arXiv subjects

Nicolas Douguet

Publications and source records attributed to Nicolas Douguet.

29 records · Page 2Linked to original sources

arXiv2019

Resonant Anisotropic Emission in Two-Photon Interferometric Spectroscopy

We theoretically explore a variant of RABBITT spectroscopy in which the attosecond-pulse train comprises isolated pairs of consecutive harmonics of the fundamental infrared probe frequency. In this scheme, one-photon and two-photon amplitudes interfere resulting in an asymmetric photoelectron emission. This interferometric principle has the potential of giving access to the time-resolved ionization of systems that exhibit autoionizing states, since it imprints the group delay of both one-photon and two-photon resonant transitions in the energy-resolved photoelectron anisotropy as a function of the pump-probe time delay. To bring to the fore the connection between the pump-probe ionization process and its perturbative analysis, on the the one side, and the underlying field-free scattering observables as well as the radiative couplings in the target system, on the other side, we test this scheme with an exactly solvable analytical one-dimensional model that supports both bound states and shape-resonances. The asymmetric photoelectron emission near a resonance is computed using perturbation theory as well as solving the time-dependent Schödinger equation; the results are in excellent agreement with the field-free resonant scattering properties of the model.

physics.atom-ph↗

arXiv2018

Application of the Complex Kohn Variational Method to Attosecond Spectroscopy

The complex Kohn variational method is extended to compute light-driven electronic transitions between continuum wavefunctions in atomic and molecular systems. This development enables the study of multiphoton processes in the perturbative regime for arbitrary light polarization. As a proof of principle, we apply the method to compute the photoelectron spectrum arising from the pump-probe two-photon ionization of helium induced by a sequence of extreme ultraviolet and infrared-light pulses. We compare several two-photon ionization pump-probe spectra, resonant with the (2s2p)1P1o Feshbach resonance, with independent simulations based on the atomic B-spline close- coupling STOCK code, and find good agreement between the two approaches. This new finite-pulse perturbative approach is a step towards the ab initio study of weak-field attosecond processes in poly-electronic molecules.

physics.atom-ph↗

arXiv2018

Attosecond angular streaking and tunnelling time in atomic hydrogen

Tunnelling, one of the key features of quantum mechanics, ignited an ongoing debate about the value, meaning and interpretation of 'tunnelling time'. Until recently the debate was purely theoretical, with the process considered to be instantaneous for all practical purposes. This changed with the development of ultrafast lasers and in particular, the 'attoclock' technique that is used to probe the attosecond dynamics of electrons. Although the initial attoclock measurements hinted at instantaneous tunnelling, later experiments contradicted those findings, claiming to have measured finite tunnelling times. In each case these measurements were performed with multi-electron atoms. Atomic hydrogen (H), the simplest atomic system with a single electron, can be 'exactly' (subject only to numerical limitations) modelled using numerical solutions of the 3D-TDSE with measured experimental parameters and acts as a convenient benchmark for both accurate experimental measurements and calculations. Here we report the first attoclock experiment performed on H and find that our experimentally determined offset angles are in excellent agreement with accurate 3D-TDSE simulations performed using our experimental pulse parameters. The same simulations with a short-range Yukawa potential result in zero offset angles for all intensities. We conclude that the offset angle measured in the attoclock experiments originates entirely from electron scattering by the long-range Coulomb potential with no contribution from tunnelling time delay. That conclusion is supported by empirical observation that the electron offset angles follow closely the simple formula for the deflection angle of electrons undergoing classical Rutherford scattering by the Coulomb potential. Thus we confirm that, in H, tunnelling is instantaneous (with an upperbound of 1.8 as) within our experimental and numerical uncertainty.

physics.atom-ph↗

arXiv2017

Dynamics of Tunneling Ionization using Bohmian Mechanics

Recent attoclock experiments and theoretical studies regarding the strong-field ionization of atoms by few-cycle infrared pulses revealed new features that have attracted much attention. Here we investigate tunneling ionization and the dynamics of the electron probability using Bohmian Mechanics. We consider a one-dimensional problem to illustrate the underlying mechanisms of the ionization process. It is revealed that in the major part of the below-the-barrier ionization regime, in an intense and short infrared pulse, the electron does not tunnel \through" the entire barrier, but rather already starts from the classically forbidden region. Moreover, we highlight the correspondence between the probability of locating the electron at a particular initial position and its asymptotic momentum. Bohmian Mechanics also provides a natural definition of mean tunneling time and exit position, taking account of the time dependence of the barrier. Finally, we find that the electron can exit the barrier with significant kinetic energy, thereby corroborating the results of a recent study [Camus et al., Phys. Rev. Lett. 119 (2017) 023201].

physics.atom-ph↗

arXiv2016

Above-threshold ionization in neon produced by combining optical and bichromatic XUV femtosecond pulses

We consider the ionization of neon induced by a femtosecond laser pulse composed of overlapping, linearly polarized bichromatic extreme ultraviolet and infrared fields. In particular, we study the effects of the infrared light on a two-pathway ionization scheme for which Ne 2s22p53s1P is used as intermediate state. Using time-dependent calculations, supported by a theoretical approach based on the strong-field approximation, we analyze the ionization probability and the photoelectron angular distributions associated with the different sidebands of the ionization spectrum. Complex oscillations of the angular distribution anisotropy parameters as a function of the infrared light intensity are revealed. Finally, we demonstrate that coherent control of the asymmetry is achievable by tuning the infrared frequency to a nearby electronic transition.

physics.atom-ph↗

arXiv2016

Photoelectron angular distribution in two-pathway ionization of neon with femtosecond XUV pulses

We analyze the photoelectron angular distribution in two-pathway interference between non\-resonant one-photon and resonant two-photon ionization of neon. We consider a bichromatic femtosecond XUV pulse whose fundamental frequency is tuned near the $2p^5 3s$ atomic states of neon. The time-dependent Schrödinger equation is solved and the results are employed to compute the angular distribution and the associated anisotropy parameters at the main photoelectron line. We also employ a time-dependent perturbative approach, which allows obtaining information on the process for a large range of pulse parameters, including the steady-state case of continuous radiation, i.e., an infinitely long pulse. The results from the two methods are in relatively good agreement over the domain of applicability of perturbation theory.

physics.atom-ph↗

arXiv2015

Theoretical study of radiative electron attachment to CN, C2H, and C4H radicals

A first-principle theoretical approach to study the process of radiative electron attachment is developed and applied to the negative molecular ions CN$^-$, C$_4$H$^-$, and C$_2$H$^-$. Among these anions, the first two have already been observed in the interstellar space. Cross sections and rate coefficients for formation of these ions by radiative electron attachment to the corresponding neutral radicals are calculated. For completeness of the theoretical approach, two pathways for the process have been considered: (i) A direct pathway, in which the electron in collision with the molecule spontaneously emits a photon and forms a negative ion in one of the lowest vibrational levels, and (ii) an indirect, or two-step pathway, in which the electron is initially captured through non-Born-Oppenheimer coupling into a vibrationally resonant excited state of the anion, which then stabilizes by radiative decay. We develop a general model to describe the second pathway and show that its contribution to the formation of cosmic anions is small in comparison to the direct mechanism. The obtained rate coefficients at 30~K are $7\times 10^{-16}$cm$^3$/s for CN$^-$, $7\times 10^{-17}$cm$^3$/s for C$_2$H$^-$, and $2\times 10^{-16}$cm$^3$/s for C$_4$H$^-$. These rates weakly depend on temperature between 10K and 100 K. The validity of our calculations is verified by comparing the present theoretical results with data from recent photodetachment experiments.

physics.chem-ph↗

arXiv2011

Theory of dissociative recombination of highly-symmetric polyatomic ions

A general first-principles theory of dissociative recombination is developed for highly-symmetric molecular ions and applied to H$_3$O$^{+}$ and CH$_3^+$, which play an important role in astrophysical, combustion, and laboratory plasma environments. The theoretical cross-sections obtained for the dissociative recombination of the two ions are in good agreement with existing experimental data from storage ring experiments.

physics.atom-ph↗

arXiv2009

Theory of dissociative recombination of a linear triatomic ion with permanent electric dipole moment: Study of HCO$^{+}$

We present a theoretical description of dissociative recombination of triatomic molecular ions having large permanent dipole moments. The study has been partly motivated by a discrepancy between experimental and theoretical cross-sections for dissociative recombination of the HCO$^+$ ion. The HCO$^{+}$ ion has a considerable permanent dipole moment ($D\approx$4 debye), which has not been taken explicitly into account in previous theoretical studies. In the present study, we include explicitly the effect of the permanent electric dipole on the dynamics of the incident electron using the generalized quantum defect theory, and we present the resulting cross section obtained. This is the first application of generalized quantum defect theory to the dissociative recombination of molecular ions.

quant-ph↗

arXiv2008

Theoretical rate of dissociative recombination of HCO$^{+}$ and DCO$^{+}$ ions

The article presents an improved theoretical description of dissociative recombination of HCO$^+$ and DCO$^+$ ions with a low energy electron. In the previous theoretical study (Phys. Rev. A {\bf 74}, 032707) on HCO$^+$, the vibrational motion along the CO coordinate was neglected. Here, all vibrational degrees of freedom, including the CO stretch coordinate, are taken into account. The theoretical dissociative recombination cross-section obtained is similar to the previous theoretical result at low collision energies ($<$0.1 eV) but somewhat larger at higher ($>$0.1 eV) energies. Therefore, the present study suggests that motion along the CO coordinate does not play a significant role in the process at low collision energies. The theoretical cross-section is still approximately 2-3 times lower than the data from a recent merged-beam experiment.

physics.chem-ph↗

arXiv2007

Correlation diagrams in collisions of three identical particles

We discuss collision of three identical particles and derive scattering selection rules from initial to final states of the particles. We use either laboratory-frame, hyperspherical, or Jacobian coordinates depending on which one is best suited to describe three different configurations of the particles: (1) three free particles, (2) a quasi-bound trimer, or (3) a dimer and a free particle. We summarize quantum numbers conserved during the collision as well as quantum numbers that are appropriate for a given configuration but may change during the scattering process. The total symmetry of the system depends on these quantum numbers. Based on the selection rules, we construct correlation diagrams between different configurations before and after a collision. In particular, we describe a possible recombination of the system into one free particle and a dimer, which can be used, for example, to identify possible decay products of quasi-stationary three-body states

physics.atom-ph↗