Generation of multi-color stimulated raman emission from two-color linearly or circularly polarized pump beams

A laser beam at two different frequencies separated by 587 cm^–1 is focused into pressurized hydrogen (rotational transition energy, 587 cm^–1) to generate multi-color stimulated Raman emission. The polarization state and the pulse energy are measured for each generated emission line using linearly and circularly polarized pump beams. The effect of the polarization is discussed by using a parameter characterizing the polarizability of hydrogen and a conservation rule for the angular momentum in four-wave mixing. Many rotational lines are generated with linearly polarized pump beams through a four-wave mixing process. This is in striking contrast to the results obtained by using a single-color circularly polarized pump beam which generates only one rotational line through a conventional stimulated Raman process.     

Generation of high-order rotational lines by four-wave Raman mixing using a high-power picosecond Ti:Sapphire laser

More than thirty rotational lines equally spaced by 587 cm^–1 are generated simultaneously in the vicinity of the fundamental line by four-wave Raman mixing using a high-power picosecond Ti:Sapphire laser as a pump source and hydrogen as a Raman medium. Since the wavelength of this multifrequency laser emission extends from the near-infrared to the near-ultraviolet, it can be utilized as a tunable light source for picosecond spectroscopy. Because of the wide spectral bandwidth available, this procedure has great potential for the generation of ultrashort laser pulses by mode-locking these emission lines.     

Stimulated Raman scattering and four-wave Raman mixing seeded by a supercontinuum generated in dibromomethane using picosecond and femtosecond laser sources

Stimulated Raman emission from liquid dibromomethane (vibrational Raman shift frequency, 588 cm⁻¹) is introduced into hydrogen gas (rotational Raman shift frequency, 587 cm⁻¹) as a seed beam, in order to generate numerous rotational lines by four-wave Raman mixing. Unexpectedly, a supercontinuum, which is generated by self-phase modulation in dibromomethane, acted as a seed beam to exclusively generate vibrational lines; the rotational lines are generated only when the supercontinuum is minimal. The former is explained by a competition between the high-gain vibrational and low-gain rotational Raman effects when strongly seeded by a supercontinuum. The latter is explained by stimulated Raman gain under the seed effect exclusively to the first-Stokes rotational line.     

Thermal loss mechanism in the generation of multifrequency laser emission via stimulated Raman scattering and four-wave Raman mixing studied by photothermal refraction spectroscopy

The heat produced in conjunction with the processes of stimulated Raman scattering and four-wave Raman mixing in hydrogen was measured by photothermal refraction spectroscopy. Many vibrational, rotational, and vibrationally shifted rotational Raman lines are exclusively/simultaneously generated by changing the polarization of the laser beam and the hydrogen pressure. Thermal loss occurs predominantly from vibrational Raman scattering, which can be ascribed to a large Raman shift frequency of 4155 cm^-1 for the vibrational transition. In contrast to stimulated Raman scattering, little or no thermal loss is observable during the process of four-wave Raman mixing. Received: 12 April 1999 / Revised version: 12 July 1999 / Published online: 20 October 1999     

High resolution emission spectra of laser-excited molecular iodine as the excitation frequency is tuned through and away from resonance

We have studied the ΔJ = 2 rotationally shifted emission lines in the region of the strong absorption of molecular iodine which occurs within the 5145 Å argon ion laser line. We used an etalon tuned, single frequency argon ion laser with a linewidth of 20 MHz to excite the iodine emission and recorded the spectra of the rotational lines with Fabry-Perot spectrometers having resolutions up to 70 MHz (0.0023 cm^-1). To overcome Doppler linewidth limitations we took spectra of the emission at small angles to the exciting beam and found the lines to have widths less than our instrumental resolution and frequencies which accurately tuned with the incident laser frequency. We recorded the emission lines for laser frequencies in the absorption line center and out into the absorption wing. Our spectra show that the intensity of the emission lines follows the absorption line profile while the frequency of the emission lines is determined by the laser frequency; the intensity is maximum at the absorption line center, falling by 10⁴ as the laser frequency is moved off the line center, while the line position maintains a constant frequency shift from the laser frequency.     

Efficiently generated rotational and vibrational stimulated raman emission by means of a two-color laser beam

When a two-color laser beam is introduced into pressurized hydrogen, about 40 laser emission lines are generated from the ultraviolet to the visible regions. This phenomenon is ascribed to the stimulated Raman effect due to a combination ofJ=1 J=3 rotational andv=0 v=1 vibrational transitions. By introducing the two-color laser beam, the threshold for generation of the rotational line is substantially reduced. The present phenomenon is attributed to four-wave mixing, which allows efficient generation of higher-order rotational and vibrational Raman lines.     

Assignments of optically pumped CD3OH laser lines

Six FIR laser lines from CD₃OH pumped by the 10R(36) and the 10R(18) CO₂ laser lines are assigned to specific rotational energy levels in the excited C–0 stretch state. It is found that their upper laser levels are shifted by a Fermi resonance between the C–0 stretch vibration and the third and forth harmonics of the torsional mode. The Fermi resonance shifts are +0.332 cm^–1 and +2.251 cm^–1 for the upper laser levels pumped by the 10R(36) and the 10R(18) CO₂ laser lines, respectively. Calculated frequencies of the pump and the laser transitions agree with those of the pump CO₂ laser lines and the observed FIR laser lines within estimated accuracy.     

The rotational resonance Raman spectrum of nitrogen dioxide and the determination of electronic state symmetry from resonance Raman selection rules

The pure rotational Raman spectrum of nitrogen dioxide has been observed and shown to be consistent with existing determinations of molecular parameters. Upon observation at 600 Torr pressure and 0.4 cm⁻¹ resolution a well-defined rotational spectrum is obtained. This spectrum is overlaid with a number of fluorescence lines. The fluorescence lines are separated from the Raman spectrum by a comparison of Stokes and anti-Stokes branches of the rotational spectrum. Out of seven strong fluorescence lines seen with 5145 Å excitation, five probably are identifiable with vibration-rotation fluorescence progressions observed by Abe.The most striking feature of these observations is the potential use of the resonance Raman effect for the analysis of complicated electronic spectra. When this rotational spectrum is observed with excitation by 5309 Å or 5145 Å excitation, the Raman spectrum follows a-axis selection rules and the Q-branches are in the noise level or barely out of it. However, at 4880 Å the ΔK = 2Q-branches become a major feature of a spectrum, indicating that an appreciable part of the absorption at this wavelength is occurring through the operation of b- or c-axis selection rules. These findings are consistent with present notions of a ²B₂ excited state dominating absorption at longer wavelengths, while at shorter wavelengths a ²B₁ excited state becomes important. Given a tunable laser, one could map the relative importance of these two possible selection rules for NO₂ without any theoretical analysis more sophisticated than that presented in this paper.A simplified statement of the selection rules for resonance rotational Raman spectra of asymmetric tops has been developed in the course of this investigation. No attempt has been made to refine the rotational parameters of NO₂ since all of the lines seen areunresolved multiplets. Our data should be regarded as a search spectrum preliminary to investigation on a high resolution instrument.     

A Semiconductor Laser of the Visible Range as an Exciting Source of Raman Scattering

A possibility of application of semiconductor lasers of the visible range as exciting sources for Raman spectroscopy is studied. An experimental set-up for measuring Raman spectra of polycrystalline dielectrics and broad-gap semiconductors excited by a semiconductor laser with a wavelength of 640 nm was created. The conditions under which the spectral width of the lasing line of a semiconductor laser was within 10^-3 cm^-1 in the continuous mode with a power of 10 mW are realized. The characteristics of various types of exciting sources used in Raman spectroscopy are compared. The results of studies of the characteristic Raman spectra excited with a semiconductor laser in polycrystalline sulfur are presented.     

Photodissociation effects on pulsed laser deposited silver oxide thin films: surface‐enhanced resonance Raman scattering

Temporal Raman scattering measurements with 488, 532 and 632 nm excitation wavelengths and normal Raman studies by varying the power (from 30 W/cm² to 2 MW/cm²) at 488 nm were performed on silver oxide thin films prepared by pulsed‐laser deposition. Initially, silver oxide Raman spectra were observed with all three excitation wavelengths. With further increase in time and power, silver oxide photodissociated into silver nanostructures. High‐intensity spectral lines were observed at 1336 ± 25 and 1596 ± 10 cm⁻¹ with 488 nm excitation. No spectral features were observed with 633 nm excitation. Surface‐enhanced resonance Raman scattering theory is used to explain the complex behavior in the intensity of the 1336/1596 cm⁻¹ lines with varying power of 488 nm excitation. Copyright © 2011 John Wiley & Sons, Ltd.     

Volume effect of laser produced plasma on X-ray emissions

An investigation of x-ray emission from Cu plasma produced by 1.054 μm Nd:glass laser pulses of 5 ns duration, at 2 × 10¹² − 2 × 10¹³ W cm⁻² is reported. The x-ray emission has been studied as a function of target position with respect to the laser beam focus position. It has been observed that x-ray emissions from ns duration plasma show a volume effect similar to subnanosecond plasmas. Due to this effect the x-ray yield increases when target is moved away relative to the best focal plane of the laser beam. This result supports the theoretical model of Tallents and has also been testified independently using suitably modified theoretical model for our experimental conditions. While above result is in good agreement with similar experimental results obtained for sub-nanosecond laser produced plasmas, it differs from result claiming filamentation rather than pure geometrical effect leading to x-ray enhancement for ns plasmas.     

Narrow-linewidth passband filter for ultraviolet rotational Raman imaging

We present a narrow-passband spectral filter capable of frequency-resolved imaging of rotational Raman light scattering with strong spectral rejection of out-of-band Raman, Rayleigh, and Mie scattering. The filter is based on mercury-vapor absorption, and subsequent resonant fluorescence and has a passband of less than 1 cm(-1). It is paired with an injection-seeded, cavity-locked, frequency-tripled Ti:sapphire laser that produces >30 mJ/pulse of single-mode, tunable light in the vicinity of 253.7 nm. The laser and filter are combined to spectrally resolve scattering from individual rotational Raman lines of nitrogen and oxygen.     

Tuning characteristics of a high pressure CO2 laser pumped CH3F Raman laser

Conclusion We described a CH₃F Raman laser pumped by a two stage 20 atmospheres CO₂ laser. The emission spectrum of the CH₃F laser at 11 Torr extends from 23 cm^–1 to 45 cm^–1 when the CO₂ laser is scanned over the 9R emission branch at a fixed pump power of 180 mJ. The emission spectrum shows a strong structure with large parts where the FIR energy decreases to zero. This fact makes the use of such a laser for spectroscopic scanning experiments in the FIR difficult. The laser is, however, very suited for working at fixed but adjustable FIR frequencies. The pulse energy in the maxima of the emission characteristics at a pump energy of 180 mJ exceeds 300 J, which corresponds a photon conversion coefficient of more than 6%.     

Doppler-limited dye laser excitation spectroscopy of DNO: Predissociation of DNO

The cw dye laser excitation spectrum of the (110)-(000) and (021)-(000) vibronic bands of the system of DNO was observed between 16530 and 16860 cm⁻¹ with Doppler-limited resolution. A rotational analysis of the two bands gave values for the rotational constants and centrifugal distortion constants. DNO was produced by the pyrolysis method and more than 1200 lines were observed in the two bands. A total of 1112 of these lines could be assigned to 9 and 11 subbands of the (110)-(000) and (021)-(000) bands, respectively. The molecular constants determined reproduce the observed transition frequencies with an average deviation of 0.011 and 0.008 cm⁻¹, respectively. Extensive perturbations in the excited state were found in most of the subbands. “Extra” lines were observed in connection with several of these perturbations. Accurate determination of the dissociation energy has been obtained; D₀ = 17010 ± 10 cm⁻¹.     

Partly tunable mid-infrared NH3 laser

Using a continously tunable pulsed 20-atmosphere CO₂ laser as a pump source, we generated pulses of mid-infrared radiation, partly tunable in frequency intervals in the range between 200 and 900 cm^–1 via stimulated Raman scattering in gaseous ammonia. As a Raman cell we used a multiple pass cell. We observed for¹⁴NH₃ and¹⁵NH₃ laser lines at 52 different frequencies with 39 lines observed for the first time. Tuning ranges up to 150 GHz and peak powers of several MW were achieved. The quantum efficiency reached 40 %.     

皮秒激光抽运高压H_2的受激拉曼散射研究

利用Nd :YAG锁模序列脉冲激光 (10 6 4nm)抽运充有高压H2 的拉曼池 ,输出光束经棱镜分光后投射在屏上 ,在可见光及近紫外光区用彩色胶卷摄得 15个受激拉曼散射光斑 ;经 1m光栅摄谱仪摄谱 ,在 36 5— 6 0 5nm波长范围内得到 6 5条受激拉曼谱线 .通过实验结果与理论计算值的比较 ,证明除了H2 的振动拉曼频移量 4 15 4 6cm- 1 外 ,还有多个振动及转动拉曼频移量共同参与作用 ,从而产生了从紫外到红外众多波长的受激拉曼散射光 .     

A comparative performance evaluation of micro-Raman spectrograph using holographic notch filter and dielectric filter

An indigenously designed and developed micro-Raman spectrograph, consisting of a diode-pumped solid-state green laser for the excitation of Raman scattering, a Raman imaging microscope, CCD as a detector and a notch filter, has been extensively studied to evaluate its performance. A dielectric edge filter (having 27 alternate layers of SiO₂ and TiO₂) and a holographic notch filter (Oriel make) have been used to block the Rayleigh scattered light from the sample to the entrance slit of the spectrograph. Holographic notch filter is found to be able to record the Raman shifts below 700 cm⁻¹ conveniently whereas dielectric edge filter (27 layers) has enabled the spectrograph to record the Raman spectra very efficiently after a wave-number shift of 700 cm⁻¹. It has also been observed that the instrument using the edge filter provides a peculiar spectrum consisting of three spectral lines having Raman shifts as 569, 1328 and 1393 cm⁻¹ in the Raman spectrum of a weakly scattering sample with large reflectivity. Similarly, a spectrum consisting of multiple lines has been observed when the instrument is being operated using a holographic notch filter. These spectral lines are not observed in the case of liquid samples such as benzene, carbon tetrachloride, ethanol, diethyl ether etc. The origin of these peculiar spectral lines has been briefly discussed in the paper. Additionally, a major motivation for this work is to utilize the results for the selection of an appropriate filter depending on the type of the sample, i.e. weakly scattered and highly reflecting sample or highly scattered and low reflecting sample.     

Picosecond pulse generation in a benzene raman generator amplifier system

Picosecond ruby laser pulses generate simultaneously Stokes pulses of the 992 cm^–1 ring breathing mode and of the 3063 cm^–1 CH-stretching mode of benzene in a Raman generator cell by stimulated Raman scattering under self-focusing conditions. The Raman generator light is spectrally filtered, collimated, and amplified in three Raman amplifier cells pumped by ruby laser pulses. Both first Stokes lines have been selectively amplified to short, low divergence, intense light pulses.     

R branch tuning characteristics of the13CH3F Raman FIR laser

Summary We described a¹³CH₃F Raman laser pumped by a grating tuned 20 atmospheres CO₂ laser. The emission characteristics of the¹³CH₃F laser extends from 14 cm^–1–35 cm^–1 and from 49 cm^–1–72 cm^–1; about 65% of these frequency ranges can be covered with tunable radiation. The characteristics shows a strong dependence on the rotaional quantum numbers of the states involved in the Raman laser transitions and, within each tuning interval, on the frequency offset with respect to the frequencies of resonant transitions. We obtained, at 51 cm^–1, a maximum FIR laser pulse energy of about 800 J (at a pump energy of 200 mJ), corresponding to a photon conversion of about 8%. In some cases we have observed simultaneous emission at a Raman and a cascade frequency. In addition, FIR emission power dependence on¹³CH₃F gas pressure and pump pulse power were investigated for different J quantum numbers.     

Powerful tunable infrared generation by stimulated Raman scattering

We report the generation of powerful infrared radiation continuously tunable between 14 000 and 2 300 cm^-1. The beam is either the output of a dye laser (with a linewidth of 0.07 cm^-1 and a full angle divergence of 0.2 mrd) or its Raman shifted components. We have obtained 20 to 60 MW peak power between 14 000 and 9 700 cm^-1, 5 to 20 MW between 9 700 and 5 500 cm^-1 and 0.5 to 2 MW between 5 500 and 2 300 cm^-1. As an application we measured the hyperpolarizability of some organic molecules.