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The Journal of Chemical Physics

Electron-spin polarization of photoions produced through photoionization from the laser-excited triplet state of Sr

Nobuaki Yonekura, Takashi Nakajima, Yukari Matsuo, T. Kobayashi, Yoshimitsu Fukuyama

Published Jan 22, 2004• 7 citations
Publisher

Abstract

We report the detailed experimental study on the production of electron-spin-polarized Sr+ ions through one-photon resonant two-photon ionization via laser-excited 5s5p 3P1 (MJ = +1) of Sr atoms produced by laser-ablation. We have experimentally confirmed that the use of laser-ablation for the production of Sr atoms prior to photoionization does not affect the electron-spin polarization. We have found that the degree of electron-spin polarization is 64+/-9%, which is in good agreement with our recent theoretical prediction. As we discuss in detail, we infer, from a simple analysis, that photoelectrons, being the counterpart of electron-spin-polarized Sr+ ions, have approximately the same degree of electron-spin polarization. Our experimental results demonstrate that the combined use of laser-ablation technique and pulsed lasers for photoionization would be a compact and effective way to realize a pulsed source for spin-polarized ions and electrons for the studies of various spin-dependent dynamics in chemical physics.

DOI
10.1063/1.1635818

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We report the detailed experimental study on the production of electron-spin-polarized Sr+ ions through one-photon resonant two-photon ionization via laser-excited 5s5p 3P1 (MJ = +1) of Sr atoms produced by laser-ablation. We have experimentally confirmed that the use of laser-ablation for the production of Sr atoms prior to photoionization does not affect the electron-spin polarization. We have found that the degree of electron-spin polarization is 64+/-9%, which is in good agreement with our recent theoretical prediction. As we discuss in detail, we infer, from a simple analysis, that photoelectrons, being the counterpart of electron-spin-polarized Sr+ ions, have approximately the same degree of electron-spin polarization. Our experimental results demonstrate that the combined use of laser-ablation technique and pulsed lasers for photoionization would be a compact and effective way to realize a pulsed source for spin-polarized ions and electrons for the studies of various spin-dependent dynamics in chemical physics.
We propose two realistic schemes for producing electron spin-polarized alkaline-earth ions. One of the schemes is based on one-photon resonant two-photon ionization via fine structure manifolds of triplet states, while the other is based on one-photon resonant one-photon ionization. For both schemes we find that the ionization must take place from a triplet state to produce spin-polarized photoions. Photoions produced from a singlet state are always unpolarized regardless of the laser polarization and a magnetic sublevel from which ionization takes place. We carry out specific analysis for both schemes with Sr atoms, and find 85%–90% and 66% polarizations for the former and the latter schemes, respectively, if the wavelengths and polarizations of lasers are judiciously chosen. In particular, if all the produced photoions are in the ground s state, we find an exact one-to-one correspondence between the spin-polarization of photoions and ejected photoelectrons.
We study the characteristics of one-photon resonant two-photon ionization of Sr through the spin-resolved detection of photoions by laser-induced fluorescence. In particular, the dependence of spin polarization on the wavelength and polarization of the ionization laser is experimentally investigated. By changing the polarization of the ionization laser from parallel linear to perpendicular linear with respect to the quantization axis defined by the circularly polarized pump laser, a significant difference is found in the degree of spin polarization, whereas the dependence on the laser wavelength at three different wavelengths (308, 266, and 248 nm) turns out to be very small. To understand the experimental results, we have also undertaken a theoretical analysis, which predicts consistent spin polarization with our experimental results for both parallel and perpendicular linear polarization for a given ratio of bound-free transition moment into the 5 s k s and 5 s k d continua. The ratio of the bound-free transition probabilities from the bound 5 s 5 p 3 P 1 state to the 5 s k s and 5 s k d continua is evaluated.
An experiment is reported on two-step photoionization of Cs via the 6P 3/2 intermediate state using circularly polarized radiation from a GaAs laser for the first step (8521 AA) and from an Ar-ion laser for the second step. Values for the ratio of ion production rates for right- and left-handed circular polarization in the second step and for the spin polarization of the photoelectrons are presented. The measurements are interpreted on the basis of a calculation which takes into account the hyperfine splitting of the levels involved in the first transition. A description in terms of fine-structure splitting of the 6P state is shown to be totally inadequate, even when allowing for possibly large spin-orbit effects in the continuum. The process is evaluated as a possible source of a spin-polarized electron beam.
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.
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.
We propose a scheme to produce spatially and temporally controlled spin-polarized photoelectrons by strong-field ionization of atoms. We calculate the momentum-resolved electron spin polarization from two spin-orbit coupled ionic states (J=1/2J=1/2J=1/2 and J=3/2J=3/2J=3/2) of krypton atoms in orthogonal two-color laser fields using the strong-field approximation, and obtain the instantaneous spin-polarization degree. With this scheme, the spin-up and -down photoelectrons can be well separated in the space, and the spin polarization is controlled on the sub-laser-cycle timescale. This study illustrates and reveals the mechanism of the generation of spin-polarized photoelectrons with an arbitrary spatially and temporally tailored laser field. We expect this work has implications for controlling the spatiotemporal spin polarization in strong-field physics.