Calculation of the dispersion of the third-order optical nonlinearity in C60 films

Using wave functions determined from ground-state local-density calculations, we have calculated the wave-dispersed free response of the optical nonlinear polarizability ⁽³⁾(–3;,,), for the C₆₀ molecule and ⁽³⁾(–3;,,) i.e. Third-Harmonic Generation (THG) for films using a sum-over-states approach. The influence of screening was determined by applying an external static electric field in separate selfconsistent calculations to evaluate induced dipole moments which was used to determine the static linear and nonlinear polarizabilities. The polarizabilities calculated in the static limit were used to determine an effective screening parameter which was, in turn, used together with an RPA approach to calculate screened wave-dispersed, third-order nonlinear optical properties such as ⁽³⁾(–3;,,) and ⁽³⁾(–3;,,). Comparing evaluated polarizabilities with experimental values we found that the non-resonant free polarizability compares well in absolute magnitude with experimental results. Inclusion of screening results in a polarizability about two orders of magnitude below the experimental values.Paper presented at the 129th WE-Heraeus-Seminar on Surface Studies by Nonlinear Laser Spectroscopies, Kassel, Germany, May 30 to June 1, 1994     

An upper bound on the free energy for classical systems with Coulomb interactions in a varying external field

The thermodynamic limit is taken using a sequence of regions all the same shape as a given region of volume ||, with a specified distribution of normal field component on . We show that with magnetostatic interactions the limiting free energy density is bounded above by jhen where (,B) is the free energy density for a system of density in a uniform external fieldB and the inf is taken over all divergence-free fieldsB with given normal component on and all densities (x) compatible with particle number constraints of the form where _i is a sub-region of . A physical argument suggests that this upper bound is the true thermodynamic limit, and that it takes account demagnetization effects. Electrostatic interactions can be treated similarly.     

Static and Vibrational Properties of Transition Metals

A model pseudopotential depending on an effective core radius but otherwise parameter free is proposed to study the equation of state by incorporating the s-d hybridization effects. Very recently proposed screening function due to Sarkar et al has been used to obtain the screened form factor. The equations of state for Cu, Ta, Mo, W and Pt have been studied up to the pressure of 1000 GPa. The vibrational properties such as phonon dispersion curves (in q and r space), phonon density of states, mode Grüneisen parameters, maximum frequency _max, mean frequency , ^21/2 = (/ ^-1)^1/2 and fundamental frequency ² and static properties such as dynamical elastic constants of rhodium and iridium are also calculated. The theoretical results are compared with experimental findings wherever possible. A good agreement between theoretical investigations and experimental findings has confirmed our formulation.     

Normal mode configuration in an inorganic medium containing defects

The vibrational structure in an inorganic medium containing defects is analyzed as a function of the frequency of the applied field. Since the dispersion relations for the medium are nonlinear, the configuration of the normal modes depends differently upon and . It is shown that exponential damping of the optic branches is observed for <₀, and that the structure of these modes changes significantly over the range 0<<₀, so that only in the neighborhood of ₀ does it correspond to long wavelength vibrations with configurations of stress deviator waves.Institute for the Physics of Strength and Materials Science, Russian Academy of Sciences, Siberian Division. Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 10, pp. 87–90, October, 1994.     

Four-wave mixing in alkali halide crystals and aqueous solutions

Noncollinear phase-matched nonresonant four-photon frequency mixing _p+ _p– _{L s} in crystals and aqueous solutions of LiCl, CsCl, KF, and KI is studied. The concentration of the aqueous solutions is varied between 0.5 mol/l and saturation. Picosecond laser pulses of a mode-locked Nd-glass laser are applied as pump pulses. The energy conversion of laser light at frequency _L to frequency _S is measured and the nonlinear susceptibilities ⁽³⁾ are calculated. The dependence of the hyperpolarizabilities on concentration is analysed and gives information on the solute-solvent interaction.     

Enhancement of activated decay of metastable states by resonant pumping

We consider the effect of a high-frequency pumping cost on the escape rate of a classical underdamped Brownian particle out of a deep potential well. The energy dependence of the oscillation frequency(E) is assumed to be weak on the scale of thermal energy,_E(0)T(0)T/V₀ (0)[_E(0) is the derivative of(E) atE= 0,V ₀ is the barrier height,V ₀ T]. The quadratic-in- contribution to the decay rate is calculated in two different regimes: (1) for the case of resonance of the pumping frequency with the nth harmonic of the internal motion at an energye, when = n(e); (2) for a rollout region of the basic resonance near the bottom of the potential well, when ¦-(0)¦ and is the damping coefficient. In the latter case the absorption spectrum and the enhancement of the decay rate are calculated as functions of two reduced parameters, the anharmonicity of the potential,v _E (0)T/, and the resonance mismatch, [ —(0)]/. It is shown that the effect of the pumping increases with diminishing ¦v¦ and at small v is proportional tov ^–1. In this regime, the dependence on is stepwise: the pumping contribution is large for v > 0 and small for v < 0. In the frame of our theory, the decay rate is invariant against the simultaneous alternation of the signs of andv. The spectrum of the energy absorption has the standard Lorentzian shape in the absence of anharmonicity,v=0, and with increasing of ¦v¦ shifts and widens retaining its bell-shape form.     

Cubic nonlinear tensor of a ferromagnet

The nonlinear properties of a ferromagnet are studied. Many-time retarded Green's functions are used to obtain an expression for the cubic nonlinearity tensor with allowance for spatial dispersion of a uniaxial ferromagnet. The components due to the dipole-dipole interaction of the spins and also due to the anisotropy energy are found. A comparative analysis is made of the different components of the cubic nonlinearity tensor in both the nonresonance case and for various resonances, in particular when ₀, 3 2w₀, 2 ₀, 3 ₀ for the case in tripling of the frequency. Here, is the frequency of the incident wave and ₀ is the frequency of uniform precession. It is shown that in the non-resonance case the largest components are those that are nonvanishing when no allowance is made for spatial dispersion; in the resonance cases the largest components are those due to the dipole-dipole interaction of the ferromagnetism spins.Translated from Izvestiya VUZ. Fizika, No. 12, pp. 53–58, December, 1973.     

The modular group and super-KMS functionals

Every normal, faithful, self-adjoint functional on a von Neumann algebraA canonically determines a one-parameter-weakly continuous *-automorphism group (the analog of the modular group) and a canonical ₂ grading onA, commuting with . We show that the functional satisfies the weak super-KMS property with respect to and Furthermore, we prove that and are the unique pair of a-weakly continuous one-parameter *-automorphism group and a grading of the algebra, commuting with each other, with respect to which is weakly super-KMS. The above results thus provide a complete extension of the theory of Tomita and Takesaki to the nonpositive case.Supported in part by the National Science Foundation under Grant DMS-8922002.     

Structure factor of substitutional sequences

We study the structure factor for a large class of sequences of two elementsa andb such that longer sequences are generated from shorter ones by a simple substitution rulea ₁(a, b) andb ₂(a, b), where the's are some sequences ofa's andb's. Such sequences include periodic and quasiperiodic systems (e.g., the Fibonacci sequence), as well as systems such as the Thue-Morse sequence, which are neither. We show that there are values of the frequency at which the structure factors of these sequences have peaks that scale withL, the size of the system likeL ⁽⁾. For a given sequence a simple one- or two-dimensional dynamical iterative map of the variable can easily be abstracted from the substitution algorithm. The basin of attraction of a given fixed point or limit cycle of this map is a set of values of at which there are peaks of the structure factor all of which share the same value of. Furthermore, only those values of which are in the basin of attraction of the origin can have()=2. All other peaks will grow less rapidly withL. We show how to construct many sequences which, like the Thue-Morse sequence, have noL ² peaks. Other qualitative features of the structure factors are presented. Our approach unifies the treatment of a large class of apparently very diverse systems. Implications for the band structure of these systems as well as for the analysis of sequences with more than two elements are discussed.     

Directed paths on percolation clusters

We consider a variant of the problem of directed polymers on a disordered lattice, in which the disorder is geometrical in nature. In particular, we allow a finite probability for each bond to be absent from the lattice. We show, through the use of numerical and scaling arguments on both Euclidean and hierarchical lattices, that the model has two distinct scaling behaviors, depending upon whether the concentration of bonds on the lattice is at or above the directed percolation threshold. We are particularly interested in the exponents and, defined by ft and xt , describing the free-energy and transverse fluctuations, respectively. Above the percolation threshold, the scaling behavior is governed by the standard random energy exponents (=1/3 and =2/3 in 1+1 dimensions). At the percolation threshold, we predict (and verify numerically in 1+1 dimensions) the exponents=1/2 and =v/v, where v and v are the directed percolation exponents. In addition, we predict the absence of a free phase in any dimension at the percolation threshold.     

Some exact models for nonspherical collapse.I

Evolution of incoherent matter distributions with cylindrical, pseudoplanar, and toroidal symmetries is considered. The system is described in terms of the scale factora (R, T) and the anisotropy factor (R, T) of the (x², x³ surfaces. A number of exact solutions is obtained under the assumptions=(a), =(R), and=(T) and their physical properties are breifly discussed. In particular, the solution with=(T) is noncollapsing and describes a matter distribution with unchanging density.     

The inverse backscattering problem in three dimensions

This article is a study of the mapping from a potentialq(x) onR ³ to the backscattering amplitude associated with the Hamiltonian –+q(x). The backscattering amplitude is the restriction of the scattering amplitudea(, , k), (, , k)S ²×S ²×₊, toa(,–, k). We show that in suitable (complex) Banach spaces the map fromq(x) toa(x/|x|, –x/|x|, |x|) is usually a local diffeomorphism. Hence in contrast to the overdetermined problem of recoveringq from the full scattering amplitude the inverse backscattering problem is well posed.     

Two repulsive lines on disordered lattices

We investigate the ground-state properties of two lines with on-site repulsion on disordered Cayley tree and (Berker) hierarchical lattices, in connection with the question of multiple pure states for the corresponding one-line problem. Exact recursion relations for the distribution of ground-state energies and of the overlaps are derived. Based on a numerical study of the recursion relations, we establish that the total interaction energy on average is asymptotically proportional to the width of the ground-state energy fluctuation of a single line for both weak and strong (i.e., hard-core) repulsion. When the lengtht of the lines is finite, there is a finite probability of ordert ^–a for (nearly) degenerate, nonoverlapping one-line ground-state configurations, in which case the interaction energy vanishes. We show thata= (t ) on hierarchical lattices. Monte Carlo transfer matrix calculation on a (1+1)-dimensional model yields the same scaling for the interaction energy but ana different from =1/3. Finitelength scalings of the distribution of the interaction energy and of the overlap are also discussed.     

Classical “freezing” of plane rotations: A proof of the Boltzmann-Jeans conjecture

Using simple known methods and results of classical perturbation theory, especially those due to Nekhoroshev and Neishtadt, we study the energy exchanges between the rotational and the translational degrees of freedom in a particular model representing the planar motion of a rigid body in a bounded analytic potential. We prove that, if the angular velocity is initially large, then the energy exchanges are small,O( ^–1), for times growing exponentially with, |t|exp. We also deduce that in a scattering process from a (smooth) potential barrier, the overall change in the rotational energy of the incoming body is exponentially small in, exp(–. The results are interpreted in the light of an old conjecture by Boltzmann and Jeans on the existence of very large time scales for equilibrium in statistical systems containing high-frequency degrees of freedom (purely classical freezing of the high-frequency degrees of freedom); the rotating object is, in this interpretation, a (classical) molecule, which moves in an external field, or collides with the wall of a container. Two different limits of large are considered, namely the limit of large rotational energy, and (as is interesting for the molecular interpretation) the limit of point mass, at finite rotational energy.     

Explaining μ+ spin-lattice relaxation in MnF2, belowT N,by scattering function

A relation between the spin-lattice relaxation rate (1/T ₁) of positive muons and the scattering functionS ^T (q,) is derived for the antiferromagnet MnF₂. We find good agreement between previousSR measurements of 1/T ₁ and our calculation using neutron scattering measurements ofS ^T (q,).     

Homogeneous and hypersurface-homogeneous shear-free perfect fluids in general relativity

Shear-free, general-relativistic perfect fluids are investigated in the case where they are either homogeneous or hypersurface-homogeneous (and, in particular, spatially homogeneous). It is assumed that the energy density and the presurep of the fluid are related by a barotropic equation of statep = p(), where +p 0. Under such circumstances, it follows that either the fluid's volume expansion rate or the fluid's vorticity (i.e., rotation) must vanish. In the homogeneous case, this leads to only two possibilities: either = = 0 (the Einstein static solution), or 0, = 0 (the Gödel solution). In the hypersurface-homogeneous case, the situation is more complicated: either = 0, 0 (as exemplified,inter alia, by the Friedmann-Robertson-Walker models), or 0, = 0 (which pertains, for example, in general stationary cylindrically symmetric fluids with rigid rotation, or = = 0 (as occurs for static spherically symmetric solutions). Each possibility is further subdivided in an invariant way, and related to the studies of other authors, thereby unifying and extending these earlier works.     

Two-photon resonance degenerate four-wave mixing in a three-level polar molecule (model calculations)

The third-order non-linear susceptibility, ⁽³⁾(; , , –), describing the phase conjugation by degenerate four-wave mixing (DFWM) is calculated for a three-level polar system under a two-photon resonance (TPR) condition. The part of the susceptibility expressed only by the transitional dipole moments and the part resulting from the permanent dipole moments are distinguished. The spectra of ⁽³⁾(; , , –), as well as the DFWM power-reflection and power-transmission spectra near to the TPR, are modelled for polar molecules. The effect of enhanced reflectivity of TPR-DFWM is obtained numerically.     

Quantum particle-like configurations of the electromagnetic field

We construct explicitly three-dimensional localized solutions of the free Maxwell's equations with a phase expi(k x - t) which move like relativistic particles. The total field energyE of the moving lump is proportional to the frequency and its momentumP is proportional to the wave vectork, withE ² =P ² +M ². Further, if the angular momentum is different from zero, thenE =. These solutions thus model the wave-particle duality of quantum particles.     

The Schrödinger equation and canonical perturbation theory

LetT ₀(, )+V be the Schrödinger operator corresponding to the classical HamiltonianH ₀()+V, whereH ₀() is thed-dimensional harmonic oscillator with non-resonant frequencies =(₁, ... , _d ) and the potentialV(q ₁, ... ,q _d) is an entire function of order (d+1)^–1. We prove that the algorithm of classical, canonical perturbation theory can be applied to the Schrödinger equation in the Bargmann representation. As a consequence, each term of the Rayleigh-Schrödinger series near any eigenvalue ofT ₀(, ) admits a convergent expansion in powers of of initial point the corresponding term of the classical Birkhoff expansion. Moreover ifV is an even polynomial, the above result and the KAM theorem show that all eigenvalues _n (, ) ofT ₀+V such thatn coincides with a KAM torus are given, up to order , by a quantization formula which reduces to the Bohr-Sommerfeld one up to first order terms in .     

Generating fields from data onH − ⋃H +andH − ⋃I +

There are series solutions for characteristic boundary value problems for fields on black hole backgrounds that converge when the data are given on =^{– +}, or on =^{– +}, but may not converge when the data are given on ^{– –}, or on ^{+ +}. We specialize to oscillatory data of frequency and calculate approximate reflection and transmission coefficientsR() andT(), using a field generated by data on =^{– +}, and again, using a field generated by data on ^{– –}. The first calculation gives qualitatively good results at all frequencies at each order of approximation, and quantitatively better results at higher orders of approximation; the second calculation, using the series which may not converge, gives bad results except at very high frequencies. Thus for the physically unnatural case of a field that vanishes on ^– and goes toe ^iv on ⁺ we have a series that is convergent, and uniformly so with respect to frequency, while for the natural case of a field that vanishes on ^– and goes toe ^iv on ^– we are limited to high frequencies. It is argued that a frequency-dependent renormalization of a series of the first type provides an approximation scheme that is convergent, and uniformly so with respect to frequency, for the physically important problems of the second type. The difficulties posed by the -dependent renormalization for the study of incident pulses are discussed.