Orientational dynamics in supercooled glycerol computed from MD simulations: self and cross contributions.

The orientational dynamics of supercooled glycerol is probed using molecular dynamics simulations for temperatures ranging from 323 K to 253 K, through correlation functions of first and second ranks of Legendre polynomials, pertaining respectively to dielectric spectroscopy (DS) and depolarized dynamic light scattering (DDLS). The self, cross, and total correlation functions are compared with relevant experimental data. The computations reveal the low sensitivity of DDLS to cross-correlations, in agreement with what is found in experimental work, and strengthen the idea of directly comparing DS and DDLS data to evaluate the effect of cross-correlations in polar liquids.

Temperature dependence of the Kirkwood correlation factor and linear dielectric constant of simple isotropic polar fluids.

The theory developed in an accompanying paper [Déjardin, Phys. Rev. E 105, 024109 (2022)10.

Kinetic Yvon-Born-Green theory of the linear dielectric constant and complex permittivity of isotropic polar fluids.

The theory of the linear static dielectric constant and linear complex permittivity of isotropic polar fluids is formulated starting from the coupled Langevin equations describing the rototranslational dynamics of long-range interacting molecules with thermal agitation and subjected to external forces and torques. To this aim, adequate reduced densities are introduced and equations governing their dynamics derived. In the equilibrium zero frequency limit, integral expressions for the Kirkwood correlation factor g_{K} are given, transparently showing that the popular method consisting in comparing g_{K} with 1 in order to deduce pair dipolar ordering has no serious theoretical grounding.

Dynamic Kerr effect in a strong uniform AC electric field for interacting polar and polarizable molecules in the mean field approximation.

Analytical formulas for the electric birefringence response of interacting polar and anisotropically polarizable molecules due to a uniform alternating electric field are derived using Berne's forced rotational diffusion model [B. J. Berne, J.

External dc bias-field effects in the nonlinear ac stationary response of dipolar particles in a mean-field potential.

External dc bias-field effects on the nonlinear dielectric relaxation and dynamic Kerr effect of a system of permanent dipoles in a uniaxial mean-field potential are studied via the rotational Brownian motion model postulated in terms of the infinite hierarchy of differential-recurrence equations for the statistical moments f_{n}(t)=〈P_{n}〉(t) (the expectation value of the Legendre polynomials P_{n}). By solving these equations, the nonlinear dielectric and Kerr-effect ac stationary responses are evaluated for arbitrary dc field strength via perturbation theory in the ac field. Simple analytic equations based on the large separation of the time scales of the fast intrawell and slow overbarrier (interwell) relaxation processes are also derived.

Stochastic dynamics of collective modes for Brownian dipoles.

The individual motion of a colloidal particle is described by an overdamped Langevin equation. When rotational degrees of freedom are relevant, these are described by a corresponding Langevin process. Our purpose is to show that the microscopic local density of colloids, in terms of a space and rotation state, also evolves according to a Langevin equation.