Excited-state absorption and third-order optical nonlinearities in symmetric π-electron organic molecules

Excited-State Absorption (ESA), Two-Photon Absorption (TPA) and the third-order polarizability (;,, – ) have been investigated for a model dichloride derivative of a symmetrically substituted benzylidene analine (SBAC), using a multielectron configuration-interaction procedure. The calculations indicate that SBAC exhibits ESA across the visible region of the spectrum, but that it is not as extensive as for molecules such as the phthalocyanines. The magnitude of the third-order polarizability is dominated by resonance enhancement from a very strongA _g B _u one-photon absorption. The calculated off-resonance value for (;,, – ) suggests that SBAC is a potential candidate for ultrafast switching applications.     

Spectral superbroadening of self-focused picosecond laser pulses in D2O

Intense picosecond light pulses of a mode-locked Nd: glass laser at _L =1054 nm (fundamental wavelength) and _SH =527 nm (second harmonic wavelength) are passed through a sample of D₂O under self-focusing conditions. Spectrally structured superbroadened, spatially bell-shaped emission in the forward direction is obtained. Primary generation processes are pump-pulse-degenerate stimulated parametric four-photon interaction (₁ + _{1 3} + ₄) and stimulated Raman scattering (_{1 R} + ), which occur concurrently (₁= _L or _SH angular pump frequency, #x03C9; _R first Stokes frequency, #x03C9; signal frequency, #x03C9;₃ signal frequency, #x03C9;₄ idler frequency). The parametric four-photon interaction occurs under collinear non-phase-matched conditions and under longitudinally phase-matched, transversally non-phase-matched (erenkov-like) conditions. Subsequent interaction processes are pump-pulse-nondegenerate four-photon interaction of the type ₁ + _{R 3} + ₄, coherent antiStokes Raman scattering (CARS, ₁ + ₁ – _{4 3}), inverse Raman scattering ( _A + ₁ + ), and cascading light up-conversion of the type ₁ + _(i) – _{R (i+1)}.     

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     

Algebraic structure of the amplitude of elastic scattering by a two-dimensional crystal

The coherent scattering of spin-S particles by a monatomic crystal film is considered, with rescattering taken into account. A relation between the amplitudes q_j of different diffraction orders and the dielectric tensor () of the two-dimensional crystal is found. The relation can be used to obtain () for an arbitrary frequency (including resonant frequencies) in terms of elastic scattering data. The possibility of bound states of the particles in the monatomic film is demonstrated.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 4, pp. 30–34, April, 1987.The author thanks V. L. Vinetskii for interest in the work and for useful discussions.     

Some exact models for nonspherical collapse. III

The gravitational nonradiative collapse of dust configurations in the presence of electromagnetic field is analyzed in terms of exact dynamical solutions for a wide range of spacetime symmetries: cylindrical, pseudoplanar, toroidal, and also spherical, planar, and pseudospherical [when the anisotropy factor of the (x ²,x ³) surfaces,(R, T), is replaced by a massless scalar field]. The condition that the collapse is nonradiative leaves three possibilities for the coordinate dependence of(R,T) (i)=(a),a (R, T) being the scale factor of the (x ²,x ³) surfaces, (ii)=(T), and (iii)=(R). Almost all (in the meaning indicated in the text) solutions for charged dust with=(a) and for dust in the external electromagnetic field with=(T) and=(R) have been obtained and discussed. A wideranging discussion concerning the topics of papers I–III is given. Special attention is paid to the question of horizon existence and formation and also the perspective of extension of the techniques developed onto the more realistic case of axial symmetry.     

A relationship between asymmetric Lévy-stable distributions and the dielectric susceptibility

This paper, as a complement to the work of Montroll and Bendler, is concerned with the Lévy-stable distributions and their connection to the dielectric response of dipolar materials in the frequency domain. The necessary and sufficient condition for this connection is found. The presented probabilistic analysis is based on the mathematically correct representation of the meaning of the relaxation function of a system of dipoles and shows why the same form of a distribution of relaxation rates, namely, the completely asymmetric Lévy-stable distribution, should apply in all different relaxing systems. This is in contrast to the traditional definition of the relaxation function, expressed as a weighted average of exponential relaxation functions, which does not explain the universality of the dielectric relaxation law. It also follows from the present considerations that not only is the imaginary part () of the dielectric susceptibility directly related to the Lévy-stable distribution (as was found by Montroll and Bendler), but so is the real part(). As a consequence the relation()/()=cot(n/2) for> _p and 0<n<1, implied by experimental results, is obtained.     

Linear and non-linear ac response of the stochastic classical model for sliding charge density waves

A comprehensive study of the ac response properties of the classical stochastic model for sliding charge density waves (CDW) in quasi one-dimensional metals is made by numerically solving the associated Fokker-Planck equation. Above the conductivity threshold a noise mechanism is indispensable to give finite line widths to the resonances of the applied ac signal of frequency with the narrow band noise frequency _OSC inherent in the model. In the present investigation a current noise of strengthT _N proportional to the CDW current is used in the Fokker-Planck equation in order to model the broad band current noise frequently observed above threshold. The present model thus incorporates three characteristic frequency scales: _OSC,T _N ,and a crossover frequency _OSC. Results are evaluated for the ac conductivity (;E ₀,E ) as function of frequency , dc bias electric fieldE ₀ and ac signal field strengthE . ForE 0 the linear ac response is obtained by a separate treatment of the Fokker-Planck equation. The resonances near =_OSC are studied in detail. Strong ac signals reduce the response at the fundamental resonance and lead to a harmonic interference structure nearn=_OSC. The overall agreement of the present results with recent measurements of the linear ac response is not good. In reality our results seem to be superimposed on a background not reproduced by the classical model with one cross over frequency. However, the peak in Im (;E ₀,E =0) vs.E ₀, when the narrow band noise frequency is near , is well reproduced. The spectral width of this peak which corresponds to the inductive dip in the susceptibility is studied as function of current noise strengthT _N .The results stress the need for a complete Fokker-Planck treatment sinceT _N is not simply related to the line width.     

QCD sum rule analysis of the coupling constant g ωσγ

We employ QCD sum rules to calculate the coupling constant g by studying the three point -correlation function. Our result complements the analysis of this coupling constant utilizing the experimental value of the ⁰⁰ decay rate studied within the framework of chiral perturbation theory including vector meson and meson intermediate states.     

The third-order electric susceptibilities of NaCl and KCl monocrystals

The dispersion of the third-order electric susceptibilities(; , , –) and(; , 0, 0) of NaCl and KCl monocrystals has been calculated by means of experimental data on the electro-optic Kerr effect. The result has been obtained by using semi-classical models of anharmonic oscillators. An ionic contribution to the electro-optic coefficients has been presented. From the result obtained it follows that the third-order electric susceptibilities are of the order of 10^–22 m² V^–2.     

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.     

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.     

One-dimensional random walk with self-interaction

A standard random walk on a one-dimensional integer lattice is considered where the probability ofk self-intersections of a path =(0, (1),..., (n) is proportional toe ^–k . It is proven that for <0,n ^–1/3(n) converges to a certain continuous random variable. For >0 the formulas are given for the asymptotic Westerwater velocity of a generic path and for the variance of the fluctuations about the asymptotic motion.     

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.     

Low frequency limits of third-order harmonic coefficients for atomic hydrogen in any level of discrete energy spectrum

In this paper the analytical expression is derived for the third-order optical harmonic coefficients x _abcd ^v (,,) of the atomic hydrogen at very low frequencies 0 in many level of the discrete energy spectrum.The author expresses his thank to Prof. Nguyen Van Hieu for suggesting the problem and fruitful discussions.     

Flow of an elastico-viscous fluid past an oscillating plate

An exact solution for the flow of an elastico-viscous fluid (Walters' liquid B') due to an oscillating infinite plate has been derived. It has been observed that forgwt=0, ( — frequency,t — time) the flow near the plate may become unstable with increasing whereas fort>0, the velocity increases with increasing. The shearing stress decreases with increasing.I wish to thank the referee for his useful comments which led to the improvement of this paper.     

Stochastic linear maps and transition probability

Some aspects of the transition probability P(, ) between states , on unital ^*-algebras are discussed. It is shown that P increases under the action of any stochastic linear map T, i.e., P(T, T)P(, ). Some properties of P are derived in starting from a recently-proved characterization of the quantity in question.     

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.     

Rate equations in the hopping transport

The usual kinetic equations for the site occupation probabilities in an external field are solved exactly in a simple one-dimensional periodic model with two kinds of atoms using a) free boundary conditions and order of limitsN, 0 needed for a proper treatment of the dc conductivity here b) boundary conditions with metallic contacts and order of limitsN, 0 and c) the same boundary conditions but reversed order of limiting processes 0,N typical of e.g. numerical and percolation treatments. (N and are the number of sites and frequency.) It is demonstrated that though the bulk dc conductivity is the same in all three cases, local bulk properties of the material are strongly dependent on the régime used. The role of the order of all three limiting processes 0,N+ andn+ (N–n+) for local shifts of the chemical potential _n in the dc limit is examined (n is the number of the relevant site calculated from a boundary of the chain). It is shown especially that the rate equation treatment (régime a) on the one hand and numerical or percolation treatments (régime c) on the other hand never yield the same bulk values of _r.     

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 .     

ВОЗНИКНОВЕНИЕ КАТОД НЫХ ПЯТЕН И РАСПРЕДЕЛЕНИЕ ПЛОТ НОСТИ ТОКА В КАТОДНЫХ ПЯТНАХ СИЛНОТОЧНОГО ЭЛЕКТРИЧЕСКОГО РАЗР ЯДА

. , 760 mm . .

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Formation of cathode spots and current density distribution in cathode spots of short-time high-intensity electric discharge

The connection between the current density distribution in a spot and the vapour jets was found for a short-time high-intensity electric discharge by studying the structure of partial cathode traces and measuring the current density on the cathode. The variation of the current density on the spot with the current gradient was also found and the etching of the cathode surface with ionic bombardment at a pressure of 760 mm Hg was observed.