Beryllium Silicate,Be2SiO4 (phenakite) – a Novel Trigonal SRS‐Active Crystal

In single crystals of the beryllium silicate Be₂SiO₄ with trigonal symmetry , known also as the mineral phenakite, χ⁽³⁾‐nonlinear lasing by stimulated Raman scattering (SRS) is investigated. All observed Stokes and anti‐Stokes lasing components are identified and ascribed to a single SRS‐promoting vibration mode with ω_SRS ≈876 cm⁻¹. With picosecond single‐wavelength pumping at one micrometer the generation of an octave‐spanning Stokes and anti‐Stokes comb is observed.     

Orthorhombic YAlO3 – a novel many‐phonon SRS‐active crystal

In single crystals of orthorhombic YAlO₃, widely known as a host‐matrix for Ln³⁺‐lasant ions, many‐phonon stimulated Raman scattering interactions as well as different manifestations of cascaded and cross‐cascaded nonlinear χ⁽³⁾↔χ⁽³⁾ processes are initiated by picosecond laser pulses. The scientific and applicative potential of YAlO₃ crystals is considerably expanded by the demonstration of its SRS properties. In particular, the studies revealed the manifestation of eight χ⁽³⁾‐active vibrational modes. The corresponding Stokes and anti‐Stokes lines have been assigned and the steady‐state Raman gain coefficients related to the strongest phonon mode have been estimated. In addition, a short review presents the stimulated emission channels of its Ln³⁺‐ions together with some χ⁽³⁾‐nonlinear laser properties of crystals belonging to the binary Y₂O₃‐Al₂O₃ system.     

Cerussite,PbCO3 – a new Stimulated Raman Scattering (SRS)‐active crystal with high‐order Stokes and anti‐Stokes lasing

Orthorhombic PbCO₃, known as natural crystal cerussite, is presented as a new Stimulated Raman Scattering (SRS)‐active crystal. With picosecond laser pumping high‐order Raman‐induced χ⁽³⁾ generation is observed. All registered Stokes and anti‐Stokes sidebands in the visible and near‐IR are identified and attributed to the SRS‐promoting phonon mode A_1g of the carbonate group, with ω_SRS ≈ 1054 cm⁻¹. The first Stokes steady‐state Raman gain coefficient in the visible spectral range is estimated as well to a value not less than 4.6 cm·GW⁻¹.     

Stimulated Raman scattering in natural crystals of fluorapatite,Ca5(PO4)3F

Hexagonal Ca₅(PO₄)₃F, known as natural crystal fluorapatite and oldest host‐crystal for Ln³⁺‐lasant ions, is presented as a Raman‐active material. High‐order Raman‐induced χ⁽³⁾‐nonlinear processes are discovered in natural crystals of fluorapatite under picosecond pumping at 1.064 μm and 0.532 μm wavelength. A multitude of Stokes and anti‐Stokes components is generated in the ultraviolet, visible and near‐infrared spectral region by stimulated Raman scattering (SRS) and Raman four‐wave mixing (FWHM), resulting in a frequency comb with a width of 520 THz. The spectral lines are identified and attributed to the ν₁(A_g) vibration mode of the tetrahedral [PO₄] units which is related to a Raman shift of ω_SRS ≈ 965 cm⁻¹. The first Stokes steady‐state Raman gain coefficient in the near‐infrared spectral range is estimated to be >0.38 cm·GW⁻¹. Finally, a short review of SRS‐promoting vibration modes and observed χ⁽³⁾‐ nonlinear interactions in all known SRS‐active natural crystals (minerals) is given.

     

Observation of stimulated Raman scattering in polar tetragonal crystals of barium antimony tartrate trihydrate,Ba[Sb2((+)C4H2O6)2]·3H2O

The non‐centrosymmetric polar tetragonal (P 4₁) barium antimony tartrate trihydrate, Ba[Sb₂((+)C₄H₂O₆)₂]·3H₂O, was found to be an attractive novel semi‐organic crystal manifesting numerous χ ⁽²⁾‐ and χ ⁽³⁾‐nonlinear optical interactions. In particular, with picosecond single‐ and dual‐wavelength pumping SHG and THG via cascaded parametric four‐wave processes were observed. High‐order Stokes and anti‐Stokes lasing related to two SRS‐promoting vibration modes of the crystal, with ω_SRS1 ≈ 575 cm^?1 and ω_SRS2 ≈ 2940 cm^?1, takes place. Basing on a spontaneous Raman investigation an assignment of the two SRS‐active vibration modes is discussed.

     

Detection of stimulated Raman scattering in the LiYbF<Subscript>4</Subscript> crystal

Stimulated Raman scattering (SRS) has been observed for the first time in a tetragonal LiYbF₄ crystal. The recorded Stokes and anti-Stokes components of χ⁽³⁾ nonlinear lasing are attributed to the two SRS-active phonon modes with ω_SRS1 ~ 325 cm^–1 and ω_SRS2 ~ 432 cm^–1 of this crystal.     

Measurement of the third‐order nonlinear optical susceptibility χ(3) for the 1002‐cm–1 mode of benzenethiol using coherent anti‐Stokes Raman scattering with continuous‐wave diode lasers

The components of the third‐order nonlinear optical susceptibility χ⁽³⁾ for the 1002‐cm^–1 mode of neat benzenethiol have been measured using coherent anti‐Stokes Raman scattering with continuous‐wave diode pump and Stokes lasers at 785.0 and 852.0 nm, respectively. Values of 2.8 ± 0.3 × 10^–12, 2.0 ± 0.2 × 10^–12, and 0.8 ± 0.1 × 10^–12 cm·g^–1·s² were measured for the xxxx, xxyy, and xyyx components of |3χ⁽³⁾|, respectively. We have calculated these quantities using a microscopic model, reproducing the same qualitative trend. The Raman cross‐section σ_RS for the 1002‐cm^–1 mode of neat benzenethiol has been determined to be 3.1 ± 0.6 × 10^–29 cm² per molecule. The polarization of the anti‐Stokes Raman scattering was found to be parallel to that of the pump laser, which implies negligible depolarization. The Raman linewidth (full‐width at half‐maximum) Γ was determined to be 2.4 ± 0.3 cm^–1 using normal Stokes Raman scattering. The measured values of σ_RS and Γ yield a value of 2.1 ± 0.4 × 10^–12 cm·g^–1·s² for the resonant component of 3χ⁽³⁾. A value of 1.9 ± 0.9 × 10^–12 cm·g^–1·s² has been deduced for the nonresonant component of 3χ⁽³⁾. Copyright © 2011 John Wiley & Sons, Ltd.     

Cascaded and cross-cascaded χ(3) nonlinear optical effects in a new SRS-active YAlO3 crystal

Stimulated Raman scattering (SRS) is discovered under picosecond laser excitation in a YAlO₃ orthorhombic crystal, and its cascaded and cross-cascaded χ⁽³⁾ nonlinear optical interactions are studied. Investigations revealed three SRS-active phonon modes of the crystal and identified all its recorded Stokes and anti-Stokes generation lines.     

Laser crystals and ceramics: recent advances

After a brief examination of known insulating laser crystals and the stimulated emission channels of their generating activator ions, this article reviews recent advances in the development of novel lasing crystals and ceramics, as well as inorganic and organic nonlinear‐laser crystals for χ⁽³⁾ and cascaded χ⁽³⁾ ↔ χ⁽²⁾ frequency converters. Several new modern attractive technologies in the physics and techniques of crystalline lasers are also discussed.     

Phosgenite,Pb2CO3Cl2 – a novel SRS‐active crystal

Lead carbonate chloride, Pb₂CO₃Cl₂, known as mineral phosgenite, is introduced as a novel SRS‐active carbonate crystal with tetragonal symmetry. Under picosecond one‐micron laser pumping Raman‐induced χ⁽³⁾‐nonlinear generation in the near‐IR is observed. All recorded high‐order Stokes and anti‐Stokes sidebands are identified and attributed to two SRS‐promoting vibration modes with ω_SRS1 ≈ 1062 cm^–1 and ω_SRS2 ≈ 86 cm^–1.

     

New nonlinear-laser effects in YbVO4 crystal: Sesqui-octave stokes and anti-Stokes comb generation and the cascaded self-frequency “tripling” of χ(3)-Stokes components under a one-micron picosecond pumping

We report the experimental investigations of nonlinear-laser effects in vanadate YbVO₄ under a onemicron picosecond Nd³⁺:Y₃Al₅O₁₂ laser pumping. In this tetragonal host-crystal for Ln³⁺ lasants, for the first time, we excited more than one-and-a-half octave (≈11661 cm^?1) Raman-induced Stokes and anti-Stokes generation combs and observed a multistep cascaded parametric χ⁽³⁾ lasing in the deep-blue spectral region. All generation lines were identified and attributed to the SRS-promoting vibration mode of the crystal (ω_SRS ≈ 897 cm^?1). We classified the ytterbium vanadate as a promising material for Raman frequency converters, wideband χ⁽³⁾-nonlinear comb generators, and as a gain medium for solid-state lasers.     

Stimulated Raman scattering in natural crystals of SrSO4, BaSO4 and PbSO4: High-order Stokes and anti-Stokes generation with?single-wavelength UV, visible, and near-IR excitation, as?well?as cascaded up-conversion nonlinear �� (3)?�� (3) lasing effects under dual-wavelength picosecond collinear coherent pumping

Orthorhombic crystals of SrSO₄, BaSO₄, and PbSO₄, known as natural crystals celestine, barite, and anglesite, were found to be attractive ?? ⁽³⁾-active nonlinear optical materials. High-order Stokes and anti-Stokes picosecond generation that spans almost two octaves has been recorded with single-wavelength laser excitation in the UV, visible, and near-IR ranges. All recorded Raman induced lasing components were identified and attributed to the SRS-promoting vibration modes of the studied crystals (?? _SRS??999?cm^?1 for SrSO₄,?? _SRS??985?cm^?1 for BaSO₄ and ?? _SRS??977?cm^?1 for PbSO₄). Under dual-wavelength (?? _f1=1.06415???m + ?? _f2=0.53207???m) collinear coherent picosecond pumping several new manifestations of cascaded ?? ⁽³⁾??? ⁽³⁾ nonlinear up-conversion lasing effects were observed in BaSO₄ and SrSO₄ crystals. We classify all three studied sulfate crystals as promising SRS-active materials for Raman laser frequency converters and as efficient ?? ⁽³⁾-crystals that efficiently generate Stokes and anti-Stokes frequency combs, which can enable experiments of ultra-short pulse syntheses.     

Raman‐induced impulsive Stokes lasing in novel SRS‐active monoclinic m‐LaVO4 crystal

Monoclinic m‐LaVO₄ vanadate with the monazite‐type structure was found to be a new favorable SRS‐active crystal. Its two‐phonon impulsive Stokes lasing has been recorded under near‐IR femtosecond pumping. Knowledge acquired about the behavior of impulsive stimulated Raman scattering in the studied crystals may be useful for the physics of coherent optical phonons and for engineering of femtosecond lasers. The fundamental results obtained here will also motivate the search for crystals able to generate multiphonon impulsive SRS. (© 2015 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

High‐order Stokes and anti‐Stokes Raman generation in monoisotopic CVD 12C‐diamond

We determined, for the first time, the room temperature phonon energy related to the F_2g vibration mode (ω_SRS(12C) ～ 1333.2 cm^–1) in a mono‐crystalline single‐isotope CVD ¹²C‐diamond crystal by means of stimulated Raman scattering (SRS) spectroscopy. Picosecond one‐micron excitation using a Nd³⁺:Y₃Al₅O₁₂‐laser generates a nearly two‐octave spanning SRS frequency comb (～12000 cm^–1) consisting of higher‐order Stokes and anti‐Stokes components. The spacing of the spectral lines was found to differ by Δω_SRS ～ 0.9 cm^–1 from the comb spacing (ω_SRS(natC) ～ 1332.3 cm^–1) when pumping a conventional CVD diamond crystal with a natural composition of the two stable carbon isotopes ¹²C (98.93%) and ¹³C (1.07%). (© 2016 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

Multiphoton SRS-Lasing in a Monoclinic β-BaYb<Subscript>2</Subscript>F<Subscript>8</Subscript> Crystal

The discovery of stimulated Raman scattering (SRS) in monoclinic fluoride β-BaYb₂F₈ known as a host matrix for Ln³⁺ lasant ions was reported. All the recorded spectral components of Stokes and anti-Stokes χ⁽³⁾-nonlinear picosecond generation were assigned to the three SRS-active photon A_g- and B_g-modes of a crystal (ω_SRS1 ~ 362 cm^–1, ω_SRS2 ~ 295 cm^–1, and ω_SRS3 ~ 230 cm^–1).     

Monoclinic niobate LaNbO<Subscript>4</Subscript> as a new SRS-active crystal

The effect of the generation of stimulated Raman scattering in monoclinic niobate LaNbO₄, which is known as a base crystal for lasant ions Ln³⁺, has been discovered. The χ⁽³⁾ nonlinear Stokes and anti-Stokes biphonon lasing of this niobate has been studied under picosecond excitation.     

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.

     

Observation of stimulated raman scattering in CVD-diamond

We report the first experimental observation of a nonlinear laser effect, stimulated Raman scattering (SRS), in manmade diamond grown from the gaseous phase by the chemical vapor deposition (CVD) technique. Multiple Stokes and anti-Stokes generation in the visible and near-IR ranges was excited under nanosecond and picosecond pumping in a 350-μ-thick plate. All the registered Raman-induced lasing wavelengths were identified. We classify the CVD-diamond as a promising χ⁽³⁾-active material for Raman laser converters in a record wide spectral range.     

Nonlinear susceptibilities of vapors and solutions of organic dyes

Results of theoretical studies of laser and Kerr nonlinear susceptibilities of vapors and solutions of organic dyes using a series of polycyclic arenes as an example are presented. Nonlinear susceptibilities of the third χ⁽³⁾ (?3ω; ω, ω, ω) and the fifth χ⁽⁵⁾ (?3ω; ω, ω, ω, ω, ?ω) orders of a series of organic dyes responsible for third harmonic generation of Nd:YAG laser radiation are calculated within the context of the free electron model. Results of calculations of their Kerr third-order nonlinear susceptibilities χ⁽³⁾ (?ω; ω, ?ω, ω) and non-linear refractive indices n ₂ are presented. The calculation results are compared with experimental data on third harmonic generation in naphthalene vapors and with χ⁽³⁾ (?ω; ω, ?ω, ω) as well as n ₂ of paraterphenyl and naphthalene solutions.     

Orthorhombic lutetium germanate NaLuGeO<Subscript>4</Subscript>: A new SRS-active crystal

The discovery of the effect of simulated Raman scattering in the NaLuGeO₄ rhombic crystal and the first results of studying the spectra of two-phonon steady χ⁽³⁾ nonlinear picosecond lasing are reported.