Far-infrared laser-emission spectroscopy on ammonia isotopomers

In this paper we report the investigation of the isotopic ammonia gases¹⁴NH₃,¹⁴NH₂D,¹⁴NHD₂,¹⁵NH₃ and¹⁵ND₃ optically pumped by a continuously tunable 20 atm CO₂-laser. We found 267 far-infrared emission lines, produced by both inversion and Raman processes, in the frequency range from 15 cm^–1 to about 250 cm^–1. 200 of these were observed for the first time. We obtained far-infrared Raman tuning ranges exceeding 3 cm^–1, photon conversion coefficients up to 12% and maximum output energies of 0.9 mJ. Furthermore, the optimum gas pressure, the polarization and the transient behavior of optically pumped ammonia have been investigated.     

Atmospheric influences in optical third-harmonic generation experiments

Third-harmonic generation in a thin solid plate surrounded by a gas is investigated. We conclude that atmospheric contributions can be suppressed in third-harmonic generation from thin solid plates. A phase-sensitive measurement of the third-order susceptibility of gases is proposed. We calibrated the third-order susceptibility of air to be X⁽³⁾ _a=(3.4±1.5)×10^–18 esu with a phase uncertainty of ±10°.     

Third order nonlinear optical properties of some organic nitroxyls

The degenerate four-wave mixing experiments have been performed in the dichloromethane solutions of 2,2,6,6-tetramethyl-pipridine-4-ol-N-oxyl p-hydroxybenzaldehyde oxime benzoic ester (TPOHBOBE) and bis-(TPOHBOBE) cobalt (II), respectively. The result is in agreement with the theoretical prediction of depending on the molecular chain length l as l ⁵. A large off-resonant third order hyperpolarizability _xxxx of 1.3 × 10^–30 esu for bis-(TPOHBOBE) cobalt (II) was obtained. The corresponding value of the third order nonlinear optical susceptibility ⁽³⁾ _xxxx for its solid state is estimated to be 7.8 × 10^–9 esu.     

New far-infrared laser lines from CH3Cl and CH3Br optically pumped with a continuously tunable high pressure CO2 laser

In this paper we report on the detection of new far-infrared laser lines from CH₃Cl and CH₃Br optically pumped with a continuously tunable high pressure CO₂ laser. We found 80 new lines for CH₃Cl and 9 new lines for CH₃Br in the frequency region between 16 cm^–1 and 41 cm^–1, all due to stimulated Raman scattering. For the Raman gain regions bandwidths up to about 700 MHz were found. We also observed high intensity short far-infrared laser pulses of durations in the nanosecond regime.Permanent address: Physics Department, State Pedagogical University, SU-119435 Moscow, USSR     

Efficient generation of FIR radiation by optical pumping of D2 18O

In this paper we show that D₂ ¹⁸O vapour, optically pumped with a continuously tunable high pressure CO₂ laser, is an excellent source for far infrared radiation. Both high photon conversion coefficients and broad Raman gain regions were found for a large number of new laser transitions spread over the frequency range from 25 cm^–1 to 240 cm^–1. We demonstrate that these Raman gain regions can be used to generate far infrared laser pulses with high intensity and durations of about 100 ps.     

Deeply virtual and exclusive electroproduction of ω-mesons

The exclusive ω electroproduction off the proton was studied in a large kinematical domain above the nucleon resonance region and for the highest possible photon virtuality (Q²) with the 5.75 GeV beam at CEBAF and the CLAS spectrometer. Cross-sections were measured up to large values of the four-momentum transfer (- t < 2.7 GeV²) to the proton. The contributions of the interference terms σ_{TT} and σ_{TL} to the cross-sections, as well as an analysis of the ω spin density matrix, indicate that helicity is not conserved in this process. The t-channel π⁰ exchange, or more generally the exchange of the associated Regge trajectory, seems to dominate the reaction γ^*p↦ωp, even for Q² as large as 5 GeV². Contributions of handbag diagrams, related to Generalized Parton Distributions in the nucleon, are therefore difficult to extract for this process. Remarkably, the high-t behaviour of the cross-sections is nearly Q²-independent, which may be interpreted as a coupling of the photon to a point-like object in this kinematical limit.     

Large third-order nonlinear optical properties of C70 fullerene in the infrared regime

The nonlinear third-order optical susceptibility of C₇₀ in a toluene solution is measured for the first time by the method of degenerate four-wave mixing using 10 ns laser pulses at 1.06 m. The third-order susceptibility X _in ⁽³⁾ is 5.6×10^–12 esu for a C₇₀ toluene solution at a concentration of 0.476 g/l. The correspondent magnitude of the hyperpolarizability ₁₁₁₁ of the C₇₀ molecule is 1.2×10^–30 esu which is in a good agreement with the prediction given by the model of a free electron in a spherical box.     

A polarized CARS investigation of the fine structure population inversion of Cl atoms from laser photolysis of ICl and the quenching of Cl(2 P 1/2) by O2

The time resolved polarized CARS technique has been used to detect Cl atoms produced by photolysis of ICl in the presence and absence of O₂. A population inversion was observed between the ground state electronic levels Cl(² P _1/2) and Cl(² P _3/2). The rate constant for Cl(² P _1/2) decay (quenching + reaction) in ICl was determined to be (3.2±0.2)×10^–13 cm³/molecule×s; the rate constant for Cl(² P _3/2) reaction with ICl was determined to be (7.8±0.5)×10^–12 cm³/molecule×s; and the rate constant for Cl(² P _1/2) quenching by O₂ was determined to be (1.9±0.2)×10^–13 cm³/molecule×s.     

Intra-cavity spectroscopy with diode lasers

A multi-mode diode laser with an external cavity is studied experimentally and theoretically for its application to intra-cavity spectroscopy. One facet of a typical Ga_0.89Al_0.11As laser diode was antireflection-coated by deposition of HfO₂ such that 10^–3 residual reflectivity was left over. This diode was placed in an external optical cavity. The emission spectrum of this diode laser is highly sensitive to any frequency-dependent loss in the cavity, and the detectivity of such a loss grows with the pump rate. Even close to threshold, the absorption at 780 nm of Rb atoms with a density of 5×10¹⁰ cm^–3 has been detected. An adequate model for diode lasers based on rate equations and including frequency-dependent gain saturation is developed and applied to the calculations of output spectra. The sensitivity of these spectra to intra-cavity absorption is determined by the overall cavity loss — which is rather high — and the fraction of spontaneous emission in the total emission, in contrast with dye lasers where it is limited by nonlinear mode coupling. Various criteria for the sensitivity are suggested. The smallest detectable absorption with a perfectly antireflection-coated laser is 10^–6 cm^–1. Improvement of the characteristics of the laser diode would increase the sensitivity.     

Development of injection-seeded, pulsed optical parametric generator/oscillator systems for high-resolution spectroscopy

We report the development and application of pulsed optical parametric generator (OPG) and optical parametric oscillator (OPO) systems that are injection seeded with near-infrared distributed feedback diode lasers. The OPG is injection seeded at the idler wavelength without the use of a resonant cavity. Two counter-rotating, beta-barium-borate (β-BBO) crystals are used in the OPG. These crystals are pumped by the third harmonic, 355-nm output of an injection-seeded Nd:YAG laser. An OPO version of the system has also been developed by placing two flat mirrors around the two β-BBO crystals to form a feedback cavity at the signal wavelength. The OPO cavity length is not actively controlled. The output signal beam from the OPG or OPO is amplified using an optical parametric amplifier (OPA) stage with four β-BBO crystals. The frequency bandwidths of the signal and idler laser radiation from OPG/OPA and OPO/OPA systems have been determined to be slightly greater than 200 MHz. The temporal pulses from each system are smooth and near-Gaussian. High-resolution optical absorption measurements of acetylene (C₂H₂) were performed as another check of the frequency spectrum of the idler beam. The frequency-doubled signal output of the OPO/OPA system was used to perform high-resolution, single-photon, laser-induced fluorescence (LIF) spectroscopic studies of the (0,0) vibrational band of the A ²Σ⁺−X ²Π electronic transition of nitric oxide (NO) at low pressure. Excellent agreement was obtained between the theory and the experiment. The signal output of the OPG/OPA system was also used for sub-Doppler, two-photon LIF spectroscopic studies of the same vibration–rotation manifold of NO.This revised version was published online in August 2005 with a corrected cover date.     

Generation and measurement of >108 intensity contrast ratio in a relativistic kHz chirped-pulse amplified laser

We report on the generation and measurement of a > 10⁸ contrast ratio between main pulse and amplified spontaneous emission (ASE) from a relativistic kHz chirped-pulse amplified laser. We have enhanced the ASE contrast ratio as much as > 400 times by employing a pulse cleaner composed of a μJ preamplifier and a saturable absorber. A third-order cross-correlator with a dynamic range of > 10⁹ and a scanning range of up to 4 ns has been developed for the contrast measurement. Detailed analysis of the cross-correlation trace shows that the random noise of spectral phase generates 20-ps pedestal structure starting from 10⁻⁶ level of the main pulse.     

Trigonal Na3Li(SeO4)2·6H2O crystal – a novel SRS‐active material with high Raman gain coefficient

We discovered and characterized the χ ⁽³⁾‐active Na₃Li(SeO₄)₂·6H₂O crystal with considerably high Raman gain coefficients for laser physics and nonlinear optics. (© 2007 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

     

Narrow-band extreme-ultraviolet laser radiation tunable in the range 90.5–95 nm

Tunable, narrowband extreme ultraviolet radiation in the range 90.5–95 nm with only limited intensity variations is produced by frequency-tripling ultraviolet light from a frequency-doubled dye laser in a gas-jet of xenon. Acetylene gas is found to be an efficient medium for third-harmonic generation in this wavelength range as well. The extreme-ultraviolet radiation is applied in a spectroscopic study of the b ¹ II _u , v=6–8 and v=10–12, o ¹ II _u , v=0 and b¹ _u ⁺ , v=9 states of molecular nitrogen. From linewidth measurements a value k _p=6×10¹⁰ s^–1 for the predissociation rate of the b ¹ II _u , v=11 state is deduced.     

Tunable frequency-controlled laser source in the near ultraviolet based on doubling of a semiconductor diode laser

Continuously tunable ultraviolet laser radiation at 397 nm was generated by doubling the output of a semiconductor diode laser. The fundamental radiation was provided by a 150 mW AlGaAs laser diode injected by a low-power AlGaAs laser diode which was frequency stabilized by optical feedback using a new scheme of a miniature external cavity. Second-harmonic generation was produced in a lithium-triborate crystal placed in a compact enhancement cavity. The fundamental radiation was used for sub-Doppler spectroscopy of the Ar I 4s ³ P ⁰ ₀–4p ¹ P ₁ transition at 795 nm; the second-harmonic radiation was used for spectroscopy of the Ca II 4² S _1/2–4² P _1/2 transition at 397 nm.     

The emission spectrum of the diatomic radical, phosphorus selenide

The emission spectrum of the PSe radical is reported for the first time. Seventy-eight reddegraded bands in the region 4000–6500 Å have been measured and assigned to the A²Π-X²Π transition of PSe. Isotope shifts observed for some bandheads have been utilized in deriving the vibrational numbering. The molecular constants have been determined as (in units of cm⁻¹): ω′ = 406.9, ω′_eχ′_e = 1.3, ω″ = 556.9, ω″_eχ″_e = 1.3, and T_e = 19477.3 for the ²Π_1/2 states; and ω′_e = 402.4, ω′_eχ′_e = 1.5, ω″_e = 556.8, ω″_eχ″_e = 1.6, and T_e = 19178.0 for the ²Π_3/2 states.     

Nonlinear optical investigations of the dynamics of hydrogen interaction with silicon surfaces

Optical second-harmonic generation (SHG) from silicon surfaces may be resonantly enhanced by dangling-bond-derived surface states. The resulting high sensitivity to hydrogen adsorption combined with unique features of SHG as an optical probe has been exploited to study various kinetical and dynamical aspects of the adsorption system H₂/Si. Studies of surface diffusion of H/Si(111)7×7 and recombinative desorption of hydrogen from Si(111)7 × 7 and Si(100)2 × 1 revealed that the covalent nature of hydrogen bonding on silicon surfaces leads to high diffusion barriers and to desorption kinetics that strongly depend on the surface structure. Recently, dissociative adsorption of molecular hydrogen on Si(100)2×1 and Si(111)7×7 could be observed for the first time by heating the surfaces to temperatures between 550 K and 1050 K and monitoring the SH response during exposure to a high flux of H₂ or D₂. The measured initial sticking coefficients for a gas temperature of 300K range from 10^–9 to 10^–5 and strongly increase as a function of surface temperature. These results demonstrate that the lattice degrees of freedom may play a decisive role in the reaction dynamics on semiconductor surfaces.     

Spectrum Invariance for a Particular Class of Optical Fields Propagated in Far Zone

This paper describes invariance of the normalized optical spectrum for a particular class of optical fields propagated in the far zone from a secondary, spatially, partially coherent source. The optical field across the secondary planar source is inhomogeneous to give the complex degree of spectral coherence such that μ = h(αω(ρ₁–ρ₂))exp(iɛω(ρ₁²–ρ₂²)), where α, ɛ are constants, ω is optical frequency, and ρ₁, ρ₂ denote two points in the secondary source. This expression for μ is the same as obtained in the Fresnel zone from a primary, spatially incoherent source. The invariance law does not hold for the spectrum of the light propagated from the primary source.     

Upconversion luminescence and kinetics in Er:YAlO3 under 652.2 nm excitation

Ultraviolet and visible upconversion properties of Er³⁺ in YAlO₃ were investigated following 652.2 nm excitation of the multiples ⁴F_9/2. The luminescence and excitation spectra were recorded. Ultraviolet (326-342 and 354-359 nm), violet (405-420 nm), blue (436-442 nm) and green (525-575 nm) upconversion and infrared downconversion luminescence were simultaneously observed. The intense green luminescence corresponds to the emissions from the thermal coupled ⁴S_3/2 and ²H_11/2 bands and ²G_9/2 level. Energy transfer upconversion processes were proposed to explain the upconversion phenomena. The luminescence kinetics was discussed in detail by the analyses of fluorescence decay curves.     

Ultra-fast nonlinear response around 1.5 μm in 2D AlGaAs/AlOx photonic crystal

We report the fast switching capabilities of a two-dimensional Al_0.3Ga_0.7As photonic crystal slab around 1.5 μm. The slab is supported by an AlOx low-index thick layer that plays the role of an efficient heat sink. By pumping at 0.8 μm in the absorption of the Al_0.3Ga_0.7As quantum wells, the optical response is modified in the transparency region: a 200% change in the reflectivity is obtained with a total response time of 8ps.     

Efficient ultraviolet photorefraction in LiNbO3

A nominally undoped LiNbO₃ crystal with a slightly broadened absorption edge is used to study beam coupling effects in the UV at 351 nm. At this wavelength the crystal exhibits a diffusion-dominated charge transport mechanism, which allows steady state beam amplification of up to 700 times, comparable to BaTiO₃ in the visible. The used crystal material was characterized by an absorption coefficient =2.68 cm^–1 at 351 nm and a maximal gain coefficient =13.94 cm^–1. This high gain value in the UV can be attributed to a hole diffusion-dominated charge transport mechanism together with a low bulk photovoltaic effect. We measured photovoltaic fields of the order of 550 V/cm.