Quantum control of ground-state rotational coherence in a linear molecule

We present an experimental and theoretical investigation of the quantum control of ground-state rotational coherence in a linear molecule. A sequence of two temporally separated laser pulses creates a rotational superposition state in ${\mathrm{CO}}_{2}$ whose evolution is monitored through a polarization technique. We study the influence of the phase difference between the two pulses. We show that the overlapping of the two wave packets, produced by each pulse, gives rise to quantum interference that affects the orientational anisotropy of the sample. Because of the large number of coherently excited levels, the interference produces well-separated temporal structures, whose magnitude can …

Shot-by-shot frequency calibration of CARS spectra: Application to the measurement of the collisional line shift in oxygen

A technique using a Fabry-Perot interferometer has been developed to calibrate high-resolution spectra obtained by Coherent Anti-Stokes Raman Spectroscopy (CARS). This technique was used to measure simultaneously the Raman frequency and the Raman signal at each laser shot. We demonstrate the accuracy of the method by measuring theQ(15) line shifts of molecular oxygen due to collisions with oxygen and water vapour.

Collisional line broadening and line shifting in N2-CO2 mixture studied by inverse Raman spectroscopy

Abstract Collisional effects in the Raman Q-branch of N 2 perturbed by CO 2 have been studied by high-resolution stimulated Raman spectroscopy. The Raman spectra recorded in the 0.3–1.0 atm and 295–1000 K pressure and temperature ranges are fitted with a theoretical profile taking into account line broadening, frequency shift and line mixing due to rotational energy transfers. The data at low density are used as basic data for the modeling of rotationally inelastic rates through sets of adjustable parameters. We have used in this study the two main models developed in the last decade and known as modified exponential gap (MEG) and energy corrected sudden (ECS) laws. Experimental spectra rec…

A new method to measure the wavelength of single-mode pulsed lasers with a scanning Michelson interferometer

We report on the possibility to measure the wave-lengths of pulsed single-mode lasers by means of a two-beam Michelson interferometer in motion [1,2]. The corner reflector moves with a nearly constant speed creating a path differenceL so thatL/C ≪ 1/Δν, Δν being the spectral width of the laser to be measured. The reference laser is a stabilized He-Ne (Spectra-Physics, model 117 A) to a precision of the order of two parts in 109. The fringe pattern of the two beams (reference beam and measured beam) is sampled simultaneously with a repetition rate of 40 ms. With this new method, the frequency doubled injection-seeded Nd: YAG laser wavelength has been measured with an accuracy of the order of…

Observation of laser-induced continuum structure in the NO molecule

0953-4075; We present experimental results on the modification of a molecular ionization continuum through a laser-induced continuum structure. The effect is demonstrated in nitric oxide where the resonant 2 + 1 multiphoton-ionization process of the X (2)Pi(3/2) electronic ground state is modified by dressing the continuum with the electromagnetically embedded M(2)Sigma(+) Rydberg state. Through selection of a two-photon rovibronic transition via the D electronic state, a single rotational ground state level is excited to the continuum with one laser field. By adding an extra dressing field, a coupling is then established between this three-photon excited ground state level and one of the M…

Characterization of self-phase modulated ultrashort optical pulses by spectral phase interferometry

0740-3224; We present the procedure for measuring self-phase modulation of ultrashort laser pulses focused in gases by use of the spectral phase interferometry for direct electric-field reconstruction (SPIDER) technique. We tested the device, which employs a noncollinear type I frequency mixing scheme, by measuring the phase induced by group-velocity dispersion either in a piece of glass or in the compressor of the laser system. Both results were validated by comparison with the expected values. The phase that resulted from self-phase modulation in H2 gas or atmospheric air was then measured and compared with calculations based on a Gaussian beam assumption. A new estimate of the nonlinear …

Spatio-temporal structures of laser-induced anisotropy

We report new observations of optical spatio-temporal structures formed in terbium gallium garnet when it is excited at resonance by a strong laser beam. We also present a theoretical description of this pattern formation, which accounts well for our observations. We finally discuss useful applications of both time and power dependence of these structures.

HIGH RESOLUTION STIMULATED RAMAN SPECTROSCOPY WITH A 3 MHz ACCURACY WAVEMETER

Accurate spectroscopic constants of nitrogen determined from stimulated Raman spectra of the fundamental and first hot bands

Nitrogen spectra of the Q-branch of the fundamental and the first hot bands were recorde with a high-resolution stimulated Raman spectrometer at atmospheric pressure and ca. 1300 K. The absolute frequencies of the Raman lines were measured with high accuracy, leading to a refinement of spectroscopic constants. A temperature estimation was also performed from the Raman intensities.

High-Resolution Photoacoustic Raman-Spectroscopy of Gases

0377-0486; A high-resolution photoacoustic Raman spectroscopy experiment is described. The resolution achieved by using two single-mode pulsed lasers is about 0.0054 cm-1 (full width at half maximum intensity). The experiment was tested first on the v1/2v2 bands of CO2 and gave an increase of at least about one order of magnitude in the signal-to-noise ratio with respect to stimulated Raman spectroscopy at low pressure (ca. 10 Torr almost-equal-to 13 kPa). The sensitivity is also demonstrated by the study of the weak hot band v1 + v2 - v2 of CO2. In both cases, the experimental line shape is well reproduced by taking into account Doppler and collisional effects. A comparison with CARS spect…

Electrodes for REMPI spectroscopy in static gases and calculation of REMPI intensities: Application to molecular oxygen

Resonance-enhanced multiphoton ionization (REMPI) of 16 O 2 X 3 Σ g − (ν = 0) through (3sσ g ) d'Π g (ν = 0) by using (2 + 1) one-colour photons is reported. This REMPI process, already observed and analysed by other authors at low pressure and low rotational temperature with mass spectrometry detection, is used to test our first detector of ionizations. Experimental difficulties have led to the design of an original arrangement of electrodes to collect electrons at room temperature and 1 Torr pressure of static molecular oxygen. A calculated spectrum is compared with the observed REMPI spectrum. The calculation uses the polarizability tensor and takes into account the competition between i…

Shaping of a ground state rotational wavepacket by frequency-chirped pulses

0953-4075; A coherent rotational superposition state is produced in the ground vibronic level of N2 through the interaction of the molecule with the electric field vector of a nonresonant laser pulse. This rotational wavepacket is shaped with a linear frequency chirp of the laser field. The structural shape of the rotational coherences shows a strong dependence with the frequency-chirp amplitude. A comparison with a theoretical model allows the interpretation of the observed effects in terms of dephasing of the wavepacket induced by the laser phase distortion. Application of the presented results to the phase characterization of short XUV pulses is suggested.

Rotationally Inelastic Rates for N2-N2 System from a Scaling Theoretical Analysis of the Stimulated Raman Q-Branch

0021-9606

High-Resolution Stimulated Raman-Spectroscopy with a 3 MHz Accuracy Wavemeter

0302-0738

Temporal phase control of bound-bound and bound-free two-photon transitions in NO with two time-delayed cross-polarized pulses

0953-4075; Temporal phase control over the multi-photoionization of NO is investigated experimentally The coherent excitation of the molecular system is achieved by a sequence of two phase-related non-Fourier-transform-limited laser pulses delivered by a nanosecond dye laser, The phase-locked pulses are produced by making use of an actively stabilized interferometer with a tunable pathlength difference. As the coherence time of the laser is comparable with the inhomogenous dephasing time of the medium, the measurements are performed with temporally overlapped pulses. In order to avoid the modulation of the ionic signal coming from optical interference, the linear polarizations of the two pu…

Concentration measurements in molecular gas mixtures with a two-pump pulse femtosecond polarization spectroscopy technique

0021-9606; Recently, we have demonstrated the ability of the Raman-induced polarization spectroscopy (RIPS) technique to accurately determine concentration or polarizability anisotropy ratio in low-pressure binary molecular mixtures [E. Hertz, B. Lavorel, O. Faucher, and R. Chaux, J. Chem. Phys. 113, 6629 (2000)]. It has been also pointed out that macroscopic interference, occurring when two revivals associated to different molecules time overlap, can be used to achieve measurements with picosecond time resolution. The applicability of the technique is intrinsically limited to a concentration range where the signals of both molecules are of the same magnitude. In this paper, a two-pump puls…

Pulse trains produced by phase-modulation of ultrashort optical pulses: tailoring and characterization

1094-4087; In this paper, creation of pulse doublets and pulse trains by spectral phase modulation of ultrashort optical pulses is investigated. Pulse doublets with specific features are generated through step-like and triangular spectral phase modulation, whereas sequences of pulses with controllable delay and amplitude are produced via sinusoidal phase modulations. A temporal analysis of this type of tailored pulses is exposed and a complete characterization with the SPIDER technique (Spectral Phase Interferometry for Direct Electric-field Reconstruction) is presented. (C) 2004 Optical Society of America.

Self-Density Frequency-Shift Measurements of Raman N2 Q-Branch Transitions

0030-4018

Application of time-resolved spectroscopy to concentration measurements in gas mixtures

1296-2147; Concentration measurements using femtosecond Raman Induced Polarization Spectroscopy (RIPS) are performed in binary gas mixtures CO2-N2 and CO2-N2O at room temperature. The principle of these measurements is based on the nonlinear rotational time response of each molecular component of the mixture, The general form of this molecular response is a series of periodic transients with a period related to the rotational constant Be The relative strength of the individual responses allows an accurate determination of the concentration. Two techniques are presented using either two pulses (one pump and one probe) or three pulses (two pumps and one probe). (C) 2001 Academie des sciences/…

Collisional broadening and shifting parameters of the RamanQbranch ofH2perturbed byN2determined from speed-dependent line profiles at high temperatures

The broadening and shifting of the {ital Q} branch of H{sub 2} diluted in N{sub 2} are studied at temperatures between 300 and 1200 K. (i) In order to account for the observed anomalies (asymmetric profiles and nonlinearity of the linewidth versus perturber concentration), the results are interpreted using a speed-dependent model in its general form. This model introduces the speed dependence of the shift and the broadening. In contrast with the previous H{sub 2}{endash}rare-gas studies, the high-temperature measurements prove the necessity to include speed-dependent broadening that was ignored in the previous studies. (ii) Concomitantly, we report as well pure H{sub 2} results including Ra…

Analysis of femtosecond Raman-induced polarization spectroscopy (RIPS) in N2 and CO2 by fitting and scaling laws

Raman-induced polarization spectroscopy (RIPS) experiments were conducted at room temperature and pressures below 2 atm in pure N2 and CO2. Both homodyne and optically heterodyne detection were used. Calculations of the signal as a function of the pump–probe delay were performed taking into account the pulse duration of the laser, the rotational dependence of the dephasing rates and the small instantaneous electronic Kerr effect. The observed decay and shape of the rotational quantum beats are in good agreement with the calculations. Several sets of linewidth coefficients corresponding to the diagonal part of the collisional–rotational relaxation matrix were used. This matrix was choosen am…

An experimental investigation of the nonlinear refractive index (n2) of carbon disulfide and toluene by spectral shearing interferometry and z-scan techniques

International audience; The recently proposed spectral shear interferometry and the well-known z-scan techniques were employed for the determination of the nonlinear refractive index n2 of CS2, toluene and fused silica. The determined n2 values by both techniques were found to be in very good agreement. In addition, the role of the repetition rate of the laser is also investigated revealing its importance for the correct determination of both the size and the sign of the nonlinearity.

High-Resolution Stimulated Raman Spectroscopy of Methane 13CD4 in the Pentad Region

Abstract We present the first Raman spectrum of 13CD4 recorded at room temperature in the pentad region by inverse Raman spectroscopy, thus including the ν1 (A1), 2ν2 (A1), 2ν4 (A1), and ν2 + ν4(F1 + F2) Q branches. It is noteworthy that the overtone bands 2ν2 and 2ν4 are observed for the first time in a methane-like molecule by a coherent Raman process. The wide frequency range investigated, covering 45 cm−1 in three parts, contains more than 300 lines with uncertainty less than 10−3 cm−1 in most cases. These Raman data are combined with high-resolution infrared data in a weighted least-squares fit of the vibration-rotation constants of the pentad, thanks to a relevant partially reduced ef…

High-resolution photoacoustic Raman spectroscopy of gases

A high-resolution photoacoustic Raman spectroscopy experiment is described. The resolution achieved by using two single-mode pulsed lasers is about 0.0054 cm −1 (full width at half maximum intensity). The experiment was tested first on the v 1 /2v 2 bands of CO 2 and gave an increase of at least about one order of magnitude in the signal-to-noise ratio with respect to stimulated Raman spectroscopy at low pressure (ca. 10 Torr ≃ 1.3 kPa). The sensitivity is also demonstrated by the study of the weak hot band v 1 +v 2 −v 2 of CO 2 . In both cases, the experimental line shape is well reproduced by taking into account Doppler and collisional effects. A comparison with CARS spectra was also made

Controlling molecular alignment rephasing through interference of Raman-induced rotational coherence

0021-9606; Quantum control over molecular alignment rephasing is experimentally investigated in gaseous CO2. The control process is achieved by illuminating the medium with a pair of pump-pulses separated in time by approximately an integer value of T0=1/8B(0), where B(0) is the rotational constant. Through a Raman-type process, each pulse alone produces rotational coherence leading to a periodic orientational anisotropy. It is the combination of the two pulses that yields to quantum interference, resulting in a modification of this anisotropy probed by a third delayed pulse. The effect is accurately analyzed for different time delays between the two pulses. A theoretical analysis supplies …

Femtosecond polarization spectroscopy in molecular gas mixtures: Macroscopic interference and concentration measurements

0021-9606; Raman-induced polarization spectroscopy (RIPS) experiments combined with homodyne detection have been conducted with a femtosecond laser at room temperature and low pressure (p < 2 atm) in CO2-N2 mixtures as well as in air (O2-N2 mixtures). Each molecule of the mixture produces its own time-dependent signal, measured as a series of recurring transients. Macroscopic interference is observed when transients of both molecules overlap in the time domain. This interference leads to a large modification of the signal, which is well reproduced by calculations. The total signal recorded in CO2-N2 or O2-N2 mixtures of known concentration is analyzed in order to measure the polarizability …