Search results for "Coherent anti-Stokes Raman spectroscopy"
showing 8 items of 48 documents
Rotational coherence imaging and control for CN molecules through time-frequency resolved coherent anti-Stokes Raman scattering
2011
Numerical wave packet simulations are performed for studying coherent anti-Stokes Raman scattering (CARS) for CN radicals. Electronic coherence is created by femtosecond laser pulses between the X²Σ and B²Σ states. Due to the large energy separation of vibrational states, the wave packets are superpositions of rotational states only. This allows for a specially detailed inspection of the second- and third-order coherences by a two-dimensional imaging approach. We present the time-frequency domain images to illustrate the intra- and intermolecular interferences, and discuss the procedure to rationally control and experimentally detect the interferograms in solid Xe environment. peerReviewed
Analytic evaluation of Raman intensities in coupled-cluster theory
2007
We present the first implementation for the analytic calculation of polarizability derivatives using coupled-cluster theory. These derivatives are related to the intensity of bands seen in Raman spectroscopy, and are therefore important quantities that can also be measured experimentally. The required theory of analytic third derivatives is discussed and also connected to response theory to allow the calculation of frequency-dependent quantities. This work includes the use of a string-based general coupled-cluster/configuration-interaction program which makes the calculation of Raman intensities for arbitrary coupled-cluster or configuration-interaction methods up to the full configuration-…
Inhomogeneous speed effects on H-2 vibrational line profiles in ternary mixtures
2000
International audience; A study of speed inhomogeneous broadening of the hydrogen vibrational line profiles in the collisional regime for ternary mixtures is reported. The Q(1) line of H-2 in H-2-Ar-N-2, H-2-He-Ar, and H-2-He-N-2 mixtures is investigated by high resolution stimulated Raman spectroscopy for various concentrations and temperatures. A model, successfully used for binary mixtures, is extended to ternary mixtures. An excellent agreement is obtained between theory and experiment for H-2-Ar-N-2, by using the collisional parameters previously obtained from binary mixtures study. For H-2-He-Ar and H-2-He-N-2, H-2-He collisions play a "hardening" effect in the H-2 soft speed memory m…
Line coupling in Anisotropic Raman Branches
1994
Direct connection between collisional Raman cross sections and state‐to‐state rotational ones permits, within the sudden approximation, to evidence drastic decouplings from isotropic to anisotropic lines. These decouplings are consistent with the results obtained by using the strong collision model. Convenient energy corrections to the sudden approximation are used for N2 to calculate the resulting effects on the isotropic and anisotropic Q‐branch profiles in a large density range (several hundred bars). The comparison of the calculations with experimental coherent anti‐Stokes Raman scattering (CARS) and stimulated Raman (SRS) spectra of nitrogen exhibits a good agreement. Such effects coul…
Enhancement of sensitivity in high-resolution stimulated Raman spectroscopy of gases: Applicaion to the 2ν2 (1285 cm−1) band of CO2
1990
The application of a multiple-pass gas cell to quasi-cw stimulated Raman scattering is demonstrated to be a powerful method for significantly increasing the sensitivity. As a consequence, such a device offers the possibility of working in the 0.1–1 Torr pressure range for weak bands. As a striking example, experimental results are given for the 2ν2 band of CO2 at 1285 cm−1. The band is almost completely resolved with a very good signal-to-noise ratio. The Raman frequencies and the collisional broadening coefficients are determined as a function of quantum number J. Moreover, the possibility of auto-stimulated Raman effect on CO2 at moderate pressure via the sharp ν1 band (1388 cm−1) is demo…
Impulsive excitation of high vibrational states in I2–Xe complex on the electronic ground state
2010
Abstract High vibrational states, up to ν = 22, are excited and investigated on the ground electronic state of a 1:1 I 2 –Xe complex isolated in solid Kr using femtosecond CARS technique and spontaneous resonant Raman measurements. The results show that this system is a promising candidate for investigations of coherent control of bimolecular reactions by using vibrational wavepackets on the ground electronic state.
High Resolution Coherent Anti-Stokes Raman Spectroscopy (CARS) Of O 2 And CO 2
1988
With the help of high spectral quality (linewidth , 6 MHz) injection-locked flashlamp-pumped dye lasers, high resolution Coherent Anti-Stokes Raman Spectroscopy (CARS) has been applied to the study of the Q-branches of 0 2 and CO 2 . The Q-branch linewidths of 02 were obtained from the first nine transitions (J 2 = 1 to 17) recorded at pressures from 0.094 to 1 atm at room temperature. A least squares program was employed to fit calculated spectra to experimental spectra by adjusting different parameters. The collisional broadening coefficients we have obtained are consistent with available Raman data. We have also studied the Q-branch of the fundamental v1 band of CO 2 in the Fermi resonan…
High Resolution Coherent Raman Spectroscopy: Studies of Molecular Structures
1992
One of the main advantages of the non-linear coherent Raman techniques is the high resolution that can be achieved in rovibrational spectroscopy. Typically an instrumental function of the order of several thousandths of a wavenumber is routinely achieved in SRS or CARS experiments. Since the first recording of the stimulated Raman spectrum of 12CH4 in 1978 [1], numerous studies of molecules have been performed [2–8]. We have built a stimulated Raman experiment in Dijon in which particular attention has been paid to the frequency measurement of the Raman lines [9]. We will describe the application of our experiment to a wide variety of molecules over the last few years: linear molecules, sph…