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International audience; Quantized nano-objects offer a myriad of exciting possibilities for manipulating electrons and light that impact photonics, nanoelectronics, and quantum information. In this context, ultrashort laser pulses combined with nanotips and field emission have permitted renewing nano-characterization and control electron dynamics with unprecedented space and time resolution reaching femtosecond and even attosecond regimes. A crucial missing step in these experiments is that no signature of quantized energy levels has yet been observed. We combine in situ nanostructuration of nanotips and ultrashort laser pulse excitation to induce multiphoton excitation and electron emission from a single quantized nano-object attached at the apex of a metal nanotip. Femtosecond induced tunneling through well-defined localized confinement states that are tunable in energy is demonstrated. This paves the way for the development of ultrafast manipulation of electron emission from isolated nano-objects including stereographically fixed individual molecules and high brightness, ultrafast, coherent single electron sources for quantum optics experiments.

International audience; Unraveling ultrafast processes induced by energetic radiation is compulsory to understand the evolution of molecules under extreme excitation conditions. To describe these photo-induced processes, one needs to perform time-resolved experiments to follow in real time the dynamics induced by the absorption of light. Recent experiments have demonstrated that ultrafast dynamics on few tens of femtoseconds are expected in such situations and a very challenging task is to identify the role played by electronic and nuclear degrees of freedom, charge, energy flows and structural rearrangements. Here, we performed time-resolved XUV-IR experiments on diamondoids carbon cages, in order to decipher the processes following XUV ionization. We show that the dynamics is driven by two timescales, the first one is associated to electronic relaxation and the second one is identified as the redistribution of vibrational energy along the accessible modes, prior to the cage opening that is involved in all fragmentation mechanisms in this family of molecules.

Modern ultrashort X-ray/XUV (extreme ultraviolet) sources provide unique opportunities to investigate the primary reactions of matter upon energetic excitation. Understanding these processes in molecules on ultrafast timescales is required to improve bespoke high-energy radiation detectors, nanomedicine schemes or to study the molecular composition of interstellar media. However, current experiments struggle to provide a general framework because of the uniqueness and complexity of each system. Here we show the universal role of correlation bands—features created by electron correlation. This is done by studying ultrafast energy relaxation of size-scalable two-dimensional molecules following ionization by an ultrashort XUV pulse. We observed long lifetimes that nonlinearly increase with the number of valence electrons. A general law based on solid-like electron–phonon scattering is proposed, which explains both our results and previously reported measurements. This offers new opportunities in attosecond science and high-energy photophysics. The size-dependent lifetimes observed in the ultrafast molecular relaxation dynamics of an entire class of polycyclic aromatic hydrocarbons can be explained by correlation bands and electron–phonon scattering, reminiscent of solid-state systems.

We have investigated photoionization delays in N2 by combining an extreme ultraviolet (XUV) attosecond pulse train generated by high harmonic generation (HHG) and a second harmonic femtosecond pulse with angularly resolved photoelectron spectroscopy. While photoionization delay measurements are usually performed by using a standard XUV-infrared scheme, here we show that the present approach allows us to separate electronic states that otherwise would overlap, thus avoiding the spectral congestion found in most molecules. We have found a relative delay between the X and A ionic molecular states as a function of the photon energy of up to 40 attoseconds, which is due to the presence of a shape resonance in the X channel. This approach can be applied to other small quantum systems with few active electronic states.

International audience; This paper presents a software solution to automatically lock and optimize the carrier envelope phase (CEP) of a femtosecond titanium:sapphire (Ti:Sa) based oscillator following the standard optical arrangement. The solution also mitigates the usual limited-range actuator problem of the slow feedback loop. The principle is to control the relevant stabilization parameters with a single computer to mimic the manual action. After calibration of the piezoelectric actuator, four preliminary measurements are required to locate the CEP-locking point. Then, the algorithm optimizes the CEP performance. Only a few seconds are required to automatically lock and optimize the CEP.

Synopsis We have investigated the photoionization dynamics of several molecular systems using attosecond in-terferometric techniques based on ultrashort extreme ultraviolet (XUV) pulses. For diatomic molecules such as N2, we can get a detailed picture of the photoionization process by measuring the attosecond delays. For polyatomic molecules such as naphthalene, such measurements can provide the average timescale over which photoionization processes at different electron energies can occur in complex quantum systems.

International audience; Understanding processes induced by XUV excitation of Polycyclic Aromatic Hydrocarbons (PAHs) is at the heart of molecular astrophysics, which aims at understanding molecular evolution in interstellar media. We used ultrashort XUV pulses to produce highly excited PAHs cations. The photo-induced dynamics is probed using a pump-probe XUV-IR spectroscopy. By studying PAH from small (naphthalene) to large (hexabenzocoronene) PAHs, we show that the dynamic is governed by the large density of states, in which many-body quantum effects are dominant.

International audience; Rapid energy transfer from electronic to nuclear degrees of freedom underlies many biological processes and astrophysical observations. The efficiency of this energy transfer depends strongly on the complex interplay between electronic and nuclear motions. In this study, we report two-color pump–probe experiments that probe the relaxation dynamics of highly excited cationic states of naphthalene, a prototypical polycyclic aromatic hydrocarbon molecule, which are produced using wavelength-selected, ultrashort extreme ultraviolet pulses. Surprisingly, the relaxation lifetimes increase with the cationic excitation energy. We postulate that the observed effect is the result of a population trapping that leads to delayed relaxation.

International audience; Processes in atoms or molecules on the attosecond timescale have been measured using XUV attosecond and IR femtosecond pulses overlapping in time and controlled with attosecond accuracy. Within this general framework, many strategies have been developed using the harmonics of the fundamental pulse. In this paper, we focus on a specific configuration where the attosecond pulse train is composed by odd harmonics and is dressed by the second harmonic of the fundamental light. Measuring the angularly resolved photoelectron spectrum as a function of the delay between the pulses, a clear oscillation of the anisotropy parameters appears revealing attosecond controlled interferences. This process, is assigned to interferences between two quantum paths involving one XUV photon, on one path, and a XUV+UV photons on the other path. The XUV-UV delay dependent up–down asymmetry can be interpreted following the usual RABBITT formalism, where the dressing photon energy corresponds to the energy separation between the XUV photons of the attosecond pulse train. This approach allows an intuitive analysis of the interference and provides a well suited method for the study of complex valence band systems thanks to the limited congestion of the resulting spectrum.

The standard velocity-map imaging (VMI) analysis relies on the simple approximation that the residual Coulomb field experienced by the photoelectron ejected from a neutral or ion system may be neglected. Under this almost universal approximation, the photoelectrons follow ballistic (parabolic) trajectories in the externally applied electric field, and the recorded image may be considered as a 2D projection of the initial photoelectron velocity distribution. There are, however, several circumstances where this approximation is not justified and the influence of long-range forces must absolutely be taken into account for the interpretation and analysis of the recorded images. The aim of this paper is to illustrate this influence by discussing two different situations involving isolated atoms or molecules where the analysis of experimental images cannot be performed without considering long-range Coulomb interactions. The first situation occurs when slow (meV) photoelectrons are photoionized from a neutral system and strongly interact with the attractive Coulomb potential of the residual ion. The result of this interaction is the formation of a more complex structure in the image, as well as the appearance of an intense glory at the center of the image. The second situation, observed also at low energy, occurs in the photodetachment from a multiply charged anion and it is characterized by the presence of a long-range repulsive potential. Then, while the standard VMI approximation is still valid, the very specific features exhibited by the recorded images can be explained only by taking into consideration tunnel detachment through the repulsive Coulomb barrier.

Femtosecond lasers, used as tools to investigate the ablation dynamics of solids, can help to develop strategies to control the deposition of nanomaterials by pulsed laser ablation. In this work, Co/ZnS targets, potential candidates for the synthesis of diluted magnetic semiconductor materials, are irradiated by sequences of two femtosecond laser pulses delayed in the picosecond time scale. The ionic composition of the ablation plasma and the dependence of the ion signals on the interpulse delay and relative fluence are determined by time-of-flight mass spectrometry. The results show that, when pulses of different fluence are used, highly asymmetric ion yields are obtained, with more intense ion signals detected when the lower fluence pulse is temporally ahead. The comparison between asymmetric and equal fluence double pulse ablation dynamics provides some understanding of the different processes that modify the properties of the layer irradiated by the first pulse and of the mechanisms affecting the coupling of the delayed pulse into the material. The final outcome of the double pulse irradiation is characterized through the analysis of the deposits produced upon ablation.

International audience; We present a simple upgrade of a time-resolved attosecond extreme ultraviolet and infrared (XUV-IR) setup designed to perform time-resolved or spectrally resolved studies of a target under similar experimental conditions. A flat XUV grating inserted in the path of an attosecond pulse train obtained via high order harmonic generation in gases is used either in the zeroth order of diffraction to follow attosecond dynamics or in the first order of diffraction to study the target spectral response with a temporally stretched single harmonic. Electron momentum measurement is performed with a velocity map imaging spectrometer, and the 10 W femtosecond laser system operating at 5 kHz provides an XUV photon flux compatible with rapid acquisition in both the monochromatic and broadband configurations. The change of experimental configuration between broadband and monochro-matic sources is rapid and performed in situ. We present the experimental implementation applied to krypton atoms and detail the capabilities and limits of this approach when an XUV grating with constant groove density is used with a converging XUV beam.

International audience; This combined experimental and theoretical study demonstrates that the surface plasmon resonance in C60 alters the valence photoemission quantum phase, resulting in strong effects in the photoelectron angular distribution and emission time delay. Electron momentum imaging spectroscopy is used to measure the photoelectron angular distribution asymmetry parameter that agrees well with our calculations from the time-dependent local density approximation (TDLDA). Significant structure in the valence photoemission time delay is simultaneously calculated by TDLDA over the plasmon active energies. Results reveal a unified spatial and temporal asymmetry pattern driven by the plasmon resonance and offer a sensitive probe of electron correlation. A semiclassical approach facilitates further insights into this link that can be generalized and applied to other molecular systems and nanometer-sized metallic materials exhibiting plasmon resonances.

International audience; XUV induced dynamics in molecules is still largely unexplored while experimental and theoretical tools are becoming available in several labs. In this work, we present a compact XUV beamline designed to induce and probe femtosecond and attosecond dynamics in gas samples (from atoms to complex molecular species). The induced processes are studied with time-resolved photoelectron or/and photoion imaging. The characterization of the performances of the experimental setup is presented. We show experimental results obtained in naphthalene molecule showing femtosecond and attosecond time-resolved photoelectron imaging experiments allowing electron wavepacket phase measurements.

International audience; We perform time-dependent local density functional calculations of the time delay in C60 HOMO and HOMO-1 photoionization at giant plasmon energies. A semiclassical model is used to develop further insights.

International audience; Hole migration is a fascinating process driven by electron correlation, in which purely electronic dynamics occur on a very short time scale in complex ionized molecules, prior to the onset of nuclear motion. However, it is expected that due to coupling to the nuclear dynamics, these oscillations will be rapidly damped and smeared out, which makes experimental observation of the hole migration process rather difficult. In this Letter, we demonstrate that the instantaneous ionization of benzene molecules initiates an ultrafast hole migration characterized by a periodic breathing of the hole density between the carbon ring and surrounding hydrogen atoms on a subfemtosecond time scale. We show that these oscillations survive the dephasing introduced by the nuclear motion for a long enough time to allow their observation. We argue that this offers an ideal benchmark for studying the influence of hole migration on molecular reactivity.

A new strategy of pulse shaping based on the quasi-direct space-to-time (QDST) conversion principle has been recently proposed theoretically [Mnguez-Vega , Opt. Express 16, 16993 (2008)]. In this letter, the working principle of this pulse shaper has been experimentally verified by using a simple second order cross-correlation setup with spatial resolution. The QDST conversion principle is evidenced through the experimental measurement of the parabolic dependence of the time delay on the focal plane versus the radii of the components of the spatial profile in the far field.

International audience; We investigate a variant of the d-scan technique, an intuitive pulse characterization method for retrieving the spectral phase of ultrashort laser pulses. In this variant a ramp of quadratic spectral phases is applied to the input pulses and the second harmonic spectra of the resulting pulses are measured for each chirp value. We demonstrate that a given field envelope produces a unique and unequivocal chirp-scan map and that, under some asymptotic assumptions, both the spectral amplitude and phase of the measured pulse can be retrieved analytically from only two measurements. An iterative algorithm can exploit the redundancy of the information contained in the chirp-scan map to discard experimental noise, artifacts, calibration errors and improve the reconstruction of both the spectral intensity and phase. This technique is compared to two reference characterization techniques (FROG and SRSI). Finally, we perform d-scan measurements with a simple grating-pair compressor.

International audience; Spatial shaping of ultrashort laser beams at the focal plane is theoretically analyzed. The description of the pulse is performed by its expansion in terms of Laguerre-Gaussian orthonormal modes. This procedure gives both a comprehensive interpretation of the propagation dynamics and the required signal to encode onto a spatial light modulator for spatial shaping, without using iterative algorithms. As an example, pulses with top-hat and annular spatial profiles are designed and their dynamics analyzed. The interference of top-hat pulses is also investigated finding potential applications in high precision pump-probe experiments (without using delay lines) and for the creation of subwavelength ablation patterns. In addition, a novel class of ultrashort pulses possessing non-stationary orbital angular momentum is also proposed. These exotic pulses provide additional degrees of freedom that open up new perspectives in fields such as laser-matter interaction and micro-machining.

10 pags, 11 figs, 2 pags, As a contribution to the ongoing controversy about the role of higher-order Kerr effect (HOKE) in laser filamentation, we first provide thorough details about the protocol that has been employed to infer the HOKE indices from the experiment. Next, we discuss potential sources of artifact in the experimental measurements of these terms and show that neither the value of the observed birefringence, nor its inversion, nor the intensity at which it is observed, appear to be flawed. Furthermore, we argue that, independently on our values, the principle of including HOKE is straightforward. Due to the different temporal and spectral dynamics, the respective efficiency of defocusing by the plasma and by the HOKE is expected to depend substantially on both incident wavelength and pulse duration. The discussion should therefore focus on defining the conditions where each filamentation regime dominates. © 2011 Pleiades Publishing, Ltd., This work was supported by the Conseil Régional de Bourgogne, the ANR COMOC, the FASTQUAST ITN Program of the 7th FP and the Swiss NSF (contracts 200021-125315 and 200021-125315-2).

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, Based on numerical simulations, we show that higher-order nonlinear indices (up to n8 and n10, respectively) of air and argon have a dominant contribution to both focusing and defocusing in the self-guiding of ultrashort laser pulses over most of the spectrum. Plasma generation and filamentation are therefore decoupled. As a consequence, ultraviolet wavelength may not be the optimal wavelength for applications requiring to maximize ionization. © 2010 The American Physical Society., This work was supported by the Conseil Régional de Bourgogne, the ANR COMOC, the FASTQUAST ITN Program of the 7th FP, and the Swiss NSF (Contracts No. 200021-116198 and No. 200021-125315).

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.

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.

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 .

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., 11 pages, 6 figures (11 panels)

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 compared with the awaited results. The technique is simple and can be easily implemented in a large class of molecular samples. Improvement to extend the performance of the method is discussed. The reported study is a decisive step toward feedback optimization and optimal control of field-free molecular alignment.

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 ratio between (i) N2 and Ar and (ii) O2 and Xe. We demonstrate in addition a progress in the scheme in order to improve the accuracy at low intensity.

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 method is assessed in N2.

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.