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arXiv:2103.07499 · Physical Review A

Circular dichroism in atomic resonance-enhanced few-photon ionization

A. H. N. C. De Silva, T. Moon, K. L. Romans, B. P. Acharya, Santwana Dubey, K. Foster, O. Russ, Cole Rischbieter, Nicolas Douguet, Klaus Bartschat, D. Fischer

Published May 28, 2021• 24 citations
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Abstract

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.

DOI
10.1103/physreva.103.053125

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We investigate few-photon ionization of lithium atoms prepared in the polarized 2p(m\ensuremathℓ=+1)2p\phantom{\rule{0.16em}{0ex}}({m}_{\ensuremath{\ell}}=+1)2p(m\ensuremathℓ​=+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\ensuremath-3s2p\text{\ensuremath{-}}3s2p\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 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.
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 study time delay in atomic photoionization by circularly polarized light. By considering the Li atom in an excited 2p2p2p state, we demonstrate a strong time-delay asymmetry between the photoemission of the target electrons that are co- and counter-rotating with the electromagnetic field in the polarization plane. In addition, we observe the time-delay sensitivity to the polar angle of the photoelectron emission in the polarization plane. This modulation depends on the shape and duration of the electromagnetic pulse.
Birefringence and dichroism in atomic systems are active areas of research. Circular dichroism is typically observed in chiral atoms, molecules (such as DNA), and optically asymmetric materials. These phenomena enable polarization-based selectivity and high-precision measurements with applications in optical systems, biomedical diagnostics, and advanced photonics.Meanwhile, negative refractive index materials offer exotic applications in optics and photonics, including super-resolution imaging, invisibility cloaking, and sub-wavelength imaging. Here, we identify a novel route to achieving birefringence and dichroism in a left-handed system for the first time.We investigate the optical activity of an atomic left-handed medium, analyzing the interaction of left- and right-circularly polarized light with different atomic states while incorporating local field corrections. Notably, our results demonstrate simultaneous left-handedness for both polarization states. Furthermore, we find that electric birefringence and dichroism are significantly enhanced with increasing control field strength, while magnetic birefringence and dichroism can be fully controlled via strong laser coupling.These findings have promising implications for spintronics, image transmission in metamaterials, and the development of optical switches and high-speed data transmission devices, opening new avenues in quantum optics and photonics.
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.