High efficiency long pulse FIR Raman conversion in ammonia

Generally the quantum efficiency of FIR Raman generation in molecular gases is below the theoretical value. This disagreement is particularly evident in Raman scattering from pulsed sources with short pulse length, when the vibrational saturation limits the power conversion. Other nonlinear processes can overcome this saturation, but they require a very intense pump power for too short a time to use the FIR radiation in high sensitive experiments with heterodyne detection. This is the case, for instance, of RFWM. In this work we describe the experimental conditions to achieve a high efficiency 90 micron Raman conversion in ammonia, with both short and long pulses.     

Investigation of SRS conversion of XeCl laser emission in lead vapor,methane, and hydrogen

We have thus optimized the conditions for SRS conversion of XeCl-laser emission in lead vapor, methane, and hydrogen. The greatest influence on the conversion efficiency is exerted for an SRS cell with lead by the divergence of the pump radiation, the focusing geometry, and the type of buffer gas. The maximum efficiency with respect to absorbed UV energy was ∼57% when xenon gas was used as the buffer, corresponding to 85% of the photon efficiency. The converted radiation could be continuously tuned in the 457.6–459.3 nm band. Addition of a light gas such as helium or hydrogen to methane raised the efficiency of conversion into Stokes components in methane to ∼24 %.     

Low-threshold lasing in stimulated Raman lasers with nanosecond pumping

We have studied the conditions resulting in maximum lowering of the excitation threshold for pulsed stimulated Raman (SRS) lasers. It has been shown theoretically that in order to achieve the lowest possible values of laser radiation pulse energy needed to excite lasing in SRS lasers, we need high reflection of the cavity mirrors and low losses at the wavelength of the 1st Stokes component, high reflection of the output mirror at the wavelength of the pump radiation, and also matching of the confocal parameters for the exciting laser radiation and the cavity with each other and with the length of the Raman-active medium. The experimentally achieved excitation threshold for an SRS laser based on a barium nitrate crystal was 6 μJ, which quantitatively corresponds well to the calculation results. Lasing of up to five Stokes components simultaneously occurred. The efficiency for conversion of the laser radiation to one component was as high as 39%. __________ Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 75, No. 2, pp. 284–290, March–April, 2008.     

SRS generation under phase matching conditions for four-wave interactions of SRS components in birefringent Raman-active crystals

The possibilities of efficient four-wave SRS generation in the schemes of cavity and cavity-amplifier SRS converters with the implementation of phase matching conditions for four-wave mixing of different SRS radiation components at an appropriate orientation of birefringent SRS crystals have been considered based on a numerical simulation. The threshold characteristics and achievable energetic parameters of the SRS generation of different frequency radiation components have been analyzed under the conditions of implementation of phase matching for four-wave mixing. Conditions have been found for a low-threshold SRS-four-wave mixing generation of an anti-Stokes wave with a conversion efficiency of up to 40%, as well as of the first, second, and third Stokes SRS components with conversion efficiencies of up to 90, 80, and 30%, respectively.     

Nonlinear frequency conversion of copper vapor laser radiation using convergent and parallel laser beams

Results of experiments are presented on the comparison of the efficiency of radiation generation at the sum frequency (λ=0.271 μm) of copper vapor laser (CVL) in a nonlinear DKDP crystal using either convergent or parallel laser beam. An intensity of UV radiation of 0.34 W and a conversion efficiency of 6% obtained under conditions of strong focusing occur to be substantially lower as compared to those obtained using a parallel laser beam of the same power (0.73 W and 12%, respectively). Experimental data on the structure of a CVL beam generated with an unstable resonator are presented, and physical reasons for the limitation of the efficiency of nonlinear frequency conversion are analyzed.     

Upconversion of IR radiation into the visible and UV ranges

A review of theoretical and experimental results on the upconversion of IR radiation due to resonant nonlinear phenomena in metal vapors is presented. Various experimental schematics providing high quantum conversion efficiency and the feasibility of converting an arbitrary IR wavelength are discussed.     

Numerical optimization of the extracavity Raman laser with barium nitrate crystal

The radiation transfer equations of the extracavity Raman laser including up to the third Stokes beams and backward Raman scattering terms were deduced in detail from the wave equation and material equations of stimulated Raman scattering. The radiation transfer equations were solved numerically to optimize the performance of the extracavity Raman lasers with barium nitrate crystal as the nonlinear medium. The optimum reflectivity of the output coupler at the first Stokes was figured out numerically to achieve the maximum conversion efficiency of the first Stokes, and found to be closely related to the pump pulse duration, peak intensity of the pump pulse, and Raman crystal length. With the resonator mirrors highly reflective at the first Stokes, the highest conversion efficiency of the second Stokes was obtained when the input mirror was highly reflective at second Stokes, whereas the output coupler was highly transmissive at the second Stokes. It was found that too high intracavity intensity of the second Stokes would impede the efficient energy extraction from the pump pulse to the first Stokes, and consequently, limit the conversion efficiency of the second Stokes.     

All-optical probing of the nonlinear acoustics of a crack

Experiments with an all-optical method for the study of the nonlinear acoustics of cracks in solids are reported. Nonlinear acoustic waves are initiated by the absorption of radiation from a pair of laser beams intensity modulated at two different frequencies. The detection of acoustic waves at mixed frequencies, absent in the frequency spectrum of the heating lasers, by optical interferometry or deflectometry provides unambiguous evidence of the elastic nonlinearity of the crack. The high contrast in crack imaging achieved by remote optical monitoring of the nonlinear acoustic processes is due to the strong dependence of the efficiency of optoacoustic conversion on the state of the crack. The highest acoustic nonlinearity is observed in the transitional state of the crack, which is intermediate between the open and the closed ones.     

Single-walled carbon nanotubes formation with a continuous CO2-laser: experiments and theory

It has been proved [1] that the use of a CO₂-laser system operating in continuous wave mode (cw) can be efficiently used for the production of carbon single-walled nanotubes (SWNTs). In this article we first describe in detail the variable experimental conditions (different ambient gases, static gas pressure, and gas flow) for SWNT formation and summarize the results of the characterization studies of the synthesized materials. Second, we analyze the influence of the different experimental conditions on the SWNTs formation process. We show that the heat transport, kinetic, and diffusion processes allow us to explain seemingly different formation conditions in a qualitative and semi-quantitative agreement with the experimental results. The presented self-consistent scenario for nanotube formation in a gas phase allowed us to propose future experiments on testing the mechanism of nanotube formation.     

Low- and high-order harmonic generation inside an air filament

We report on the generation of third-order (TH) and high-order harmonics (HH) directly inside a self-guided femtosecond filament in air. By terminating the filament with a steep density gradient behind a pinhole placed at different distances from the geometric focus, the evolution of the generated radiation is tracked along the nonlinear interaction zone. Spectra are recorded in the visible (VIS), ultraviolet (UV) and extreme ultraviolet (XUV) spectral range under identical conditions. The VIS and UV spectral bandwidth undergoes significant broadening. The input pulse parameters are varied systematically to optimize the TH bandwidth. Recorded spectra show Fourier-limits below 5 fs pulse duration centered at 264 nm wavelength. We observe conversion to HH up to the 25th order and use the HH generation process as a nonlinear probe for the on-axis intensity evolution along the filament.     

Relativistically strong electromagnetic radiation in a plasma

Physical processes in a plasma under the action of relativistically strong electromagnetic waves generated by high-power lasers have been briefly reviewed. These processes are of interest in view of the development of new methods for acceleration of charged particles, creation of sources of bright hard electromagnetic radiation, and investigation of macroscopic quantum-electrodynamical processes. Attention is focused on nonlinear waves in a laser plasma for the creation of compact electron accelerators. The acceleration of plasma bunches by the radiation pressure of light is the most efficient regime of ion acceleration. Coherent hard electromagnetic radiation in the relativistic plasma is generated in the form of higher harmonics and/or electromagnetic pulses, which are compressed and intensified after reflection from relativistic mirrors created by nonlinear waves. In the limit of extremely strong electromagnetic waves, radiation friction, which accompanies the conversion of radiation from the optical range to the gamma range, fundamentally changes the behavior of the plasma. This process is accompanied by the production of electron–positron pairs, which is described within quantum electrodynamics theory.     

Electro-optic detection of continuous-wave mid-infrared radiation

We demonstrate coherent detection of continuous-wave mid-infrared radiation. This radiation is produced by use of conventional difference-frequency mixing and detected via the linear electro-optic effect. The detection process allows for the simultaneous measurement of the amplitude and phase properties of the infrared field. Both processes require an amplitude-modulated optical beam that is derived from the superimposed output of two single-frequency lasers. With appropriate choice of lasers and nonlinear optical crystals, the technique may be applied to any wavelength throughout the far and mid infrared.     

Spatiotemporal dynamics of the amplitude-phase characteristics of stimulated Raman scattering

A numerical model describing the processes of generation of stimulated Raman scattering (SRS) is developed; the calculations are performed and different scenarios of generation of Stokes radiation in compressed hydrogen are analyzed. The spatiotemporal profiles of intensities and phases of interacting waves, the radiation spectra, and the functions of spatial coherence are obtained by way of numerical simulation for different conditions of SRS generation. A substantial difference between these parameters in the cases of nonstationary and quasi-stationary regimes of SRS generation is revealed. The nonstationary regime of generation is characterized by more complicated spatiotemporal dependences than the quasi-stationary regime. However, in the quasi-stationary regime, the phase of the Stokes wave radiation varies over a larger interval during the pump pulse duration, which leads to a decrease in the degree of spatial coherence to lower values. For both regimes of generation, the value of the degree of spatial coherence decreases with an increase in the conversion factor to a certain threshold value and then stabilizes, which is in agreement with experimental data. The presence of a moving focus of SRS focusing of the Stokes beam is demonstrated. This effect is governed by the spatiotemporal shape of the pump beam intensity (the Gaussian profile), by a high SRS gain, and by the processes of diffraction. The results of the numerical simulation are in qualitative and quantitative agreement with experimental data obtained previously.     

非均匀等离子体中受激Raman散射非线性行为

鉴于实际中等离子体不均匀性和非周期性边界条件，建立了受激Ｒａｍａｎ散射（ＳＲＳ）和受激Ｂｒｉｌｌｏｕｒｉｎ散射（ＳＢＳ）非线性耦合模型。ＳＢＳ对ＳＲＳ的影响主要表现在两方面：１）Ｌａｎｇｍｕｉｒ波与离子声波的非线性相互作用，２）ＳＢＳ与ＳＲＳ的竞争。本文研究了离子声衰变不稳定性、离子声波对Ｌａｎｇｍｕｉｒ波的非共振散射两种非线性过程在ＳＲＳ发展过程中的作用，给出一维不均匀等离子体中ＳＲＳ发展图象。Ｌａｎｇｍｕｉｒ波向短波转换，从而被强烈阻尼是抑制ＳＲＳ的重要机制。文中给出了ＳＢＳ／ＳＲＳ耦合过程中决定ＳＲ 关键词：     

Advantages of plasma harmonic generation using high pulse repetition rate lasers: Review of recent studies

The studies of coherence properties of the harmonics generating in laser-produced plasmas, the analysis of the optical nonlinearities of deoxyribonucleic acid components, the resonance enhancement of harmonic in the cases of excitation of indium plasma by multi- and few-cycle pulses, and the application of nanoparticle-based emitters of harmonics using high-pulse repetition rate lasers are reviewed. The analysis of various aspects of plasma harmonic generation at the conditions of optimal excitation of the ablated targets irradiating by 1 kHz lasers is presented. The growth of plasma harmonic conversion efficiency, single harmonic emission, nonlinear spectroscopy of complex organic components, as well as high coherency of harmonic radiation show the advantages of using plasma harmonic technique for optimization of the sources of coherent extreme ultraviolet radiation and for the material science studies. These studies allowed a significant growth of the average power of harmonics compared with the case of 10 Hz lasers.     

Pump spectral linewidth influence on stimulated Brillouin scattering (SBS) and stimulated Raman scattering (SRS) and self‐termination behavior of SRS in liquids

The threshold, temporal behavior, and conversion efficiency of stimulated Brillouin scattering (SBS) and stimulated Raman scattering (SBS) in three liquids (benzene, hexane, and dimethyl sulfoxide) and two crystals (calcite and barium nitrate) have been investigated under three largely different spectral linewidth conditions. Pumped with 532‐nm and nanosecond duration laser pulses of ≤ 0.01 cm^?1 linewidth, only SBS can be generated in all tested liquids with a high nonlinear reflectivity. However when the pump spectral linewidth is ～0.07 cm^?1 or ～0.8 cm^?1, both SBS and SRS can be observed in benzene while only SRS can be generated in dimethyl sulfoxide; in all these cases SRS is the dominant contribution to the stimulated scattering but the efficiency values are drastically decreased due to the self‐termination behavior of SRS in liquids, which arises from the thermal self‐defocusing of both pump beam and SRS beam owing to Stokes‐shift related opto‐heating effect. In contrast, for SRS process in the two crystals, the thermal self‐defocusing influence is negligible benefitting from their much greater thermal conductivity, and a higher conversion efficiency of SRS generation can be retained under all three pump conditions.