Narrowing broadening and shifting parameters for R(2) and P(14) lines in the HCl fundamental band perturbed by N2 and rare gases from tunable diode laser spectroscopy

High resolution measurements of room temperature absorption with a controlled tunable diode laser (TDL) spectrometer have been made for R(2) and P(14) lines in the HCl fundamental band perturbed by N₂, Xe, Ar and He at pressures lower than one atmosphere. Pressure broadening, shift and collisional narrowing parameters have been extracted by least-squares fitting of several collisional profiles to the spectra. Asymmetries are observed for P(14) broadened by Xe at the lowest pressures and attributed to correlations between velocity- and phase-changing collisions.     

H2-broadening,shifting and mixing coefficients of the doublets in the ν2 and ν4 bands of PH3 at room temperature

The broadening, shifting and mixing coefficients of the doublet spectral lines in the ν₂ and ν₄ bands of PH₃ perturbed by H₂ have been determined at room temperature. Indeed, the collisional spectroscopic parameters: intensities, line widths, line shifts and line mixing parameters, are all grouped together in the collisional relaxation matrix. To analyse the collisional process and physical effects on spectra of phosphine (PH₃), we have used the measurements carried out using a tunable diode-laser spectrometer in the ν₂ and ν₄ bands of PH₃ perturbed by hydrogen (H₂) at room temperature. The recorded spectra are fitted by the Voigt profile and the speed-dependent uncorrelated hard collision model of Rautian and Sobelman. These profiles are developed in the studies of isolated lines and are modified to account for the line mixing effects in the overlapping lines. The line widths, line shifts and line mixing parameters are given for six A₁ and A₂ doublet lines with quantum numbers K = 3n,?(n = 1,?2, …) and overlapped by collisional broadening at pressures of less than 50 mbar.     

Diode laser measurements of temperature-dependent collisional-narrowing and broadening parameters of Ar-perturbed H2O transitions at 1391.7 and 1397.8 nm

High-resolution absorption lineshapes of two H₂O transitions near 7185.60 and 7154.35 cm⁻¹ have been recorded in a heated static cell as a function of temperature (296-1100 K) and pressure (6-830 Torr) using two distributed-feedback diode lasers. The measured absorption spectra are least squares fit to both Voigt and Galatry profiles. Strong collisional-narrowing effects are observed in the Ar-broadened H₂O spectra at near-atmospheric pressure due to the relatively weak collisional broadening induced by Ar-H₂O collisions, while collisional narrowing is not significant for pure H₂O absorption lineshapes. Line strengths and self-broadening coefficients are inferred from the pure H₂O absorption spectra and compared with published data. Temperature dependences of the Ar-induced broadening, narrowing, and shift coefficients are determined using Galatry fits to the absorption data. The measured collisional-narrowing parameters have similar temperature dependence to the collisional-broadening coefficients.     

Collision broadening in MO-electron spectra in Kr-Kr and Kr-Ar collisions

The energy spectrum of MO Auger electrons produced in ion-atom collisions is determined by the behaviour of the energyE(R) and the autoionizing widthΓ _A (R) of a quasimolecular level as a function of the internuclear distanceR and by the collisional broadening mechanism. The collisional broadening (cb) of a MO-electron spectrum is caused by the nuclear motion and mainly concerns transitions between the quasimolecular autoionizing state and the continuum. In the present work the dependences of cb on the projectile velocityv _p and on the united atomic numberZ of the projectile-target systems are studied.     

ABSORPTION INTENSITIES, PRESSURE-BROADENING AND LINE MIXING PARAMETERS OF SOME LINES OF NH3 IN THE ν4 BAND

The intensities and foreign gas broadening coefficients of 57 selected lines of the ν₄ band of NH₃ have been measured in the region of 1550 cm^-1 using a high resolution Brucker Fourier transform spectrometer. The line intensities were obtained by using the methods of absorbance at the line center and by fitting Voigt profiles to the measured shapes of the lines. The latter method also provides the collisional widths of the lines. In addition, collision cross relaxation coefficients of O₂ and air foreign gases were measured for 9 doublets of NH₃ in the ν₄ band. The J and K quantum numbers dependencies of pressure-broadening coefficients and line intensities are discussed. The observed air broadening and cross relaxation coefficients were found to be in reasonable quantitative agreement with the concentration-weighted average of the N₂ and O₂ broadening coefficients. The comparison of our present and previous results obtained for the NH₃–H₂, NH₃–air, NH₃–N₂ and NH₃–CO₂ collisions shows an increase of the pressure broadening and cross relaxation coefficients with quadrupole moment of the foreign gas. The analysis of the line intensities was based on the third-order theory of line strengths and yields effective transition moments, vibrational band strengths and correction parameters of the symmetric and antisymmetric partial bands of the fundamental ν₄ band.     

Transverse-momentum distribution of J/Ψ's in Pb-Pb collisions and gluon rescattering

We study anomalous J/Ψ suppression and p _t broadening in the model of prompt gluons. The anomalous suppression can be successfully described in this model. The transverse-momentum dependence of J/Ψ suppression in relativistic heavy-ion collisions is calculated from initial-state gluon rescattering with both nucleons and prompt gluons produced in nucleon-nucleon collisions in the early phase of the reaction. It seems impossible to describe simultaneously anomalous suppression and p _t broadening in Pb-Pb collisions within the model of prompt gluons with reasonable values of the parameters. Received: 27 September 2001 / Accepted: 12 November 2002 / Published online: 17 January 2003 RID="a" ID="a"e-mail: zhuangpf@mail.singhua.edu.cn Communicated by A. Molinari     

Linewidth studies on the Ar+ 476.5 nm and 480.6 nm lines excited in a helium-agron hollow cathode discharge

The spectral line shapes of the Ar⁺ 476.5 nm and 480.6 nm lines, excited in a He-Ar hollow cathode (HC) discharge, were measured using the Fabry-Perot technique. The collisional and Doppler linewidths were determined for the two lines. The collisional broadening constants are estimated to be (5±3) MHz/mbar and (6±3) MHz/mbar, respectively. The temperature obtained from the two Ar ion transitions was found to be 260 K higher than that expected for the rest of the gas mixture from earlier measurements. The possibility is discussed, that this excess temperature is caused by Ar ions partially created in the HC discharge by charge transfer collisions with He ₂ ⁺ molecules.     

Memory effects in speed-changing collisions and their consequences for spectral line shape

The kinetic model accounting for speed-memory effects on the spectral line shape proposed in I [D. Robert, L. Bonamy, Eur. Phys. J. D 2, 245 (1998)] is extended for any density range, within the binary collision framework. The additional Doppler contribution requires to consider the 3D velocity-memory function instead of the 1D speed one, with distinct treatments for the velocity-orientation and velocity-modulus memory mechanisms. Both the collisional confinement narrowing of the Doppler distribution and the radiator speed-dependence of the collisional broadening and shifting parameters are thus conveniently taken into account. In the high density regime, this model leads to the same results as in I. At lower densities, it generalizes the very well-known hard and soft collision models for the Dicke narrowing of the Doppler distribution, but it also includes the second source of inhomogeneity tied to the speed-dependent collisional parameters and, concomitantly, the speed class exchanges. Numerical applications to H₂-N₂ and H₂-Ar gaseous mixtures are in close agreement with experiments. This allows one to clearly analyze the specific role of speed and velocity memory effects on the line profile.Received: 18 June 2004, Published online: 3 November 2004PACS: 34.10. + x General theories and models of atomic and molecular collisions and interactions (including statistical theories, transition state, stochastic and trajectory models, etc.) - 33.70.Jg Line and band widths, shapes, and shifts     

水汽分子对CO_2谱线加宽的影响

报道了以高分辨力连续可调谐中红外差频激光为探测光源,结合可调长光程怀特池,利用直接吸收的方法探测了CO2的10011←10002带R支以及部分P支在室温下的水汽加宽吸收光谱。在2422cm-1到2457cm-1范围内共有26条吸收谱线被探测到,采用Voigt线型对吸收谱线进行拟合,得到了CO2光谱的水汽加宽系数,结果显示CO2的水汽加宽系数平均比干燥空气的加宽系数大52%。利用实验测得的CO2的水汽加宽系数与HITRAN04数据库中CO2谱线的线位置、线强和干燥的空气加宽系数进行比较,分析了在实际大气中(海平面,10km光程)不存在水汽和存在水汽(含有2.0kPa水汽)时该波段CO2的大气透过率,结果表明潮湿空气与干燥空气之间的最大透过率差约为0.5‰。     

Study of the rates of collisional decay of population, orientation, and alignment by stimulated photon echo in a molecular gas

A stimulated photon echo technique with specially selected linear polarizations of the coherent resonant driver pulses is used to study depolarizing collisions in the molecular gas SF₆ and in mixtures of it with buffer He and Xe. The collisional decay rates of the population, orientation, and alignment in an ensemble of gas particles are determined for the first time in a single experiment. These relaxation rates are measured as a function of the longitudinal translational velocities of the resonant particles. To within the experimental accuracy, no significant dependence of the collisional decay rates on the translational velocities of the particles was observed. This result confirms the conventional theoretical approach to depolarizing collisions. In pure SF₆ the decay rates for the orientation and alignment were lower than the relaxation constant for collisions involving a change in the longitudinal velocity (elastic collisions) that is known from experimental observations of the ordinary photon echo. This means that only some of the elastic collisions participate in destroying the multipole moments of the levels. Evidence is found that the relaxation of the multipole moments created by polarized radiation in a resonant medium of molecular SF₆ gas depends on j, the total angular momentum of the level. Zh. éksp. Teor. Fiz. 113, 826–833 (March 1998)     

High temperature O2-CARS thermometry

O₂ temperature measurements at T=1910K have been performed by coherent anti-Stokes Raman scattering (CARS) inside a homogeneously heated gas volume of a tube furnace. The oxygen CARS spectrum can now be modeled accurately within the higher vibrational levels of the Q-branch manifold populated at flame temperatures using recently available spectroscopic data and collisional broadening coefficients.     

Extracting Information About Few-Body Breakup Thresholds from High-Energy Collisions

We show that the analysis of high-energy collisions provides an alternative, and sometimes advantageous, method of gathering information on a breakup system at threshold. We demonstrate the applicability of this approach by extracting the s-wave scattering length a₀ for the collision of electrons by neutral atoms in metastable states from measurements of photo- and collisional detachment of electrons from negative ions and electron capture to continuum states of neutral projectiles in atomic ionization collisions. Finally, we discuss how to generalize these ideas to gather information about an N-body threshold behavior.Fax: +54 2944 445299, Phone: +54 2944 445234     

Energy and angular momentum transfer in atom-diatom collisions from polarized laser fluorescence

We report a study of collisional reorientation of diatomic lithium molecules by rare gas atoms using high resolution circularly polarized laser fluorescence. As in the case of I₂ we find that elastic collisions are very inefficient at reorienting Li₂ molecules and a selection rule ΔM′ _J = 0 appears to be in operation. Rotationally inelastic collisions, particularly those with argon, cause some degree of reorientation and are the result of relatively long range intermolecular interactions. Vibrational transfer features are more strongly depolarized. Optical pumping studies of oriented ¹Σ _g Li₂ molecules have yielded a cross section for inelastic transfer of 35 ± 15 Ų.     

CARS investigations of quenching and photochemical reactions in the Na+H2 collision system

Summary We have carried out parallel studies of the quenching process in Na(3p)+H₂ collisions and the possible reactive process in Na(3p)+H₂ (v ^″=1,2,3) collisions. Rich CARS spectra which were obtained at H₂ pressure of 100 mbar and oven temperature of 600 K indicate the presence of vibrationally excited H₂ and photochemically produced NaH molecules. Temporal resolution of NaH CARS lines was employed in order to rule out competing collisional processes. We make use of resonantly enhanced CARS methods which enabled us to achieve very high sensitivity for NaH detection. Paper presented at the ?XI European CARS Workshop?, Florence, Italy, 23–25 March, 1992.     

O2 broadening of carbon disulphide 12C32S2 in the v 3 and v 3—v 1 bands

Using a tunable diode laser spectrometer, we have measured O₂ broadening coefficients of ¹²C³²S₂ for 31 lines in the v ₃ fundamental band near 6.5 μm and 12 lines in the v ₃—v ₁ band near 11.4 μm. The collisional halfwidths are obtained by fitting the spectral lines with a Voigt and a Rautian profile. The broadening coefficients of ¹²C³²S₂-O₂ are also calculated from semiclassical theory involving, in addition to electrostatic interactions, successively the atom-atom Lennard-Jones model and a simple formulation for the anisotropic dispersion forces, leading to more satisfactory results.     

Collisional effects upon optical coherences: Experimental study in a xenon three-level system

Laser induced nonlinear absorption profiles in a three-level system have been recorded to study the effect of elastic collisions upon optical coherences. In our particular system, the signal is due to a pure double-quantum term, where we have separated the effect of phase-interrupting collisions from the effect of velocity-changing collisions. Experimental results show that the effect of velocity-changing collisions is very small, and that broadening of the signal is due to phase-interrupting collisions mainly. We are able to determine the increase of the decay rate of the coherent superposition (the “coherence”) of two levels of same parity [Dγ ₁₃/dp=(6.5±1) MHz/Torr] and an upper limit for the mean velocity change (ũ≲5m/s).     

Collisional broadening of infra-red absorption lines

The Lorentz half-widths of collision-broadened lines in the rotation-vibration bands of diatomic molecules vary with line number |m| in the P and R branches. The observed variation of half-width for lines in the 0 → 1 and 0 → 2 bands of CO and HCl are interpreted in terms of a simple fitting procedure. One dominant source of line broadening is assumed to consist of diabatic hard collisions involving transitions from each rotational level to all higher rotational levels; the effectiveness of this process, which varies from line to line, is described in terms of an empirically adjusted collision cross section, a maximum collision parameter related to independently measured molecular properties, and upon the availability of the required energy and angular momentum in molecular collisions. The second source of line broadening, assumed to be the same for all lines, includes all other types of collisions and is represented by a single empirically adjusted cross section. The simple fitting procedure is applied successfully to self-broadening of CO lines and to foreign-gas broadening of CO and HCl; for HCl self-broadening an additional cross section for resonant-dipole processes must be included. Possible applications of the fitting procedure to HBr, HF, and CO₂ are discussed. The simple procedure presented represents an approximation that may prove useful pending the development of readily applicable complete theories based on first principles.     

A self-consistent kinetic modeling of a 1-D, bounded, plasma in equilibrium

A self-consistent kinetic treatment is presented here, where the Boltzmann equation is solved for a particle conserving Krook collision operator. The resulting equations have been implemented numerically. The treatment solves for the entire quasineutral column, making no assumptions about λ_mfp/L, where λ_mfp is the ion-neutral collision mean free path and L the size of the device. Coulomb collisions are neglected in favour of collisions with neutrals, and the particle source is modeled as a uniform Maxwellian. Electrons are treated as an inertialess but collisional fluid. The ion distribution function for the trapped and the transiting orbits is obtained. Interesting findings include the anomalous heating of ions as they approach the presheath, the development of strongly non-maxwellian features near the last λ_mfp, and strong modifications of the sheath criterion.