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arXiv:2006.07408 · Physical Review Letters

Using Circular Dichroism to Control Energy Transfer in Multiphoton Ionization

A. H. N. C. De Silva, David Atri-Schuller, Santwana Dubey, B. P. Acharya, K. L. Romans, K. Foster, O. Russ, Katrina Compton, Cole Rischbieter, Nicolas Douguet, Klaus Bartschat, D. Fischer

Published Jan 12, 2021• 38 citations
arXivHTMLPDF

Abstract

Chirality causes symmetry breaks in a large variety of natural phenomena ranging from particle physics to biochemistry. We investigate one of the simplest conceivable chiral systems, a laser-excited, oriented, effective one-electron Li target. Prepared in a polarized p state with |m|=1 in an optical trap, the atoms are exposed to co- and counterrotating circularly polarized femtosecond laser pulses. For a field frequency near the excitation energy of the oriented initial state, a strong circular dichroism is observed and the photoelectron energies are significantly affected by the helicity-dependent Autler-Townes splitting. Besides its fundamental relevance, this system is suited to create spin-polarized electron pulses with a reversible switch on a femtosecond timescale at an energy resolution of a few meV.

DOI
10.1103/physrevlett.126.023201

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Chirality causes symmetry breaks in a large variety of natural phenomena ranging from particle physics to biochemistry. We investigate one of the simplest conceivable chiral systems, a laser-excited, oriented, effective one-electron Li target. Prepared in a polarized p state with |m|=1 in an optical trap, the atoms are exposed to co- and counterrotating circularly polarized femtosecond laser pulses. For a field frequency near the excitation energy of the oriented initial state, a strong circular dichroism is observed and the photoelectron energies are significantly affected by the helicity-dependent Autler-Townes splitting. Besides its fundamental relevance, this system is suited to create spin-polarized electron pulses with a reversible switch on a femtosecond timescale at an energy resolution of a few meV.
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 theoretically investigate the resonant two-photon ionization of a hydrogen atom in the counter-rotating circularly polarized double-pulse sequences, by solving the time-dependent Schr\"odinger equation. Due to the induced Rabi oscillations between the ground and excited states, the well-known Autler-Townes doublet is observed in the photoelectron spectra. More interestingly, our numerical results reveal an additional peak located between the Autler-Townes doublets, which originates from single-photon ionization from the excited state by the second pulse. By adjusting the laser intensity of the two pulses, the photoelectron yields of the three peaks can be sensitively modulated, under the control of completed Rabi cycles within the first pulse. In addition, our results show a potential of manipulating the photoemission anisotropy by both the laser intensity and the two-pulse time delay, through adjusting the competition of different partial waves generated by the two pulses.
We consider few-photon ionization of atomic lithium by linearly polarized femtosecond laser pulses and demonstrate that asymmetries of the electron angular distribution can occur for initially polarized (2p,(2p,(2p, mmm=+1)+1)+1) target atoms. The dependence of the photoelectron emission angle relative to the electric field direction is investigated at different laser intensities and wavelengths. The experimental spectra show excellent agreement with numerical solutions of the time-dependent Schr\"odinger equation. In the perturbative picture, the angular shift is traced back to interferences between partial waves with mean magnetic quantum number $\ensuremath{\langle}m\ensuremath{\rangle}\ensuremath{\ne}0$. This observation allows us to obtain quantum mechanical information on the final electronic state.
Scalar spin chirality, a three-body spin correlation that breaks time-reversal symmetry, is revealed to couple directly to circularly polarized laser. This is shown by the Floquet formalism for the periodically driven repulsive Hubbard model with a strong-coupling expansion. A systematic derivation of the effective low-energy Hamiltonian for a spin degree of freedom reveals that the coupling constant for scalar spin chirality can become significant for a situation in which the driving frequency and the on-site interaction are comparable. This implies that the scalar chirality can be induced by circularly polarized lights, or that it can be used conversely for probing the chirality in Mott insulators as a circular dichroism.
We investigate two-pathway interferences between nonresonant one-photon and resonant two-photon ionization of atomic hydrogen. In particular, we analyze in detail the photoionization mediated by the fundamental frequency and the second harmonic of a femtosecond VUV pulse when the fundamental is tuned near an intermediate atomic state. Following our recent study [Phys. Rev. A 91, 063418 (2015)] of such effects with linearly polarized light, we analyze a similar situation with circularly polarized radiation. As a consequence of the richer structure in circularly polarized light, characterized by its right-handed or left-handed helicity, we present and discuss various important features associated with the photoelectron angular distribution.