ABSTRACT
We study theoretically the kinetics of noninteracting photoswitchable guest molecules (model azo-dye) dispersed at low concentration in host (model polymer matrix) in the all-optical poling process close to the glass transition temperature Tg. We modify kinetic Monte Carlo model used in our previous studies of nonlinear optical processes in host-guest systems. The polymer matrix is simulated using the bond-fluctuation model. The kinetics of multiple trans-cis-trans cycles is formulated in terms of transition probabilities which depend on local free volume in the matrix and its dynamics. Close to Tg, the buildup of polar order, monitored in terms of angular probability density functions, follows a power-law in time while the evolution of the nonlinear susceptibilities related to second harmonic generation effect follows the stretched-exponential law. This complex dynamics of guest molecules implies the presence of dynamic heterogeneities of the matrix in space and time which spread the complexity from the matrix to the otherwise simple dynamics of noninteracting guest molecules. A qualitative physical picture of mosaic-like states-intertwined areas of free- and hindered angular motion of guest molecules-is proposed and the role of related short and longer scales in space for the promotion of complex dynamics of guest molecules is discussed. A brief comparison of the theory to available experimental data is given.
ABSTRACT
We show that nanosphere dispersed liquid crystal (NDLC) metamaterial can be characterized in near IR spectral region as an indefinite medium whose real parts of effective ordinary and extraordinary permittivities are opposite in signs. Based on this fact we designed an electro-optic effect: an external electric-field-driven switch between normal refraction, negative refraction, and reflection of TM incident electromagnetic wave from the boundary vacuum/NDLC. A detailed analysis of its functionality is given based on effective medium theory combined with a study of negative refraction in anisotropic metamaterials and finite elements simulations.
ABSTRACT
We present a design of an infrared cylindrical cloak using nanosphere dispersed nematic liquid crystal (NLC) metamaterial following the approach of Smith's group [Science 314, 977 (2006)]. Cloaking conditions require spatial distribution of liquid crystal birefringence with constant extraordinary index of refraction and radially dependent ordinary index of refraction. An approximate analytical formula for the latter is derived. Finite element (FE) simulations confirm the cloaking effect. Owing to the tunable birefringence of the liquid crystal component, such cloaking material offers the interesting possibilities of real-time control of invisibility. The possibility of experimental realization is briefly discussed.
ABSTRACT
Analysis of the metrical and topological features of the local structure in a freezing two-dimensional Lennard-Jones system found that in a narrow strip [Formula: see text] of thermodynamic states close to the melting line, the liquid becomes a complex liquid characterized by a super-Arrhenius increase of relaxation times, stretched-exponential decay of correlations in time, and a power-law distribution of waiting times for changes in the local order. In [Formula: see text], the structure of the liquid and its dynamics are spatially heterogeneous; the sizes of ordered clusters are power-law distributed. Those features are governed by local structure evolution between solid-like and liquid-like (disordered) patterns. The liquid inside the strip [Formula: see text] gives a unique opportunity to study how heterogeneous structure, dynamics and complexity are intertwined with each other on a microscopic level.
ABSTRACT
Conditions towards effective electric field poling in two dimensions (2D) of octupolar molecules which can be achieved are being addressed, based on a lattice model which mimics the basic features of poling. The model is studied using the complementary approaches of analytical methods in statistical mechanics and Monte Carlo simulations. The poling field is imparted by a system of adequately shaped cylindrical electrodes. A topologically rich structure of local and global inhomogeneous octupolar order, including octupolar vortices, is present in the system. The poling criteria are shown to vary strongly throughout the cell: in close proximity to the contact points of neighboring electrodes, a high quality local octupolar order appears at temperature T ≃ 0.1 K while octupoling in the center of the cell requires temperatures as low as 10(-4) K. The highly demanding octupoling criteria are ascribed to symmetry-driven effects which decrease the quality of the octupolar phase even in the ground state, as well as to thermal fluctuations and numerical factors at above zero temperatures. Based on our results and using plausible conjectures related to the generalization of the model, it is argued that a weak global octupolar order can be reached at liquid Helium temperatures (a few Kelvins), based on current advances in optical techniques and nanotechnologies.
ABSTRACT
Experimental studies of second harmonic generation (SHG) from electric-field poled PMMA - DR1 system show occurrence of a maximum in diagonal and off diagonal tensor components χ(2)(-2ω;ω,ω) at 15 mol % concentration and a rapid decrease above, with a stabilization. The origin of the observed concentration dependence is studied using the Monte Carlo (MC) modeling. We find that presence of maximum is conditioned by the pre-poling history of the sample, when entanglement of linear dipolar structures takes place. Length of the pre-poling interval is an important kinetic parameter which differentiates between various nonexponential kinetics of build-up of polar phase responsible for strong/weak SHG susceptibility.
Subject(s)
Optics and Photonics , Polymers/chemistry , Algorithms , Computer Simulation , Equipment Design , Kinetics , Models, Statistical , Monte Carlo Method , Static ElectricityABSTRACT
Thermodynamic properties of one-dimensional lattice models exhibiting entropy-driven phase transformations are discussed in quantum and classical regimes. Motivated by the multistability of compounds exhibiting photoinduced phase transitions, we consider systems with asymmetric, double, and triple well on-site potential. One finds that among a variety of regimes, quantum versus classical, discrete versus continuum, a key feature is asymmetry distinguished as a "shift" type and "shape" type in limiting cases. The behavior of the specific heat indicates one phase transformation in a "shift" type and a sequence of two phase transformations in "shape"-type systems. Future analysis in higher dimensions should allow us to identify which of these entropy-driven phase transformations would evolve into phase transitions of the first order.
