Interpretation of negative birefringence observed in strong-field optical pump-probe experiments: High-order Kerr and plasma grating effects

The analysis of negative birefringence optically induced in major air components (Loriot et al., [1, 2]) is revisited in light of the recently reported plasma grating-induced phase-shift effect predicted for strong field pump-probe experiments (Wahlstrand and Milchberg, [3]). The nonlinear birefrin- gence induced by a short and intense laser pulse in argon is measured by femtosecond time-resolved polarimetry. The experiments are performed with degenerate colors, where the pump and probe beam share the same spectrum, or with two different colors and non-overlapping spectra. The in- terpretation of the experimental results is substantiated using a numerical 3D+1 model accounting for nonlinear…

Field-free molecular alignment of asymmetric top molecules using elliptically polarized laser pulses

International audience; We show theoretically that a short specific elliptically polarized laser pulse driving an asymmetric top molecule can induce postpulse revivals of three-dimensional (3-D) alignment. By choosing the field ellipticity resulting in the best compromise between the alignment of two molecular axes, we demonstrate that efficient 3-D alignment can be achieved at low temperature. In the experiment, the field-free alignment of moderately cool ethylene molecules is probed by using a technique based on the optical Kerr effect. Control of 3-D field-free alignment opens the door to a large range of applications in chemistry as well as in molecular optics.

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 …

Nonintrusive monitoring and quantitative analysis of strong laser-field-induced impulsive alignment

We report the observation of impulsive alignment of $\mathrm{C}{\mathrm{O}}_{2}$ molecules produced through their interaction with a nonresonant, strong laser pulse. The periodic alignment is monitored using a polarization technique generally employed in optical Kerr effect experiments; the birefringence produced by alignment of the molecular sample is measured with a weak pulse, time-delayed with respect to the alignment pulse. The technique provides a signal proportional to $⟨{\mathrm{cos}}^{2}\phantom{\rule{0.2em}{0ex}}\ensuremath{\theta}⟩\ensuremath{-}\frac{1}{3}$, where $\ensuremath{\theta}$ is the polar angle between the molecular axis and the strong-field polarization axis. Experimen…

Femtosecond time resolved coherent anti-Stokes Raman spectroscopy: Experiment and modelization of speed memory effects on H2-N2 mixtures in the collision regime

194317; With the aim of temperature diagnostic, femtosecond time-resolved CARS (coherent anti-Stokes Raman spectroscopy) is applied to probe H2 in H2-N2 mixtures. In a first part, a Lorentzian profile is used to model the femtosecond CARS response. A difference between the experimental broadening and the expected one is observed in the collision regime. The observed broadening increases strongly in an inhomogeneous way with respect to the perturber concentration. This is of considerable importance for temperature measurements. In a second part, we show that in the collision regime, this inhomogeneous broadening is due to the speed dependence of the collisional parameters and the memory effe…

Dynamical Stark Effect in the nu(2)/nu(4) Vibrational Polyad of SiH(4): Theory and Observation.

We report a theoretical and experimental investigation of the dynamical Stark effect in a tetrahedral molecule, silane (SiH(4)). We use a tetrahedral formalism and Floquet theory to calculate the absorption spectra for the molecule dressed by an intense nonresonant pulsed laser. Experimentally, the dynamical Stark effect is observed for transitions of the nu(2)/nu(4) vibrational polyad of SiH(4) by means of nanosecond diode laser absorption spectroscopy and a Nd:YAG laser excitation. Copyright 2000 Academic Press.

Quantum Control in Atomic Systems

We review a series of recent experiments demonstrating quantum control of atomic processes and products induced by the interaction of the atom with coherent bichromatic electromagnetic fields. Since the effects under consideration are electromagnetically induced, control is established through the field parameters i.e. frequency, amplitude and phase. The controlled processes include resonant and non resonant multiphoton ionization, autoionization, radiative decay in multiple continua (ionization branching ratios) and third harmonic generation.

Contrôle de paquets d'ondes rotationnels par impulsions laser ultrabrèves modulées en phase

Une superposition lineaire d'etats rotationnels est produite dans le niveau vibronique de base de la molecule d'azote (Ni) par une impulsion laser ultra-breve non resonnante. Un controle precis de ce paquet d'ondes, a travers la modulation de phase spectrale du champ electrique excitateur, est demontre experimentalement. L'excitation relative entre modes Raman associes a des niveaux de parite donnee est realisee. L'evolution temporelle du paquet d'ondes rotationnel mis en forme est observee par une technique de spectroscopie de polarisation. Les resultats experimentaux sont confortes par une analyse theorique menee dans l'espace des temps et des frequences.

Field-free molecular alignment for probing collisional relaxation dynamics

International audience; We report the experimental study of field-free molecular alignment in CO2 gas mixtures induced by intense femtosecond laser pulses in the presence of collisional processes. We demonstrate that the alignment signals exhibit specific features due to nontrivial collisional propensity rules that tend to preserve the orientation of the rotational angular momentum of the molecules. The analysis is performed with a quantum approach based on the modeling of rotational J- and M-dependent state-to-state transfer rates. The present work paves the way for strong-field spectroscopy of collisional dynamics.

Higher-order Kerr effect in ultrashort laser pulse propagation and laser filamentation

We discuss the contribution of the higher-order Kerr effect (HOKE) to the propagation of ultrashort laser pulses in several contexts. We show that their consideration is necessary to adequately reproduce experimental data about harmonics generation, propagation in hollow-core fibers, and laser filamentation. In the latter case, our results show that the HOKE play a key role for short pluses and/or long wavelengths, while the plasma contributes more for long pulses and/or short wavelengths.

Measurement of high order Kerr refractive index of major air components: erratum

A clarification is missing concerning the high order Kerr non-linearities deduced from our experimental data published in [Opt. Express 17, 13429-13434 (2009)]. Here, we rectify this omission by making explicit the distinction between cross-Kerr and Kerr effects, and by extrapolating the value of the nonlinear refractive index for the last effect. Since the occurrence of sign inversion in the Kerr effect is not affected, the overall report in [Opt. Express 17, 13429-13434] remains valid.

Probing ultrafast thermalization with field-free molecular alignment

International audience; The rotation-translation thermalization of CO2 gas is investigated 500 ps after its preheating by a nonresonant short and intense laser pulse. The temperature of thermalization is optically determined with two additional short laser pulses enabling a field-free molecular alignment process and its probing, respectively. The measurements are performed for various intensities of the preheat pulse, leading to the observation of different temperatures which are in very good agreement with classical molecular dynamics simulations. The results can be regarded as a step towards real-time tracking of ultrafast relaxation pathways in molecular motion.

Molecular alignment in CO2 mixtures induced by a short nonresonant intense pulse : effect of collisional relaxation

Observation of two-XUV-photon ionization using harmonic generation from a short, intense laser pulse

We report the observation of a two-photon ionization process in the XUV wavelength regime. In a near-resonant 1 + 1 ionization scheme, Ar atoms are ionized absorbing the 15 eV third harmonic photons produced in a gas jet by the 0.5 ps intense laser pulses of a KrF excimer laser emitting at 248.6 nm. The present demonstration of a non-linear process in the XUV regime reveals feasibility of high-intensity applications utilizing the uniquely high peak power of non-conventional short wavelength radiation sources based on harmonic generation.

Measurement of high order Kerr refractive index of major air components

International audience; We measure the instantaneous electronic nonlinear refractive index of N2 , O2 , and Ar at room temperature for a 90 fs and 800 nm laser pulse. Measurements are calibrated by post-pulse molecular alignment through a polarization technique. At low intensity, quadratic coefficients n2 are determined. At higher intensities, a strong negative contribution with a higher nonlinearity appears, which leads to an overall negative nonlinear Kerr refractive index in air above 26 TW/cm2 .

Field-free one-dimensional alignment of ethylene molecule

International audience; We report an experimental study of non-adiabatic laser-induced molecular alignment of ethylene (C2H4) using a linearly polarized short laser pulse of moderate intensity. The information about the confinement of the C=C bond axis along the direction of the applied electric field is obtained by measuring the depolarization of a second short pulse of weak intensity interacting with the molecules after they have been exposed to the first pulse. The experimental data are compared with the numerical simulation of the Schr¨odinger equation written for the non-resonant interaction of an asymmetric top rigid rotor with a linearly polarized electric field. The field-free align…

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…

Orientation of Polar Molecules by Laser Induced Adiabatic Passage

International audience; We show that two overlapping linearly polarized laser pulses of frequencies ω and its second harmonic 2ω can strongly orient linear polar molecules, by adiabatic passage along dressed states. The resulting robust orientation can be interpreted as a laser-induced localization in the effective double well potential created by the fields, which induces a preliminary molecular alignment. The direction of the orientation can be selected by the relative phase of the fields.

Optical kerr effect in the strong field regime

The optical Kerr response of hydrogen atom submitted to a strong and short near infrared laser pulse excitation is studied by solving the full 3D time-dependent Schro¨dinger equation. The nonlinear polarization evaluated at the driving field frequency is compared to the canonical expression derived from perturbation theory. A discrepancy between the two models is observed at large intensity affecting the nonlinear propagation of short and intense laser pulses.

Using molecular alignment to track ultrafast collisional relaxation

Field-free molecular alignment has been used in order to track the collisional relaxation occurring in a molecular gas. CO${}_{2}$ molecules were initially irradiated by a short linearly polarized laser pulse resulting in the increase of their rotational energy. The evolution of the subsequent ultrafast relaxation process was optically probed after irradiating the sample with a second, weaker, short pulse leading to the alignment of the preheated molecules. Using classical molecular dynamic simulations, we were able to quantitatively reproduce the experimental shapes and amplitudes of the recorded revival transients for a time interval extending from 25 to 500 ps until thermalization of the…

Echo-assisted impulsive alignment of room-temperature acetone molecules

International audience; We experimentally and theoretically investigate the field-free alignment of the asymmetric-top acetone molecule. Our study shows that the production of postpulse aligned molecules in a dense sample (0.05-0.2 bar) of room-temperature acetone using a single-pulse excitation can be significantly improved by rotational alignment echoes induced in a two-pulse excitation scheme. We report the observation of fractional echoes that can be used to reveal the nonlinearity of the molecular system. In a proof-of-principle experiment, a pre-aligned sample of acetone is also used for third-harmonic generation. The analysis of the experimental data with numerical simulations based …

Ultrafast buffering by molecular gas

A simple molecular gas sample can be used to achieve ultrafast optical buffering in two-dimensional optical imaging, thus serving as a promising extension of the well-developed liquid-crystal display technology.

L'alignement moléculaire comme une méthode de calibration pour la détermination de probabilité d'ionisation

Par le biais d'une methode originale, nous avons determine experimentalement la probabilite d'ionisation de l'azote (N 2 ) soumis a un champ laser non resonnant et ultracourt (100 fs). La technique de defocalisation croisee mis en oeuvre dans ce travail est sensible a l'alignement moleculaire post-impulsion et a l'ionisation. L'analyse du signal experimental permet d'extraire une probabilite d'ionisation calibree par une mesure d'alignement.

Strong-field molecular ionization: determination of ionization probabilities calibrated with field-free alignment

International audience; We report an original optical method providing the probability of molecular ionization induced by femtosecond laser pulses. The approach consists of exploiting molecular alignment in order to extract reliable information about ionization. The cross defocusing technique implemented for this purpose reveals a sensitivity with respect to post-pulse alignment, as well as to free electron density induced by the ultra-short laser pulse. The analysis of the resulting signal gives thus access to absolute single-ionization probabilities calibrated through the degree of alignment provided that free electrons are mainly produced from single-ionization. The relevance of the meth…

Orientation and Alignment Echoes

We present one of the simplest classical systems featuring the echo phenomenon---a collection of randomly oriented free rotors with dispersed rotational velocities. Following excitation by a pair of time-delayed impulsive kicks, the mean orientation or alignment of the ensemble exhibits multiple echoes and fractional echoes. We elucidate the mechanism of the echo formation by the kick-induced filamentation of phase space, and provide the first experimental demonstration of classical alignment echoes in a thermal gas of ${\mathrm{CO}}_{2}$ molecules excited by a pair of femtosecond laser pulses.

Temperature measurement in gas mixtures by femtosecond Raman-induced polarization spectroscopy

The potential of femtosecond Raman-induced polarization spectroscopy (RIPS) for the simultaneous determination of temperature and concentrations was investigated. These measurements were related to the rotational time response of the molecular gas mixture, which was measured as a function of the pump-probe time delay. The change of the polarizability anisotropy with respect to the vibrational levels was taken into account. The results of temperature measurements in pure CO2 showed good agreement with the values obtained by a thermocouple. The RIPS technique was also applied to a CO2-N2 gas mixture to determine simultaneously temperatures and concentrations at temperatures up to 600 K. The a…

Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses

We show that a linear molecule subjected to a short specific elliptically polarized laser field yields postpulse revivals exhibiting alignment alternatively located along the orthogonal axis and the major axis of the ellipse. The effect is experimentally demonstrated by measuring the optical Kerr effect along two different axes. The conditions ensuring an optimal field-free alternation of high alignments along both directions are derived.

Measurement of laser-induced alignment of molecules by cross defocusing

0146-9592; The field-free alignment of CO2 produced in response to the excitation of a molecule by a high-intensity femtosecond pump pulse is measured with a simple coronography-like technique. The technique is based on the defocusing of a time-delayed probe pulse produced by the spatial distribution of aligned molecules. In the intensity regime explored here, the technique is shown to give valuable information about dynamic alignment. With the help of simulations, the degree of alignment is extracted from the data. (C) 2005 Optical Society of America.

Mid-infrared supercontinuum generation from 2 to 14 μm in various chalcogenide glasses optical fibers

Chalcogenide glasses optical fibers with step index or microstructured profiles are drawn from low toxicity compositions. Supercontinuum generation lead to an infrared spectrum spanning from 2 to 14µm with a 10µm core fiber of 40mm length.

Wavelength dependence of multiphoton ionization of xenon

We have studied the multiphoton ionization of xenon atoms by $160\phantom{\rule{0.3em}{0ex}}\mathrm{fs}$ pulses at intensities of $5\ifmmode\times\else\texttimes\fi{}{10}^{12}$ and $1.3\ifmmode\times\else\texttimes\fi{}{10}^{13}\phantom{\rule{0.3em}{0ex}}\mathrm{W}∕{\mathrm{cm}}^{2}$ and present photoelectron kinetic energy and angular distribution spectra measured with a photoelectron imaging spectrometer. A noncollinear optical parametric amplifier allows us to tune the wavelength of the laser pulse over a range between 500 and $700\phantom{\rule{0.3em}{0ex}}\mathrm{nm}$. Resonant and nonresonant processes as well as channel switching effects have been observed in this intensity and wavel…

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.

Field-free molecular alignment for measuring ionization probability

International audience; We have shown in a recent letter (Loriot et al 2006 Opt. Lett. 31 2897) the possibility of determining the ionization probability of linear molecules by using an all-optical technique that takes advantage of post-pulse molecular alignment. To that end, we have implemented a ‘cross-defocusing' technique producing a signal sensitive to both alignment and ionization. The analysis of the signal provides a quantitative measurement of the ionization probability calibrated with molecular alignment. In the present work, the method is discussed in more detail and applied to the measurement of the ionization probability of N2 as well as to the determination of the ionization r…

Optically Probed Laser-Induced Field-Free Molecular Alignment

Molecular alignment induced by laser fields has been investigated in research laboratories for over two decades. It led to a better understanding of the fundamental processes at play in the interaction of strong laser fields with molecules, and also provided significant contributions to the fields of high harmonic generation, laser spectroscopy, and laser filamentation. In this chapter, we discuss molecular alignment produced under field-free conditions, as resulting from the interaction of a laser pulse of duration shorter than the rotational period of the molecule. The experimental results presented will be confined to the optically probed alignment of linear as well as asymmetric top mol…

Laser spatial profile effects in measurements of impulsive molecular alignment

0953-4075; We use a non-intrusive technique based on a polarization scheme to probe the periodic alignment of the CO2 and N2 molecules induced by a strong laser pulse linearly polarized. A weak probe field experiences the birefringence resulting from the alignment of the molecules. By comparing the probe depolarization signal with the numerical simulation of the time-dependent Schrödinger equation, it is possible to quantify the alignment of the molecular sample. The modelling takes into account the spatial profile of the pump intensity. It allows from the alignment signal to determine the onset of saturation due to ionization, despite the intrinsic saturation of the alignment arising for a…

Controlling ground-state rotational dynamics of molecules by shaped femtosecond laser pulses

We report controlled excitation of ground-state rotational wave packet by pulse-shaping technique. The experiment is conducted in nitrogen $({\mathrm{N}}_{2})$ at room temperature and atmospheric pressure. A femtosecond laser pulse produces rotational coherences in the vibronic ground state of ${\mathrm{N}}_{2}$ through an impulsive Raman process. The laser pulse is tailored using a spatial light modulator producing spectral phase modulation. Periodic phase steps are applied in order to control the excitation of specific rotational Raman transitions. The outcome is the modification of the relative excitation between odd and even rotational states which allows the control of the symmetry and…

Transition from plasma-driven to Kerr-driven laser filamentation.

While filaments are generally interpreted as a dynamic balance between Kerr focusing and plasma defocusing, the role of the higher-order Kerr effect (HOKE) is actively debated as a potentially dominant defocusing contribution to filament stabilization. In a pump-probe experiment supported by numerical simulations, we demonstrate the transition between two distinct filamentation regimes at 800 nm. For long pulses (1.2 ps), the plasma substantially contributes to filamentation, while this contribution vanishes for short pulses (70 fs). These results confirm the occurrence, in adequate conditions, of filamentation driven by the HOKE rather than by plasma.

Filament-induced visible-to-mid-IR supercontinuum in a ZnSe crystal: Towards multi-octave supercontinuum absorption spectroscopy

Abstract We report on the generation of multiple-octave supercontinuum laser source spanning from 0.5 μm to 11 μm induced by multi-filamentation in a ZnSe crystal. The generated supercontinuum is both spatially and spectrally characterized. It is then exploited in a proof-of-principle experiment for methane spectroscopy measurements by means of the supercontinuum absorption spectroscopy technique. The entire absorption spectrum is successfully recorded within the whole spectral bandwidth of the supercontinuum. Experimental results are in fairly good agreement with the HITRAN database, confirming the reliability and stability over several hours of the generated supercontinuum.

Postpulse molecular alignment measured by a weak field polarization technique

We report a direct nonintrusive observation of alignment and planar delocalization of ${\mathrm{C}\mathrm{O}}_{2}$ after an intense linearly polarized femtosecond laser pulse excitation. The effects are measured by a polarization technique involving a perturbative probe that itself does not induce appreciable alignment. We show that this technique allows one to measure a signal proportional to $⟨{cos}^{2}\ensuremath{\theta}⟩\ensuremath{-}1/3$, with $\ensuremath{\theta}$ the angle between the molecular axis and the laser polarization. Simulations that support this analysis allow one to characterize the experimentally observed alignment and planar delocalization quantitatively.

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…

Molecular quantum interface for storing and manipulating ultrashort optical vortex

Light beams carrying orbital angular momentum (OAM) have become over the past few years a subject of widespread interest with unprecedented applications in various fields such as optical communication, super-resolution imaging, optical tweezers, or quantum processing. We demonstrate in the present work that gas-phase molecules can be used as a quantum interface to store an OAM carried by an ultrashort laser pulse. The interplay between spin angular momentum and OAM is exploited to encode the spatial phase information of light beams into rotational coherences of molecules. The embedded spatial structure is restored on-demand with a reading beam by taking advantage of field-free molecular ali…

Spectral dependence of purely-Kerr driven filamentation in air and argon

5 pags, 4 figs.-- PACS number(s): 42.65.Jx, 42.65.Tg, 78.20.Ci. -- Publisher error corrected 27 September 2010, Erratum Phys. Rev. A 82, 039905 (2010): https://doi.org/10.1103/PhysRevA.82.033826

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…

Field-free molecular alignment of CO2 mixtures in presence of collisional relaxation

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…

Realization of time-resolved two-vacuum-ultraviolet-photon ionization

International audience; Ultrafast dynamics of excited molecules is studied through time-resolved two-vacuum-ultraviolet (vuv)- photon ionization using a nonlinear volume autocorrelator unit. The two-vuv-photon process is induced by the intense fifth harmonic radiation of a femtosecond Ti:sapphire laser. In a proof-of-principle experiment, ultrafast dynamics of excited ethylene and oxygen molecules are investigated. Molecular decay times are deduced by comparing the experimental data with the results of a numerical model that accounts for the spatial and temporal characteristics of the harmonic field. The present experiments pave a convenient way for time domain investigations in the vuv-xuv s…

Harmonic Generation and Nonlinear Propagation: When Secondary Radiations Have Primary Consequences

In this Letter, it is experimentally and theoretically shown that weak odd harmonics generated during the propagation of an infrared ultrashort ultraintense pulse unexpectedly modify the nonlinear properties of the medium and lead to a strong modification of the propagation dynamics. This result is in contrast with all current state-of-the-art propagation model predictions, in which secondary radiations, such as third harmonic, are expected to have a negligible action upon the fundamental pulse propagation. By analyzing full three-dimensional ab initio quantum calculations describing the microscopic atomic optical response, we have identified a fundamental mechanism resulting from interfere…

Laser-induced field-free alignment of the OCS molecule

We investigate the dynamical alignment of jet-cooled OCS molecules induced by a short laser pulse. The alignment is measured through the orientational contribution of the optical Kerr effect using a second weak laser pulse as a probe. Maximum alignment is observed at conditions close to saturation of ionization. The results are analysed with a quantum mechanical model solving for the rotational dynamics.

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.

Observation of laser-induced field-free permanent planar alignment of molecules

International audience; Permanent planar alignment of gas-phase linear molecules is achieved by a pair of delayed perpendicularly polarized short laser pulses. The experiment is performed in a supersonic jet, ensuring a relatively high number density of molecules with moderately low rotational temperature. The effect is optically probed on a femtosecond time scale by the use of a third short pulse, enabling a time-resolved birefringence detection performed successively in two perpendicular planes of the laboratory frame. The technique allows for an unambiguous estimation of the molecular planar delocalization produced within the polarization plane of the pulse pair after the turn-off of the…

General approach to spatiotemporal modulational instability processes

International audience; In this article, we derive the general exact solution of the modulation instability gain. The solution described here is valid for 1-D, 2-D, and 3-D cases considering any temporal response function of the medium and with possible higher order Kerr nonlinearities. In particular, we show that the gain induced by modulation instability is initial condition dependent, while the usual calculations do not lead to such a dependence. Applications for current and high-interest nonlinear propagation problems, such as 1-D optical fiber propagation with delayed Raman response and 2-D filamentation in gases, are investigated in detail. More specifically, we demonstrate that the 2-D …

Higher-order Kerr effects improve quantitative modelling of harmonics generation and laser filamentation

The consideration of the higher-order Kerr effect (HOKE) drastically improves the quantitative agreement between measured and simulated harmonic yield as well as intensity and electron density in laser filaments generated by pulses below a few hundreds of fs. In longer pulses, the plasma defocusing plays a much more important role.

Field-free molecular alignment in presence of collisional relaxations

Determination of concentrations in ternary and quaternary molecular gas mixtures using femtosecond Raman spectroscopy

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 discussed. Copyright © 2002 John Wiley & Sons, Ltd.

Field-free molecular orientation of1Σand2Πmolecules at high temperature

We analyze the control of field-free molecular orientation at high temperature by use of a two-color laser bipulse strategy proposed in Zhang et al. [Phys. Rev. A 83, 043410 (2011)]. A general study shows that there exist two types of linear molecules for which a different mechanism has to be used. For molecules with a large hyperpolarizability, a monochromatic laser pre-pulse is applied before the two-color laser pulse at a time close to the rotational period ${T}_{r}$, while for molecules with a small hyperpolarizability, the optimal delay is found close to ${T}_{r}/4$ or $3{T}_{r}/4$. We extend this analysis to the case of a ${}^{2}\phantom{\rule{-0.16em}{0ex}}\ensuremath{\Pi}$ molecule …

Tracking Autoionizing-Wave-Packet Dynamics at the 1-fs Temporal Scale

We present time-resolved studies and Fourier transform spectroscopy of inner-shell excited states undergoing Auger decay and doubly excited autoionizing states, utilizing coherent extreme-ultraviolet (XUV) radiation continua. Series of states spanning a range of ∼4  eV are excited simultaneously. An XUV probe pulse tracks the oscillatory and decaying evolution of the formed wave packet. The Fourier transform of the measured trace reproduces the spectrum of the series. The present work paves the way for ultrabroadband XUV spectroscopy and studies of ultrafast dynamics in all states of matter.

Observation of field phase dependent autoionization

We report on the observation of a field phase dependent autoionization rate of calcium in the region of the doubly excited state. Excitation of the autoionizing state occurs from the atomic ground state through two phase related and hence interfering channels, namely a three photon channel and a single photon channel , being the third harmonic of . The autoionization rate exhibits a sinusoidal modulation as a function of the relative phase of the two excitation fields. Both ionizing fields are not focused in the interaction region, thus demonstrating the possibility of phase control in a large interaction volume and free of phase shift effects associated with focused geometries.

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/…

Filamentation-induced spectral broadening and pulse shortening of infrared pulses in Tellurite glass

Abstract Filamentation of infrared femtosecond pulses in Tellurite glass is reported, leading to the generation of a supercontinuum generation spanning from the visible up to 4 μm. The angular distribution of the supercontinuum shows clear evidence of conical waves generation, in particular, in the visible region. Moreover, taking advantage of the spatio-temporal self-focusing effect occurring in the Tellurite glass, a twofold pulse shortening is demonstrated. Tellurite glass appears as a very convenient, versatile and promising medium for femtosecond nonlinear optics in the infrared region.

Control of field-free molecular alignment by phase-shaped laser pulses

We report an experimental study of the control of molecular alignment of ${\mathrm{N}}_{2}$ by use of spectrally modulated pulses at an intensity regime below the intrinsic saturation of the alignment. By manipulating the relative timing of the alignment revival pattern arising from the even subset of the thermal ensemble as compared to the odd subset, we demonstrate that the angular distribution of the aligned molecule can be converted into planar delocalization at specific times. We also show that the angular focusing of the molecular axis can be switched off by applying a specific bipulse.

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…

Field-free molecular alignment induced by elliptically polarized laser pulses: Noninvasive three-dimensional characterization

International audience; An investigation of field-free molecular alignment produced by elliptically polarized laser pulses is reported. Experiments are conducted in CO2 at room temperature. A noninvasive all-optical technique, based on the cross defocusing of a probe pulse, is used to measure the alignment along two orthogonal directions which is sufficient to provide a three-dimensional characterization. The field-free molecular alignment produced by a laser of elliptical polarization is in good agreement in terms of amplitude and shape with theoretical predictions. It turns out to be almost equivalent to the superposition of the effects that one would obtain with two individual cross-pola…

Femtosecond Raman Spectroscopy of C2H4 and CH4 molecules

Optical gratings induced by field-free alignment of molecules

We analyze the alignment of molecules generated by a pair of crossed ultra-short pump pulses of different polarizations by a technique based on the induced time-dependent gratings. Parallel polarizations yield an intensity grating, while perpendicular polarizations induce a polarization grating. We show that both configurations can be interpreted at moderate intensity as an alignment induced by a single polarized pump pulse. The advantage of the perpendicular polarizations is to give a signal of alignment that is free from the plasma contribution. Experiments on femtosecond transient gratings with aligned molecules were performed in CO2 at room temperature in a static cell and at 30 K in a …

Optimization of field-free molecular alignment by phase-shaped laser pulses

We theoretically demonstrate the optimization of field-free molecular alignment by phase-shaped femtosecond laser pulses. The effect is assessed in ${\mathrm{O}}_{2}$ at $T=60\phantom{\rule{0.3em}{0ex}}\mathrm{K}$ under realistic conditions of intensity and pulse shaping. The spectral laser phase is sampled through 128 control parameters and a self-learning evolutionary algorithm combined with a nonperturbative regime calculation is used in order to design the specific phase that maximizes the degree of alignment. The postpulse molecular alignment appears significantly enhanced compared to a Fourier-transform-limited pulse of same energy. The analysis of the target state reveals that the so…

High rate concentration measurement of molecular gas mixtures using a spatial detection technique

International audience; Concentration measurement in molecular gas mixtures using a snapshot spatial imaging technique is reported. The approach consists of measuring the birefringence of the molecular sample when field-free alignment takes place, each molecular component producing a signal with an amplitude depending on the molecular density. The concentration measurement is obtained on a single-shot basis by probing the time-varying birefringence through femtosecond time-resolved optical polarigraphy (FTOP). The relevance of the method is assessed in air.

Spectroscopie Raman Anti-Stokes Cohérente femtoseconde (DRASC – fs) : expériences et modélisation dans le cas du mélange H2 – N2 à basse pression

Dans l'objectif du diagnostic de la temperature dans les milieux en combustion, la Diffusion Raman Anti-Stokes Coherente resolue en temps (DRASC - fs) est utilisee pour sonder H 2 dans les melanges H 2 -N 2 a basse pression. Le dispositif DRASC mis en place est decrit en detail. Un nouveau modele de la reponse DRASC temporelle, prenant en compte tous les effets collisionnels specifiques a l'hydrogene (effets dits « de vitesse ») est presentee, ainsi que la comparaison avec l'experience, l'accord se revelant tres satisfaisant.

Higher-order Kerr terms allow ionization-free filamentation in gases.

We show that higher-order nonlinear indices ($n_4$, $n_6$, $n_8$, $n_{10}$) provide the main defocusing contribution to self-channeling of ultrashort laser pulses in air and Argon at 800 nm, in contrast with the previously accepted mechanism of filamentation where plasma was considered as the dominant defocusing process. Their consideration allows to reproduce experimentally observed intensities and plasma densities in self-guided filaments.

Snapshot imaging of postpulse transient molecular alignment revivals

Laser induced field-free alignment of linear molecules is investigated by using a single-shot spatial imaging technique. The measurements are achieved by femtosecond time-resolved optical polarigraphy (FTOP). Individual alignment revivals recorded at high resolution in ${\text{CO}}_{2}$, as well as simultaneous observation of several alignment revivals produced within the rotational period of the ${\text{O}}_{2}$ molecule are reported. The data are analyzed with a theoretical model describing the alignment experienced by each molecule standing within the interaction region observed by the detector. The temporal dynamics, intensity dependence, and degree of alignment are measured and compare…

Speed-memory effects in H2-N2 mixtures studied by CARS femtosecond. Experiments and modelization from the collisional to the Doppler regime

High-field quantum calculation reveals time-dependent negative Kerr contribution

The exact quantum time-dependent optical response of hydrogen under strong field near infrared excitation is investigated and compared to the perturbative model widely used for describing the effective atomic polarization induced by intense laser fields. By solving the full 3D time-dependent Schr\"{o}dinger equation, we exhibit a supplementary, quasi-instantaneous defocusing contribution missing in the weak-field model of polarization. We show that this effect is far from being negligible in particular when closures of ionization channels occur and stems from the interaction of electrons with their parent ions. It provides an interpretation to higher-order Kerr effect recently observed in v…

Visualizing coherent molecular rotation in a gaseous medium

Inducing and controlling the ultrafast molecular rotational dynamics using shaped laser fields is essential in numerous applications. Several approaches exist that allow following the coherent molecular motion in real-time, including Coulomb explosion-based techniques and recovering molecular orientation from the angular distribution of high harmonics. We theoretically consider a non-intrusive optical scheme for visualizing the rotational dynamics in an anisotropic molecular gas. The proposed method allows determining the instantaneous orientation of the principal optical axes of the gas. The method is based on probing the sample using ultra-short circularly polarized laser pulses and recor…

Femtosecond Raman time-resolved molecular spectroscopy

International audience; The applicability of several femtosecond time resolved non-linear coherent techniques such as Raman induced polarization spectroscopy (RIPS), degenerate four-wave mixing (DFWM) and coherent anti-Stokes Raman spectroscopy (CARS) for molecular spectroscopy is presented. All methods rely on the initial coherent excitation of molecular states producing wavepackets, whose time evolution is then measured. In the case of RIPS and DFWM only pure rotational transitions are involved, whereas in CARS vibrational states can be excited. First the methodology of concentration and temperature measurements using RIPS in gas mixtures involving N2, CO2, O2, and N2O is shown. In additi…

Controlling ionization products through laser-induced continuum structure

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.

Suppression of plasma contribution in femtosecond degenerate four-wave mixing (fs-DFWM) at high intensity

Femtosecond degenerate four-wave mixing (fs-DFWM) experiments in CO2 exhibit a strong background due to plasma produced at high intensity (≥20 TW/cm2), when significant molecular alignment is likely to arise. This perturbing phenomenon renders the measurements of alignment very difficult. It is shown that the plasma contribution can be avoided by employing perpendicular polarizations for the two pump pulses. The effect is explained on the basis of the different diffraction angles between signals produced by molecular alignment and plasma. Copyright © 2007 John Wiley & Sons, Ltd.

Femtosecond Raman time-resolved molecular spectroscopy

Abstract The applicability of several femtosecond time resolved non-linear coherent techniques such as Raman induced polarization spectroscopy (RIPS), degenerate four-wave mixing (DFWM) and coherent anti-Stokes Raman spectroscopy (CARS) for molecular spectroscopy is presented. All methods rely on the initial coherent excitation of molecular states producing wavepackets, whose time evolution is then measured. In the case of RIPS and DFWM only pure rotational transitions are involved, whereas in CARS vibrational states can be excited. First the methodology of concentration and temperature measurements using RIPS in gas mixtures involving N2, CO2, O2, and N2O is shown. In addition some applica…

Optical Imaging of Coherent Molecular Rotors

International audience; Short laser pulses are widely used for controlling molecular rotational degrees of freedom and inducing molecular alignment, orientation, unidirectional rotation and other types of coherent rotational motion. To follow the ultra-fast rotational dynamics in real time, several techniques for producing molecular movies have been proposed based on the Coulomb explosion of rotating molecules, or recovering molecular orientation from the angular distribution of high-harmonics. The present work offers and demonstrates a novel non-destructive optical method for direct visualization and recording of movies of coherent rotational dynamics in a molecular gas. The technique is b…

Ultrafast collisional dissipation of symmetric-top molecules probed by rotational alignment echoes

We experimentally and theoretically investigate the ultrafast collisional dynamics of a symmetric-top molecule (${\mathrm{C}}_{2}{\mathrm{H}}_{6}$) in pure gas and mixtures with He at high density by employing the rotational alignment echo created by a pair of time-delayed intense laser kicks. The decrease of the amplitude of the echo when increasing the delay between the two laser pulses, reflecting the collisional relaxation of the system, is measured by probing the transient birefringence induced in the medium. The theoretical predictions, carried using purely classical molecular dynamics simulations, reproduce well the observed features, as demonstrated previously for a linear molecule.…

Rotational echoes as a tool for investigating ultrafast collisional dynamics of molecules

We show that recently discovered rotational echoes of molecules provide an efficient tool for studying collisional molecular dynamics in high-pressure gases. Our study demonstrates that rotational echoes enable the observation of extremely fast collisional dissipation, at timescales of the order of a few picoseconds, and possibly shorter. The decay of the rotational alignment echoes in ${\mathrm{CO}}_{2}$ gas and ${\mathrm{CO}}_{2}\text{\ensuremath{-}}\mathrm{He}$ mixture up to 50 bar was studied experimentally, delivering collision rates that are in good agreement with the theoretical expectations. The suggested measurement protocol may be used in other high-density media, and potentially …

Dissipation of post-pulse laser-induced alignment of CO2through collisions with Ar

In this paper, laser-induced field-free alignment of CO2 in mixtures with Ar is investigated under dissipative conditions (up to 15 bars) at room temperature. The degree of alignment is temporally monitored by a polarization spectroscopy technique, where a weak probe pulse measures the transient birefringence resulting from the alignment. The data are analyzed with a quantum mechanical density matrix formalism using properly J-dependent and M-dependent state-to-state transfer rates, which was previously successfully tested on pure CO2 and CO2–He mixtures. The same consistency is obtained between experiments and calculations, in particular the decay times of both the transient revivals and t…

Spatiotemporal rotational dynamics of laser-driven molecules

Molecular alignment and orientation by laser fields has attracted significant attention in recent years, mostly due to new capabilities to manipulate the molecular spatial arrangement. Molecules can now be efficiently prepared for ionization, structural imaging, orbital tomography, and more, enabling, for example, shooting of dynamic molecular movies. Furthermore, molecular alignment and orientation processes give rise to fundamental quantum and classical phenomena like quantum revivals, Anderson localization, and rotational echoes, just to mention a few. We review recent progress on the visualization, coherent control, and applications of the rich dynamics of molecular rotational wave pack…

Polarization shaping for unidirectional rotational motion of molecules.

Control of the orientation of the angular momentum of linear molecules is demonstrated by means of laser polarization shaping. For this purpose, we combine two orthogonally polarized and partially time-overlapped femtosecond laser pulses so as to produce a spinning linear polarization which in turn induces unidirectional rotation of N2 molecules. The evolution of the rotational response is probed by a third laser beam that can be either linearly or circularly polarized. The physical observable is the frequency shift imparted to the probe beam as a manifestation of the angular Doppler effect. Our experimental results are confirmed by theoretical computations, which allow one to gain a deep p…

Optical Diagnostics with Ultrafast and Strong Field Raman Techniques

In this chapter, we will discuss some coherent techniques, namely Raman Induced Polarization Spectroscopy (RIPS) and femtosecond Coherent Raman Anti-Stokes Spectroscopy (fs-CARS). We will demonstrate their ability to be used as non-invasive optical diagnostic tools for temperature, density, or concentration measurements, as well as a means of testing collision induced energy transfer models (in a low field regime), and studying the so-called inhomogeneous lineshape effects that are particularly enhanced in the case of hydrogen. We will also show how molecular alignment achieved in a strong field regime can provide additional information about collisional relaxation processes. In all cases, …

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 …

Rotational Raman spectroscopy of ethylene using a femtosecond time-resolved pump-probe technique.

154309; Femtosecond Raman-induced polarization spectroscopy (RIPS) was conducted at low pressure (250 mb at 295 K and 400 mb at 373 K) in ethylene. The temporal signal, resulting from the beating between pure rotational coherences, was measured with a heterodyne detection. The temporal traces were converted to the frequency domain using a Fourier transformation and then analyzed thanks to the D2hTDS software (http://www.u-bourgogne.fr/LPUB/shTDS.html) dedicated to X2Y4 molecules with D2h symmetry. The effective Hamiltonian was expanded up to order 2, allowing the determination of five parameters with an rms of 0.017 cm(-1). Special care was taken in the precise modeling of intensities, taki…

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 …

Molecular alignment echoes probe collision-induced rotational-speed changes

International audience; We show that the decays with pressure of the rotational alignment echoes induced in N 2 O-He gas mixtures by two ultrashort laser pulses with various delays show detailed information about collision-induced changes of the rotational speed of the molecules. Measurements and classical calculations consistently demonstrate that collisions reduce the echo amplitude all the more efficiently when the echo appears late. We quantitatively explain this behavior by the filamentation of the classical rotational phase space induced by the first pulse and the narrowing of the filaments with time. The above mentioned variation of the echo decay then reflects the ability of collisi…