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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

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

Felipe Morales, Jivesh Kaushal, Alexander Hartung, M. Kunitski, K. Henrichs, Alina Laucke, Martin Richter, T. Jahnke, Anton Kalinin, Markus S Schöffler, Lothar Ph. H. Schmidt, R. Dörner, Misha Ivanov, Olga V. Smirnova

Published Jun 1, 2017• 0 citations

Abstract

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.

DOI: 10.1109/cleoe-eqec.2017.8086812

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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.

We show that ionization of noble gas atoms by a strong infrared circularly polarized laser field under standard experimental conditions can yield electrons with up to 100

%

spin polarization in energy-resolved measurements. Spin polarization arises due to the interplay of the electron-core entanglement and the sensitivity of ionization in circularly polarized fields to the sense of electron rotation in the initial state.

We study the effect of spin flip on tunneling ionization in the attoclock settings. Our study is based on a fully relativistic approach in which we seek a numerical solution of the time-dependent Dirac equation. We find that spin flip during strong field ionization significantly increases the attoclock offset angle, indicating longer tunneling delay relative to electrons with no spin flip. To interpret our numerical findings, we conduct additional modeling within the perturbative Breit-Pauli approach, which allows us to elucidate the role of different relativistic mechanisms. We show that the spin-orbit interaction is mainly responsible for the spin flip, rather than interaction with the magnetic component of the laser field. We further discuss the dynamic mechanisms of the spin-flip effect, suggesting that it takes place while the electron is still bound. Our findings indicate that the attoclock can be used to investigate electron spin-flip dynamics during the tunnel ionization process.

Attosecond chronoscopy represents a major breakthrough in the study of ultrafast phenomena and has the potential to revolutionize our understanding of the fundamental physics of matter. We theoretically investigate the spin-orientation-resolved attosecond chronoscopy for the first time by the circular RABBIT technique for Kr atoms. Due to the spin-orbit interaction and the sensitivity of ionization in circularly polarized fields to the sense of electron rotation in the initial state, the spin-resolved ionization rates of photoelectrons emitted from

^2P_{1/2}

and

^2P_{3/2}

channels can be expressed via

m

-resolved ionization rates of initial state, where

m

is the orbital magnetic quantum number. We demonstrate that the yields difference between spin-up and spin-down photoelectrons from each channel are closely associated with the different behaviors of corresponding Wigner time delay. We find that the Wigner time delay between spin-up and spin-down photoelectrons in the polarization plane can reach several tens of attoseconds in the co-rotating geometry, but a few attoseconds in the counter-rotating geometry. Our approach opens up a new avenue for probing the spin-dependent behavior of Wigner time delay, and lays the foundation for spin-orientation-resolved attosecond chronoscopy, which can be verified by the current experimental techniques.

We show how spin polarization of photoelectrons produced in strong-field ionization of noble-gas atoms can be used to detect highly unexpected electron orbits created in strong, circularly polarized near-infrared fields. In such fields, ionization is expected to generate photoelectrons rapidly moving away from the ionic core, freezing their initial spin due to the short-range nature of the spin-orbit interaction between the photoelectron and the core. However, we find clear evidence of spin flips in the photoelectron spectra at low photoelectron energies and confirm that they happen because a photoelectron has been trapped near the core. The presence of such highly unexpected orbits explains the marked deviations between the recent experimental measurements of spin polarization [Nat. Photonics 10, 526 (2016)NPAHBY1749-488510.1038/nphoton.2016.109] and simulations with frozen spin.

The ionization of the prealigned nitric oxide molecule by strong circularly polarized laser fields is studied via theoretical simulations of the spin-resolved photoelectron momentum distributions by solving numerically the three-dimensional time-dependent Schr\"odinger equation. Due to the spin-orbit entanglement in the ground state of nitric oxide and the sensitivity of the tunnel ionization of its doubly degenerate valence $2{\ensuremath{\pi}}_{\ifmmode\pm\else\textpm\fi{}}$ orbitals carrying opposite electron ring currents to the sense of the laser-field rotation, the momentum-resolved spin-polarized photoelectrons are produced. We show that the spin polarization exhibits strong dependence on the kinetic energy as well as the emitting angle of the photoelectron. In addition to the laser control, the momentum gate in strong-field experiments would enable full control of the spin polarization.

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.