Chiral topological light for detection of robust enantiosensitive observables

TY - JOUR

T1 - Chiral topological light for detection of robust enantiosensitive observables

AU - Mayer, Nicola

AU - Ayuso, David

AU - Ivanov, Misha

AU - Decleva, Piero

AU - Khokhlova, Margarita

AU - Pisanty, Emilio

AU - Smirnova, Olga

N1 - Publisher Copyright: © The Author(s) 2024.

PY - 2024/8/13

Y1 - 2024/8/13

N2 - The topological response of matter to electromagnetic fields is a highly demanded property in materials design and metrology due to its robustness against noise and decoherence, stimulating recent advances in ultrafast photonics. Embedding topological properties into the enantiosensitive optical response of chiral molecules could therefore enhance the efficiency and robustness of chiral optical discrimination. Here we achieve such a topological embedding by introducing the concept of chiral topological light—a light beam which displays chirality locally, with an azimuthal distribution of its handedness described globally by a topological charge. The topological charge is mapped onto the azimuthal intensity modulation of the non-linear optical response, where enantiosensitivity is encoded into its spatial rotation. The spatial rotation is robust against intensity fluctuations and imperfect local polarization states of the driving field. Our theoretical results show that chiral topological light enables detection of percentage-level enantiomeric excesses in randomly oriented mixtures of chiral molecules, opening a way to new, extremely sensitive and robust chiro-optical spectroscopies with attosecond time resolution.

AB - The topological response of matter to electromagnetic fields is a highly demanded property in materials design and metrology due to its robustness against noise and decoherence, stimulating recent advances in ultrafast photonics. Embedding topological properties into the enantiosensitive optical response of chiral molecules could therefore enhance the efficiency and robustness of chiral optical discrimination. Here we achieve such a topological embedding by introducing the concept of chiral topological light—a light beam which displays chirality locally, with an azimuthal distribution of its handedness described globally by a topological charge. The topological charge is mapped onto the azimuthal intensity modulation of the non-linear optical response, where enantiosensitivity is encoded into its spatial rotation. The spatial rotation is robust against intensity fluctuations and imperfect local polarization states of the driving field. Our theoretical results show that chiral topological light enables detection of percentage-level enantiomeric excesses in randomly oriented mixtures of chiral molecules, opening a way to new, extremely sensitive and robust chiro-optical spectroscopies with attosecond time resolution.

UR - http://www.scopus.com/inward/record.url?scp=85201277852&partnerID=8YFLogxK

U2 - 10.1038/s41566-024-01499-8

DO - 10.1038/s41566-024-01499-8

M3 - Article

SN - 1749-4885

JO - Nature Photonics

JF - Nature Photonics

ER -