0000000001078139
AUTHOR
Edouard Hertz
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…
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 …
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.
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.
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 .
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…
Fiber laser mode locked through an evolutionary algorithm
Mode locking of fiber lasers generally involves adjusting several control parameters, in connection with a wide range of accessible short-pulse dynamics. In this Letter, we experimentally demonstrate the ability of an evolutionary algorithm to prescribe a set of cavity parameters entailing specific self-starting mode locking. The prescribed parameters are applied to electrically driven polarization controllers, thus shaping the effective nonlinear transfer function at play within the fiber cavity. According to the specifications of the objective function used for the optimization procedure, various short-pulse regimes are obtained. Our versatile method represents an effective novel avenue f…
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…
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.
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.
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…
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.
Field-free permanent molecular planar alignment
We show the existence of a permanent molecular planar alignment in field-free conditions. We present different control strategies using shaped laser pulses to reach this state. The strategies are robust with respect to the temperature and can be implemented with the state of the art technology. They can be applied not only to linear molecules but also to symmetric or asymmetric top molecules along the most polarizable molecular axis. We propose potential applications of this planar alignment such as the increase of the adsorption on a surface.
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…
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.
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 …
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/…
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.
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…
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.
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…
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…
Ultimate field-free molecular alignment by combined adiabatic-impulsive field design
We show that a laser pulse designed as an adiabatic ramp followed by a kick allows one to reach a perfect postpulse molecular alignment, free of saturation. The mechanism is based on an optimized distribution of the energy between a weakly efficient but non saturating adiabatic ramp and an efficient but saturating impulsive field. Unprecedent degrees of alignment are predicted using state-of-the-art pulse shaping techniques and non-destructive field intensities. The scheme can be extended to reach high degrees of orientation of polar molecules using designed half-cycle pulses.
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…
CHARACTERISATION OF A RADIATION PULSE BY TIME-RESOLVED OPTICAL WINDOWING
The invention relates to a system (10) for characterising a pulse (I) of electromagnetic radiation by time-resolved optical windowing, which comprises an device (1) for forming an interference which is suitable for superimposing four parts of the pulse. The system also comprises a matrix image sensor (3) which selectively captures an interference pattern formed by the pulse from two-photon absorptions. Said system allows the pulse shape to be obtained completely and accurately, and is particularly suitable for characterising ultrashort pulses. In various embodiments, the two-photon absorption can be produced in the matrix image sensor, or replaced by optical frequency doubling which is prod…
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 …
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 …
Selective excitation of bright and dark plasmonic resonances of single gold nanorods.
Plasmonic dark modes are pure near-field resonances since their dipole moments are vanishing in far field. These modes are particularly interesting to enhance nonlinear light-matter interaction at the nanometer scale because radiative losses are mitigated therefore increasing the intrinsic lifetime of the resonances. However, the excitation of dark modes by standard far field approaches is generally inefficient because the symmetry of the electromagnetic near-field distribution has a poor overlap with the excitation field. Here, we demonstrate the selective optical excitation of bright and dark plasmonic modes of single gold nanorods by spatial phase-shaping the excitation beam. Using two-p…
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…