Picosecond stimulated Raman scattering in crystals

The comparative values of the peak and integral cross sections of spontaneous Raman scattering and the optical dephasing time of molecular vibrations were determined for several oxide crystals by spontaneous Raman spectroscopy. The spectral, time, and energy parameters of stimulated Raman scattering (SRS) were measured for ten crystals using picosecond YLF: Nd laser pumping with a radiation wavelength of 1047 nm. An analysis of the experimental dependence of the threshold energy of pumping SRS on the integral and peak cross sections of spontaneous Raman scattering showed that the SRS gain increment explicitly depended on the integral cross section and was independent of the peak cross section of spontaneous Raman scattering as the ratio between the pumping pulse width (11 ps) and the time of optical dephasing of molecular vibrations changed from 0.42 to 9.3. The gain coefficients of steady-state stimulated Raman scattering under threshold stimulated Raman scattering conditions were determined for all the crystals studied on the basis of the measured threshold SRS pumping energies, the duration and width of the spectrum of pulses, the nonlinear interaction length, the intensity of pumping, and the theoretical dependences that relate the steady-state and transient SRS gain increments. The steady-state SRS gain coefficients obtained in this work fitted well a linear dependence on the peak cross sections of spontaneous Raman scattering, which substantiated the correctness of our analysis and measurements.     

Temperature dependence of the radiation-stimulated conductivity of CsI crystals upon picosecond excitation by electron beams

The temperature dependence of the pulse conductivity for CsI crystals upon excitation with an electron beam (0.2 MeV, 50 ps, 400 A/cm²) at a time resolution of 150 ps is investigated. Under experimental conditions, the time of bimolecular recombination of electrons and holes (V _k centers) is directly measured in the temperature range 100–300 K. This made it possible to calculate the temperature dependence of the effective recombination cross section S(T)=7.9×10^?8 T² cm². The temperature dependence of the conductivity σ(T) is interpreted within the model of the separation of genetically bound electron-hole pairs. The activation energy of this process is found to be E _G =0.07 eV.     

Micromagnetic investigation of the sub-nanosecond magnetic pulse driven domain wall motion in CoFeB nanowire

We report our micromagnetic simulations based on Landau-Lifshitz-Gilbert (LLG) equation for CoFeB nanowire which was exposed by sub-nanosecond magnetic pulse with varied pulse width between 100 and 1000 ps. It is found that the Walker Breakdown field (H_WB) shifted as the field pulse duration decreased and reached at the highest value in case of 100 ps pulse width, then decreased steeply with respect to the pulse width up to 400 ps. H_WB values are not significantly dependent for pulses longer than 500 ps. It is observed that, below the H_WB, the exchange energy is larger than the demagnetization energy in the wider nanowire. By energy density analysis, it is understood that the increase of H_WB values in the cases of narrower pulse width was to compensate the energy needed to move the DW.     

Threshold and conversion experiments on seeded stimulated Raman scattering

High energy-conversion efficiencies in Stimulated Raman Scattering (SRS) are demonstrated both in experiments and by simulations for pump powers below SRS threshold. The scattering is induced by a short seed pulse at the Stokes frequency, the pulse width of which is much shorter than the pump pulse width and which is comparable with the medium's dephasing time.     

Dynamics of first- and second-order phase transitions in amorphous magnetooptic TbFeCo films

The dynamics of phase transformations in thin amorphous TbFeCo films under the action of ～ 1 ps laser pulses is investigated. The films are heated to the Curie temperature in the amorphous state (T _C1), to the crystallization temperature (T _ac), and to the Curie temperature in the crystalline phase (T _C2). The change in magnetization is detected by Faraday magnetooptic effect during and after the action of the heating pulse. A static external magnetic fieldH～1?12 kOe, whose flux lines are directed perpendicular to the plane of the film, is used in the experiments. Amorphous TbFeCo films possess a perpendicular magnetic anisotropy, which on crystallization becomes reoriented in the plane of the film. It is observed that crystallization and magnetization reorientation occur during the heating pulse (within ～ 1 ps). The spin subsystem is heated to the Curie temperature several picoseconds after the end of the laser pulse. The characteristic spin relaxation time is ～ 10 ps. A model of the dynamics of the electronic, spin, and phonon subsystems that makes it possible to explain the experimental results is proposed on the basis of the data obtained.     

Solvent and Temperature Dependence of Spin Echo Dephasing for Chromium(V) and Vanadyl Complexes in Glassy Solution

The solvent and temperature dependence of the rate constant for spin echo dephasing, 1/T_m, for 0.2 to 1.2 mM glassy solutions of chromyl bis(1-hydroxy-cyclohexanecarboxylic acid), CrO(HCA)⁻₂; aquo vanadyl ion, VO²⁺(aq), and vanadyl bis(trifluoroacetylacetonate), VO(tfac)₂were examined. At low temperatures where 1/T₁⪡ 1/T_m, 1/T_min 1:1 H₂O:glycerol is dominated by solvent protons. At low temperature 1/T_mincreases in the order 1:1 H₂O:glycerol or 9:1 CF₃CH₂OH:ethyleneglycol (no methyl groups) < 9:1i-PrOH:MeOH (hindered methyl groups) < 9:1n-PrOH:MeOH (less hindered methyl groups). This solvent dependence of 1/T_mis similar to that observed for nitroxyl radicals, which indicates that the effect of solvent methyl groups on spin-echo dephasing at low temperature is quite general. At higher temperatures the echo dephasing is dominated by spin–lattice relaxation and is concentration dependent. As the glass softens, echo dephasing is dominated by the onset of molecular tumbling.     

Pico-second photoelectric characteristic in manganite oxide La0.67Ca0.33MnO3 films

Ultrafast photoelectric characteristic has been observed in La_0.67Ca_0.33MnO₃ films on tilted SrTiO₃ substrates. A pico-second (ps) open-circuit photovoltage of the perovskite manganese oxide films has been obtained when the films were irradiated by a 1.064μm laser pulse of 25 ps duration. The rise time and full width at half-maximum of the photovoltage pulse are ～300 ps and ～700 ps, respectively. The photovoltaic sensitivity was as large as ～500 mV/mJ.     

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.     

Investigations of self-, H2- and He-broadening for rotational transitions of HCCC15N,CF3D and CF3CCH by the microwave transient emmission technique

The pressure dependence of coherent dephasing time T₂ has been determined by investigating transient emission signals of molecular gas samples, following pulsed microwave excitation. Experimental results on cyanoacetylene (HCCC¹⁵N), deuterated fluoroform (CF₃D) and 3,3,3-trifluoropropyne (CF₃CCH) are reported for the pure gas and also for mixtures with H₂ and He for rotational transitions in the frequency range from 5.8 GHz to 19.6 GHz.     

Microcavity polariton scattering probed by coherent control experiments

We present coherent control experiments which simultaneously probe both the coherence and the population dynamics of the exciton–photon polariton states in a semiconductor microcavity. The coherent manipulation of either the spin orientation or the density of polaritons is demonstrated leading to the measurement of the optical dephasing time. The polariton scattering by acoustical phonons or by mutual collision processes are investigated by a simultaneous measurement of both the optical dephasing time T₂and the decay time T₁of the radiant states. These results clearly evidence a quenching of the different scattering processes at resonance.     

Subpicosecond photon echoes by using nanosecond laser pulses

Subpicosecond time resolutions have been obtained in photon echoes when a sample was excited by two nanosecond dye laser pulses with a smooth and broad spectrum. The dye laser was pumped by second harmonics of a Q-switched Nd:YAG laser, and the pulse width was 10 ns. The sample was 3% Nd³⁺-doped silicate glass, and the center frequency of the dye laser was tuned at 5910 Å on resonance with the ⁴I_{$\text{9}\text{2}$} ? ²G_{$\text{7}\text{2}$}, ⁴G_{$\text{5}\text{2}$} transition of Nd³⁺. The homogeneous transverse relaxation time T₂ was measured to be 91 ps at 10 K in agreement with the previous measurements by picosecond pulses.     

Passive compression of KrCl excimer laser pulses in naphthalene solutions

The width of KrCl laser pulses has been compressed from 5.2 ns to less than 800 ps using naphthalene as the saturable absorber dye. It was found that the width of the compressed laser pulse decreased with both the input laser intensity and the concentration of naphthalene in the solution. The pulse shortening mechanism is attributed to excited state S₂-S_n transitions in naphthalene.     

Investigation on third-order nonlinear optical properties of two Au(dmit)2/PMMA thin films by Z-scan technique in picosecond pulse regime

The third-order nonlinear optical properties of two Au(dmit)₂/PMMA compound thin films, hexadecyltrimethylammonium bis(1,3-dithiole-2-thione-4,5-dithiolato)aurate and tetramethylammonium bis(1,3-dithiole-2-thione-4,5-dithiolato)aurate (abbreviated as MeAu and CtAu, respectively) with a doping concentration of 1?wt.% deposited on quartz-glass substrate were characterized by a single beam Z-scan technique at 1064?nm with 20?ps laser pulse width and 10?Hz repetition rate. The dominant nonlinear refraction and tiny nonlinear absorption of both materials lead to a larger possibility for them to be applied as promising candidates of all-optical switching. The results of two figures of merit, |W|?1 and |T|?1, were also calculated; this further validated the excellent properties of the materials for applications of the nonlinear optics.     

Biexponential intersubband relaxation in n-modulation-doped quantum-well structures

Intersubband scattering in an n-modulation-doped GaAs/Al_0.31Ga_0.69As quantum-well structure is systematically investigated as a function of temperature and pump intensity. For the first time biexponential relaxation is observed during infrared bleaching experiments. The fast component with a time constant of ∼1 ps, which represents the depopulation of the first excited well subband, is found to dominate the signal more and more with decreasing temperature and pump intensity. The decay time of the slower component rises with decreasing temperature from τ₂=8 ps atT=300 K to τ₂=23 ps atT=10 K. This component is believed to be connected with a carrier transfer to the potential minima in the barrier layers. The intensity dependent excitation mechanism and the relaxation processes are discussed with the help of detailed numerical simulations.     

Influence of zeolite water on paramagnetic and ferromagnetic resonances in the Co2[Nb(CN)8] · 8H2O molecular magnet

The contributions of Co²⁺ and Nb⁴⁺ ions to the high-frequency dynamic magnetic susceptibility of the Co₂[Nb(CN)₈] · 8H₂O molecular magnet in the paramagnetic state at T > 12 K are separated. It is found that the ferromagnetic ordering, which leads to the reconstruction of the electron paramagnetic resonance spectrum into the ferromagnetic resonance spectrum, occurs at T < 12 K. The influence of zeolite water on the spectra of the paramagnetic and ferromagnetic resonances is found. Dehydration leads to a decrease in the time of the spin relaxation of the ferromagnetic system from 50 ps to 17 ps at T = 4 K and to the variation in the temperature dependences of the widths of the lines and g factors in the electron spin resonance spectra.     

Vibrational dephasing in highly compressed liquid nitrogen studied with time-resolved stimulated raman gain spectroscopy

Abstract

In liquid nitrogen at 295 K we observe for the first time the minimum in the variation of the vibrational dephasing rate T^?1 ₂ with density at ρ = 2.15 × 10²². cm^?3. At higher densities the dephasing rate shows a steep rise with density. The observed behaviour shows good agreement with results of previously published molecular dynamics simulations.     

Photon echoes in single- and trilayer semiconductor films of different nanosized thicknesses and their properties

A femtosecond stimulated photon echo is detected for the first time in thin semiconductor films with thicknesses of 100, 800, and 2400 nm. It is established that relaxation time T ₁ varies with ZnO film thickness, taking values of 0.96, 2.96, and 4.312 ps at thicknesses of 2400, 800, and 100 nm, respectively. For ZnO/Si⁺/Si^? trilayer films, the relaxation time is T ₁ = 12.73 ps.     

High-energy sub-nanosecond optical pulse generation with a semiconductor laser diode for pulsed TOF laser ranging utilizing the single photon detection approach

Bulk and quantum well laser diodes with a large equivalent spot size of d _a /Γ _a  ≈ 3 µm and stripe width/cavity length of 30 µm/3 mm were realized and tested. They achieved a pulse energy and pulse length of the order of ~1 nJ and ~100 ps, respectively, with a peak pulse current of 6–8 A and a current pulse width of 1 ns. The 2D characteristics of the optical output power versus wavelength and time were also analyzed with a monochromator/streak camera set-up. The far-field characteristics were studied with respect to the time-homogeneity and energy distribution. The feasibility of a laser diode with a large equivalent spot size in single photon detection based laser ranging was demonstrated to a non-cooperative target at a distance of a few tens of meters.     

Coherent dynamics in InGaAs quantum dots and quantum dot molecules

We measure the dephasing time of the exciton ground state transition in InGaAs quantum dots (QD) and quantum dot molecules (QDM) using a sensitive four-wave mixing technique. In the QDs we find experimental evidence that the dephasing time is given only by the radiative lifetime at low temperatures. We demonstrate the tunability of the radiatively limited dephasing time from 400 ps up to 2 ns in a series of annealed QDs with increasing energy separation of 69–330 meV from the wetting layer continuum. Furthermore, the distribution of the fine-structure splitting δ₁ and of the biexciton binding energy δ_B is measured. δ₁ decreases from 96 to with increasing annealing temperature, indicating an improving circular symmetry of the in-plane confinement potential. The biexciton binding energy shows only a weak dependence on the confinement energy, which we attribute to a compensation between decreasing confinement and decreasing separation of electron and hole. In the QDM we measured the exciton dephasing as function of interdot barrier thickness in the temperature range from 5 to 60 K. At 5 K dephasing times of several hundred picoseconds are found. Moreover, a systematic dependence of the dephasing dynamics on the barrier thickness is observed, showing how the quantum mechanical coupling in the molecules affects the exciton lifetime and acoustic-phonon interaction.