arXiv subjects

Francois Légaré

Publications and source records attributed to Francois Légaré.

4 recordsLinked to original sources

arXiv2026

Detecting the full photoemission cone from laser-based ARPES experiments by leveraging deflector technology

Angle-resolved photoemission spectroscopy (ARPES) provides a direct access to the electronic band structure of solid and molecular systems. The momentum range accessible by this technique depends directly on the photon energy used, and low-photon-energy sources are insufficient to photoemit electrons over the full Brillouin zone of most quantum materials. In addition, while electrons are emitted over a 2$π$ solid angle, conventional hemispherical analyzers only collect a small subset of those electrons. A previous work [RSI 92, 123907 (2021)] demonstrated that electrons emitted over a larger field-of-view can be acquired in one fixed configuration by accelerating them towards the analyzer with a bias voltage. Here, we extend this work by leveraging the deflector technology of novel ARPES hemispherical analyzers. We demonstrate the ability to detect all $2π$ photoemitted electrons in a fixed configuration for various materials such as gold, cuprates and transition-metal dichalcogenides. This approach is especially advantageous for time-resolved ARPES, as electron dynamics over a large momentum range can be accessed with identical measurement conditions.

cond-mat.mtrl-sci↗

arXiv2017

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

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.

physics.atom-ph↗

arXiv2016

Relaxation Dynamics in Photoexcited Chiral Molecules Studied by Time-Resolved Photoelectron Circular Dichroism: Toward Chiral Femtochemistry

Unravelling the main initial dynamics responsible for chiral recognition is a key stepin the understanding of many biological processes. However this challenging task requires a sensitive enantiospecic probe to investigate molecular dynamics on their natural femtosecond timescale. Here we show that, in the gas phase, the ultrafast relaxationdynamics of photoexcited chiral molecules can be tracked by recording Time-ResolvedPhotoElectron Circular Dichroism (TR-PECD) resulting from the photoionisation bya circularly polarized probe pulse. A large forward/backward asymmetry along theprobe propagation axis is observed in the photoelectron angular distribution. Its evolution with pump-probe delay reveals ultrafast dynamics that are inaccessible in theangle-integrated photoelectron spectrum nor via the usual electron emission anisotropyparameter ($β$). PECD, which originates from the electron scattering in the chiral molecular potential, appears as a new sensitive observable for ultrafast molecular dynamicsin chiral systems.

physics.chem-ph↗

arXiv2016

Generation of high harmonics from silicon

We generate high-order harmonics of a mid-infrared laser from a silicon single crystal and find their origin in the recollision of coherently accelerated electrons with their holes, analogously to the atomic and molecular case, and to ZnO [Vampa et al., Nature 522, 462-464 (2015)], a direct bandgap material. Therefore indirect bandgap materials are shown to sustain the recollision process as well as direct bandgap materials. Furthermore, we find that the generation is perturbed with electric fields as low as 30 V/$μ$m, equal to the DC damage threshold. Our results extend high-harmonic spectroscopy to the most technologically relevant material, and open the possibility to integrate high harmonics with conventional electronics.

physics.optics↗