Jl. Dejardin, DERIVATION OF THE INERTIAL AC RESPONSE FOR THE KERR-EFFECT RELAXATIONFROM THE LANGEVIN EQUATION IN 3-DIMENSIONAL SPACE, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics, 52(5), 1995, pp. 4646-4660
The Kerr-effect response of an assembly of noninteracting dipolar and
anisotropically polarizable spherical molecules is calculated from the
Euler-Langevin stochastic differential equations. The solution is obt
ained using combinations of the Legendre polynomials and the associate
d Legendre functions as angular variables, together with the Hermite p
olynomials as angular velocity variables. The molecules are compelled
to rotate in three-dimensional space and are acted on by a de bias fie
ld, superimposed on which is an ac electric field in the same directio
n. When the response is restricted to second order in the applied fiel
d, the coupling of the fields gives rise to two distinct nonlinear har
monic components of the complex birefringence, varying at the fundamen
tal (omega) and the second harmonic (2 omega) of the ac field. Small i
nertial effects are considered, and their importance is illustrated in
numerous dispersion and Cole-Cole plots for various values of the par
ameter P measuring the balance between induced and permanent dipole mo
ments and a fixed value of the inertial parameter gamma. Special empha
sis is placed on the phase angles between in-phase and out-of-phase ha
rmonic terms whose values may be multiplied by a factor of 2 at high f
requencies, compared to those obtained in the rotational diffusion lim
it (Debye's model), thus allowing possible practical applications. The
transition matrix that is appropriate to dielectric relaxation is als
o given, since a knowledge of it in the nonlinear case, unlike the aft
ereffect solution, is needed for the description of the dynamic Kerr e
ffect.