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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 (Verlagsversion), 833KB
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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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Supplemental material. -The file contains technical details on the methodology, as well as some additional results.
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externe Referenz:
https://dx.doi.org/10.1103/PhysRevResearch.3.L032006 (Verlagsversion)
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https://arxiv.org/abs/2010.14182 (Preprint)
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Urheber

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 Urheber:
Neufeld, O.1, 2, Autor           
Hübener, H.1, Autor           
Rubio, A.1, 3, Autor           
de Giovannini, U.1, 4, Autor           
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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 Zusammenfassung: 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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Sprache(n): eng - English
 Datum: 2020-10-022021-06-112021-07-062021-07
 Publikationsstatus: Erschienen
 Seiten: -
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1103/PhysRevResearch.3.L032006
arXiv: 2010.14182
 Art des Abschluß: -

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Projektname : We thank Shaked Rozen from Weisman Institute, Israel, and Bernard Pons from Université Bordeaux, France, for helpful discussions. We acknowledge financial support from the European Research Council (Grant No. ERC-2015-AdG-694097), the Cluster of Excellence ‘CUI: Advanced Imaging of Matter’ of the Deutsche Forschungsgemeinschaft (DFG) - EXC 2056 - project ID 390715994, Grupos Consolidados (IT1249-19), partially supported by the Federal Ministry of Education and Research Grant RouTe-13N14839, the SFB925 “Light induced dynamics and control of correlated quantum systems”. The Flatiron Institute is a division of the Simons Foundation. O.N. gratefully acknowledges the support of the Adams Fellowship Program of the Israel Academy of Sciences and Humanities and support from the Alexander von Humboldt foundation.
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Quelle 1

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Titel: Physical Review Research
Genre der Quelle: Zeitschrift
 Urheber:
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Ort, Verlag, Ausgabe: College Park, Maryland, United States : American Physical Society (APS)
Seiten: - Band / Heft: 3 (3) Artikelnummer: L032006 Start- / Endseite: - Identifikator: ISSN: 2643-1564
CoNE: https://pure.mpg.de/cone/journals/resource/2643-1564