Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Journal of Physics B Atomic Molecular and Optical Physics

Spin-polarized electrons produced by a sequence of two femtosecond pulses. Calculation of differential and global polarization rates

M. A. Bouchène, Sébastien Zamith, B. Girard

Published Apr 6, 2001• 16 citations
Publisher

Abstract

This paper presents a theoretical analysis of the possibilities of producing spin-polarized electrons with a sequence of two ultra-short time-delayed laser pulses. The first pulse, which is right circularly polarized, excites resonantly the fine structure n p level of potassium atoms leading to a spin-flip and thus polarizing the atom. The second pulse ionizes the system thereby resulting in spin-polarized electron release. We examine and compare several situations corresponding to different polarizations of the ionizing pulse (σ + ,σ - and π). For each case we derive analytical expressions for the angular and global electron spin-polarization rates as well as for the differential cross sections. The obtained rates can be very high (up to 100%) and can be controlled accurately on the femtosecond time scale by varying the time delay between the pulses.

DOI
10.1088/0953-4075/34/8/313

Related papers

Polarization-dependent pump-probe studies in atomic fine-structure levels: towards the production of spin-polarized electrons

Emma J. Sokell, Sébastien Zamith, M. A. Bouchène +1 more

The precession of orbital and spin angular momentum vectors has been observed in a pump-probe study of the 4P fine-structure states of atomic potassium. A femtosecond pump pulse prepared a coherent superposition of the two fine-structure components. A time-delayed probe pulse then ionized the system after it had been allowed to evolve freely. Oscillations recorded in the ion signal reflect the evolution of the orientation of the orbital and spin angular momentum due to spin-orbit coupling. This interpretation gives physical insight into the cause of the half-period phase shift observed when the relative polarizations of the laser pulses were changed from parallel to perpendicular. Finally, it is shown that these changes in the orientation of the spin momentum vector of the system can be utilized to produce highly spin-polarized free electrons on the femtosecond scale

Journal of Physics B Atomic Molecular and Optical Physics•May 16, 2000•21 citations

Control of the spin-polarization of photoelectrons/photoions using short laser pulses (Invited Paper)

Takashi Nakajima

We present a scheme to control the spin-polarization of photoelectrons/photoions using short laser pulses. It is based on the pump-probe method. By exciting fine structure manifolds of a system by the short pump pulse with a sufficient bandwidth, a superposition of fine structure states is created. After the pump pulse, the coherently superposed excited state evolves in time under the field-free condition with a period determined by the inverse of energy difference between them. In terms of the spin state, this suggests that the different spin state evolves differently in time, leading to the time-varying spin-polarization. Therefore, varying the time delay between the pump and probe pulses leads to the control of spin states upon photoionization. Specific theoretical results are presented for two-valence-electron atoms, in particular for Mg, which demonstrate that, under certain conditions, not only the degree of spin-polarization but also its polarity can be manipulated through time delay. Furthermore, we propose a new technique to accelerate the coupling time by the introduction of a dressing laser with a few ns duration. Since the underline physics is rather general and transparent, the presented scheme may be potentially applied to nanostructures such as quantum wells and quantum dots.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Apr 13, 2005•0 citations

Polarization phenomena in bichromatic ionization of Ne and Ar induced by circularly polarized VUV femtosecond pulses

A N Grum-Grzhimailo, Грызлова Елена Владимировна, Maria M. Popova

Synopsis Interference effects resulting from direct single-photon and resonant two-photon ionization of neon and argon by bichromatic circularly polarized radiation were investigated in the framework of the perturbation theory. Analytical formulas are obtained for the differential cross section of the process in multielectron noble gas atoms. The possibility of coherent control of the photoelectron angular distribution and spin polarization will be discussed.

Journal of Physics Conference Series•Jan 1, 2020•0 citations

Molecular Free Electron Vortices in Photoionization by Polarization-Tailored Ultrashort Laser Pulses

Tim Bayer, M. Wollenhaupt

Atomic and molecular free electron vortices (FEVs), characterized by their spiral-shaped momentum distribution, have recently attracted a great deal of attention due to their varied shapes and their unusual topological properties. Shortly after their theoretical prediction by the single-photon ionization (SPI) of He atoms using pairs of counterrotating circularly polarized attosecond pulses, FEVs have been demonstrated experimentally by the multiphoton ionization (MPI) of alkali atoms using single-color and bichromatic circularly polarized femtosecond pulse sequences. Recently, we reported on the analysis of the experimental results employing a numerical model based on the ab initio solution of the time-dependent Schrödinger equation (TDSE) for a two-dimensional (2D) atom interacting with a polarization-shaped ultrashort laser field. Here, we apply the 2D TDSE model to study molecular FEVs created by SPI and MPI of a diatomic molecule using polarization-tailored single-color and bichromatic femtosecond pulse sequences. We investigate the influence of the coupled electron-nuclear dynamics on the vortex formation dynamics and discuss the effect of CEP- and rotational averaging on the photoelectron momentum distribution. By analyzing how the molecular structure and dynamics is imprinted in the photoelectron spirals, we explore the potential of molecular FEVs for ultrafast spectroscopy.

Frontiers in Chemistry•Jun 2, 2022•10 citations

Electron spin polarization in strong-field ionization and the effect of spin in attoclock measurements

Felipe Morales, Jivesh Kaushal, Alexander Hartung +11 more

Summary form only given. Spin plays a fundamental role in the electronic structure of matter, from single atoms and molecules through to condensed matter. However, spin dynamics and the spin response of electrons to ultra-short, strong laser pulses has remained largely unexplored until today. In 2011 and 2013, pioneering theoretical work [1, 2] extended the fundamental PPT theory [3] to treat ionization of p+ and p” electrons by circular fields. This work predicted the sensitivity of ionization probabilities in strong field ionization using circular fields to the magnetic quantum number, showing that counter rotating electrons can tunnel ionize easier. It also predicted the possibility to obtain spin polarized electrons from strong, circularly polarized fields with a high degree of efficiency. The preference of ionization was later confirmed experimentally by [4], however, the experiment in [4] did not provide a confirmation of the spin polarization predictions.

Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)•Jun 1, 2017•0 citations

Two-photon ionization of caesium via the 62P3/2intermediate state: analysis of photoelectron spin polarization and saturation effects

Ernst H.A. Granneman, M Klewer, Marnix J. van der Wiel

The authors have investigated the two-step process 6 2 S 1/2 to 6 2 P 3/2 to (epsilon 2 S 1/2 , epsilon 2 D 3/2 , epsilon 2 D 5/2 ) in Cs for circular polarization of the radiation in both steps. Theoretical expressions are presented for the photoelectron spin polarization P z and the ion count-rate 'asymmetry' A i (ratio of ion rates for right or left circular polarization in the second step), based on the hyperfine-coupling scheme for the first step. These expressions contain ratios of the three radial matrix elements involved in the ionizing step. The experimental determination of P z and A i , for different groups of hyperfine transitions, permits an evaluation of these ratios. The experiment was performed on a Cs atomic beam using a pulsed GaAs laser at 8521 AA for the first step and a pulsed Ar-ion laser at 5017-4545 AA for the second step. Effects of saturation in the first transition are studied and optimal conditions for use of the process in a spin-polarized electron source are discussed.

Journal of Physics B Atomic and Molecular Physics•Nov 11, 1976•20 citations
This paper presents a theoretical analysis of the possibilities of producing spin-polarized electrons with a sequence of two ultra-short time-delayed laser pulses. The first pulse, which is right circularly polarized, excites resonantly the fine structure n p level of potassium atoms leading to a spin-flip and thus polarizing the atom. The second pulse ionizes the system thereby resulting in spin-polarized electron release. We examine and compare several situations corresponding to different polarizations of the ionizing pulse (σ + ,σ - and π). For each case we derive analytical expressions for the angular and global electron spin-polarization rates as well as for the differential cross sections. The obtained rates can be very high (up to 100%) and can be controlled accurately on the femtosecond time scale by varying the time delay between the pulses.
The precession of orbital and spin angular momentum vectors has been observed in a pump-probe study of the 4P fine-structure states of atomic potassium. A femtosecond pump pulse prepared a coherent superposition of the two fine-structure components. A time-delayed probe pulse then ionized the system after it had been allowed to evolve freely. Oscillations recorded in the ion signal reflect the evolution of the orientation of the orbital and spin angular momentum due to spin-orbit coupling. This interpretation gives physical insight into the cause of the half-period phase shift observed when the relative polarizations of the laser pulses were changed from parallel to perpendicular. Finally, it is shown that these changes in the orientation of the spin momentum vector of the system can be utilized to produce highly spin-polarized free electrons on the femtosecond scale
We present a scheme to control the spin-polarization of photoelectrons/photoions using short laser pulses. It is based on the pump-probe method. By exciting fine structure manifolds of a system by the short pump pulse with a sufficient bandwidth, a superposition of fine structure states is created. After the pump pulse, the coherently superposed excited state evolves in time under the field-free condition with a period determined by the inverse of energy difference between them. In terms of the spin state, this suggests that the different spin state evolves differently in time, leading to the time-varying spin-polarization. Therefore, varying the time delay between the pump and probe pulses leads to the control of spin states upon photoionization. Specific theoretical results are presented for two-valence-electron atoms, in particular for Mg, which demonstrate that, under certain conditions, not only the degree of spin-polarization but also its polarity can be manipulated through time delay. Furthermore, we propose a new technique to accelerate the coupling time by the introduction of a dressing laser with a few ns duration. Since the underline physics is rather general and transparent, the presented scheme may be potentially applied to nanostructures such as quantum wells and quantum dots.
Atomic and molecular free electron vortices (FEVs), characterized by their spiral-shaped momentum distribution, have recently attracted a great deal of attention due to their varied shapes and their unusual topological properties. Shortly after their theoretical prediction by the single-photon ionization (SPI) of He atoms using pairs of counterrotating circularly polarized attosecond pulses, FEVs have been demonstrated experimentally by the multiphoton ionization (MPI) of alkali atoms using single-color and bichromatic circularly polarized femtosecond pulse sequences. Recently, we reported on the analysis of the experimental results employing a numerical model based on the ab initio solution of the time-dependent Schrödinger equation (TDSE) for a two-dimensional (2D) atom interacting with a polarization-shaped ultrashort laser field. Here, we apply the 2D TDSE model to study molecular FEVs created by SPI and MPI of a diatomic molecule using polarization-tailored single-color and bichromatic femtosecond pulse sequences. We investigate the influence of the coupled electron-nuclear dynamics on the vortex formation dynamics and discuss the effect of CEP- and rotational averaging on the photoelectron momentum distribution. By analyzing how the molecular structure and dynamics is imprinted in the photoelectron spirals, we explore the potential of molecular FEVs for ultrafast spectroscopy.
Summary form only given. Spin plays a fundamental role in the electronic structure of matter, from single atoms and molecules through to condensed matter. However, spin dynamics and the spin response of electrons to ultra-short, strong laser pulses has remained largely unexplored until today. In 2011 and 2013, pioneering theoretical work [1, 2] extended the fundamental PPT theory [3] to treat ionization of p+ and p” electrons by circular fields. This work predicted the sensitivity of ionization probabilities in strong field ionization using circular fields to the magnetic quantum number, showing that counter rotating electrons can tunnel ionize easier. It also predicted the possibility to obtain spin polarized electrons from strong, circularly polarized fields with a high degree of efficiency. The preference of ionization was later confirmed experimentally by [4], however, the experiment in [4] did not provide a confirmation of the spin polarization predictions.
The authors have investigated the two-step process 6 2 S 1/2 to 6 2 P 3/2 to (epsilon 2 S 1/2 , epsilon 2 D 3/2 , epsilon 2 D 5/2 ) in Cs for circular polarization of the radiation in both steps. Theoretical expressions are presented for the photoelectron spin polarization P z and the ion count-rate 'asymmetry' A i (ratio of ion rates for right or left circular polarization in the second step), based on the hyperfine-coupling scheme for the first step. These expressions contain ratios of the three radial matrix elements involved in the ionizing step. The experimental determination of P z and A i , for different groups of hyperfine transitions, permits an evaluation of these ratios. The experiment was performed on a Cs atomic beam using a pulsed GaAs laser at 8521 AA for the first step and a pulsed Ar-ion laser at 5017-4545 AA for the second step. Effects of saturation in the first transition are studied and optimal conditions for use of the process in a spin-polarized electron source are discussed.