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1. Coherent energy exchange between carriers and phonons in Peierls-distorted bismuth unveiled by broadband XUV pulses

Author: Romain Géneaux, Iurii Timrov, Christopher J. Kaplan, Andrew D. Ross, Peter M. Kraus, and Stephen R. Leone
Subjects: Physics, QC1-999
Abstract: In Peierls-distorted materials, photoexcitation leads to a strongly coupled transient response between structural and electronic degrees of freedom, always measured independently of each other. Here we use transient reflectivity in the extreme ultraviolet to quantify both responses in photoexcited bismuth in a single measurement. With the help of first-principles calculations based on density-functional theory (DFT) and time-dependent DFT, the real-space atomic motion and the temperature of both electrons and holes as a function of time are captured simultaneously, retrieving an anticorrelation between the A_{1g} phonon dynamics and carrier temperature. The results reveal a coherent, bidirectional energy exchange between carriers and phonons, which is a dynamical counterpart of the static Peierls-Jones distortion, providing validation of previous theoretical predictions.
Published: 2021
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2. Coherent energy exchange between carriers and phonons in Peierls-distorted bismuth unveiled by broadband XUV pulses

Author: Peter Kraus, Stephen R. Leone, Iurii Timrov, Christopher J. Kaplan, Romain Géneaux, Andrew D. Ross, Biomolécules Excitées (DICO), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), University of California [Berkeley], University of California, Theory and Simulation of Materials (THEOS) and National Centre for Computational Design and Discovery of Novel Materials, Lawrence Berkeley National Laboratory [Berkeley] (LBNL), ANR-10-LABX-0039,PALM,Physics: Atoms, Light, Matter(2010), Dynamique et Interactions en phase Condensée (DICO), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), University of California [Berkeley] (UC Berkeley), and University of California (UC)
Subjects: electron, Phonon, spectra, Degrees of freedom (physics and chemistry), chemistry.chemical_element, FOS: Physical sciences, 02 engineering and technology, Electron, 01 natural sciences, Bismuth, [PHYS.MECA.MEMA]Physics [physics]/Mechanics [physics]/Mechanics of materials [physics.class-ph], Condensed Matter::Materials Science, Distortion, 0103 physical sciences, surface, Transient response, 010306 general physics, density-functional theory, Physics, Condensed Matter - Materials Science, crystal-structure, Materials Science (cond-mat.mtrl-sci), dynamics, 021001 nanoscience & nanotechnology, excitations, Photoexcitation, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, chemistry, Extreme ultraviolet, phase-stability, Condensed Matter::Strongly Correlated Electrons, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Atomic physics, 0210 nano-technology, te
Abstract: International audience; In Peierls-distorted materials, photoexcitation leads to a strongly coupled transient response between structural and electronic degrees of freedom, always measured independently of each other. Here we use transient reflectivity in the extreme ultraviolet to quantify both responses in photoexcited bismuth in a single measurement. With the help of first-principles calculations based on density-functional theory (DFT) and time-dependent DFT, the real-space atomic motion and the temperature of both electrons and holes as a function of time are captured simultaneously, retrieving an anticorrelation between the A$_{1g}$ phonon dynamics and carrier temperature. The results reveal a coherent, bidirectional energy exchange between carriers and phonons, which is a dynamical counterpart of the static Peierls-Jones distortion, providing validation of previous theoretical predictions.
Published: 2021
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3. Coupled valence carrier and core-exciton dynamics in WS2 probed by few-femtosecond extreme ultraviolet transient absorption spectroscopy

Author: Yi-De Chuang, Christopher T. Chen, Alexander Guggenmos, Daniel M. Neumark, Juwon Oh, Stephen R. Leone, Romain Géneaux, Shaul Aloni, Hung-Tzu Chang, and Adam M. Schwartzberg
Subjects: Physics, Valence (chemistry), business.industry, Exciton, 02 engineering and technology, 021001 nanoscience & nanotechnology, 01 natural sciences, Spectral line, Condensed Matter::Materials Science, Semiconductor, Extreme ultraviolet, 0103 physical sciences, Ultrafast laser spectroscopy, Atomic physics, 010306 general physics, 0210 nano-technology, Spectroscopy, Absorption (electromagnetic radiation), business
Abstract: Author(s): Chang, Hung-Tzu; Guggenmos, Alexander; Chen, Christopher T; Oh, Juwon; Geneaux, Romain; Chuang, Yi-De; Schwartzberg, Adam M; Aloni, Shaul; Neumark, Daniel M; Leone, Stephen R | Abstract: Few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy, performed with optical 500-1000 nm supercontinuum and broadband XUV pulses (30-50 eV), simultaneously probes dynamics of photoexcited carriers in WS$_{2}$ at the W O$_3$ edge (37-45 eV) and carrier-induced modifications of core-exciton absorption at the W N$_{6,7}$ edge (32-37 eV). Access to continuous core-to-conduction band absorption features and discrete core-exciton transitions in the same XUV spectral region in a semiconductor provides a novel means to investigate the effect of carrier excitation on core-exciton dynamics. The core-level transient absorption spectra, measured with either pulse arriving first to explore both core-level and valence carrier dynamics, reveal that core-exciton transitions are strongly influenced by the photoexcited carriers. A $1.2\pm0.3$ ps hole-phonon relaxation time and a $3.1\pm0.4$ ps carrier recombination time are extracted from the XUV transient absorption spectra from the core-to-conduction band transitions at the W O$_{3}$ edge. Global fitting of the transient absorption signal at the W N$_{6,7}$ edge yields $\sim 10$ fs coherence lifetimes of core-exciton states and reveals that the photoexcited carriers, which alter the electronic screening and band filling, are the dominant contributor to the spectral modifications of core-excitons and direct field-induced changes play a minor role. This work provides a first look at the modulations of core-exciton states by photoexcited carriers and advances our understanding of carrier dynamics in metal dichalcogenides.
Published: 2021
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4. Two-dimensional phase cartography for high-harmonic spectroscopy

Author: Antoine Camper, Emmanouil Skantzakis, Romain Géneaux, François Risoud, Elizabeth English, Zsolt Diveki, Nan Lin, Vincent Gruson, Thierry Auguste, Bertrand Carré, Robert R. Lucchese, Alfred Maquet, Richard Taïeb, Jérémie Caillat, Thierry Ruchon, Pascal Salières
Published: 2021
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5. Attosecond-resolved photoionization of chiral molecules

Author: Gil Porat, Dominique Descamps, Yann Mairesse, Nirit Dudovich, J. Caillat, Samuel Beaulieu, Thierry Ruchon, Antoine Comby, Romain Géneaux, Stéphane Petit, Valérie Blanchet, Baptiste Fabre, Alex Clergerie, François Légaré, R. Taїeb, Bernard Pons, Centre d'Etudes Lasers Intenses et Applications (CELIA), Université de Bordeaux (UB)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Weizmann Institute of Science [Rehovot, Israël], Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Institut National de la Recherche Scientifique [Québec] (INRS), Department of Physics of Complex System, Attophysique (ATTO), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Bordeaux (UB), ANR-14-CE32-0014,MISFITS,Imagerie Moléculaire par effet tunnel et recollision en champ fort(2014), ANR-14-CE32-0010,Xstase,Étude du moment angulaire de faisceaux lumineux XUV: synthèse et transferts(2014), ANR-10-IDEX-0003,IDEX BORDEAUX,Initiative d'excellence de l'Université de Bordeaux(2010), ANR-11-IDEX-0004,SUPER,Sorbonne Universités à Paris pour l'Enseignement et la Recherche(2011), ANR-15-CE30-0001,CIMBAAD,Contrôle de l'ionisation moléculaire aux échelles attoseconde et Angström(2015), European Project: 682978,EXCITERS, and European Project: 284464,EC:FP7:INFRA,FP7-INFRASTRUCTURES-2011-1,LASERLAB-EUROPE(2012)
Subjects: Physics::Instrumentation and Detectors, Atomic Physics (physics.atom-ph), Wave packet, media_common.quotation_subject, Attosecond, FOS: Physical sciences, 02 engineering and technology, Electron, Photoionization, Asymmetry, 01 natural sciences, Measure (mathematics), Physics - Atomic Physics, law.invention, law, Physics - Chemical Physics, Electric field, 0103 physical sciences, Physics::Atomic and Molecular Clusters, Physics - Atomic and Molecular Clusters, Physics::Atomic Physics, 010306 general physics, Circular polarization, media_common, Chemical Physics (physics.chem-ph), [PHYS]Physics [physics], Physics, Multidisciplinary, Resonance, Photoelectric effect, 021001 nanoscience & nanotechnology, Laser, Interferometry, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Atomic physics, Enantiomer, Atomic and Molecular Clusters (physics.atm-clus), 0210 nano-technology
Abstract: Clocking departures from chiral origins Just as the atoms in a molecule can be arranged in a left- or right-handed manner, the field in a beam of light can circulate like a left- or right-handed corkscrew. Matches or mismatches in this mutual handedness give rise to an asymmetric distribution of trajectories as electrons are ejected during photoionization. Beaulieu et al. used an interferometric approach to uncover the temporal dynamics associated with this asymmetry. They probed the mirror-image isomers of camphor with circularly polarized light, which revealed the angle-dependent delays between trajectories that spanned up to 24 attoseconds. Science , this issue p. 1288
Published: 2017
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6. Source noise suppression in attosecond transient absorption spectroscopy by edge-pixel referencing

Author: Romain Géneaux, Adam M. Schwartzberg, Hung-Tzu Chang, Hugo J. B. Marroux, Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)
Subjects: Physics - Instrumentation and Detectors, Attosecond, Free electron lasers, FOS: Physical sciences, Optical Physics, 02 engineering and technology, Power spectra, 01 natural sciences, physics.data-an, 010309 optics, Absorption spectroscopy, Optics, Power spectral density, 0103 physical sciences, Singular value decomposition, [PHYS.PHYS.PHYS-INS-DET]Physics [physics]/Physics [physics]/Instrumentation and Detectors [physics.ins-det], Sensitivity (control systems), Electrical and Electronic Engineering, physics.ins-det, Laser sources, Physics, Communications Technologies, Pixel, business.industry, ray, Atomic layer deposition, Detector, Spectral density, dynamics, Instrumentation and Detectors (physics.ins-det), 021001 nanoscience & nanotechnology, Noise floor, [PHYS.PHYS.PHYS-GEN-PH]Physics [physics]/Physics [physics]/General Physics [physics.gen-ph], Atomic and Molecular Physics, and Optics, Noise, Physics - Data Analysis, Statistics and Probability, physics.optics, 0210 nano-technology, business, [PHYS.PHYS.PHYS-DATA-AN]Physics [physics]/Physics [physics]/Data Analysis, Statistics and Probability [physics.data-an], Data Analysis, Statistics and Probability (physics.data-an), Physics - Optics, Optics (physics.optics)
Abstract: Attosecond transient absorption spectroscopy (ATAS) is used to observe photoexcited dynamics with outstanding time resolution. The main experimental challenge of this technique is that high-harmonic generation sources show significant instabilities, resulting in sub-par sensitivity when compared to other techniques. This paper proposes edge-pixel referencing as a means to suppress this noise. 'lino approaches are introduced: the first is deterministic and uses a correlation analysis, while the second relies on singular value decomposition. Each method is demonstrated and quantified on a noisy measurement taken on WS2 and results in a fivefold increase in sensitivity. The combination of the two methods ensures the fidelity of the procedure and can be implemented on live data collection but also on existing datasets. The results show that edge-referencing methods bring the sensitivity of ATAS near the detector noise floor. An implementation of the post-processing code is provided to the reader. (C) 2021 Optical Society of America under the terms of the OSA Open Access Publishing Agreement
Published: 2020
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7. Attosecond time-domain measurement of core-excitonic decay in magnesium oxide

Author: Peter M. Kraus, Lun Yue, Mette B. Gaarde, Mi-Ying Huang, Michael Zürch, Daniel M. Neumark, Christopher J. Kaplan, Jens Egebjerg Bækhøj, Kenneth J. Schafer, Romain Géneaux, Alexander Guggenmos, Stephen R. Leone, Hung-Tzu Chang, and Andrew D. Ross
Subjects: Physics, Condensed Matter - Materials Science, Infrared, Exciton, Attosecond, General Physics and Astronomy, Materials Science (cond-mat.mtrl-sci), FOS: Physical sciences, Condensed Matter::Mesoscopic Systems and Quantum Hall Effect, 01 natural sciences, Condensed Matter::Materials Science, Extreme ultraviolet, 0103 physical sciences, Quasiparticle, Atomic physics, 010306 general physics, Spectroscopy, Ultrashort pulse, Excitation
Abstract: Excitation of ionic solids with extreme ultraviolet pulses creates localized core-excitons, which in some cases couple strongly to the lattice. Here, core-excitonic states of magnesium oxide are studied in the time domain at the Mg $\text{L}_{2,3}$ edge with attosecond transient reflectivity spectroscopy. Attosecond pulses trigger the excitation of these short-lived quasiparticles, whose decay is perturbed by time-delayed near infrared optical pulses. Combined with a few-state theoretical model, this reveals that the optical pulse shifts the energy of bright core-exciton states as well as induces features arising from dark core-excitons. We report coherence lifetimes for the first two core-excitons of $2.3 \pm 0.2$ and $1.6 \pm 0.5$ femtoseconds and show that these short lifetimes are primarily a consequence of strong exciton-phonon coupling, disclosing the drastic influence of structural effects in this ultrafast relaxation process.
Published: 2019

8. Transfer of Orbital Angular Momentum in High Harmonic Generation using two Driving Beams

Author: Thierry Ruchon, Giovanni De Ninno, O. Gobert, David Bresteau, C Chappuis, Thierry Auguste, David Gauthier, and Romain Géneaux
Subjects: Quantum optics, Wavefront, Physics, 0303 health sciences, Angular momentum, Photon, business.industry, Attosecond, Physics::Optics, Polarization (waves), 01 natural sciences, 03 medical and health sciences, Optics, 0103 physical sciences, High harmonic generation, Light beam, 010306 general physics, business, 030304 developmental biology
Abstract: Light beams may carry both a spin and an orbital angular momentum (OAM). While the former is associated to their polarization state, the latter stems from the geometrical properties of their wavefront. In their prototypical form, beams with OAM have "donuts-like" intensity profile and helicoidal wavefront, carrying integral multiples of h as angular momenta. Since their "rediscovery" in the late 90's, beams with OAM of visible wavelengths have found innumerable applications in quantum optics, microscopy or information transfer. A major recent development was the generation of such beams with much smaller wavelengths — in the extreme ultraviolet (XUV) — using synchrotron sources, free electron lasers as well as high harmonic sources (HHG). In this latter case, it creates ultrashort XUV sources of beams with OAM, suited for time-resolved applications at femtosecond and attosecond time scales. Remarkably, we showed that even though HHG is a non-perturbative process, the OAM transfer from the driving beam to the harmonics was purely parametric; i.e., the q-th harmonic — which can be thought as the upconversion of q infrared photons — carries q times the OAM of the driver [3, 4]. However, this rule limits severely the flexibility in choosing the OAM of the XUV emission.
Published: 2019
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9. Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids

Author: Hugo J. B. Marroux, Daniel M. Neumark, Alexander Guggenmos, Romain Géneaux, and Stephen R. Leone
Subjects: Physics, General Mathematics, Attosecond, General Engineering, Complex system, General Physics and Astronomy, 02 engineering and technology, Articles, 021001 nanoscience & nanotechnology, 01 natural sciences, Computational physics, Picosecond, 0103 physical sciences, Ultrafast laser spectroscopy, High harmonic generation, 010306 general physics, 0210 nano-technology, Spectroscopy, Ultrashort pulse, Excitation
Abstract: Attosecond science opened the door to observing nuclear and electronic dynamics in real time and has begun to expand beyond its traditional grounds. Among several spectroscopic techniques, X-ray transient absorption spectroscopy has become key in understanding matter on ultrafast time scales. In this review, we illustrate the capabilities of this unique tool through a number of iconic experiments. We outline how coherent broadband X-ray radiation, emitted in high-harmonic generation, can be used to follow dynamics in increasingly complex systems. Experiments performed in both molecules and solids are discussed at length, on time scales ranging from attoseconds to picoseconds, and in perturbative or strong-field excitation regimes. This article is part of the theme issue ‘Measurement of ultrafast electronic and structural dynamics with X-rays’.
Published: 2019

10. Beam optimization in a 25 TW femtosecond laser system for high harmonic generation

Author: Tianyi Guo, Stephen R. Leone, Jonathon White, Paul B. Corkum, Matthew Weidman, Yi Wu, Christopher J. Kaplan, Kai Hu, Graham G. Brown, Romain Géneaux, Marieke F. Jager, Daniel M. Neumark, Jialin Li, Zenghu Chang, and Yang Wang
Subjects: Physics, business.industry, Physics::Optics, Condensed Matter Physics, Laser, 7. Clean energy, 01 natural sciences, high harmonic generation, Atomic and Molecular Physics, and Optics, law.invention, 010309 optics, Optics, law, XUV, Extreme ultraviolet, 0103 physical sciences, Femtosecond, Physics::Atomic and Molecular Clusters, High harmonic generation, Physics::Atomic Physics, 010306 general physics, business, wavefront correction, Beam (structure)
Abstract: It has been demonstrated in the past that high fluxes of extreme ultraviolet (XUV) light could be obtained by driving high harmonic generation (HHG) with high energy lasers. However, the peak intensity at the focal point of a femtosecond laser with more than 100 mJ can be too high for phase-matched HHG in gases. We propose a method to optimize the spatial profile at off-focus locations of the high energy driving laser to avoid fully ionizing the target atoms. The beam profile before or after the focal point depends on the wavefront quality of the laser beam and the near field intensity distribution. The beam spot diameter reaches three times that at the focus by adding customized wavefront terms. An XUV pulse energy of 5.6 μJ was obtained from HHG when a larger off-focus spot of a 500 mJ Ti: sapphire laser beam was applied in an argon gas cell.
Published: 2020
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11. Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom

Author: Claire Vallance, Jérôme Palaudoux, Stefan Düsterer, Marc Simon, Evgeny Savelyev, Tatiana Marchenko, Hansjochen Köckert, Kasra Amini, Jongmin Lee, Benjamin Erk, R. Guillemin, Marie Géléoc, Cédric Bomme, Per Johnsson, Sebastian Trippel, Nora Schirmel, David M. P. Holland, Francis Penent, Barbara Cunha de Miranda, Jonathan G. Underwood, Rebecca Boll, Pavel K. Olshin, Sadia Bari, Thomas Kierspel, Maria Novella Piancastelli, Jochen Küpper, Jan Lahl, Michael Burt, I. Ismail, Simone Techert, Serguei Patchkovskii, Sylvain Maclot, Alexander S. Gentleman, Gildas Goldsztejn, Artem Rudenko, Felix Brauße, Terence Mullins, Daniel Rolles, Mark Brouard, Oksana Travnikova, Thierry Ruchon, Andrey S. Mereshchenko, Bastian Manschwetus, Dimitrios Rompotis, Joss Wiese, Arnaud Rouzée, Pascal Lablanquie, Romain Géneaux, Stuart R. Mackenzie, Loïc Journel, Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie (MBI), University of Oxford, Deutsches Elektronen-Synchrotron [Hamburg] (DESY), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Structures BioMoléculaires (SBM), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Attophysique (ATTO), Lund University [Lund], Center for Free-Electron Laser Science (CFEL), Universität Hamburg (UHH), Saint Petersburg State Polytechnical University (SPSPU), Department of Physics and Astronomy [Uppsala], Uppsala University, Kansas State University, Max-Planck-Institut für Biophysikalische Chemie - Max Planck Institute for Biophysical Chemistry [Göttingen], Max-Planck-Gesellschaft, Department of Physics and Astronomy [UCL London], University College of London [London] (UCL), ANR-14-CE32-0010,Xstase,Étude du moment angulaire de faisceaux lumineux XUV: synthèse et transferts(2014), ANR-16-CE30-0001,ATTOMEMUCHO,Dynamique électronique attoseconde dans les molécules organiques isolées par la spectroscopie 'core-hole clock'(2016), European Project: 238671,EC:FP7:PEOPLE,FP7-PEOPLE-ITN-2008,ICONIC(2009), European Project: 641789,H2020,H2020-MSCA-ITN-2014,MEDEA(2015), University of Oxford [Oxford], Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), and Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Chemical Physics (physics.chem-ph), Physics, 010304 chemical physics, Atom and Molecular Physics and Optics, Chemical structure, Photodissociation, technology, industry, and agriculture, FOS: Physical sciences, Configuration interaction, 01 natural sciences, Molecular physics, Dissociation (chemistry), 3. Good health, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, X-ray photoelectron spectroscopy, Ionization, Physics - Chemical Physics, 0103 physical sciences, Physics::Atomic and Molecular Clusters, Molecule, ddc:530, Atom- och molekylfysik och optik, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], 010306 general physics, Spectroscopy
Abstract: International audience; Due to its element and site specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here, we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH3I) is investigated by ionization above the iodine 4d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal-field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.
Published: 2018
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12. Probing ultrafast dynamics of chiral molecules using time-resolved photoelectron circular dichroism

Author: Laurent Nahon, Samuel Beaulieu, Antoine Comby, Yann Mairesse, Valérie Blanchet, Stéphane Petit, Dominique Descamps, Thierry Ruchon, François Légaré, Bernard Pons, A. Ferré, Gustavo A. Garcia, Romain Géneaux, Baptiste Fabre, Centre d'Etudes Lasers Intenses et Applications (CELIA), Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Bordeaux (UB), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Institut National de la Recherche Scientifique [Québec] (INRS), Attophysique (ATTO), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), and Université de Bordeaux (UB)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Circular dichroism, education.field_of_study, Chemistry, [PHYS.PHYS.PHYS-ATM-PH]Physics [physics]/Physics [physics]/Atomic and Molecular Clusters [physics.atm-clus], Relaxation (NMR), Population, 02 engineering and technology, 021001 nanoscience & nanotechnology, 01 natural sciences, symbols.namesake, Tunnel ionization, Extreme ultraviolet, Ionization, 0103 physical sciences, Physics::Atomic and Molecular Clusters, Rydberg formula, symbols, Physics::Atomic Physics, Physical and Theoretical Chemistry, Atomic physics, 010306 general physics, 0210 nano-technology, education, Ultrashort pulse
Abstract: International audience; Measuring the ultrafast dynamics of chiralmolecules in the gas phase has been a long standing and challenging quest of molecular physics. The main limitation to reach that goal has been the lack of highly sensitive chiroptical measurement. By enabling chiral discrimination with up to several 10% of sensitivity, photoelectron circular dichroism (PECD) offers a solution to this issue. However, tracking ultrafast processes requires measuring PECD with ultrashort light pulses. Here we compare the PECD obtained with different light sources, from the extreme ultraviolet to the mid-infrared range, leading to different ionization regimes: single-photon, resonance-enhanced multiphoton, above-threshold and tunnel ionization. We use single and multiphoton ionization to probe the ultrafast relaxation of fenchone molecules photoexcited in their first Rydberg states. We show that time-resolved PECD enables revealing dynamics much faster than the population decay of the Rydberg states, demonstrating the high sensitivity of this technique to vibronic relaxation.
Published: 2016
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13. Photoexcitation Circular Dichroism in Chiral Molecules

Author: Romain Géneaux, Yann Mairesse, Alex G. Harvey, Valérie Blanchet, Olga Smirnova, Gustavo A. Garcia, Stéphane Petit, Baptiste Fabre, Antoine Comby, Samuel Beaulieu, Dominique Descamps, Laurent Nahon, François Légaré, Zdeněk Mašín, Andres F. Ordonez, Bernard Pons, Centre d'Etudes Lasers Intenses et Applications (CELIA), Université de Bordeaux (UB)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Institut National de la Recherche Scientifique [Québec] (INRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Attophysique (ATTO), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Max-Born-institut, Berlin, Technical University of Berlin / Technische Universität Berlin (TU), ANR-14-CE32-0014,MISFITS,Imagerie Moléculaire par effet tunnel et recollision en champ fort(2014), ANR-14-CE32-0010,Xstase,Étude du moment angulaire de faisceaux lumineux XUV: synthèse et transferts(2014), European Project: 682978,EXCITERS, European Project: 641789,H2020,H2020-MSCA-ITN-2014,MEDEA(2015), Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Bordeaux (UB), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), and Technische Universität Berlin (TU)
Subjects: Chemical Physics (physics.chem-ph), Physics, Circular dichroism, High Energy Physics::Lattice, High Energy Physics::Phenomenology, FOS: Physical sciences, General Physics and Astronomy, Metamaterial, 02 engineering and technology, 021001 nanoscience & nanotechnology, Linear dichroism, 01 natural sciences, Photoexcitation, Excited state, Physics - Chemical Physics, 0103 physical sciences, Physics - Atomic and Molecular Clusters, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Atomic physics, Optical rotation, Atomic and Molecular Clusters (physics.atm-clus), 010306 general physics, 0210 nano-technology, Excitation, Circular polarization
Abstract: International audience; Chiral effects appear in a wide variety of natural phenomena and are of fundamental importance in science, from particle physics to metamaterials. The standard technique of chiral discrimination—photoabsorption circular dichroism—relies on the magnetic properties of a chiral medium and yields an extremely weak chiral response. Here, we propose and demonstrate an orders of magnitude more sensitive type of circular dichroism in neutral molecules: photoexcitation circular dichroism. This technique does not rely on weak magnetic effects, but takes advantage of the coherent helical motion of bound electrons excited by ultrashort circularly polarized light. It results in an ultrafast chiral response and the efficient excitation of a macroscopic chiral density in an initially isotropic ensemble of randomly oriented chiral molecules. We probe this excitation using linearly polarized laser pulses, without the aid of further chiral interactions. Our time-resolved study of vibronic chiral dynamics opens a way to the efficient initiation, control and monitoring of chiral chemical change in neutral molecules at the level of electrons.
Published: 2018
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14. Electron dynamics in transition metal dichalcogenides utilizing attosecond transient absorption spectroscopy

Author: Xuan Wei, Steven G. Louie, Yufeng Liang, Stephen R. Leone, Felipe H. da Jornada, Alexander Guggenmos, Chang-Ming Jiang, Romain Géneaux, Diana Y. Qiu, Hung-Tzu Chang, Adam M. Schwartzberg, Yen-Chang Chen, Vincent Tung, David Prendergast, Michael Zürch, and Daniel M. Neumark
Subjects: Condensed Matter::Quantum Gases, Materials science, Absorption spectroscopy, Condensed Matter::Other, Exciton, Attosecond, 02 engineering and technology, Electron, Condensed Matter::Mesoscopic Systems and Quantum Hall Effect, 021001 nanoscience & nanotechnology, 01 natural sciences, Molecular physics, Condensed Matter::Materials Science, Transition metal, 0103 physical sciences, Ultrafast laser spectroscopy, Physics::Atomic and Molecular Clusters, 010306 general physics, 0210 nano-technology, Spectroscopy, Absorption (electromagnetic radiation)
Abstract: © OSA 2018. Strong enhancement of exciton binding has been observed in valence-excitons in the optical regime of 2D materials. We report direct observation of long-lived core-exciton states in transition metal dichalcogenides by attosecond transient absorption spectroscopy in the XUV.
Published: 2018
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15. Coulomb explosion imaging of CH3I and CH2CII photodissociation dynamics

Author: Barbara Cunha de Miranda, Per Johnsson, Romain Géneaux, Stuart R. Mackenzie, I. Ismail, Hansjochen Köckert, David M. P. Holland, Dimitrios Rompotis, Marie Géléoc, Jérôme Palaudoux, Loic Journel, Jonathan G. Underwood, Farzaneh Ziaee, Jan Lahl, Robert Mason, Kasra Amini, Mark Brouard, Gildas Goldsztejn, Artem Rudenko, Stefan Düsterer, Sylvain Maclot, Maria Novella Piancastelli, Arnaud Rouzée, Thierry Ruchon, Daniel Rolles, Michael Burt, Jongmin Lee, Rebecca Boll, Oksana Travnikova, Andrey S. Mereshchenko, Joss Wiese, Sebastian Trippel, Marc Simon, Francis Penent, Felix Allum, Felix Brauße, Bastian Manschwetus, Simone Techert, Evgeny Savelyev, Tatiana Marchenko, Henrik Stapelfeldt, Renaud Guillemin, Nora Schirmel, Cédric Bomme, Benjamin Erk, Alexander S. Gentleman, Claire Vallance, Pavel K. Olshin, Sadia Bari, Jochen Küpper, University of Oxford, Deutsches Elektronen-Synchrotron [Hamburg] (DESY), Saint Petersburg State Polytechnical University (SPSPU), KVI Atomic and Molecular Physics (KVI), University of Groningen [Groningen], Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie (MBI), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Attophysique (ATTO), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Microbiology Laboratory, Middlemore Hospital, Laboratoire des collisions atomiques et moléculaires (LCAM), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Department of Physics, Lund Institute of Technology, Lund University [Lund]-Lund University [Lund], Lund University [Lund], Centre de recherche sur les Ions, les MAtériaux et la Photonique (CIMAP - UMR 6252), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Physical and Theoretical Chemistry Laboratory, Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interdisciplinaire Carnot de Bourgogne (ICB), Université de Bourgogne (UB)-Centre National de la Recherche Scientifique (CNRS), Kansas State University, Georg-August-University = Georg-August-Universität Göttingen, Department of Physics and Astronomy [UCL London], University College of London [London] (UCL), Center for Free-Electron Laser Science (CFEL), ANR-16-CE30-0001,ATTOMEMUCHO,Dynamique électronique attoseconde dans les molécules organiques isolées par la spectroscopie 'core-hole clock'(2016), University of Oxford [Oxford], Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interdisciplinaire Carnot de Bourgogne (LICB), Georg-August-University [Göttingen], Centre National de la Recherche Scientifique (CNRS)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Caen Normandie (UNICAEN), and Normandie Université (NU)
Subjects: Atom and Molecular Physics and Optics, Imaging spectrometer, General Physics and Astronomy, 02 engineering and technology, Physical Chemistry, 01 natural sciences, Molecular physics, Mass spectrometry imaging, Ion, 0103 physical sciences, Molecule, ddc:530, Physical and Theoretical Chemistry, 010306 general physics, ComputingMilieux_MISCELLANEOUS, Fysikalisk kemi, Physics, Coupling, Range (particle radiation), Photodissociation, Coulomb explosion, 021001 nanoscience & nanotechnology, 3. Good health, Atom- och molekylfysik och optik, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], 0210 nano-technology
Abstract: The journal of chemical physics 149(20), 204313 (2018). doi:10.1063/1.5041381, The photodissociation dynamics of CH$_3$I and CH$_2$ClI at 272 nm were investigated by time-resolved Coulomb explosion imaging, with an intense non-resonant 815 nm probe pulse. Fragment ion momenta over a wide m/z range were recorded simultaneously by coupling a velocity map imaging spectrometer with a pixel imaging mass spectrometry camera. For both molecules, delay-dependent pump-probe features were assigned to ultraviolet-induced carbon-iodine bond cleavage followed by Coulomb explosion. Multi-mass imaging also allowed the sequential cleavage of both carbon-halogen bonds in CH$_2$ClI to be investigated. Furthermore, delay-dependent relative fragment momenta of a pair of ions were directly determined using recoil-frame covariance analysis. These results are complementary to conventional velocity map imaging experiments and demonstrate the application of time-resolved Coulomb explosion imaging to photoinduced real-time molecular motion., Published by American Institute of Physics, Melville, NY
Published: 2018
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16. Coulomb-explosion imaging of concurrent CH2BrI photodissociation dynamics

Author: Renaud Guillemin, Maria Novella Piancastelli, Alexander S. Gentleman, Artem Rudenko, Jérôme Palaudoux, Thierry Ruchon, O. Travnikova, Rebecca Boll, Felix Brausse, Rolf Treusch, Marc Simon, Arnaud Rouzée, Mark Brouard, Stefan Düsterer, Joss Wiese, Stuart R. Mackenzie, Jochen Küpper, Sebastian Trippel, Loic Journel, Jonathan G. Underwood, Claire Vallance, Michael Burt, Nora Schirmel, Kasra Amini, David M. P. Holland, Farzaneh Ziaee, Francis Penent, Benjamin Erk, Jan Lahl, Per Johnsson, Romain Géneaux, Barbara Cunha de Miranda, Hansjochen Köckert, Andrey S. Mereshchenko, Jongmin Lee, Marie Géléoc, Gildas Goldsztejn, Bastian Manschwetus, Sylvain Maclot, Henrik Stapelfeldt, Daniel Rolles, Cédric Bomme, Iyas Ismail, Simone Techert, Evgeny Savelyev, Tatiana Marchenko, Erland Müller, Dimitrios Rompotis, Pavel K. Olshin, and Sadia Bari
Subjects: Physics, Photon, Photodissociation, Coulomb explosion, 010402 general chemistry, medicine.disease_cause, Laser, 01 natural sciences, 0104 chemical sciences, Chemical Dynamics, law.invention, law, Ionization, 0103 physical sciences, Femtosecond, medicine, Atomic physics, 010306 general physics, Ultraviolet
Abstract: The dynamics following laser-induced molecular photodissociation of gas-phase CH2BrI at 271.6 nm were investigated by time-resolved Coulomb-explosion imaging using intense near-IR femtosecond laser pulses. The observed delay-dependent photofragment momenta reveal that CH2BrI undergoes C-I cleavage, depositing 65.6% of the available energy into internal product states, and that absorption of a second UV photon breaks the C-Br bond of CH2Br. Simulations confirm that this mechanism is consistent with previous data recorded at 248 nm, demonstrating the sensitivity of Coulomb-explosion imaging as a real-time probe of chemical dynamics.
Published: 2017
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17. Lowered threshold energy for femtosecond laser induced optical breakdown in a water based eye model by aberration correction with adaptive optics

Author: Anja Hansen, Axel Günther, Tammo Ripken, A. Krüger, and Romain Géneaux
Subjects: Wavefront, Materials science, Photodisruption, business.industry, ocis:(330.4460) Ophthalmic optics and devices, Laser, Threshold energy, Atomic and Molecular Physics, and Optics, law.invention, ocis:(140.3300) Laser beam shaping, Lens (optics), ocis:(110.1080) Active or adaptive optics, Optics, law, Achromatic lens, ocis:(170.4470) Ophthalmology, ocis:(330.3350) Vision - laser damage, Research-Article, ocis:(140.3440) Laser-induced breakdown, business, Adaptive optics, Eye laser surgery, Biotechnology
Abstract: In femtosecond laser ophthalmic surgery tissue dissection is achieved by photodisruption based on laser induced optical breakdown. In order to minimize collateral damage to the eye laser surgery systems should be optimized towards the lowest possible energy threshold for photodisruption. However, optical aberrations of the eye and the laser system distort the irradiance distribution from an ideal profile which causes a rise in breakdown threshold energy even if great care is taken to minimize the aberrations of the system during design and alignment. In this study we used a water chamber with an achromatic focusing lens and a scattering sample as eye model and determined breakdown threshold in single pulse plasma transmission loss measurements. Due to aberrations, the precise lower limit for breakdown threshold irradiance in water is still unknown. Here we show that the threshold energy can be substantially reduced when using adaptive optics to improve the irradiance distribution by spatial beam shaping. We found that for initial aberrations with a root-mean-square wave front error of only one third of the wavelength the threshold energy can still be reduced by a factor of three if the aberrations are corrected to the diffraction limit by adaptive optics. The transmitted pulse energy is reduced by 17% at twice the threshold. Furthermore, the gas bubble motions after breakdown for pulse trains at 5 kilohertz repetition rate show a more transverse direction in the corrected case compared to the more spherical distribution without correction. Our results demonstrate how both applied and transmitted pulse energy could be reduced during ophthalmic surgery when correcting for aberrations. As a consequence, the risk of retinal damage by transmitted energy and the extent of collateral damage to the focal volume could be minimized accordingly when using adaptive optics in fs-laser surgery.
Published: 2013

18. Phase-Resolved Two-Dimensional Spectroscopy of Electronic Wavepackets by Laser-Induced XUV Free Induction Decay

Author: Samuel Beaulieu, Yann Mairesse, L. Barreau, Dominique Descamps, Antoine Comby, Stéphane Petit, Romain Géneaux, François Légaré, Etienne Bloch, Centre d'Etudes Lasers Intenses et Applications (CELIA), Université de Bordeaux (UB)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Institut National de la Recherche Scientifique [Québec] (INRS), Attophysique (ATTO), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Bordeaux (UB), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), and Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Physics, [PHYS]Physics [physics], Atomic Physics (physics.atom-ph), Dephasing, Wave packet, FOS: Physical sciences, Laser, 7. Clean energy, 01 natural sciences, 3. Good health, law.invention, Physics - Atomic Physics, 010309 optics, Free induction decay, Amplitude, law, Extreme ultraviolet, 0103 physical sciences, Heterodyne detection, Atomic physics, 010306 general physics, Spectroscopy
Abstract: We present a novel time- and phase-resolved, background-free scheme to study the extreme ultraviolet dipole emission of a bound electronic wavepacket, without the use of any extreme ultraviolet exciting pulse. Using multiphoton transitions, we populate a superposition of quantum states which coherently emit extreme ultraviolet radiation through free induction decay. This emission is probed and controlled, both in amplitude and phase, by a time-delayed infrared femtosecond pulse. We directly measure the laser-induced dephasing of the emission by using a simple heterodyne detection scheme based on two-source interferometry. This technique provides rich information about the interplay between the laser field and the Coulombic potential on the excited electron dynamics. Its background-free nature enables us to use a large range of gas pressures and to reveal the influence of collisions in the relaxation process., Comment: In press, PRA Rapid Communications
Published: 2017
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19. Tunable orbital angular momentum in high-harmonic generation

Author: A. Camper, Thierry Ruchon, Fabio Frassetto, Luca Poletto, Ganesh Adhikary, Guillaume Dovillaire, C Chappuis, Carlo Spezzani, Louis F. DiMauro, Paolo Miotti, Barbara Ressel, Matija Stupar, David Gauthier, Riccardo Cucini, G. De Ninno, P. Rebernik Ribič, Romain Géneaux, Elettra Sincrotrone Trieste, Laboratory of Quantum Optics, University of Nova Gorica, Ohio State University [Columbus] (OSU), Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Attophysique (ATTO), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Imagine Optic, AFOP, CNR Inst Photon & Nanotechnol, Laboratoire de Physique des Solides (LPS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), ANR-14-CE32-0010,Xstase,Étude du moment angulaire de faisceaux lumineux XUV: synthèse et transferts(2014), and Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Genetics and Molecular Biology (all), Angular momentum, Photon, Science, General Physics and Astronomy, FOS: Physical sciences, Physics::Optics, angular momentum, 01 natural sciences, Biochemistry, Article, General Biochemistry, Genetics and Molecular Biology, 010309 optics, high-order laser harmonics, Physics and Astronomy (all), Optics, 0103 physical sciences, High harmonic generation, Light beam, 010306 general physics, Physics, [PHYS]Physics [physics], Multidisciplinary, business.industry, Chemistry (all), Optical physics, General Chemistry, Dichroism, Femtosecond, Biochemistry, Genetics and Molecular Biology (all), business, Optical vortex, Optics (physics.optics), Physics - Optics
Abstract: Optical vortices are currently one of the most intensively studied topics in optics. These light beams, which carry orbital angular momentum (OAM), have been successfully utilized in the visible and infrared in a wide variety of applications. Moving to shorter wavelengths may open up completely new research directions in the areas of optical physics and material characterization. Here, we report on the generation of extreme-ultraviolet optical vortices with femtosecond duration carrying a controllable amount of OAM. From a basic physics viewpoint, our results help to resolve key questions such as the conservation of angular momentum in highly nonlinear light–matter interactions, and the disentanglement and independent control of the intrinsic and extrinsic components of the photon's angular momentum at short-wavelengths. The methods developed here will allow testing some of the recently proposed concepts such as OAM-induced dichroism, magnetic switching in organic molecules and violation of dipolar selection rules in atoms., The controlled generation of extreme-ultraviolet beams with controllable topological charge has not been demonstrated. Here, Gauthier et al. report on the generation of extreme-ultraviolet optical vortices with femtosecond duration carrying a controllable amount of orbital angular momentum.
Published: 2017
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20. Determination of accurate electron chiral asymmetries in fenchone and camphor in the VUV range: sensitivity to isomerism and enantiomeric purity

Author: Uwe J. Meierhenrich, Gustavo A. Garcia, Ivan Powis, Iuliia Myrgorodska, Vincent Wanie, Romain Géneaux, Samuel Beaulieu, Lipsa Nag, Valérie Blanchet, Laurent Nahon, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Institut de Chimie de Nice (ICN), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Côte d'Azur (UCA)-Université Nice Sophia Antipolis (... - 2019) (UNS), COMUE Université Côte d'Azur (2015-2019) (COMUE UCA)-COMUE Université Côte d'Azur (2015-2019) (COMUE UCA), Centre d'Etudes Lasers Intenses et Applications (CELIA), Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Bordeaux (UB), Attophysique (ATTO), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), School of Chemistry, The University of Nottingham, University Park, Nottingham, NG7 2RD, UK., School of Chemistry, The University of Nottingham, University Park, Nottingham, NG7 2RD, UK. Code (UMR, EA, ...), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Université Nice Sophia Antipolis (1965 - 2019) (UNS), COMUE Université Côte d'Azur (2015-2019) (COMUE UCA)-COMUE Université Côte d'Azur (2015-2019) (COMUE UCA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Côte d'Azur (UCA), and Université de Bordeaux (UB)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS]Physics [physics], Spectrometer, Chemistry, Analytical chemistry, General Physics and Astronomy, Synchrotron radiation, Photoionization, Electron, Photoelectric effect, 010402 general chemistry, 01 natural sciences, 0104 chemical sciences, Ion, 0103 physical sciences, Physical and Theoretical Chemistry, Enantiomer, 010306 general physics, Enantiomeric excess
Abstract: International audience; Photoelectron circular dichroism (PECD) manifests itself as an intense forward/backward asymmetry in the angular distribution of photoelectrons produced from randomly-oriented enantiomers by photoionization with circularly-polarized light (CPL). As a sensitive probe of both photoionization dynamics and of the chiral molecular potential, PECD attracts much interest especially with the recent performance of related experiments with visible and VUV laser sources. Here we report, by use of quasi-perfect CPL VUV synchrotron radiation and using a double imaging photoelectron/photoion coincidence (i2PEPICO) spectrometer, new and very accurate values of the corresponding asymmetries on showcase chiral isomers: camphor and fenchone. These data have additionally been normalized to the absolute enantiopurity of the sample as measured by a chromatographic technique. They can therefore be used as benchmarking data for new PECD experiments, as well as for theoretical models. In particular we found, especially for the outermost orbital of both molecules, a good agreement with CMS-Xα PECD modeling over the whole VUV range. We also report a spectacular sensitivity of PECD to isomerism for slow electrons, showing large and opposite asymmetries when comparing R-camphor to R-fenchone (respectively −10% and +16% around 10 eV). In the course of this study, we could also assess the analytical potential of PECD. Indeed, the accuracy of the data we provide are such that limited departure from perfect enantiopurity in the sample we purchased could be detected and estimated in excellent agreement with the analysis performed in parallel via a chromatographic technique, establishing a new standard of accuracy, in the ±1% range, for enantiomeric excess measurement via PECD. The i2PEPICO technique allows correlating PECD measurements to specific parent ion masses, which would allow its application to analysis of complex mixtures
Published: 2016
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21. Enhanced high-order harmonic generation driven by a wavefront corrected high-energy laser

Author: Yi Wu, Jian Zhao, Yang Wang, Stephen R. Leone, Yanchun Yin, Jie Li, Christian Reinhold Ott, Zenghu Chang, Daniel M. Neumark, Tianyi Guo, Matthew Weidman, Xiaoming Ren, Christopher J. Kaplan, Marieke F. Jager, Jialin Li, and Romain Géneaux
Subjects: Wavefront, Physics, Argon, business.industry, chemistry.chemical_element, Condensed Matter Physics, Laser, 01 natural sciences, 7. Clean energy, Atomic and Molecular Physics, and Optics, Deformable mirror, law.invention, 010309 optics, Optics, chemistry, Physics::Plasma Physics, law, Harmonics, Extreme ultraviolet, 0103 physical sciences, High harmonic generation, 010306 general physics, business, Beam splitter
Abstract: We developed and implemented an experimental setup for the generation of high-energy high-order harmonics in argon gas for nonlinear experiments in the extreme ultraviolet (XUV) spectral range. High-order harmonics were generated by loosely focusing a high-energy laser pulse centered around 800 nm into a gas cell filled with argon in a phase-matching condition. The wavefront distortions of the driving pulse were corrected by a deformable mirror, and the XUV conversion efficiency was significantly improved due to the excellent beam profile at focus. A high-damage-threshold beam splitter was used to eliminate high-energy driving pulses co-propagating with high-order harmonics. The setup has a potential to provide intense ultrashort XUV pulses reaching the intensity levels required for nonlinear experiments in the XUV spectral range.
Published: 2018
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22. Synthesis and characterization of attosecond light vortices in the extreme ultraviolet

Author: Thierry Ruchon, O. Gobert, Thierry Auguste, A. Camper, J. Caillat, Romain Géneaux, Richard Taïeb, Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Ohio State University [Columbus] (OSU), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Pierre et Marie Curie - Paris 6 (UPMC)
Subjects: Attosecond, Science, General Physics and Astronomy, FOS: Physical sciences, Physics::Optics, Astrophysics::Cosmology and Extragalactic Astrophysics, 7. Clean energy, 01 natural sciences, General Biochemistry, Genetics and Molecular Biology, Article, 010309 optics, Optics, 0103 physical sciences, Physics::Atomic and Molecular Clusters, Light beam, 010306 general physics, Physics, [PHYS.PHYS.PHYS-OPTICS]Physics [physics]/Physics [physics]/Optics [physics.optics], Multidisciplinary, business.industry, General Chemistry, Photon upconversion, Extreme ultraviolet, Femtosecond, [SPI.OPTI]Engineering Sciences [physics]/Optics / Photonic, Optoelectronics, Photonics, business, Ultrashort pulse, Optical vortex, Optics (physics.optics), Physics - Optics
Abstract: Infrared and visible light beams carrying orbital angular momentum (OAM) are currently thoroughly studied for their extremely broad applicative prospects, among which are quantum information, micromachining and diagnostic tools. Here we extend these prospects, presenting a comprehensive study for the synthesis and full characterization of optical vortices carrying OAM in the extreme ultraviolet (XUV) domain. We confirm the upconversion rules of a femtosecond infrared helically phased beam into its high-order harmonics, showing that each harmonic order carries the total number of OAM units absorbed in the process up to very high orders (57). This allows us to synthesize and characterize helically shaped XUV trains of attosecond pulses. To demonstrate a typical use of these new XUV light beams, we show our ability to generate and control, through photoionization, attosecond electron beams carrying OAM. These breakthroughs pave the route for the study of a series of fundamental phenomena and the development of new ultrafast diagnosis tools using either photonic or electronic vortices., Twisted light beams have found several applications in the infrared and visible regime, but reaching the extreme ultraviolet has been difficult due to lack of sources. Here the authors report generation of helically shaped extreme ultraviolet trains of attosecond pulses via high harmonic generation.
Published: 2016
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23. Probing Ultrafast Molecular Chirality

Author: Antoine Comby, Laurent Nahon, Gustavo García, Mathieu Dumergue, A. Ferré, Sébastien J. Weber, Romain Géneaux, L. Merceron, David Staedter, Thierry Ruchon, Frédéric Burgy, C. Handschin, Bernard Pons, Valérie Blanchet, Stéphane Petit, Eric Mével, Yann Mairesse, Dominique Descamps, and Baptiste Fabre
Subjects: Circular dichroism, Photon, Chemistry, High Energy Physics::Lattice, Relaxation (NMR), Analytical chemistry, Physics::Optics, Photoionization, Molecular physics, Ionization, Physics::Atomic and Molecular Clusters, Physics::Atomic Physics, Physics::Chemical Physics, Chirality (chemistry), Ultrashort pulse, Circular polarization
Abstract: We investigate the photoionization of chiral molecules in different ionization regimes : one photon-, multiphoton above threshold-, and tunnel-ionization. We use the photoelectron circular dichroism to track the ultrafast relaxation of a chiral molecule.
Published: 2016
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24. Toward Femtochemistry with Circular Polarized Pulses

Author: Stéphane Petit, Dominique Descamps, Laurent Nahon, Thierry Ruchon, A. Ferré, François Légaré, Antoine Comby, Gustavo García, Valérie Blanchet, Yann Mairesse, Bernard Pons, Samuel Beaulieu, Romain Géneaux, Baptiste Fabre, Centre d'Etudes Lasers Intenses et Applications (CELIA), Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Bordeaux (UB), Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Advanced Laser Light Source-INRS-EMT, Énergie Matériaux Télécommunications - INRS (EMT-INRS), Institut National de la Recherche Scientifique [Québec] (INRS)-Université du Québec à Montréal = University of Québec in Montréal (UQAM)-Institut National de la Recherche Scientifique [Québec] (INRS)-Université du Québec à Montréal = University of Québec in Montréal (UQAM), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Centre de Recherche des Cordeliers (CRC), Université Paris Diderot - Paris 7 (UPD7)-École pratique des hautes études (EPHE), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Université Paris Descartes - Paris 5 (UPD5)-Institut National de la Santé et de la Recherche Médicale (INSERM), Femto (LCAR), Laboratoire Collisions Agrégats Réactivité (LCAR), Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées, Université de Bordeaux (UB)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Université Pierre et Marie Curie - Paris 6 (UPMC)-École Pratique des Hautes Études (EPHE), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris Descartes - Paris 5 (UPD5)-Institut National de la Santé et de la Recherche Médicale (INSERM), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université de Toulouse (UT)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Bordeaux (UB)-Centre National de la Recherche Scientifique (CNRS), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS), Institut National de la Recherche Scientifique [Québec] (INRS)-Université du Québec à Montréal (UQAM)-Institut National de la Recherche Scientifique [Québec] (INRS)-Université du Québec à Montréal (UQAM), Université Paris Diderot - Paris 7 (UPD7)-École pratique des hautes études (EPHE)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Université Paris Descartes - Paris 5 (UPD5)-Institut National de la Santé et de la Recherche Médicale (INSERM), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), and Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse)
Subjects: Physics, [PHYS]Physics [physics], Extreme ultraviolet, High harmonic generation, Observable, Atomic physics, Polarization (waves), Femtochemistry, ComputingMilieux_MISCELLANEOUS
Abstract: Femtochemistry induced by circularly polarization light coupled to velocity map imaging of photoelectron gives an access to new and sensitive observables that have to be compared to the standard ones.
Published: 2016
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25. A table-top ultrashort light source in the extreme ultraviolet for circular dichroism experiments

Author: L. Merceron, Romain Géneaux, Valérie Blanchet, Dominique Descamps, Stéphane Petit, Eric Mével, Yann Mairesse, Gustavo A. Garcia, Frédéric Burgy, David Staedter, Laurent Nahon, Antoine Comby, C. Handschin, Thierry Ruchon, A. Ferré, Mathieu Dumergue, Sébastien J. Weber, Baptiste Fabre, Bernard Pons, Centre d'Etudes Lasers Intenses et Applications (CELIA), Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Bordeaux (UB), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Collisions Agrégats Réactivité (LCAR), Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Bordeaux (UB)-Centre National de la Recherche Scientifique (CNRS), Attophysique (ATTO), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Biomolécules Excitées (DICO), Femto (LCAR), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées, Université de Bordeaux (UB)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay, Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Dynamique et Interactions en phase Condensée (DICO), Université de Toulouse (UT)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université de Toulouse (UT)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), and Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC)
Subjects: Physics, [PHYS]Physics [physics], Circular dichroism, [PHYS.PHYS.PHYS-OPTICS]Physics [physics]/Physics [physics]/Optics [physics.optics], business.industry, Attosecond, Physics::Optics, Photoionization, Laser, 7. Clean energy, Atomic and Molecular Physics, and Optics, Electronic, Optical and Magnetic Materials, law.invention, Pulse (physics), Optics, law, Extreme ultraviolet, Femtosecond, High harmonic generation, business, ultrashort, ComputingMilieux_MISCELLANEOUS
Abstract: International audience; Circular dichroism in the extreme ultraviolet range is broadly used as a sensitive structural probe of matter, from the molecular photoionization of chiral species1, 2, 3 to the magnetic properties of solids4. Extending such techniques to the dynamical regime has been a long-standing quest of solid-state physics and physical chemistry, and was only achieved very recently5 thanks to the development of femtosecond circular extreme ultraviolet sources. Only a few large facilities, such as femtosliced synchrotrons6, 7 or free-electron lasers8, are currently able to produce such pulses. Here, we propose a new compact and accessible alternative solution: resonant high-order harmonic generation of an elliptical laser pulse. We show that this process, based on a simple optical set-up, delivers bright, coherent, ultrashort, quasi-circular pulses in the extreme ultraviolet. We use this source to measure photoelectron circular dichroism on chiral molecules, opening the route to table-top time-resolved femtosecond and attosecond chiroptical experiments.
Published: 2015
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26. Universality of photoelectron circular dichroism in the photoionization of chiral molecules

Author: Thierry Ruchon, Yann Mairesse, R. Canonge, A. Ferré, Romain Géneaux, Samuel Beaulieu, François Légaré, Valérie Blanchet, Dominique Descamps, Nikita Fedorov, Stéphane Petit, Baptiste Fabre, Bernard Pons, Centre d'Etudes Lasers Intenses et Applications (CELIA), Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Bordeaux (UB), Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Attophysique (ATTO), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Advanced Laser Light Source-INRS-EMT, Énergie Matériaux Télécommunications - INRS (EMT-INRS), Institut National de la Recherche Scientifique [Québec] (INRS)-Université du Québec à Montréal = University of Québec in Montréal (UQAM)-Institut National de la Recherche Scientifique [Québec] (INRS)-Université du Québec à Montréal = University of Québec in Montréal (UQAM), Université de Bordeaux (UB)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Physics, Circular dichroism, [PHYS.PHYS]Physics [physics]/Physics [physics], media_common.quotation_subject, General Physics and Astronomy, Photoionization, Electron, Dichroism, 010402 general chemistry, 01 natural sciences, Asymmetry, 0104 chemical sciences, Tunnel ionization, Ionization, 0103 physical sciences, Vibrational circular dichroism, Physics::Atomic and Molecular Clusters, Physics::Atomic Physics, Atomic physics, 010306 general physics, media_common
Abstract: International audience; Photoionization of chiral molecules by circularly polarized radiation gives rise to a strong forward/backward asymmetry in the photoelectron angular distribution, referred to as photoelectron circular dichroism (PECD). Here we show that PECD is a universal effect that reveals the inherent chirality of the target in all ionization regimes: single photon, multiphoton, above-threshold and tunnel ionization. These different regimes provide complementary spectroscopic information at electronic and vibrational levels. The universality of the PECD can be understood in terms of a classical picture of the ionizing process, in which electron scattering on the chiral potential under the influence of a circularly polarized electric field results in a strong forward/backward asymmetry.
Published: 2016
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26 results on '"Romain Géneaux"'

1. Coherent energy exchange between carriers and phonons in Peierls-distorted bismuth unveiled by broadband XUV pulses

2. Coherent energy exchange between carriers and phonons in Peierls-distorted bismuth unveiled by broadband XUV pulses

3. Coupled valence carrier and core-exciton dynamics in WS2 probed by few-femtosecond extreme ultraviolet transient absorption spectroscopy

4. Two-dimensional phase cartography for high-harmonic spectroscopy

5. Attosecond-resolved photoionization of chiral molecules

6. Source noise suppression in attosecond transient absorption spectroscopy by edge-pixel referencing

7. Attosecond time-domain measurement of core-excitonic decay in magnesium oxide

8. Transfer of Orbital Angular Momentum in High Harmonic Generation using two Driving Beams

9. Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids

10. Beam optimization in a 25 TW femtosecond laser system for high harmonic generation

11. Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom

12. Probing ultrafast dynamics of chiral molecules using time-resolved photoelectron circular dichroism

13. Photoexcitation Circular Dichroism in Chiral Molecules

14. Electron dynamics in transition metal dichalcogenides utilizing attosecond transient absorption spectroscopy

15. Coulomb explosion imaging of CH3I and CH2CII photodissociation dynamics

16. Coulomb-explosion imaging of concurrent CH2BrI photodissociation dynamics

17. Lowered threshold energy for femtosecond laser induced optical breakdown in a water based eye model by aberration correction with adaptive optics

18. Phase-Resolved Two-Dimensional Spectroscopy of Electronic Wavepackets by Laser-Induced XUV Free Induction Decay

19. Tunable orbital angular momentum in high-harmonic generation

20. Determination of accurate electron chiral asymmetries in fenchone and camphor in the VUV range: sensitivity to isomerism and enantiomeric purity

21. Enhanced high-order harmonic generation driven by a wavefront corrected high-energy laser

22. Synthesis and characterization of attosecond light vortices in the extreme ultraviolet

23. Probing Ultrafast Molecular Chirality

24. Toward Femtochemistry with Circular Polarized Pulses

25. A table-top ultrashort light source in the extreme ultraviolet for circular dichroism experiments

26. Universality of photoelectron circular dichroism in the photoionization of chiral molecules

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26 results on '"Romain Géneaux"'

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