOMENA
In this section, two related phenomena, photo-induced cur-
rent modulation, are presented.
4.1. Conductance Modulation Due
to the Molecular Photodesorption
Conductance of an individual semiconducting SWCNT
decreases by 10% upon ultraviolet (UV) illumination in air,
NO
2
, and NH
3
atmosphere, contrary to the photoconductive
response [52]. The conductance recovers after the light is
turned off. This reaction occurs in reverse by repeating irra-
diation of light. This is caused by photodesorption of gases
which acts as an electron donor or accepter. Through pho-
todesorption of molecules, SWCNTs becomes intrinsic semi-
conductors without any carrier doping and its conductance
decreases. Therefore, when UV illumination is performed
in a high vacuum, the conductance decreases drastically by a
few orders of magnitude, and exhibit no appreciable recov-
ery when the light was switched off.
4.2. Photo-Induced Tunneling Current
in STM Measurements
It is expected that the local photocurrent can be measured
by the scanning tunneling microscopy (STM) method [53].
A photo-induced tunneling current is observed for semi-
conducting and metallic SWCNTs, only when the photon
energy exceeds energy difference of the rst symmetrical
pairs of VHS in the density of state. It is observed at both
a positive and negative bias voltage of STM measurements,
and increases linearly to the light intensity and is reversible.
Although this behavior is preferred to observations of pho-
toconductive response and electronic structure modulation
through light irradiation in nanometer scale spatial resolu-
tion, it is necessary to clarify the extrinsic effects, such as
the effect of thermal expansion of the CNT sample and the
tip of STM to tunnel current, which is extremely sensitive to
the distance between the sample and the tip.
5. SUMMARY
In this chapter, we have reviewed current states of photo-
conductivity of carbon nanotubes. Photoconductive proper-
ties for the bundles of SWCNTs with a diameter of 1.4 nm
and the SWCNTs with a diameter of 0.4 nm in Zeolite
single crystals are presented. Two types of photo-induced
current modulation are also presented. The mechanism of
photoconductivity is still unclear because of its short his-
tory. However, from the viewpoint both of nanoscale sci-
ence and practical application for nano-scale devices, the
Photoconductivity of Carbon Nanotubes 573
understanding of this phenomenon is very important. It is
expected that the origin of photocarriers, the conduction
characteristic of a semiconductor nanotubeballistic or dif-
fusive will be claried from the detailed experiments on the
temperature dependence of photoconductivity. In addition
to this, the effect of the one dimensionality and the contribu-
tion of the exciton for the carrier generation will be claried
by comparing the photoconductive properties between these
two types of SWCNTs with different diameters. This eld is
now ongoing and will develop further.
GLOSSARY
Carbon nanotube (CNT) A tubular molecule made of car-
bon with nanometer diameter.
Exciton A mobile, electrically neutral, excited condition of
holes and electrons in a crystal. One example is a weakly
bound electron-hole pair.
Multiwall carbon nanotube (MWCNT) A type of carbon
nanotube with the structure that a concentric tubular struc-
ture can be made of two or more nanotubes with different
diameters.
Optical parametric oscillator (OPO) A laser-pumped crys-
tal with nonlinear optical properties that generates coher-
ent light whose output can be tuned continuously over wide
range of wavelengths.
Photoconductivity An electrical conductivity increase
exhibited by some nonmetallic materials, resulting from the
free carriers generated when photon energy is absorbed in
electronic transitions.
Photocurrent A current produced by photoelectric or pho-
tovoltaic effects.
Scanning electron microscope (SEM) A type of electron
microscope that uses a beam of electrons to scan the sample
surface, ejecting secondary electrons that form the picture
of the sample.
Scanning tunneling microscope (STM) A high-solution
microscope that can detect and measure the positions and
heights of individual atoms on the surface of the sample.
Single-wall carbon nanotube (SWCNT) A type of car-
bon nanotube with the structure that a single graphite
(graphene) sheet rolled into a cylindrical shape.
Transmission electronic microscope (TEM) A type of
electron microscope that uses magnetic lenses to transmit
a beam of electrons through the sample; the electrons are
then focused on a uorescent screen to form an enlarged
image or a diffraction image.
van Hove singularity (VHS) A singularity observed in
energy spectrum of density of states for electrons and
phonons, showing divergences of the slope.
ACKNOWLEDGMENTS
The authors wish to thank Dr. H. Suematsu at Japan
Synchrotron Radiation Research Institute and Professor
K. Miyano, Professor N. Nagasawa, and Mr. N. Ogawa at the
University of Tokyo for the continuous discussions and/or
collaboration on this problem.
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