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  Strong chiral dichroism and enantiopurification in above-threshold ionization with locally chiral light

Neufeld, O., Hübener, H., Rubio, A., & de Giovannini, U. (2021). Strong chiral dichroism and enantiopurification in above-threshold ionization with locally chiral light. Physical Review Research, 3(3): L032006. doi:10.1103/PhysRevResearch.3.L032006.

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PhysRevResearch.3.L032006.pdf (Publisher version), 833KB
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PhysRevResearch.3.L032006.pdf
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Open Access. - Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Open access publication funded by the Max Planck Society.
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SM_PRR_resub2_fin.pdf (Supplementary material), 608KB
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Supplemental material. -The file contains technical details on the methodology, as well as some additional results.
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https://arxiv.org/abs/2010.14182 (Preprint)
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 Creators:
Neufeld, O.1, 2, Author              
Hübener, H.1, Author              
Rubio, A.1, 3, Author              
de Giovannini, U.1, 4, Author              
Affiliations:
1Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
2Physics Department and Solid State Institute, Technion–Israel Institute of Technology, ou_persistent22              
3Center for Computational Quantum Physics (CCQ), The Flatiron Institute, ou_persistent22              
4IKERBASQUE, Basque Foundation for Science, ou_persistent22              

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 Abstract: We derive here a highly selective photoelectron-based chirality-sensing technique that utilizes “locally chiral” laser pulses. We show that this approach results in strong chiral discrimination, where the standard forwards/backwards asymmetry of photoelectron circular dichroism (PECD) is lifted. The resulting dichroism is larger and more robust than conventional PECD (especially in the high-energy part of the spectrum), is found in all hemispheres, and is not symmetric or antisymmetric with respect to any symmetry operator. Remarkably, chiral dichroism of up to 10% survives in the angularly integrated above-threshold ionization (ATI) spectra, and chiral dichroism of up to 5% survives in the total ionization rates. We demonstrate these results through ab initio calculations in the chiral molecules bromochlorofluoromethane, limonene, fenchone, and camphor. We also explore the parameter space of the locally chiral field and show that the observed dichroism is strongly correlated to the degree of chirality of the light, validating it as a measure for chiral-interaction strengths. Our results pave the way for highly selective probing of ultrafast chirality in ATI and motivate the use of locally chiral light for enhancing ultrafast spectroscopies. Most importantly, the technique can be implemented to achieve all-optical enantiopurification of chiral samples.

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Language(s): eng - English
 Dates: 2020-10-022021-06-112021-07-062021-07
 Publication Status: Published in print
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 Rev. Type: Peer
 Identifiers: DOI: 10.1103/PhysRevResearch.3.L032006
arXiv: 2010.14182
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Title: Physical Review Research
Source Genre: Journal
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Publ. Info: College Park, Maryland, United States : American Physical Society (APS)
Pages: - Volume / Issue: 3 (3) Sequence Number: L032006 Start / End Page: - Identifier: ISSN: 2643-1564
CoNE: https://pure.mpg.de/cone/journals/resource/2643-1564