High-order stimulated electronic Raman scattering from lithium vapor

An intense radiation at 395.0 nm has been observed when lithium vapor is optically pumped in a heat pipe with a pulsed dye laser whose output wavelength is tuned near the Li 2s–4s two-photon resonance transition. The radiation is emitted in the direction along the pump laser beam. It is proposed that the 395.0 nm radiation is mainly generated through three-photon excitation and one-Raman-photon scattering followed by two-cascade (spontaneous) emission. The overall reaction mechanism can be described by a parametric six-wave mixing process. The quantum efficiency of the observed process is estimated to be of the order of 2 × 10^–6.This work was partially supported by the USC Faculty Research and Innovation Fund     

Tunable picosecond infrared pulses generated by stimulated electronic Raman scattering of a mode-locked Ti:Sapphire laser in potassium vapor

A down-conversion to the mid-infrared region by using Stimulated Electronic Raman Scattering (SERS) in potassium vapor is described. The pump radiation is a frequency-doubled regeneratively amplified Ti:Sapphire laser with a pulse duration of 2 ps, pulse energy of 0.2 mJ, and repetition rate of 10 Hz. With the pumping frequency tuned around the potassium 4s-5p transition, nearly transform-limited infrared radiation tunable between 2.2 and 3.4 m has been generated with a peak infrared energy of 12 µJ, corresponding to a quantum efficiency of 17%, and with a pulse duration of 2 ps. The present tuning range could be extended by extending the tuning range of the pump laser. In comparison, intense infrared radiation of 90 µJ energy but with a very narrow tunability around 2.9 m has also been generated by SERS in barium vapor.     

Influence of gas circulation on stimulated Raman scattering and amplification of ultrashort laser pulses in methane

Applying gas recirculation in a high pressure cell, laser pulses of 1 ps at 400 nm and with a repetition rate of 1 kHz were frequency shifted by stimulated Raman scattering and amplification in methane gas at high pressure. We studied the influence of gas recirculation on the conversion efficiencies into the Stokes and anti-Stokes components as well as on their spatial distributions and spectral shapes using generator and generator-amplifier arrangements. For high pump energies, recirculation in the generator cell decreases conversion efficiency into the first Stokes component whereas it increases conversion into higher Stokes and anti-Stokes components. It results in a significantly improved spatial characteristics of the frequency-shifted radiation, however, is accompanied by a substantial spectral broadening. Using gas recirculation in the generator-amplifier arrangement we achieved a conversion efficiency into the first Stokes component of about 50% with highly improved spatial and spectral characteristics.     

Efficient multi-frequency generation of ultrashort light pulses using stimulated Raman scattering and optical parametric amplification

Optical parametric amplification of multi-frequency seed pulses generated in a mixture of compressed hydrogen and methane by stimulated Raman scattering of 1 ps, 1 kHz laser pulses at 395.8 nm has been studied. Efficient generation of spectrally narrow ultrashort pulses with a spatial distribution close to the Gaussian profile of the pump beam was obtained in the visible and near infrared ranges.     

Determination of temperature by stimulated raman scattering of molecular nitrogen,oxygen, and carbon dioxide

We have determined the temperature from SRS spectra of N₂-N₂, N₂-CO₂, O₂-O₂, and CO₂-CO₂ recorded in wide pressure and temperature ranges. The fitting procedure takes simultaneously into account the Dicke effect and motional narrowing. We have quantified the accuracy of the MEG and ECS-P models for rotational relaxation. The temperature extracted from each model is compared with thermocouple measurements. The influence of vibrational broadening and shifting is discussed in detail.     

Mechanism of phase conjugation via stimulated Brillouin scattering in narrow band gap semiconductors

We develop a theoretical model to study optical phase conjugation via stimulated Brillouin scattering (OPC-SBS) in narrow band gap transversely magnetized semiconductors. Threshold value of pump electric field and reflectivity of the image radiation for the onset of OPC-SBS are estimated. The analysis is applied to both cases viz. centrosymmetric (CS) and non-centrosymmetric (NCS) crystals. Numerical estimates made for n-type InSb crystal at liquid nitrogen temperature duly irradiated by nanosecond pulsed 10.6 μm CO₂ laser shows that high OPC-SBS reflectivity (90%) can be achieved in NCS crystals at moderate pump electric fields if the crystal is used as an optical waveguide with relatively large interaction length (L = 5 mm) which proves its potential in practical applications such as fabrication of phase conjugate mirrors.     

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.     

Cascaded compression of the first and second Stokes pulses during forward transient stimulated Raman amplification

The results of numerical modelling of cascaded compression of the first and second Stokes pulses during regenerative regime of the forward transient stimulated Raman amplification are presented for the case when the walk-off length of the first Stokes pulse due to group velocity mismatch is shorter than the length of the nonlinear medium. The influence of the initial amplitudes of the seed first Stokes pulses, its durations and its time delay with respect to the pump pulse, the Kerr nonlinearity of the medium on the conversion efficiency, duration and propagation factor M² of the first and second Stokes pulse are studied. It is demonstrated that for the pump pulse duration of 1 ps the duration of the compressed second Stokes pulses in a KGW crystal near the beam axis may be approximately 14 times shorter than the pump pulse duration. It is shown that the propagation factor of the compressed pulses increases significantly because of complex spatial-temporal dynamics of compression and the influence of Kerr nonlinearity of Raman medium.     

Efficient compression of femtosecond pulses by stimulated Raman scattering

Femtosecond pulses at 496 nm were Raman-shifted in methane with 20% efficiency. The pulse duration could be reduced up to 6.5 times from 560 fs at the fundamental to 85 fs at the Stokes frequency (580nm), which is the shortest pulse duration generated in this way. It was shown experimentally that chirped-pulse Raman scattering avoids the limitations arising from self-phase modulation.     

Stimulated raman scattering of fuel droplets

The strong stimulated Raman scattering (SRS) from diesel fuel droplets has the potential of providing the relative concentration of multicomponent fuel and the absolute size of individual droplets. The morphology-dependent resonances (MDRs) of a sphere cause the droplet to act as an optical resonator which greatly lowers the SRS threshold. The number density, quality factor, and frequency shift of several MDRs are calculated as a function of the ratio of the index of refraction of the liquid and the surrounding gas, which approaches unity at the thermodynamic critical condition for the fuel spray. The SRS spectra of monodispersed droplets of toluene, pentane, Exxon-Aromatic-150, and Mobil D-2 are presented. The exponential growth region of the SRS intensity I _1S as a function of the input laser intensity I _input is investigated for the toluene carbon ring breathing mode v ₂ and the pentane C-H stretching region. The I _1S ratio of toluene and pentane is measured as a function of the ratio of the toluene and pentane concentration for monodispersed droplets. The reduced fluctuation in I _1S when I _input is changed from multimode to single-mode is displayed as a histogram of the I _1S of the v ₂ mode of toluene droplets.     

Origin of low-frequency spectrum structure of four-photon scattering in liquid water

-1 has been found experimentally in liquid water. The theoretical interpretation relates these spectral features to an interference of strictional and orientational contributions to the scattered signal. Received: 16 October 1996     

Structural changes in excited states and photoisomers determined by time-resolved Raman scattering

Molecules in the excited singlet and triplet state and photoproducts occuring after photoisomerization or proton transfer are investigated by time-resolved resonance Raman and resonance CARS spectroscopy with nanosecond time resolution. From the time-resolved spectra information on structures and bond strengths of these short-lived species and on their kinetics are obtained.     

Threshold reduction of stimulated Brillouin scattering (SBS) using fiber loop schemes

SBS mirrors as self-pumped and easy to handle non-linear optical devices are frequently used in high-power laser systems for improving the beam quality based on optical phase conjugation. Because of the non-linear behaviour, a certain pulse energy or power of incident light is needed to generate enough reflectivity for practical purposes. Therefore, reducing this “threshold” is still a main topic in the development of new schemes for optical phase conjugation. In addition to the taper concept reported earlier, this paper deals with loop schemes for reducing the power requirements. A reduction of the so-called “threshold” by a factor of between two and four was obtained with the schemes investigated using liquids and fibers. Received: 4 September 2001 / Revised version: 22 October 2001 / Published online: 23 November 2001     

The interplay of thermal and pump fluctuations in stimulated Brillouin scattering

We present a experimental and theoretical investigation of spontaneously initiated stimulated Brillouin scattering in which the interplay of two independent noise sources (thermal and pump) can be studied by controlling the relative importance of each source. We vary the pump noise by adding a controlled amount of Gaussian noise to the input pulses, and we control the contribution of the thermal noise by examining the energy statistics of both entire scattered pulses and of temporal slices of the scattered pulses. We show that the energy of the whole Stokes pulses follow a Gaussian distribution but that the energy of the Stokes pulse slices do not.     

Dispersion of the third-order susceptibility of a cyanine dye measured by coherent anti-Stokes Raman scattering

The dispersion of the third-order susceptibility of the cyanine dye bis-(dimethylamino)-heptamethinium chloride was measured by Coherent Anti-Stokes Raman Scattering (CARS) over a wide wavelength range from 530 to 830 nm. Large negative values of the real part of the second-order hyperpolarizability are observed. The data are analyzed with the help of theoretical calculations based on a perturbative approach for the nonlinearities. The dispersion behavior of the third-order susceptibility is governed by the resonant enhancement due to vibrational transitions of the first excited electronic state and, to lesser extent, by an electronic two-photon resonance around 600 nm.     

Near-UV sub-Doppler spectroscopy on a metastable Mg beam by a frequency-doubled diode laser

Near-UV radiation is generated by doubling the frequency of a semiconductor laser in a nonlinear crystal. The crystal is contained in a resonant cavity in order to improve the conversion efficiency. The cavity increases the efficiency by about three orders of magnitude. This radiation has been used to perform spectroscopy of metastable magnesium in an atomic beam. We observed the (3s3p)³ P–(3s3d)³ D transition multiplet, which is of interest for metrological applications. The isotopic shift between²⁴Mg and²⁶Mg was measured and new information on the hyperfine structure of²⁵Mg was obtained. This radiation source is promising also in order to improve the Mg frequency standard.     

Coherent anti-Stokes Raman scattering velocimetry with nearly degenerate pumps

The time evolution of the anti-Stokes signal produced from the non-linear interaction of a short Stokes pulse and two long pump pulses that are nearly degenerate in frequency has been investigated. It is shown that this approach allows us to specify the accuracy of CARS (coherent anti-Stokes Raman scattering) velocimetry and to extend the range of operation of the method. In addition, an original optical scheme capable of delivering short visible pulses with good spatial and spectral properties is reported. The optical bench has been used for the characterisation of a low-pressure laminar Mach-10 flow. Received: 24 October 2001 / Revised version: 8 January 2002 / Published online: 14 March 2002     

Nonlinear behaviour of atomic fluorescence in mercury vapours following double-resonance laser excitation

When mercury atoms, present with a buffer gas (N₂ or Ar) in a quartz cell or in a graphite furnace are excited into the 7³ S ₁ level by means of two pulsed dye lasers tuned at 253.652 nm (6¹ S _o 6³ P ₁) and 435.835 nm (6³ P ₁ 7³ S ₁), a laser-like, collimated emission is observed along the axis of the cell at the green mercury line (7³ S ₁ 6³ P ₂), 546.074 nm). This radiation exhibits a pronounced non-linear dependence upon the number density of the mercury atoms in the cell. This behaviour is interpreted as being due to amplified spontaneous emission (ASE), which occurs as a result of the transient population inversion between the 7s ³ S ₁ and 6p ³ P ₂ ^o levels. The parameters governing the population inversion can be deduced by applying a rate equation analysis to the atomic system. A time-resolved observation of both ASE and spontaneous fluorescence signals confirms the totally different characteristics of the two emission processes.     

Magnetic-grating free-induction decay and magnetic-grating echo using ultrafast excitation pulses

The interaction of atoms with ultrafast, counterpropagating optical fields is considered. The magnetic degeneracy and hyperfine splitting of the atomic levels are included in the calculations, which are carried out for arbitrary polarizations of the incident fields. The counterpropagating fields produce spatial harmonics in the ground state density matrix (gratings) which can be monitored by backscattering of a traveling wave probe pulse. Two types of excitation schemes are analyzed. The Magnetic-Grating Free-Induction Decay (MGFID) consists of excitation with a single counterpropagating wave field, while the Magnetic-Grating Echo (MGE) involves excitation by two counterpropagating wave fields, separated in time by T. The atomic response to the probe pulse is calculated in lowest-order perturbation theory for atoms cooled below the Doppler limit of laser cooling. Both the MGFID and MGE signals consist of pulses having a duration of order of the excited state lifetime, modulated at frequencies corresponding to the various hyperfine transitions. As a function of the delay between pulses, the signals oscillate at frequencies determined by the ground state hyperfine splittings. General expressions for the MGFID and MGE signals are derived and specific results are presented for the D₂ line in Na.