Chaotic orientational behavior of a nematic liquid crystal subjected to a steady shear flow Go ¨ tz Riena ¨ cker, 1 Martin Kro ¨ ger, 1,2,3 and Siegfried Hess 1,2, * 1 Institut fu ¨r Theoretische Physik, Technische Universita ¨t Berlin, Fakulta ¨t II, Hardenbergstrasse 36, D-10623 Berlin, Germany 2 Institute for Theoretical Physics, University of California Santa Barbara, California 93106-4030 3 Polymer Physics, Material Sciences, ETH Zu ¨rich, CH-8092 Zu ¨rich, Switzerland Received 12 April 2002; published 29 October 2002 Based on a relaxation equation for the second rank alignment tensor characterizing the molecular orientation in liquid crystals, we report on a number of symmetry-breaking transient states and simple periodic and irregular, chaotic out-of-plane orbits under steady flow. Both an intermittency route and a period-doubling route to chaos are found for this five-dimensional dynamic system in a certain range of parameters shear rate, tumbling parameter at isotropic-nematic coexistence, and reduced temperature. A link to the corresponding rheochaotic states, present in complex fluids, is made. DOI: 10.1103/PhysRevE.66.040702 PACS numbers: 61.30.Gd, 61.30.Cz A nematic liquid crystal LCsubjected to a steady shear flow can either go to a stationary flow aligned state or re- spond with a time dependent molecular orientation depend- ing on the magnitude of the tumbling parameter 1–3. Both flow alignment and time dependent orientation, fre- quently referred to as ‘‘tumbling’’ behavior are observed in thermotropic, lyotropic, and polymeric LC’s 4In the tum- bling regime, however, the dynamics are more complex than the Ericksen-Leslie director theory can describe. The second alignment tensor is needed to characterize the molecular ori- entation. Detailed theoretical studies 5, based on the solu- tions of a generalized Fokker-Planck equation 6,7, revealed that in addition to the tumbling motion, wagging and kayak- ing types of motions, as well as combinations thereof occur. Recently, also chaotic motions were inferred from a moment approximation to the Fokker-Planck equation leading to a 65-dimensional dynamical system 8for uniaxial particles. While we consider uniaxial particles in this note, one may notice that for long triaxial ellipsoidal non-Brownian par- ticles chaotic behavior had also been predicted in Ref. 9. Here we report on our discovery 10that a closed nonlinear relaxation equation for the alignment tensor, being equiva- lent to a five-dimensional dynamical system and strongly related to the full Fokker-Planck equation, leads to a chaotic behavior for particular values of the tumbling parameter and in certain ranges of the shear rate. Both the frequency dou- bling route, as in Ref. 8, and the intermittency route to chaos are found for the simpler system. Due to the coupling between the alignment and stress tensor a relationship is given below, one may attempt to model the time dependent and also chaotic rheological behavior seen in the recent ex- periments on micellar materials 11, dense lamellar phases 12, and dense suspensions 13—and discussed in more general theoretical considerations on rheochaos 14—by variants of the dynamic system to be characterized in this paper. An illustrative example is given in Ref. 15, where equations similar to the one to be discussed below were used to describe the effect of nonchaoticshear thickening. The quantity , specified below, is the derivative of a Landau-de Gennes free energy with respect to the align- ment tensor, it contains terms of first, second, and third order in a. The equation stated here was first derived within the framework of irreversible thermodynamics 16, where the relaxation time coefficients a 0 and ap are considered as phenomenological parameters. It had been shown in Refs. 6,17that a and ap are proportional to the Ericksen-Leslie viscosity coefficients 1 and 2 , respectively. The basic equation used here can also be derived, within certain ap- proximations, from a Fokker-Planck equation for the orien- tational distributions function that contains a torque associ- ated with the molecular field proportional to a 6,7,18. Then a and the ratio - ap / a can be related to the rotational diffusion coefficent and to a nonsphericity parameter associ- ated with the shape of a particle. Equation 1is applicable to both the isotropic and the nematic phases. Limiting cases that follow from this equation are the pretransitional behav- ior of the flow birefringence 19,20in the isotropic phase ( a) is approximated by its term linear in a] and the Ericksen-Leslie theory in the uniaxial nematic phase. In the latter case, the Ericksen-Leslie viscosity coefficients 1 and 2 are proportional to a and ap , respectively, and =- 2 / 1 . Equation 1has been applied to the study of the influence of a shear flow on the isotropic-nematic phase transition 19,20, and discussed intensively in recent, in par- ticular, experimental works, see e.g., Refs. 3,4and refer- ences cited therein. *Corresponding author. RAPID COMMUNICATIONS PHYSICAL REVIEW E 66, 040702R2002 1063-651X/2002/664/0407024/$20.00 ©2002 The American Physical Society 66 040702-1