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     

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.     

Special frequencies and Lifshitz singularities in binary random harmonic chains

We consider a one-dimensional chain of coupled harmonic oscillators; the mass of each atom is a random variable taking only two values (M or 1). We investigate the integrated density of statesH(²) near special frequencies: a given frequency _s with rational wavelength becomes special if the mass ratioM exceeds a certain critical valueM _c . We show thatH has essential singularities of the typesH _sg exp(–C ₁ ¦²– _s ² ¦^–1/2) or exp(–C ₂¦²– _s ² ¦^–1), according to the value ofM and the sign of (²– _s ² ). The Lifshitz singularity at the band edge is analyzed in the same way. In each case, the constantC ₁ orC ₂ is evaluated explicitly and compared with a vast amount of numerical work. All these exponential singularities are modulated by periodic amplitudes. The properties of the eigenfunctions with frequencies close to the special values are also discussed, and are illustrated by numerical data.     

Ultrasound in spin glasses

The change of the sound velocity v(,T) and the damping of sound waves (,T) in spin glasses are calculated in the frame-work of an Ising model with a random distribution of exchange interactions. The calculation is based on linearized equations of motion for the spins and on an improved mean field approximation which includes the Onsager reaction field. Near to the freezing temperatureT _f and at high temperatures v(,T) and (,T) turn out to be approximately proportional to the real and the imaginary parts of the dynamical susceptibility. For the special case of infinite range interactions atT=T _f one has v(, T_f) ( )^1/2 and (, T_f) (/)^1/2 where is the relaxation time of independent spins. However, already slightly aboveT _f the frequency dependence of both quantities becomes rather small for RKKY spin glasses. At high temperatures both, v(,T) and (,T) vary asT ^–1.SFB 125 Aachen-Jülich-Köln     

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.     

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.     

Fractional Moment Estimates for Random Unitary Operators

We consider unitary analogs of d-dimensional Anderson models on l²( $$\mathbb(z)$$^d) defined by the product U=D S where S is a deterministic unitary and D is a diagonal matrix of i.i.d. random phases. The operator S is an absolutely continuous band matrix which depends on parameters controlling the size of its off-diagonal elements. We adapt the method of Aizenman–Molchanov to get exponential estimates on fractional moments of the matrix elements of U(U –z)^–1, provided the distribution of phases is absolutely continuous and the parameters correspond to small off-diagonal elements of S. Such estimates imply almost sure localization for U.     

Large time behavior of the vorticity of two-dimensional viscous flow and its application to vortex formation

We consider the Cauchy problem for the two-dimensional vorticity equation. We show that the solution behaves like a constant multiple of the Gauss kernel having the same total vorticity as time tends to infinity. No particular structure of initial data ₀=(x, 0) is assumed except the restriction that the Reynolds numberR=|₀|dx/v is small, wherev is the kinematic viscosity. Applying a time-dependent scale transformation, we show a stability of Burgers' vortex, which physically implies formation of a concentrated vortex.Partly supported by Grant-in-Aid for Scientific Research No. B60460042, the Japan Ministry of Education, Science and Culture     

Four-wave mixing in CO via the C 1Σ+ (υ′=0) state

Coherent vacuum ultraviolet (VUV) radiation was generated by four-wave difference frequency mixing (_VUV=2₁–₂) of pulsed dye laser radiation in carbon monoxide (CO). The frequency ₁ was tuned to the C ¹⁺(=0)X ¹⁺(=0) two-photon transition, while the dye laser frequency ₂ was scaned around 17650 cm^–1 which corresponds to the A ¹(=7)«C ¹⁺(=0) transition energy. The VUV intensity was found to be strongly wavelength dependent. The analysis of the spectrum revealed (i) that the VUV intensity was enhanced by the rotational levels of the A ¹(=7) state and (ii) that the off-resonance excitation in the C ¹⁺(=0)X ¹⁺(=0) two-photon transition greatly contributed to the present four-wave mixing process. The effects of pumping laser detuning, saturation and foreign gases are briefly discussed.     

Harmonic mixing by weakly pinned charge density waves

Third order harmonic mixing voltageE ₀ in case of frequency matching, =₂–₁=0, and third order pseudo harmonic mixing currentj() in the detuned case, 0, are evaluated for the one-dimensional Fukuyama-Lee-Rice model for weakly pinned charge density waves in the region of sub-threshold bias electric fields. After a perturbation expansion of the phase response to the ac driving fields the impurity averaging is performed diagrammatically. Specific statistical properties of the charge density wave phase in the weak pinning limit and a non-trivial result for the pinning of the static phase are utilized to expressE ₀ andj() in terms of the dielectric function (). A recent evaluation of () within the self-consistent Born approximation is used to present the results explicitly in a number of diagrams. In comparison to the overdamped anharmonic oscillator the following differences are found: Randomness leads to interference contributions which increase the amplitudes and decrease the phase shifts. The more realistic form for () at lower frequencies lead to a downward shift in the maximum ofj() when ₁ is decreased below the cross-over frequency _c . The present theory retains inertia in the dynamical equations and remains valid for frequencies near and above the pinning frequency. It fails, however, for small frequencies _{1 c} due to the neglect of metastable states and screening.     

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.     

A theory of 1/f noise

Letu() be an absolutely integrable function and define the random process where thet _i are Poisson arrivals and thes _i, are identically distributed nonnegative random variables. Under routine independence assumptions, one may then calculate a formula for the spectrum ofn(t), S _n(), in terms of the probability density ofs, p_s(). If any probability density p_s() having the property p_s() I for small is substituted into this formula, the calculated S_n() is such that S_n() 1 for small . However, this is not a spectrum of a well-defined random process; here, it is termed alimit spectrum. If a probability density having the property p_s() for small , where > 0, is substituted into the formula instead, a spectrum is calculated which is indeed the spectrum of a well-defined random process. Also, if the latter p_s is suitably close to the former p_s, then the spectrum in the second case approximates, to an arbitrary, degree of accuracy, the limit spectrum. It is shown how one may thereby have 1/f noise with low-frequency turnover, and also strict 1/f ^1– noise (the latter spectrum being integrable for > 0). Suitable examples are given. Actually, u() may be itself a random process, and the theory is developed on this basis.     

s-Polarized nonlinear surface polaritons

An exact solution of Maxwell's equations is found, corresponding to ans-polarized nonlinear surface polarition, at the planar interface between two dielectric media, one of which is optically unaxial and is characterized by a diagonal dielectric tensor whose elements depend on the amplitude of the electric field according to ₁₁=₂₂=₀()+a() (|E ₁|²+|E ₂|²), ₃₃=(). Such modes have no counterpart in the corresponding linear system.     

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)}.     

Kinematics of four-wave decay of high-frequency plasma oscillations into upper hybrid and electron-cyclotron plasma waves under multiple electron gyroresonance conditions

We consider the conditions for four-wave decay of two primary plasmons with wave vector and frequency ₀ close to the multiple gyroresonance frequency n_Be into two secondary plasmons with frequencies ₁ > ₀ and ₂ < ₀. The secondary plasmons belong to the upper hybrid and the electron cyclotron branches. It is shown that the main features of the broad upshifted maximum (BUM) in the SEE spectrum can be explained in the context of the proposed process. The BUM feature appears in the region of frequencies having a positive shift from the high-power radio wave frequency. In particular the broad band nature of the BUM can be a result of the broad spectrum of wave number k₀ of the primary plasma waves. In this case the observed cut-off frequency f_cutoff limiting the BUM spectrum on the lower side can result from the lower bound of k₀ (the increase in ₁ corresponds to decay of shorter wave plasmons). In our approach we assume that the generation of primary plasma oscillations by the high-power radio wave and the conversion of secondary plasma waves into the electromagnetic waves is due to coherent scattering of corresponding waves by small-scale magnetic-field-aligned artificial irregularities or to another nonlinear processes.Published from Izvestiya Vysshikh Uchebnykh Zavedenii, Radiofizika, Vol. 39, No. 3, pp. 301–317, March, 1996.     

830 nm emission in sodium vapor

We demonstrate that the intriguing 830 nm coherent emission, which is observed when sodium vapor is pumped with a high-power pulsed laser tuned near the 3S4D two-photon transition, is due to an axially phase-matched six-wave mixing process. This conclusion is based upon the observation of emission near 584 nm, which is coupled to the 830 nm emission in the six-wave mixing process: ₁+₂=2_L–_4D4P –_4P3D . In addition, we have observed coherent emission near 1.16 m, which is due to an analogous process involving cascade through the 4S (as opposed to the 3D) state. We calculate the wavelengths of all photons involved in these processes using the standard formulas of parametric wave-mixing theory, and show that they can be predicted to within experimental uncertainties. Finally we report observations of significant blue shifts of the 830 nm and 1.16 m emissions in a mixed sodium-potassium vapor. These shifts can be readily understood by considering the effect of the potassium on the frequency-dependent refractive index of the vapor. Due to these results, other recent interpretations of the 830 nm emission as stimulated excimer emission on the Na₂ 1³ _g ⁺ 1³ _u ⁺ band must now be rejected.     

Systematic perturbation calculation for a non commutative model for a metallic glas

We present a systematic perturbation calculation up to the 4th order in the interaction for a metallic-glas-model with an anisotropic coupling of the conduction electrons to a local two-level-system. The logarithmic-(infrared-)divergent terms for the electronic lifetime are suppressed by exponentially small prefactors in the region I (ET) whereas in the region II (ET) they survive in the general case of non-commuting elastic and inelastic couplings in the Hamiltonian, whereE denotes the level-splittings of the local-system, the excitation energy of the conduction electrons above the Fermi level, andT the thermal energy.     

Radiation damping of waves in a cold magnetized two-component plasma

It is shown in this paper that the damping decrements of electromagnetic waves with right circular polarization and the decrements of plasma oscillations near the cyclotron and hybrid frequencies in a strong magnetic field _eBpe are proportional to the square of the cyclotron frequencies _eB and _iB. In a weak magnetic field _eBpe the damping decrements of all modes are proportional to the square of the plasma oscillation frequencies _pe, _pi. Taking account of ions results in a nonzero damping decrement for electromagnetic waves with left circular polarization.Deceased.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 10, p. 8–11, October, 1982.In conclusion, I am grateful to L. S. Kuz'menkov and P. Polyakov for constant attention to the research and for useful remarks.     

Dynamic structure factor in a random diffusion model

Let {X _t:0} denote random walk in the random waiting time model, i.e., simple random walk with jump ratew ^–1(X _t), where {w(x):x^d} is an i.i.d. random field. We show that (under some mild conditions) theintermediate scattering function F(q,t)=E ₀ (q^d) is completely monotonic int (E ₀ denotes double expectation w.r.t. walk and field). We also show that thedynamic structure factor S(q, w)=2 ₀ cos(t)F(q, t) exists for 0 and is strictly positive. Ind=1, 2 it diverges as 1/||^1/2, resp. –ln(||), in the limit 0; ind3 its limit value is strictly larger than expected from hydrodynamics. This and further results support the conclusion that the hydrodynamic region is limited to smallq and small such that ||D |q|², whereD is the diffusion constant.     

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.