Search results for "Rotational coherence"
showing 9 items of 9 documents
Dynamique induite par champ laser femtoseconde intense : alignement moléculaire en milieu gazeux dense et effet Kerr
2011
This thesis is devoted to the study of dynamics induced by intense femtoseconds lasers pulses. The first studied dynamics deals with molecular alignment of CO2-X mixtures (X=CO2, Ar, N2), in dense gases (up to 20 bar). Up to now, this regime has never been studied experimentally. In the field-free regime (after laser/matter interaction), molecular alignment exhibits two components : a permanent alignment and a transient one. The influence of collisions appears through population transfers between rotational states, which leads to a decrease of these two contributions. Permanent alignment relaxation time is only tied to inelastics collisions whereas transient alignment relaxation time is tie…
Determination of concentrations in ternary and quaternary molecular gas mixtures using femtosecond Raman spectroscopy
2002
European Conference on Nonlinear Optical Spectroscopy MAR 18-19, 2002 VILLIGEN, SWITZERLAND; Measurements of concentrations in gas mixtures of three and four molecular components are presented. They rely on a femtosecond time-resolved pump-probe technique based on Raman-induced polarization spectroscopy. The rotational time response of the molecular gas mixture is measured as a function of the pump-probe time delay. No selective frequency tunability is needed as the molecular rotational spectra are excited within the laser bandwidth. The results obtained from experiments performed at room temperature in N2O-CO2-N2 and N2O-CO2-O2-N2 mixtures are presented and the accuracy of the method is di…
Alignment of linear molecules by short duration laser pulses
2005
Alignment of linear molecules is efficiently induced by strong linearly polarized laser pulses. In the case of short pulses with respect to molecular rotation, periodic alignment appears in field-free conditions after the extinction of the field. This manuscript presents three techniques where the value of allows to quantify alignment without molecular dissociation nor additional alignment. They use a weak time-delayed probe pulse which experiences the optical properties of an aligned sample and shows modification of its characteristics. The first of them measures a depolarization due to the birefringence of the sample. The second one is based on the defocusing produced by the spatial distr…
ALIGNEMENT UNI ET TRIDIMENSIONNEL DE MOLÉCULES PAR IMPULSION LASER FEMTOSECONDE
2007
This thesis is devoted to the study of the alignment of linear and asymmetric top molecules generated by an intense laser pulse. In the case of short pulses with respect to molecular rotation, periodic alignment appears in field-free conditions after the extinction of the field. We study theoretically and experimentally the effects of intensity, temperature and polarization of the electric field on produced alignment. If the field is linearly polarized, the interaction leads to the alignment of the most polarizable axis of the molecule. If the field is elliptically polarized, the pulse can generate a simultaneous alignment of the three principal axes of inertia of an asymmetric top molecule…
Concentration measurements in molecular gas mixtures with a two-pump pulse femtosecond polarization spectroscopy technique
2001
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…
Field-free molecular alignment of CO2 mixtures in presence of collisional relaxation
2008
The present work explores the extension of the concept of short-pulse-induced alignment to dissipative environments within quantum mechanical density matrix formalism (Liouville equation) from the weak to the strong field regime. This is illustrated within the example of the CO2 molecule in mixture with Ar and He, at room temperature, for which a steep decrease of the alignment is observed at moderate pressure because of the collisional relaxation. The field-free alignment is measured by a polarization technique where the degree of alignment is monitored in the time domain by measuring the resulting transient birefringence with a probe pulse Raman induced polarization spectroscopy (RIPS) Co…
Application of time-resolved spectroscopy to concentration measurements in gas mixtures
2001
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/…
Alignement moléculaire par impulsions laser ultrabrèves : Mesures & Applications
2009
The interaction of an intense ultrashort laser pulse with a molecular sample leads, after the end of the pulse, to molecular alignment at specific time under field-free conditions. This thesis is dedicated to the measurements and applications of this effect. The degree of alignment is determined through the variation of the refractive index induced by the rearrangement of the molecular dipoles. A two-dimensional technique allowing to measure molecular alignment on a single-shot basis is reported in this document. The alignment is then exploited in order to determine physical quantities which are usually difficult to estimate through others methods. The "cross-defocusing technique" has been …
Femtosecond polarization spectroscopy in molecular gas mixtures: Macroscopic interference and concentration measurements
2000
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 …