Nonlinear photoresponse of disordered elastomers

We model the polarization-dependent photocontractions of polydomain nematic elastomers. Contraction initially arises by light-induced director rotation. At higher light intensity, strain recovers because the local order parameter diminishes. Thus we predict photostrains to be nonmonotonic with light intensity and predict the induction of a negative global order parameter for the system of polydomains. Nonmonotonic strains would give curvature reversal in thick samples. Our model also predicts an elongational strain response to nonpolarized light.     

Thermal diffusion and bending kinetics in nematic elastomer cantilever

Vertically aligned monodomain nematic liquid-crystal elastomers contract when heated. If a temperature gradient is applied across the width of such a cantilever, inhomogeneous strain distribution leads to bending motion. We modelled the kinetics of thermally induced bending in the limit of a long thin strip and the predicted time variation of curvature agreed quantitatively with experimental data from samples with a range of critical indices and nematic-isotropic transition temperatures. We also deduced a value for the thermal diffusion coefficient of the elastomer.     

External field-induced switching in nematic elastomers: A Monte Carlo study

We present a Monte Carlo study of external field-induced switching in nematic elastomers, employing a coarse-grained shearable lattice model. In large enough systems a full-wavelength Fréedericksz effect is observed --as opposed to the half-wavelength effect seen in ordinary nematics-- that clearly reflects in simulated polarized light textures, as well as in deuterium magnetic resonance spectra. The reorientation of mesogenic units is accompanied by pronounced shear deformations.     

Near-field effect in two-atom system

The self-consistent problem is solved for the interaction of two dipole atoms situated at arbitrary distance from one another with the field of quasiresonant light wave. Atoms are considered to be linear Lorenz oscillators. Polarizing fields inside the system include both Coulomb and retarding parts. The solutions obtained are investigated for the case when atoms have the same polarizabilities and interatomic distance is much less than external light wavelength. Formulas for electric fields inside and outside of small object are obtained. It is shown that longitudinal and transverse optical oscillations are possible to exist inside small two-atom object. Dispersion laws of these oscillations depend upon interatomic distance and upon angle between axis of the system and the direction of propagation of external wave. The field outside the small object in wave zone is linearly polarized with the choice of linear polarization of external field. However, the directions of polarization of these waves are different and depend essentially upon frequency. The amplitude of field outside small object in wave zone is shown to depend essentially on the frequency of external field and interatomic distance. The results obtained are treated as near-field effect in the optics of small objects making it possible to investigate the structure of small objects with optical radiation. Received 26 October 1998 and Received in final form 26 January 2000     

Intrinsic optical bistability in Kerr ferroelectric materials

In this paper we investigate the intrinsic optical bistability (IOB) in a ferroelectric (FE) single layer using an alternative analysis. The FE material is considered to have an intensity-dependent refractive index where the third order nonlinear susceptibility χ⁽³⁾ acts like Kerr coefficient. The nonlinear response of the FE medium is modeled using the Landau-Khalatnikov (LK) dynamical equation with the nonlinear anharmonic potential obtained from the Landau-Devonshire free energy expressed in terms of polarization. Within a single frequency approximation, the electromagnetic wave equation is written in terms of the polarization P rather than the electric field E as the dependent variable. With the application of the nonlinear boundary conditions we have derived expressions for both reflectance and transmittance as a function of the electric field incident amplitude, polarization and other material parameters. The formalism proves to be more suitable for FE materials since most of these materials have highly linear and nonlinear coefficients especially when the operating frequency is in the resonance region. The effects of thickness, operating frequency and temperature on BaTiO₃ single film are investigated theoretically. The results presented here agree in principle with the recent experimental observations of intrinsic OB in BaTiO₃ monocrystal and other FE photorefractive materials.     

Deformation of cholesteric elastomers by uniaxial stress along the helix axis

The deformation of cholesteric elastomers by mechanical stress applied parallel to the helix axis is studied by calculation of the free-energy density. The Frank-elasticity contribution is taken into account. A chiral solvent, present at cross-linking time, is in general considered to be replaced after cross-linking by a solvent with different chirality. Two special cases considered are zero and unchanged solvent chirality, the first known as that of imprinted cholesteric elastomers, the latter equivalent to intrinsic cholesteric elastomers with chemically attached chiral groups. Depending on material parameters and imposed strain, the director can show a tilt towards the helix axis up to the maximum tilt, corresponding to a nematic state. In case of intrinsic elastomers with low conformation anisotropy, direct transitions from untilted to nematic states can be induced by straining. The helix structure of the director field is coarsened with an average wave number different to that of the information inscribed in the network at cross-linking time, if this lowers the average free-energy density. Switching between different states can be achieved with electric fields of reasonable values applied parallel to the helix axis. Spectra of the reflection of polarized light are calculated.     

Dielectric properties of side chain liquid crystalline elastomers: influence of crosslinking on side chain dynamics

Dielectric response, from 1 Hz to 10 MHz, of liquid crystalline side chain elastomers has been compared to the one of analogous uncrosslinked materials. Results are discussed in terms of mobility of the mesogens. Two different systems have been investigated: smectic A elastomers allow to determine the influence of crosslinking on the relaxation (i.e. the reorientation of the whole mesogen around the chain), a S _C ^* elastomer shows the drastic influence of the polymer network on the Goldstone mode. Received 12 October 1998     

Impact of spin-zero particle-photon interactions on light polarization in external magnetic fields

If the recent PVLAS results on polarization changes of a linearly polarized laser beam passing through a magnetic field are interpreted by an axion-like particle, it is almost certain that it is not a standard QCD axion. Considering this, we study the general effective interactions of photons with spin-zero particles without restricting the latter to be a pseudo-scalar or a scalar, i.e., a parity eigenstate. At the lowest order in effective field theory, there are two dimension-5 interactions, each of which has previously been treated separately for a pseudo-scalar or a scalar particle. By following the evolution in an external magnetic field of the system of spin-zero particles and photons, we compute the changes in light polarization and the transition probability for two experimental set-ups: one-way propagation and round-trip propagation. While the first may be relevant for astrophysical sources of spin-zero particles, the second applies to laboratory optical experiments like PVLAS. In the one-way propagation, interesting phenomena can occur for special configurations of polarization where, for instance, transition occurs but light polarization does not change. For the round-trip propagation, however, the standard results of polarization changes for a pseudoscalar or a scalar are only modified by a factor that depends on the relative strength of the two interactions.     

Shear modulus of polydomain, mono-domain and non-mesomorphic side-chain elastomers: Influence of the nematic order

We investigate the behavior of the complex shear modulus of a series of elastomers including mono-domain and poly-domain liquid crystal samples, and a non-mesomorphic sample. We find that the dynamics of the glass transition are strongly modified by the nematic order. This result explains why the truly elastic response of liquid crystal elastomers can only be observed in the isotropic phase at very high temperatures and at very low frequencies. Between the elastic regime and the glassy state, the elastomers have a visco-elastic regime, which is characterized by a Rouse-like behavior for mono-domain and poly-domain samples, and by a Zimm-like behavior for the non-mesomorphic sample. We also show that the mono-domain sample exhibits marked anisotropy of the shear-modulus G ^′. This anisotropy, which is observed for the first time, is a function of frequency and is inverted between low and high frequencies, due to relaxation effects of the orientational order. Received 28 January 2000 and Received in final form 16 October 2000     

Renormalization of the two-photon vacuum polarization and the self energy vacuum polarization for a tightly bound electron

The renormalization method of Bogoljubov-Parasiuk-Hepp-Zimmermann (BPHZ) is used in order to derive the renormalized energy shift due to the gauge invariant K?llén-Sabry diagram of the two-photon vacuum polarization (VPVP) as well as the self energy vacuum polarization S(VP)E beyond the Uehling approximation. It is outlined, that no outer renormalization is required for the two-photon vacuum polarization and that only the inner renormalization has to be accomplished. It is shown that the so-called nongauge invariant spurious term is absent for a wide class of vacuum polarization (VP) diagrams if one applies the widely used spherical expansion of bound and free-electron propagator. This simplifies significantly calculations in bound state quantum electrodynamics. As one result of our paper the use of the BPHZ-approach in bound state QED is established. Received 28 September 2001     

Lamb shift in muonic hydrogen—II. Analysis of the discrepancy of theory and experiment

Currently, both the g factor measurement of the muon as well as the Lamb shift 2S–2P measurement in muonic hydrogen are in disagreement with theory. Here, we investigate possible theoretical explanations, including proton structure effects and small modifications of the vacuum polarization potential. In particular, we investigate a conceivable small modification of the spectral function of vacuum polarization in between the electron and muon energy scales due to a virtual millicharged particle and due to an unstable vector boson originating from a hidden sector of an extended standard model. We find that a virtual millicharged particle which could explain the muonic Lamb shift discrepancy alters theoretical predictions for the muon anomalous magnetic moment by many standard deviations and therefore is in conflict with experiment. Also, we find no parameterizations of an unstable virtual vector boson which could simultaneously explain both “muonic” discrepancies without significantly altering theoretical predictions for electronic hydrogen, where theory and experiment currently are in excellent agreement. A process-dependent correction involving electron screening is evaluated to have the right sign and order-of-magnitude to explain the observed effect in muonic hydrogen. Additional experimental evidence from light muonic atoms and ions is needed in order to reach further clarification.     

Effect of misfit strain on the electrocaloric effect of polydomain epitaxial ferroelectric thin films

The effect of misfit strain on the electrocaloric effect in polydomain epitaxial BaTiO 3 thin films at room temperature is investigated using the Ginzburg-Landau-Devonshire thermodynamic theory. Numerical calculations indicate that the misfit strain has a large impact on the ferroelectric polarization states and the electrocaloric effect. Most importantly, the electrocaloric effect in the polydomain ca 1 /ca 2 /ca 1 /ca 2 phase is much larger than that in the monodomain c phase and the other polydomain phases. Consequently, a large electrocaloric effect can be obtained by carefully controlling the misfit strain, which may provide potential applications in refrigeration devices.     

Field-temperature phase diagrams in chiral tilted smectics,evidencing ferroelectric and ferrielectric phases

Usual ferroelectric compounds undergo a paraelectric-to-ferroelectric phase transition when the susceptibility of the electric polarization density changes its sign. The temperature is the only thermodynamic field that governs the phase transition. Chiral tilted smectics may also present an improper ferroelectricity when there is a tilt angle between the average long axis direction and the layer normal. The tilt angle is the order parameter of the phase transition which is governed by the temperature. Although the electric susceptibility remains positive, a polarization proportional to the tilt appears due to their linear coupling allowed by the chiral symmetry. Further complications come in when the chirality increases, as new phases are encountered with the same tilt inside the layers but a distribution of the azimuthal direction which is periodic with a unit cell of two (SmC(A)*, three (SmC(Fi1)*, four (SmC(Fi2)* or more (SmC(alpha)* layers. In most of these phases, the layer normal is a symmetry axis so there is no macroscopic polarization except for the SmC(Fi1)* in which the average long axis is tilted so the phase is ferrielectric. By studying a particular compound with only a SmC(Fi2)* and a SmC(alpha)* phase, we show that we recover the uniformly tilted ferroelectric SmC* when applying an electric field. We are thus led to build field-temperature phase diagrams for this class of compounds by combining different experimental techniques described here.     

Structure and mobility in ferroelectric liquid crystalline elastomers

Time-resolved Fourier transform infrared (FTIR) spectroscopy with polarized light was employed to study the structure and mobility of a homologous series of ferroelectric liquid crystalline polymers (FLCPs) and ferroelectric liquid crystalline elastomers (FLCEs) in response to an external electric field. The chemical composition of the samples, besides the cross-linking units, is similar. For the elastomers, two different cross-linking architectures are realized: “intralayer” cross-linking leads to the formation of two-dimensional networks, whereas “interlayer” cross-linking forms three-dimensional networks. Due to its specificity, FTIR spectroscopy enables analysis of the reorientational dynamics for the different molecular moieties in detail, thus revealing information about reorientation times, angular excursion, and the phase relationship in the rearrangement of the various molecular groups. In comparison to the un-cross-linked FLCP, both elastomeric samples exhibited smaller reorientation angles and an increase of the reorientation times. In the case of the interlayer cross-linked FLCE, an elastic memory effect was observed: For the reversal from negative to positive field polarity, the reorientation times were longer than for those in the opposite direction. For the intralayer cross-linked sample, it was shown that the backbone molecules reorient slower than the other molecular units (“locomotive effect”). For the un-cross-linked FLCP and the two FLCE samples, different coupling mechanisms between the network and the mesogenic parts are derived from the measurements.     

The elastic anisotropy of nematic elastomers

We examine the robustness of order in nematic elastomers under mechanical strains imposed along and perpendicularly to the director when director rotation is prohibited. In contrast to electric and magnetic fields applied to conventional nematics, mechanical fields are shown theoretically and experimentally to greatly affect the degree of nematic order and related quantities. Unlike in liquid nematics, one can impose fields perpendicular to the director, thereby inducing biaxial order which should be susceptible to experimental detection. Nematic elastomers with unchanging director and degree of order should theoretically have the same elastic moduli for longitudinal and transverse extensions. This is violated when nematic order is permitted to relax in response to strains. Near the transition we predict the longitudinal modulus to be smaller than the transverse modulus; at lower temperatures the converse is true, with a crossover a few degrees below the transition. The differences are ascribed to the different temperature dependence of the stiffness of uniaxial and biaxial order. We synthesised side chain single-crystal nematic polymer networks, performed DSC, X-ray, birefringence, and thermo-mechanical characterisations, and then obtained linear moduli from stress-strain measurements. Received 29 September 2000     

Magnetic field effects on coherent backscattering of light

We have studied the influence of magneto-optical Faraday rotation on coherent backscattering of light experimentally, theoretically and by computer simulations of Monte-Carlo type. The consistency of these three approaches reveals new aspects of the propagation of vector waves in turbid media with and without Faraday rotation. Experimentally, we have demonstrated that the Faraday rotation may almost completely destroy the reciprocity of light paths. However, as shown by the simulations, the cone of coherent backscattering may not only be destroyed but also shifted off the exact backscattering direction, parallel to the magnetic field, as long as the amount of circular polarization is not completely destroyed by the multiple scattering. The relationship between coherent backscattering, depolarization and Faraday rotation are explained by a simple path model of vector waves. This leads to a new characteristic correlation length required to properly describe the influence of Faraday rotation on multiple light scattering. Received 28 January 2000     

Light scattering by aggregates of varying porosity and the opposition phenomena observed in the low-albedo particulate media

The rule that the opposition phenomena in brightness and linear polarization observed in many regolith surfaces usually accompany each other is violated in the cases of very dark asteroids and particulate samples: practically no nonlinear surge of brightness to opposition is observed while the branch of negative polarization at small phase angles exists. To explain this fact, we model the light scattering by particulate media with ensembles of spherical particles (with size comparable to the wavelength) of varying packing density and refractive index. The superposition T-matrix method is used. The increase in the absorption and/or packing density diminishes the amplitude of the brightness opposition peak, and its profile becomes wider. The influence on the branch of negative polarization is more complex and depends on the relation between the size parameters of the constituents, the refractive index, and the porosity. However, the feature common to all considered cases is that the negative branch changes its shape and the polarization minimum moves to the inversion point. This behavior radically differs from that observed in nonabsorbing ensembles of particles and reflects the fact that the efficiency of the coherent backscattering, which mainly determines these characteristics in nonabsorbing ensembles (to the packing density of about 30%), decreases. Moreover, since the angular profiles are not simply damped, but the polarization minimum changes its angular position, we may conclude that the near-field interaction of the constituents becomes important: the shielding of particles by each other eliminates many constituents from the scattering and the near-field effects promote the negative polarization and smooth the backscattering brightness surge. Due to this, when the packing density exceeds 10-20%, the opposition phenomena in absorbing ensembles are caused not only by the coherent backscattering, and situations, when the opposition brightness surge is practically suppressed, but the negative branch of polarization still survives, are possible. This may explain the fact that the dark regolith surfaces show no brightness opposition effect, but produce the branch of negative polarization with the minimum shifted from opposition.     

Elastic stabilization of a single-domain ferroelectric state in nanoscale capacitors and tunnel junctions

Taking into account the electrostrictive coupling between inhomogeneous polarization fluctuations and lattice strains in ferroelectric films, we show that, in heterostructures involving strained epitaxial films and metal electrodes, the single-domain state may remain stable against the transformation into a polydomain state down to the nanometer scale. This result indicates that the ferroelectric states with opposite remanent polarizations can be stabilized even in nanoscale capacitors and tunnel junctions, which opens the possibility of their application for memory storage.