Energy characteristics of photothermal vibrational instability at stimulated Raman and Mandelstam-Brillouin scattering in aerosol droplets

The threshold intensity and the combination frequencies for photothermal vibrational instability in high-Q aqueous aerosol droplets in the two-mode regime have been calculated. The selection rules for coupling electromagnetic and temperature modes in a droplet are obtained. A comparative analysis of the threshold excitation intensities of photothermal vibrational instability, stimulated Mandelstam-Brillouin scattering, and stimulated Raman scattering in droplets is performed. It is shown that photothermal vibrational instability in the two-mode regime can be developed at a pump intensity of about 10⁴ W/cm² for droplets with radii of 2–20 μm for a pump wavelength of 0.532 μm. A method of remote measurement of the microphysical droplet parameters from the additional periodic temperature shift of droplet eigenfrequencies in the spectrum of stimulated Raman scattering and lasing is proposed.     

Giant Raman optical activity of the 128-cm-1 mode in α-quartz

The threshold intensity of stimulated Raman scattering along the c-axis in α-quartz was measured for the 128-cm^-1 optical lattice vibration as a function of pump laser polarization at T = 10 K. In a right-handed, optically active quartz crystal the Raman threshold intensity for left-handed, circularly polarized pump light was lower by a factor of about 1.5 than for right-handed, circularly polarized light. The difference in threshold intensity is discussed in terms of Raman optical activity.     

Pre-resonant Raman scattering in antracene crystals

The pre-resonant Raman scattering (PRRS) of anthracene crystals (T = 4.2?30 K) has been studied. A tunable dye laser (v_exc = 25000?25100 cm^-1 was used to produce an excitation close to the lowest exciton band bottom (v₀ = 25097 cm^-1). A sharp increase of the PRRS intensity when approaching the excitation light frequency v_exc to v₀ and then the not less sharp drop of the PRRS intensity close to resonance (v₀ ? v_exc ≈ 35?15 cm^-1) where observed. An extremely high PRRS sensitivity to temperature and the excitation light intensity was found. The results are explained within the framework of stimulated PRRS in anthracene crystals.     

Time-resolved photoluminescence on the stimulated emission in polycrystalline ZnO nanoparticles

The detailed room temperature stimulated emission including its optical characteristics from ZnO nanoparticles, which were prepared by a homogenous precipitation method, has been investigated by the time-resolved spectroscopy. The light emission originates from a free exciton recombination at a lower excitation level; the amplified spontaneous emission appears at a moderate excitation level, in which the threshold excitation intensity is 0.65 GW cm⁻². The resonant stimulated emission was observed in ZnO nanoparticles at a higher excitation intensity. Also, the emission lifetime is drastically reduced. Compared to the fluorescence decay curves, the time-resolved spectrum of the stimulated emission suggests the Gaussian-like decay time with only a few of picoseconds. The dynamic processes of lasing behavior and the characteristics of lasing emission in ZnO nanoparticles could provide the information on the crystal quality, the exciton and the lasing action in the particles.     

Parametric excitation of temperature oscillations in a high-Q dielectric microwave resonator in liquid helium vapor

We study the threshold conditions of the parametric excitation of temperature oscillations using pulsed microwave pumping in three-mode regime for high-Q ferroelectric cryogenic resonators made of SrTiO₃ and KTaO₃. Comparative analysis is performed for the threshold power of the excitation of temperature oscillations and the threshold power of the ponderomotive parametric excitation of acoustic oscillations in the resonator. It is shown that in three-mode regime, temperature oscillations can develop under a rather moderate pump power of about 0.1–8 μW, depending on the combination of interacting temperature and electromagnetic modes. The calculated low threshold powers allow one to apply resonators in practice as high-sensitivity infrared sensors, resonant bolometers, and parametric amplifiers. Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Radiofizika, Vol. 52, No. 2, pp. 172–180, February 2009.     

Raman study of BiFeO3 with different excitation wavelengths

Raman spectra of bismuth ferrite (BiFeO₃) over the frequency range of 100-1500 cm⁻¹ have been systematically investigated with different excitation wavelengths. The intensities of the two-phonon modes are enhanced obviously under the excitation of 532 nm wavelength. This is attributed to the resonant behavior when incident laser energy closes to the intrinsic bandgap of BiFeO₃. The Raman spectra of BiFeO₃ excited at 532 nm were measured over the temperature range from 77 to 678 K. Besides the abnormal changes of the peak position and the linewidth of the A₁ mode at 139 cm⁻¹, the prominent frequency shift, the line broadening and the decrease of the intensity for the two-phonon mode at 1250 cm⁻¹ were observed as the temperature increased to Néel temperature (T_N). All these results indicate the existence of strong spin-phonon coupling in BiFeO₃.     

Generation of frequency shifted picosecond pulses with low temporal jitter

Transient stimulated Raman scattering is used for the generation of a frequency shifted picosecond light pulse; part of this Raman shifted pulse is subsequently coherently scattered at a material excitation of a second Raman cell. Starting with the second harmonic pulse (t_p = 4 ps) of a mode-locked Nd : glass laser system, both the stimulated and the coherently produced pulses have durations of 2.3 ps at different wavelengths. By the appropriate choice of the Raman medium pulses between 13 000 and 21 000 cm^-1 can be generated. The coherent generation process minimizes the temporal jitter between the two pulses and allows to obtain a high time resolution of better than 0.3 ps in excite and probe experiments.     

光纤共振和预共振喇曼光谱

在液芯光纤内产生共振和预共振喇曼效应,喇曼光谱强度可以大幅度提高,最高可达10⁹倍.本文介绍获得光纤(预)共振喇曼光谱的可行性、实验及实验结果.用远离吸收带的激光激发获得了α甲基吡啶预共振喇曼光谱.用小功率激光(0.8mW)、低浓度溶液(9.6×10¹²mol/L)还获得了β叶红素在CS₂中的共振喇曼光谱.     

Two-photon correlations of luminescence at the Bose-Einstein condensation of dipolar excitons

Correlations of the luminescence intensity (the second-order correlation function g ⁽²⁾(τ)), where τ is the delay time between the photons detected in pairs) under the conditions of the Bose-Einstein condensation (BEC) of dipolar excitons has been studied in a temperature range of 0.45–4.2 K. Photoexcited dipolar excitons have been accumulated in a lateral trap in a GaAs/AlGaAs Schottky diode with a 25-nm wide single quantum well with an electric bias applied across the heterolayers. Two-photon correlations have been measured with the use of a two-beam intensity interferometer with a time resolution of }~0.4 ns according to the well-known classical Hanbury-Brown-Twiss scheme. The photon bunching has been observed at the onset of Bose-Einstein condensation manifested by the appearance of a narrow exciton condensate line in the luminescence spectrum at an increase in the optical pumping (the line width near the threshold is ?200 μeV). At the same time, the two-photon correlation function itself obeys the super-Poisson distribution, g ⁽²⁾(τ) > 1, at time scale τ_c ? 1 ns of the system coherence. The photon bunching is absent at a pumping level substantially below the condensation threshold. The effect of bunching also decreases at pumping significantly above the threshold, when the narrow exciton condensate line starts to dominate in the luminescence spectra, and finally disappears with the further increase in the optical excitation. In this region, the distribution of pair photon correlations is a Poisson distribution manifesting the united quantum coherent state of the exciton condensate. Under the same conditions, the first-order spatial correlation function g ⁽¹⁾(r) determined from the interference pattern of the luminescence signals from the spatially separated parts of the condensate at constant pumping remains noticeable at distances of no less than 4 μm. The discovered effect of photon bunching is very sensitive to temperature and decreases by several times with a temperature increase in the range of 0.45–4.2 K. Assuming that the luminescence of the dipolar excitons directly reflects the coherence properties of the gas of interacting excitons, the discovered photon bunching at the onset of condensation, where the fluctuations of the exciton density and, consequently, of the luminescence intensity are most significant, indicates a phase transition in the interacting Bose gas of excitons, which is an independent way of detecting the Bose-Einstein condensation of excitons.     

Hot electrons produced from long scale-length laser-produced droplet plasmas

Microplasmas produced from 15 μm methanol droplets irradiated by 100 fs laser pulses in the intensity range 10¹⁴–10¹⁶ W cm^?2 are investigated via measurements of the hot electron temperature and x-ray yields under different conditions of intensity, polarization state, and plasma scale-length. The scale length of the drop-let plasma is increased with an intentional prepulse that is 10 ns ahead of the main pulse. Hot electron temperatures up to 48 keV have been measured at intensities of 2.5 × 10¹⁵W cm^?2 and the scaling of temperature as a function of intensity is determined for a long scale-length droplet plasma. The polarization and ellipticity dependence of the hard x-ray yield from the microdroplet plasmas are used to probe the shape of the droplet after irradiation by a prepulse.     

Observation of general behaviour of Resonance Raman Spectra in the model system KBr(MnO-4)

Employing KBr(MnO^-₄) crystals as model specimens, the authors have observed for the first time the theoretically predicted peculiarities of the impurity resonance Raman scattering (RRS) resulting from excitation to a vibronic-structured absorption band, those peculiarities being the sharp irregularity of the RRS spectrum in case of excitation to Frank-Condon sublevel, the strong dependence of the spectrum on excitation frequency, the temperature dependences of the RRS line intensity which are significantly different for different orders of scattering. The observational data have been compared with calculations of cross-sections for multi-phonon RRS.     

Increase of the stimulated Raman scattering threshold at droplets by spectral broadening of nanosecond laser pulses

We show that the threshold of stimulated Raman scattering (SRS) from single micro‐droplets increases with the bandwidth of the pulsed excitation laser radiation. SRS thresholds were experimentally investigated for two droplet sizes and two excitation bandwidths. For the narrowband excitation, a frequency doubled Nd:YAG laser with a central wavelength of 532 nm, a full width half maximum (FWHM) bandwidth of 0.05 nm and a repetition rate of 10 Hz was used. For the comparison with the broadband excitation, a dye resonator containing Rhodamine 6G being pumped by the Nd:YAG laser was utilized with a central wavelength of 566 nm and a FWHM bandwidth of 4 nm. Droplets of 89 and 116 µm diameters, respectively, were illuminated by a vertical light sheet. If the broadband excitation is applied instead of the narrowband excitation ‐ for both droplet sizes ‐ the pulsed excitation energies can be increased by a factor of approximately 5 before the SRS threshold is reached. The multiplication register of an emCCD detector was used to detect low signals. The gain factor of the detector was calibrated and adapted to different excitation energies and signal intensities. Copyright © 2012 John Wiley & Sons, Ltd.     

Vibrational Raman scattering temperature measurements

Experimental data and analyses are presented for the determination of gas temperature by measurements of vibrational Raman scattering intensity ratios of Stokes Q-branch fundamental bands. The method is demonstrated for two thermal equilibrium experiments: (1) CO₂ (a gas well-suited for use in multi-component mixtures near ambient temperatures) in a test cell, and (2) N₂ (a gas well-suited for use at elevated temperatures) in a flame. This method of temperature measurement is of particular value for non-thermal equilibrium conditions, for which vibrational excitation temperatures can be assigned to each pair of vibrational level corresponding to observable Raman bands.     

Resonant Raman scattering of polymeric sulfur nitride modified by iodine

Resonance Raman spectra of (SNI_y)_x crystals have been measured at 150 K. The energies of the principal Raman lines of the chromophore (109 and 154 cm^?1) and their intensity behaviour with exciting laser frequency are consistent with the formation of a charge-transfer complex in which iodine enters the interfiber regions of the (SN)_x lattice as I₅^- or I₃^- linked to distorted I₂ units. This structural model is supported by comparison of these Raman data with the excitation profiles of the chromophoric group in starch-iodine and α-cyclodextrine-iodine complexes. Possible mechanisms for the conductivity increase on the basis of the proposed charge transfer model are also discussed.     

Nonlinear properties in InxGa1 − xAs/GaAs multiple quantum well laser structures

In this paper we investigated nonlinear properties and lasing in In_xGa_1 − xAs/GaAs multiple quantum wells grown by metal-organic chemical vapour deposition. A systematic study, performed by high excitation photoluminescence measurements as a function of excitation intensity, allowed us to identify the minimum well width for observing stimulated emission from well states. We also determined the threshold for stimulated emission for well and barrier lasing. Radiative recombination energies are identified by using theoretical data obtained in the effective mass approximation, including boundary conditions and strain.     

Electrothermal Oscillatory Instability in Spherical Ferroelectric Resonators. Three-Mode Case

We consider the equations of interaction between electromagnetic oscillations and the temperature in a nonlinear dielectric resonator and study the dynamics of the oscillatory instability in the system. The threshold conditions (power and self-modulation frequency) of electrothermal excitation are calculated for microwave potassium-tantalate resonators for the case of three-mode interaction. The conditions for observing electrothermal excitation in the three-mode case are found to be quite favorable. In this case, the threshold power of excitation of temperature oscillations is smaller than that in the two-mode case and can amount to a few microwatts.     

Spin-dependent phonon Raman scattering in CdCr2Se4

Influences of ferromagnetic ordering on the phonon Raman scattering are studied for CdCr₂Se₄ through the intensity measurements of Raman spectra between 25 and 300 K with various wavelengths of excitation light (488.0–676.4 nm). Spin-dependent enhancements of Raman cross section are observed for optical phonon lines D(168 cm^?1) and F(238 cm^?1) with excitation wavelengths of about 630 and 550 nm, respectively. This kind of phenomenon in spinel-type chalcogen chromites seems to originate in spin-dependent intermediate interactions in the excited states of specific electronic transitions with which the incident or scattered light is resonant.     

High-Resolution Stimulated Raman Spectroscopy of Cl2, Cl2, and ClCl

A high-resolution rovibrational Raman spectrum of a sample of Cl₂ has been recorded at room temperature using a quasi-cw stimulated Raman technique. Three Q-branch structures belonging to the fundamental vibrations of the three chlorine isotopomers present in the sample in natural abundances and two weaker Q branches belonging to the first hot bands of the two more abundant isotopomers, ³⁵Cl₂ and ³⁵Cl³⁷Cl, have been observed. Lines with values of J up to 60 for the fundamentals and 50 for the hot bands have been measured in these fully resolved structures. Some additional lines belonging to O and S branches of the fundamentals and hot bands have also been recorded. The analysis of these data has rendered a new and more precise set of rotational molecular constants and band origins for the first three vibrational states of the chlorine isotopomers.     

Effect of crystal orientation on picosecond-laser bulk microstructuring and Raman lasing in diamond

In the paper we report on picosecond-laser bulk microstructuring and stimulated Raman scattering (SRS) in type IIa single-crystal diamond in the course of multipulse irradiation at λ=532 nm wavelength using an advanced ps-laser system equipped with additional setups for on-line video imaging and photoluminescence spectra measurements. The effect of crystal orientation (relative to the incident laser beam) on (i) optical breakdown thresholds, (ii) character of bulk modifications, and (iii) generation of stimulated Raman scattering in diamond during irradiation with picosecond pulses of different durations (τ ₁=10 ps and τ ₂=44 ps) is studied. It is shown that the processes of laser-induced breakdown in the bulk of diamond (at the backside of the crystals) and bulk microstructure growth are governed by the dielectric breakdown mechanism. It is found that generation of high-order stimulated Raman scattering in diamond crystals has a considerable effect on the threshold of laser-induced breakdown and bulk microstructuring. Conditions of the efficient SRS lasing are determined, depending on the pulse duration and the direction ([100] and [110]) of the laser beam incidence. A method of local temperature measurements in the bulk of diamond based on the Stokes-to-anti-Stokes intensity ratio in the recorded SRS spectra is proposed, its applicability to determine a “pre-breakdown” temperature of diamond during multipulse ps-laser irradiation is discussed.     

Oscillations in the excitation function for complete fusion of 6O+12C at low energies

The excitation function of the complete fusion of ¹⁶O + ¹²C has been measured in the range E_c.m.=8.5?12.9 MeV. It contains oscillations which have already been observed at higher energies. Some of these oscillations are tentatively in terms of a rotational band.