Hard X-ray helical dichroism of disordered molecular media

Chirality is a structural property of molecules lacking mirror symmetry that has strong implications in diverse fields, ranging from life sciences to materials science. Chirality-sensitive spectroscopic methods, such as circular dichroism, exhibit weak signal contributions on an achiral background....

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Bibliographic Details
Published in:Nature photonics 2022-08, Vol.16 (8), p.570-574
Main Authors: Rouxel, Jérémy R., Rösner, Benedikt, Karpov, Dmitry, Bacellar, Camila, Mancini, Giulia F., Zinna, Francesco, Kinschel, Dominik, Cannelli, Oliviero, Oppermann, Malte, Svetina, Cris, Diaz, Ana, Lacour, Jérôme, David, Christian, Chergui, Majed
Format: Article
Language:English
Subjects:
639/624/400/1106
639/638/440
639/766/36
639/766/930/527
Angular momentum
Applied and Technical Physics
Asymmetry
Chemical Physics
Chirality
Circular dichroism
Dichroism
Fresnel zones
Helicity
Iron
Linear polarization
Materials science
Optics
Physics
Physics and Astronomy
Quantum Physics
Salts
Spectra
X-rays
Zone plates
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Summary:Chirality is a structural property of molecules lacking mirror symmetry that has strong implications in diverse fields, ranging from life sciences to materials science. Chirality-sensitive spectroscopic methods, such as circular dichroism, exhibit weak signal contributions on an achiral background. Helical dichroism, which is based on the orbital angular momentum (OAM) of light, offers a new approach to probe molecular chirality, but it has never been demonstrated on disordered samples. Furthermore, in the optical domain the challenge lies in the need to transfer the OAM of the photon to an electron that is localized on an ångström-size orbital. Here we overcome this challenge using hard X-rays with spiral Fresnel zone plates, which can induce an OAM. We present the helical dichroism spectra of a disordered powder sample of enantiopure salts of the molecular complex of [Fe(4,4′-diMebpy) 3 ] 2+ at the iron K edge (7.1 keV) with OAM-carrying beams. The asymmetry ratios for the helical dichroism spectra are within one to five percent for OAM beams with topological charges of one and three. These results open a new window into the studies of molecular chirality and its interaction with the OAM of light. Linearly polarized orbital angular momentum-carrying hard X-ray beams are induced using spiral Fresnel zone plates. By sending the hard X-ray beams to disordered enantiopure molecular complexes, the helicity-dependent and chiral-sensitive signal is obtained.
ISSN:1749-4885
1749-4893
DOI:10.1038/s41566-022-01022-x