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)}.     

Generation of more than 40 laser emission lines from the ultraviolet to the visible regions by two-color stimulated raman effect

An intense and monochromatic laser beam consisting of more than 40 vibrational and rotational lines is generated by the stimulated Raman effect, when two-color laser beams separated by 590 cm^–1 are tightly focused into pressurized hydrogen. This phenomenon is reasonably explained by four-wave mixing; one beam is used for two-step excitation (₁+₁) to an imaginary level and another beam (₂) acts as a seed beam, generating a fourth beam (2₁–₂). Through cascade processes, so many laser emissions appear with a frequency difference of (₁–₂) in entire ultraviolet and visible regions.     

CW coherent VUV radiation generated by resonant sum-frequency mixing in metal vapors

Resonant third-order sum-frequency mixing of continuous-wave visible and ultraviolet laser light is investigated in the metal vapors of Sr, Ca, Mg, and Zn. The laser radiation (with the frequencies ₁, ₂, and ₃) is generated by single-mode dye- and argonion lasers. The third-order nonlinear susceptibility is enhanced by tuning the laser frequencies 2₁ or ₁+₂ to a two-photon resonance. The wavelength of the generated coherent VUV radiation (with the frequency _VUV=3₁, _VUV=2₁+₂ or _VUV=₁+₂+₃) is tunable in spectral regions between 133 and 217 nm. For most conversion processes an additional enhancement of the nonlinearity is provided by an autoionizing level or by a highly excited state close to E=_VUV. With laser powers of 0.2–3 W the power of the generated sum frequencies is in the range of 5×10⁵–6×10¹⁰ photons s^–1 (0.5 pW–60 nW).     

Tunable UV radiation at short wavelengths (188–240 nm) generated by sum-frequency mixing in lithium borate

Sum-frequency mixing (₃=₁+₂) of UV laser radiation (₁=266 nm and 213 nm) and tunable coherent infrared light (₂=1.2–2.6 m) in lithium borate (LBO) generates radiation at short wavelengths (₃=188–242 nm). The UV radiation at ₁ is produced by the fourth and fifth harmonic of a pulsed Nd-YAG laser. The infrared light is generated with an optical parametric oscillator of beta barium borate. The phase-matching angle is measured as function of ₃ and compared with calculated values. For UV laser radiation at shorter wavelengths (173 nm₁213 nm) the calculations predict an extension of the tuning range of the sum-frequency generated at ₃ to wavelengths as short as the LBO transmission cutoff at 160 nm.     

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.     

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.     

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.     

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.     

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.     

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     

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.     

Theoretical investigation of noncollinear phase-matched parametric four-photon amplification of ultrashort light pulses in isotropic media

The amplification of light signals (angular frequency _S in some isotropic media (D₂O, fused silica, and Schott type SF10 glasses) by noncollinear phase-matched parametric four-photon interaction ₁+_2S+₁ is studied theoretically. Computer simulations are carried out for fundamental and second-harmonic pump pulses of a mode-locked Nd: glass laser. Degenerate interaction (wavelength ₁=₂=1054nm or 527 nm) and nondegenerate interaction (₁=1054nm, ₂=527 nm are considered. Characteristic phase-matching parameters and gain parameters versus wavelength are determined. Limitations by spectral bandwidth, optical absorption, optical damage, self-phase modulation, self-focusing and stimulated Raman scattering are analysed.     

Extensible Embeddings of Black-Hole Geometries

Removing a black hole conic singularity by means of Kruskal representation is equivalent to imposing extensibility on the Kasner–Fronsdal local isometric embedding of the corresponding black hole geometry. Allowing for globally non-trivial embeddings, living in Kaluza–Klein-like M ₅ × S ₁ (rather than in standard Minkowski M ₆ ) and parametrized by some wave number k, extensibility can be achieved for apparently forbidden frequencies in the range ₁ (k) ₂ (k). As k 0, _{1, 2} (0) _H (e.g., _H = 1/4M in the Schwarzschild case) such that the Hawking–Gibbons limit is fully recovered. The various Kruskal sheets are then viewed as slices of the Kaluza–Klein background. Euclidean k discreteness, dictated by imaginary time periodicity, is correlated with flux quantization of the underlying embedding gauge field.     

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.     

Effective method of phase conjugation of multifrequency radiation in “pseudo”-four-wave interaction

The possibility is considered of formation of a multifrequency-radiation wave front (with a wide line spectrum in the interval , +), reversed with respect to the wave front of a signal wave of frequency ₀ unequal to the frequencies in the indicated spectrum. The wave front reversal (phase conjugation) is achieved by diffraction of a multifrequency light wave in a direction counter to that of the signal, on a three-dimensional dynamic hologram produced by electromagnetic fields of frequency ₀ in a resonant medium (with thermal nonlinearity) that is fully transparent to the multifrequency radiation. A single direction of the radiation diffraction at all frequencies of the spectrum is ensured by preliminary passage of the initial multifrequency wave through a simple dispersive prism that deflects the direction in each spectral line in proportion to the frequency change. The basic equations describing a similar phase conjugation method are derived, and the efficiency of the conjugation are estimated using as an example multifrequency emission of a chemical cw HF laser.P. N. Lebedev Instiute of Physics. Translated from Preprint No. 205 of the lebedev Institute of Physics of the Academy of Sciences of the USSR, Moscow, 1989.     

Plasma instability in a strong,circularly polarized electromagnetic wave

Conclusions In summary, we have studied the parametric instability of a cold electron plasma in a strong, circularly polarized electromagnetic wave, taking into account the relativistic nature of the electron motion. We have shown that an instability of longitudinal waves occurs at frequencies _p/ and _p/, while an instability of transverse waves occurs at frequencies ₀±₀ and ₀±_p/. The results of a numerical solution of the dispersion relation for large pump amplitudes, in which case the approximation of a weak coupling between waves is not applicable, show that the growth rates and the bands of the instabilities increase with increasing pump amplitude. We have found that in the case of the excitation of electromagnetic plasma waves, even at low pump amplitudes, the relativistic nature of the electron motion can be of decisive importance for the effect.T. G. Shevchenko Kiev State University. Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Radiofizika, Vol. 19, No. 10, pp. 1481–1488, October, 1976.     

Lifshitz tails for periodic plus random potentials

We prove that the integrated density of states () for a potentialW =V _per +V has Lifshitz tails where V_per is a periodic potential with reflection symmetry andV is a random potential, e.g., of the formV =q _i ()f(x–i).research partially supported by DFG.research partially supported by USNSF under grant No. MCS-81-20833.     

A Boltzmann map for quantum oscillators

We define a map on the space of quasifree states of the CCR or CAR of more than one harmonic oscillator which increases entropy except at fixed points ofx. The map is the composition of a doubly stochastic map T^* and the quasifree reductionQ. Under mixing conditions onT, iterates of take any initial state to the Gibbs state, provided that the oscillator frequencies are mutually rational. We give an example of a system with three degrees of freedom with energies ₁, ₂, and ₃ mutually irrational, but obeying a relation n₁₁+n₂₂=n₃₃,n _i . The iterated Boltzmann map converges from an initial statep to independent Gibbs states of the three oscillators at betas (inverse temperatures) ₁,₂, ₃ obeying the equation n₁₁₁+n₂₂₂=n₃₃₃. The equilibrium state can be rewritten as a grand canonical state. We show that for two, three, or four fermions we can get the usual rate equations as a special case.     

A theory of the weakly pinned Fröhlich mode

Extending earlier work of Littlewood (1987) a theory for the collective mode (Fröhlich mode) response of weakly pinned charge density waves (CDW) is given. Long range Coulomb interaction is incorporated in both a proper definition of the measured ac conductivity _CDW() and in the Fukuyama-Lee-Rice treatment of phason dynamics. The frequency and wave number dependent quasi particle resistivity is shown to appear only in the internal phason lines in the perturbation expansion of the impurity averaged phason propagatorD _ren. Quantitative results for _CDW() are evaluated within the self-consistent Born approximation toD _ren in three spatial dimensions taking anisotropy into account. Besides the low frequency relaxation mode we find a significant effect of the longitudinal optical phason _LO on the Fröhlich mode pinning frequency when descreening sets in at low temperatures. This is yet another manifestation of selection rule breaking by inhomogeneous pinning and establishes the special role that _LO plays in the dynamics of CDW. An explicit analytical formula for _CDW() is given and discussed in some detail including the important analyticity properties. Available measurements of the linear ac response in a wide range of frequencies and conductivities are compared with the theory and found to agree with the theoretical predictions supporting the concept of weak pinning in CDW.