Enantiosensitive steering of free-induction decay

TY - JOUR

T1 - Enantiosensitive steering of free-induction decay

AU - Khokhlova, Margarita

AU - Pisanty, Emilio

AU - Patchkovskii, Serguei

AU - Smirnova, Olga

AU - Ivanov, Misha

N1 - Funding Information: We acknowledge funding from Engineering and Physical Sciences Research Council (MURI-MIR EP/N018680/1); Deutsche Forschungsgemeinschaft (IV 152/6-2, SM 292/5-2, SPP 1840); and Horizon 2020 research and innovation (899794). M.K. acknowledges funding from the Alexander von Humboldt Foundation. E.P. acknowledges URF funding from the Royal Society. O.S. acknowledges HE ERC-2021-ADG 101054696 Ulisses. Publisher Copyright: Copyright © 2022 The Authors, some rights reserved

PY - 2022/6/15

Y1 - 2022/6/15

N2 - Chiral discrimination, a problem of vital importance, has recently become an emerging frontier in ultrafast physics, with remarkable progress achieved in multiphoton and strong-field regimes. Rydberg excitations, unavoidable in the strong-field regime and intentional for few-photon processes, arise in all these approaches. Here, we show how to harness this ubiquitous feature by introducing a new phenomenon, enantiosensitive free-induction decay, steered by a tricolor chiral field at a gentle intensity, structured in space and time. We demonstrate theoretically that an excited chiral molecule accumulates an enantiosensitive phase due to perturbative interactions with the tricolor chiral field, resulting in a spatial phase gradient steering the free-induction decay in opposite directions for opposite enantiomers. Our work introduces a general, extremely sensitive, all-optical enantiosensitive detection technique that avoids strong fields and takes full advantage of recent advances in structuring light.

AB - Chiral discrimination, a problem of vital importance, has recently become an emerging frontier in ultrafast physics, with remarkable progress achieved in multiphoton and strong-field regimes. Rydberg excitations, unavoidable in the strong-field regime and intentional for few-photon processes, arise in all these approaches. Here, we show how to harness this ubiquitous feature by introducing a new phenomenon, enantiosensitive free-induction decay, steered by a tricolor chiral field at a gentle intensity, structured in space and time. We demonstrate theoretically that an excited chiral molecule accumulates an enantiosensitive phase due to perturbative interactions with the tricolor chiral field, resulting in a spatial phase gradient steering the free-induction decay in opposite directions for opposite enantiomers. Our work introduces a general, extremely sensitive, all-optical enantiosensitive detection technique that avoids strong fields and takes full advantage of recent advances in structuring light.

UR - http://www.scopus.com/inward/record.url?scp=85132460631&partnerID=8YFLogxK

U2 - 10.1126/sciadv.abq1962

DO - 10.1126/sciadv.abq1962

M3 - Article

SN - 2375-2548

VL - 8

JO - Science Advances

JF - Science Advances

IS - 24

M1 - eabq1962

ER -