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arXiv:1510.01092 · Physical Review A

Opportunities for detecting ring currents using an attoclock setup

Jivesh Kaushal, Felipe Morales, Olga V. Smirnova

Published Dec 7, 2015• 41 citations
arXivHTMLPDF

Abstract

Strong field ionization by circularly polarized laser fields from initial states with internal orbital momentum has an interesting propensity rule: electrons counter-rotating with respect to the laser field can be liberated more easily than co-rotating electrons [Barth and Smirnova, Phys. Rev. A 84, 063415 (2011)]. Here we show that application of few-cycle IR pulses allows one to use this propensity rule to detect ring currents associated with such quantum states, by observing angular shifts of the ejected electrons. Such shifts present the main observable of the attoclock method. We use time-dependent analytical $R$-matrix theory to show that the attoclock measured angular shifts of an electron originating from two counter-rotating orbitals (${p}^{+}$ and ${p}^{\ensuremath{-}}$) are noticeably different. Our work opens opportunities for detecting ring currents excited in atoms and molecules, using the attoclock setup.

DOI
10.1103/physreva.92.063405

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Strong field ionization by circularly polarized laser fields from initial states with internal orbital momentum has an interesting propensity rule: electrons counter-rotating with respect to the laser field can be liberated more easily than co-rotating electrons [Barth and Smirnova, Phys. Rev. A 84, 063415 (2011)]. Here we show that application of few-cycle IR pulses allows one to use this propensity rule to detect ring currents associated with such quantum states, by observing angular shifts of the ejected electrons. Such shifts present the main observable of the attoclock method. We use time-dependent analytical RRR-matrix theory to show that the attoclock measured angular shifts of an electron originating from two counter-rotating orbitals (p+{p}^{+}p+ and p\ensuremath−{p}^{\ensuremath{-}}p\ensuremath−) are noticeably different. Our work opens opportunities for detecting ring currents excited in atoms and molecules, using the attoclock setup.
Attosecond angular streaking (or "attoclock") is an insightful technique for probing the ultrafast electron dynamics in strong laser fields. Up until recently, this technique relied solely on an accurate measurement of the photoelectron momentum distribution and has remained restricted to atomic targets. Here, we propose a novel attosecond angular streaking scheme applicable to molecules, for which the ionic fragments of dissociative ionization are detected in the polarization plane of a close-to-circular polarized laser light. Our ionic attoclock measurements are consistent with theoretical results from a numerical solution of the time-dependent Schrödinger equation and an upper bound of 10 as on the tunneling time from the attoclock readings in the H_{2} molecule has been given, which is significantly smaller than any definitions of tunneling time available in the literatures.
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.
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 2P1/2^2P_{1/2}2P1/2​ and 2P3/2^2P_{3/2}2P3/2​ channels can be expressed via mmm-resolved ionization rates of initial state, where mmm 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 investigate few-photon ionization of lithium atoms prepared in the polarized $2p\phantom{\rule{0.16em}{0ex}}({m}_{\ensuremath{\ell}}=+1)$ state when subjected to femtosecond light pulses with left- or right-handed circular polarization at wavelengths between 665 and 920 nm. We consider whether ionization proceeds more favorably for the electric field co- or counter-rotating with the initial electronic current density. Strong asymmetries are found and quantitatively analyzed in terms of ``circular dichroism'' (CD). While the intensity dependence of the measured CD values is rather weak throughout the investigated regime, a very strong sensitivity on the center wavelength of the incoming radiation is observed. While the co-rotating situation overall prevails, the counter-rotating geometry is strongly favored around 800 nm due to the $2p\text{\ensuremath{-}}3s$ resonant transition, which can only be driven by counter-rotating fields. The observed features provide insights into the helicity dependence of light-atom interactions, and on the possible control of electron emission in atomic few-photon ionization by polarization-selective resonance enhancement.
We utilize the reconstruction of attosecond beating by interference of two-photon transitions (RABBIT) technique to study the phase of a Rabi-cycling atom using circularly polarized extreme ultraviolet and infrared (IR) fields, where the IR field induces Rabi oscillations between the 2s and 2p states of lithium. Autler-Townes splittings are observed in sidebands of the photoelectron spectra and the relative phases of outgoing electron wave packets are retrieved from the azimuthal angle. In this RABBIT scheme, more ionization pathways beyond the usual two-photon pathways are required. Our results show that the polar-angle-integrated and polar-angle-resolved RABBIT phases have different behaviors when the XUV and IR fields have co- and counter-rotating circular polarizations, which are traced back to the different ionization channels according to the selection rules in these two cases and their competition relying on the propensity rule in laser-assisted photoionization.