Three-dimensional model for light-induced chaotic rotations in liquid crystals under spin and orbital angular momentum transfer processes Etienne Brasselet Centre de Physique Moléculaire Optique et Hertzienne, Université Bordeaux 1, CNRS, 351 Cours de la Libération, 33405 Talence Cedex, France Bruno Piccirillo * and Enrico Santamato * Dipartimento di Scienze Fisiche, Università di Napoli “Federico II,” via Cintia, 80126 Napoli, Italy Received 9 April 2008; revised manuscript received 22 August 2008; published 3 September 2008 Liquid crystals interacting with light represent a unique class of soft-matter systems that exhibit various generic nonlinear behaviors, including chaotic rotational dynamics. Despite several experimental observations, complex nematic liquid crystal director rotations in presence of spin and orbital angular momentum transfer processes were left unexplained. We present a self-consistent three-dimensional model able to describe the previous experimental observations, accounting for the dependence on the incident beam intensity, polariza- tion, finite size and shape. More generally, our model is able to describe quantitatively the dynamics of, and beyond, the optical Fréedericksz transition under realistic experimental conditions almost three decades after its experimental discovery. DOI: 10.1103/PhysRevE.78.031703 PACS numbers: 42.70.Df, 05.45.a, 42.65.Sf I. INTRODUCTION Dynamical systems that are described by a set of coupled first-order autonomous differential equations are usually characterized in terms of rotational motions, which is a ge- neric feature of many processes in physics, chemistry, or biology. This is especially the case when such nonlinear sys- tems exhibit chaotic dynamics. Then, the system trajectory can be considered as going through an infinite number of rotationlike motions characterized by a suitable definition of the phase 1, which is of special interest in the framework of phase synchronization 2,3. Due to the modeling difficulties and/or achievable computational handling of real dynamical systems exhibiting chaotic rotations, their description is usu- ally reduced to standard nonlinear models, such as the Lor- entz 4or Rössler 5systems. Exact modeling of real sys- tems exhibiting chaotic rotations is much less widespread. Quite recently, chaotic rotations generated by a light field in nematic liquid crystals NLCshave been reported 6,7. In these experiments, the light was circularly polarized and sent at normal incidence onto a homeotropically aligned nematic film. In Ref. 6an elliptically shaped light beam was used, while in Ref. 7the incident beam shape was cylindrically symmetric. In both cases the observations were left unexplained despite some attempt to describe the NLC continuum medium as a discrete set of coupled nonlinear rotators driven by light, which led to a generic Kuramoto model 7,8. The major difficulty in modeling this kind of experiment is that the dynamics of the NLC director is strongly affected by the finite size and shape of the incoming light beam so that the plane-wave approach, where all the fields depend on one coordinate only, is inapplicable. All the three space coordinates and time must be retained. A previ- ous attempt to model complex rotational dynamics account- ing for the finite size of the light beam, but neglecting higher order reorientational modes and nonadiabatic propagation of light in the distorted liquid crystal, failed to retrieve experi- mental observations 9and to give the expected sequence of bifurcations in the plane-wave limit 10. Therefore a suit- able model is still lacking. In this paper, we present the derivation of a set of coupled ordinary differential equations ODEsfor the motion of the local averaged molecular orientation defined by a unit vector n, called director, from the fundamental equations for LCs and electromagnetic waves. The dependence of the liquid crystal dynamics on the incident beam intensity, polarization, finite size and shape are obtained, which naturally accounts for spin angular momentum SAMand orbital angular mo- mentum OAMtransfer processes between light and matter. This is another interesting yet intriguing feature of this class of experiments where both the photon SAM and OAM come into play and couple with the NLC anisotropic fluid. The model capabilities are illustrated in the case where SAM and OAM transfer processes are simultaneously present and a successful description of the complex sequence of director rotations observed in Ref. 6is obtained. More generally, our model is able to describe quantitatively the dynamics of, and beyond, the optical Fréedericksz transition OFTunder realistic experimental conditions almost three decades after its experimental discovery. From a general point of view, the angular momentum balance in NLCs can be written in the form 11r v˙ = div L ˆ + w and In n˙ = div S ˆ - w where an upper dot stands for partial time derivative, , I, and v are, respectively, the density, inertial momentum, and velocity field of the fluid, L ˆ and S ˆ are the orbital and spin total matter + lightangular momentum flux tensors and, finally, w is the internal torque density due to the anisotropy of the elastic constants of the material. Note that L ˆ and S ˆ can be uniquely split into a mat- * Also at Consorzio Nazionale Interuniversitario per la Struttura della Materia CNISM, Sezione di Napoli, Italy. PHYSICAL REVIEW E 78, 031703 2008 1539-3755/2008/783/0317034©2008 The American Physical Society 031703-1