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On the Lorentz-Lorenz formula and the

Lorentz model of dielectric dispersion


Kurt E. Oughstun and Natalie A. Cartwright
College of Engineering & Mathematics, University of Vermont, Burlington, VT 05405-0156
Oughstun@emba.uvm.edu, Ncartwri@emba.uvm.edu

Abstract: The combination of the Lorentz-Lorenz formula with the Lorentz


model of dielectric dispersion results in a decrease in the effective
resonance frequency of the material when the number density of Lorentz
oscillators is large. An equivalence relation is derived that equates the
frequency dispersion of the Lorentz model alone with that modified by the
Lorentz-Lorenz formula. Negligible differences between the computed
ultrashort pulse dynamics are obtained for these equivalent models.
©2003 Optical Society of America
OCIS codes: (260.2030) Dispersion; (320.5550) Pulses.

References and Links


1. H. A. Lorentz, Versuch einer Theorie der Electrischen und Optischen Erscheinungen in Bewegten Körpern
(Teubner, 1906); see also H. A. Lorentz The Theory of Electrons (Dover, 1952).
2. H. A. Lorentz, “Über die Beziehungzwischen der Fortpflanzungsgeschwindigkeit des Lichtes der
Körperdichte,” Ann. Phys. 9, 641-665 (1880).
3. L. Lorenz, “Über die Refractionsconstante,” Ann. Phys. 11, 70-103 (1880).
4. M. Born and E. Wolf, Principles of Optics, 7th (expanded) edition (Cambridge U. Press, 1999) Ch. 2.
5. J. M. Stone, Radiation and Optics (McGraw-Hill, 1963) Ch. 15.
6. H. M. Nussenzveig, Causality and Dispersion Relations (Academic Press, 1972) Ch. 1.
7. A. Sommerfeld, “Über die Fortpflanzung des Lichtes in Disperdierenden Medien,” Ann. Phys. 44, 177-202
(1914).
8. L. Brillouin, “Über die Fortpflanzung des Licht in Disperdierenden Medien,” Ann. Phys. 44, 203-240
(1914).
9. L. Brillouin, Wave Propagation and Group Velocity (Academic Press, 1960).
10. K. E. Oughstun and G. C. Sherman. “Propagation of electromagnetic pulses in a linear dispersive medium
with absorption (the Lorentz medium),” J. Opt. Soc. Am. B 5, 817-849 (1988).
11. K. E. Oughstun and G. C. Sherman, Electromagnetic Pulse Propagation in Causal Dielectrics (Springer-
Verlag, 1994).
12. B. K. P. Scaife, Principles of Dielectrics (Oxford, 1989) Ch. 7.

_____________________________________________________________________________

1. Introduction
The classical Lorentz model [1] of dielectric dispersion due to resonance polarization is of
fundamental importance in optics as it provides a physically appealing, accurate description of
both normal and anomalous dispersion phenomena in the extended optical region of the
electromagnetic spectrum from the far infrared up to the near ultraviolet. Of equal importance
is the Lorentz-Lorenz formula [2,3] which, as stated in Born and Wolf [4], “connects
Maxwell’s phenomenological theory with the atomistic theory of matter.” It is typically
assumed [4,5] that the number density of molecules is sufficiently small so that the Lorentz-
Lorenz formula can be simplified to a simple linear relationship between the mean molecular
polarizability and the dielectric permittivity. Although the influence of the Lorentz-Lorenz
formula on the resulting frequency dispersion can be striking when the number density
becomes sufficiently large, the fundamental frequency structure is not altered from that

#2595 - $15.00 US Received June 11, 2003; Revised June 20, 2003
(C) 2003 OSA 30 June 2003 / Vol. 11, No. 13 / OPTICS EXPRESS 1541
described by the Lorentz model alone; a frequency band of anomalous dispersion with high
absorption surrounded by lower and higher frequency regions exhibiting normal dispersion
with small absorption.
The fact that the Lorentz model is a causal model [6] of temporal dispersion has cast it in
a central role in both the classical [7-9] and modern [10-11] asymptotic theories of linear
dispersive pulse propagation. Although the asymptotic theory is independent of the particular
material parameter values chosen for the Lorentz model dielectric considered, the material
parameters originally chosen by Brillouin [8,9] and employed in much of the modern
asymptotic theory [10-11] correspond to a highly absorptive material for which the Lorentz-
Lorenz formula must be applied without approximation. The purpose of this paper is to
establish an approximate equivalence relation that equates the frequency dispersion of the
Lorentz model alone with that modified by the Lorentz-Lorenz formula. This result then
extends the domain of applicability of the asymptotic theory to include the optically dense
material originally considered by Brillouin [8,9].
2. The Lorentz-Lorenz formula and the Lorentz model of dielectric dispersion
The Lorentz force acting on a bound electron in a material depends upon the local or effective
electromagnetic field present at that molecular site. The effective electric field Eeff ( r , t )
acting on a molecule at space-time position ( r,t ) in a polarizable medium with polarization
P( r,t ) is given by [3]
4p
Eeff ( r , t ) = E( r , t ) + P( r , t ) , (1)
3

where E( r,t ) is the external, applied electric field. In a locally linear, homogeneous,
isotropic material the electric dipole moment for each molecule is linearly related to the
effective electric field through the causal relation

p( r , t ) = Ú aˆ (t - t ¢)Eeff ( r , t ¢)dt ¢
t
(2)
-•

with Fourier transform p˜ ( r , w ) = a (w ) E˜ eff ( r , w ) , where a (w ) is the mean polarizability


at angular frequency w . If N denotes the number density of molecules in the material, then
the spectrum of the induced polarization in Eq. (1) is given by P ˜ ( r , w ) = Np˜ ( r , w ) . With
substitution from the Fourier transform of Eq. (1) one then obtains the expression

P˜ ( r , w ) = c e (w ) E˜ ( r , w ) , (3)

where

Na (w )
c e (w ) = (4)
1 - ( 4p 3) Na (w )

is the electric susceptibility. With the expression e (w ) = 1 + 4pc e (w ) for the relative
dielectric permittivity, one then obtains the Lorentz-Lorenz formula [2,3]

3 e (w ) - 1
a (w ) = , (5)
4pN e (w ) + 2

#2595 - $15.00 US Received June 11, 2003; Revised June 20, 2003
(C) 2003 OSA 30 June 2003 / Vol. 11, No. 13 / OPTICS EXPRESS 1542
which is also referred to as the Clausius-Mossotti relation [12]. It is typically assumed that
e (w ) is sufficiently close to unity that e (w ) + 2 ª 3 in which case the Lorentz-Lorenz
formula simplifies to e (w ) ª 1 + 4pNa (w ) , which is equivalent to the approximation that
Eeff ( r , t ) ª E( r , t ) .
The Lorentz model [1] of resonance polarization in dielectrics is based upon the damped
harmonic oscillator equation

me ( r˙˙(t ) + 2dr˙(t ) + w 02 r (t )) = - qe Eeff (t ) (6)

r (t ) relative to the nucleus of a bound electron of mass me and charge


for the position vector
magnitude qe with (undamped) resonance frequency w 0 and phenomenological damping
constant d under the action of the local Lorentz force Floc (t ) = - qe Eeff (t ) due to the
electric field alone, the magnetic field contribution being assumed negligible by comparison.
The solution to this o.d.e. is obtained in the Fourier frequency domain as

qe me
r˜ (w ) = E˜ (w ) . (7)
w - w 02 + 2idw eff
2

The local induced dipole moment is then given by p˜ (w ) = - qe r˜ (w ) which then results in
the expression

- qe2 me
a (w ) = (8)
w 2 - w 02 + 2idw
for the molecular polarizability. Substitution of this expression into the Lorentz-Lorenz
formula then yields the final expression

1 - (2b 2 3) (w 2 - w 02 + 2idw )
e (w ) = (9)
1 + (b 2 3) (w 2 - w 02 + 2idw )

for the complex, relative dielectric permittivity. The complex index of refraction
n(w ) = e (w ) is then given by the branch of the square root of the expression in Eq. (9)
that yields a positive imaginary part (attenuation) along the positive real frequency axis. [12].
( )
When the inequality b 6dw 0 << 1 is satisfied, the denominator in Eq. (9) may be
2

approximated by the first two terms in its power series expansion so that

Ê 2b 2 3 ˆÊ b2 3 ˆ b2
e (w ) ª Á1 - 2 ˜ Á1 - ˜ ª1- 2 , (10)
Ë w - w 02 + 2idw ¯ Ë w 2 - w 02 + 2idw ¯ w - w 02 + 2idw

which is the usual expression [1,4-11] for the frequency dispersion of a single resonance
Lorentz model dielectric.
As an example, consider the Lorentz model material parameters chosen by Brillouin [8,9],
viz. w 0 = 4 ¥ 10 r / s , d = 0.28 ¥ 10 r / s , b = 20 ¥ 10 r / s , which correspond
16 16 16

to a highly absorptive dielectric. The angular frequency dispersion of the complex index of
refraction for the Lorentz model alone [as given by the square root of the final approximation
in Eq. (10)] is illustrated by the solid blue curve in Figure 1. Part (a) of the figure describes

#2595 - $15.00 US Received June 11, 2003; Revised June 20, 2003
(C) 2003 OSA 30 June 2003 / Vol. 11, No. 13 / OPTICS EXPRESS 1543
the frequency dispersion of the real index of refraction nr (w ) = ¬ { e (w ) } while part (b)
describes that for imaginary part ni (w ) = ¡ { e (w ) } . The corresponding solid green
curves in Fig. 1 describe the resultant frequency dispersion for this Lorentz model dielectric
when the Lorentz-Lorenz relation is used [cf. Eq. (9)]. As can be seen, the Lorentz-Lorenz
modified frequency dispersion primarily shifts the resonance frequency to a lower frequency
value while increasing both the absorption and the below resonance index of refraction.
( )
Notice that b 6dw 0 = 2.976 for this choice of material parameters. If the plasma
2

frequency is decreased to the value b = 2 ¥ 1016 r / s so that b 2 (6dw 0 ) = 0.2976 ,


then the modification of the Lorentz model by the Lorentz-Lorenz relation is relatively small,
as exhibited by the second set of curves in Fig. 1.
3 3

b2 = 20X1032r /s
2.5 2.5

b2 = 20X1032r/s

2 2
nr(w)

ni(w)
1.5 1.5

1 b2 = 2X1032r/s
1

0.5 0.5
b2=2X1032r/s

0 0
0 1 2 3 4 5 6 7 8 9 10 0 1 2 3 4 5 6 7 8 9 10
(a) w - r/s 16
x 10 (b) w - r/s 16
x 10

Fig. 1. Angular frequency dependence of the real (a) and imaginary (b) parts of the complex
index of refraction for a Lorentz model dielectric with (green curves) and without (blue curves)
the Lorentz-Lorenz formula for two different values of the material plasma frequency.

3. An approximate equivalence relation


Since the primary effect of the Lorentz-Lorenz formula on the Lorentz model is to downshift
the effective resonance frequency and increase the low frequency refractive index, consider
then determining the resonance frequency w * appearing in the Lorentz-Lorenz formula for a
Lorentz model dielectric that will yield the same value for e (0) as given by the Lorentz
model alone with resonance frequency w 0 . From Eqs. (9) and (10) one then has that

1 + (2 3)(b 2 w *2 )
1 + b 2 w 02 = , (11)
1 - (1 3)(b 2 w *2 )

with solution

w * = w 02 + b 2 3 . (12)

Consider then comparison of the frequency dependence of the expression [cf. Eq. (9)]

1 - (2b 2 3) (w 2 - w *2 + 2idw )
e (w ) = (13)
1 + (b 2 3) (w 2 - w *2 + 2idw )

#2595 - $15.00 US Received June 11, 2003; Revised June 20, 2003
(C) 2003 OSA 30 June 2003 / Vol. 11, No. 13 / OPTICS EXPRESS 1544
of the relative dielectric permittivity for the Lorentz-Lorenz modified Lorentz model dielectric
with undamped resonance frequency w * given by the equivalence relation (12), with the
expression [cf. Eq. (10)]

b2
e app (w ) = 1 - (14)
w 2 - w 02 + 2idw

of the approximate relative dielectric permittivity for a Lorentz model dielectric with
undamped resonance frequency w 0 . The other two material parameters b and d are the
same in these two expressions.
3 2.5

2.5
2

1.5
nr(w)

ni(w)
1.5

0.5
0.5

0 0
0 1 2 3 4 5 6 7 8 9 10 0 1 2 3 4 5 6 7 8 9 10
(a) w - r/s 16
x 10 (b) w - r/s 16
x 10

Fig. 2. Comparison of the angular frequency dependence of the real (a) and imaginary (b) parts
of the complex index of refraction for a single resonance Lorentz model dielectric alone (solid
blue curves) and for the equivalent Lorentz-Lorenz formula modified Lorentz model (green
circles).

A comparison of the angular frequency dependence described by Eqs. (14) and (13) with
w * given by the equivalence relation (12) is presented in Fig. 2 for Brillouin’s choice of the
material parameters ( w 0 = 4 ¥ 10 r / s , d = 0.28 ¥ 10 r / s , b = 20 ¥ 10 r / s ).
16 16 16

The rms error between the two sets of data points presented in Fig. 2 is approximately
2.310-16 for the real part and 2.010-16 for the imaginary part of the complex index of
-16
refraction, with a maximum single point rms error of ~2.510 . The corresponding rms
-15
error for the relative dielectric permittivity is ~1.110 for both the real and imaginary
-14
parts with a maximum single point rms error of ~1 10 . Variation of any of the
remaining material parameters in the equivalent Lorentz-Lorenz modified Lorentz model
dielectric, including the value of the plasma frequency from that specified in Eq. (12), only
results in an increase in the rms error. This approximate equivalence relation between the
Lorentz-Lorenz formula modified Lorentz model dielectric and the Lorentz model dielectric
alone is then seen to provide a “best fit” in the rms sense between the frequency dependence
of the two models.
4. Conclusions
An approximate equivalence relation between the Lorentz-Lorenz formula modified Lorentz
model dielectric and the Lorentz model alone for the complex index of refraction of a single
resonance dielectric has been presented. Numerical results show that this approximate
equivalence relation provides a “best fit” in the rms sense between the frequency dependence
of the two models. This result then extends the domain of applicability of the asymptotic

#2595 - $15.00 US Received June 11, 2003; Revised June 20, 2003
(C) 2003 OSA 30 June 2003 / Vol. 11, No. 13 / OPTICS EXPRESS 1545
theory of dispersive pulse propagation in a Lorentz model dielectric to include the optically
dense material originally considered by Brillouin [8,9] and subsequently used as an example
in the modern asymptotic theory [10,11]. In fact, the results are indistinguishable when the
two equivalent models are used in a numerical determination of the propagated field due to an
input rectangular envelope pulse in a single resonance Lorentz model dielectric using
Brillouin’s choice of the material parameters, including the leading and trailing edge
precursors.
Acknowledgement
The research presented in this paper was supported, in part, by the United States Air Force
Office of Scientific Research under AFOSR Grant # 49620-01-0306.

#2595 - $15.00 US Received June 11, 2003; Revised June 20, 2003
(C) 2003 OSA 30 June 2003 / Vol. 11, No. 13 / OPTICS EXPRESS 1546

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