Journal ArticleDOI
Enantiomer-specific detection of chiral molecules via microwave spectroscopy
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TLDR
This work uses nonlinear resonant phase-sensitive microwave spectroscopy of gas phase samples in the presence of an adiabatically switched non-resonant orthogonal electric field to map the enantiomer-dependent sign of an electric dipole Rabi frequency onto the phase of emitted microwave radiation.Abstract:
Chirality plays a fundamental part in the activity of biological molecules and broad classes of chemical reactions, but detecting and quantifying it remains challenging. The spectroscopic methods of choice are usually circular dichroism and vibrational circular dichroism, methods that are forbidden in the electric dipole approximation. The resultant weak effects produce weak signals, and thus require high sample densities. In contrast, nonlinear techniques probing electric-dipole-allowed effects have been used for sensitive chiral analyses of liquid samples. Here we extend this class of approaches by carrying out nonlinear resonant phase-sensitive microwave spectroscopy of gas phase samples in the presence of an adiabatically switched non-resonant orthogonal electric field; we use this technique to map the enantiomer-dependent sign of an electric dipole Rabi frequency onto the phase of emitted microwave radiation. We outline theoretically how this results in a sensitive and species-selective method for determining the chirality of cold gas-phase molecules, and implement it experimentally to distinguish between the S and R enantiomers of 1,2-propanediol and their racemic mixture. This technique produces a large and definitive signature of chirality, and has the potential to determine the chirality of multiple species in a mixture.read more
Citations
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Journal ArticleDOI
Electromagnetic chirality: from fundamentals to nontraditional chiroptical phenomena
Jungho Mun,Minkyung Kim,Younghwan Yang,Trevon Badloe,Jincheng Ni,Yang Chen,Cheng-Wei Qiu,Junsuk Rho +7 more
TL;DR: This review presents a comprehensive overview of the theoretical aspects of chirality in light, nanostructures, and nanosystems and their chiroptical interactions and describes the strong intrinsic and extrinsic chiral properties in plasmonic nanoparticle systems.
Journal ArticleDOI
Perspective: Ultracold molecules and the dawn of cold controlled chemistry
TL;DR: A brief account of recent progress on the experimental and theoretical fronts on cold and ultracold molecules and the opportunities and challenges they provide for a fundamental understanding of bimolecular chemical reaction dynamics is presented.
Journal ArticleDOI
Quantum control of molecular rotation
TL;DR: The angular momentum of molecules is naturally quantized, time evolution is governed by a well-known Hamiltonian with only a few accurately known parameters, and transitions between rotational levels can be driven by external fields from various parts of the electromagnetic spectrum.
Journal ArticleDOI
Probing molecular chirality on a sub-femtosecond timescale
Raluca Cireasa,Raluca Cireasa,A. E. Boguslavskiy,A. E. Boguslavskiy,Bernard Pons,M. C. H. Wong,Dominique Descamps,Stéphane Petit,H. Ruf,Nicolas Thiré,Nicolas Thiré,A. Ferré,J. Suarez,J. Higuet,Bruno E. Schmidt,A. F. Alharbi,A. F. Alharbi,François Légaré,Valérie Blanchet,Valérie Blanchet,Baptiste Fabre,Serguei Patchkovskii,Olga Smirnova,Yann Mairesse,V. R. Bhardwaj +24 more
TL;DR: In this paper, the authors used high-harmonic generation from a randomly oriented gas of molecules subjected to an intense laser field, to probe chiral interactions on these sub-femtosecond timescales.
Journal ArticleDOI
Direct Determination of Absolute Molecular Stereochemistry in Gas Phase by Coulomb Explosion Imaging
M. Pitzer,Maksim Kunitski,Allan S. Johnson,Allan S. Johnson,Till Jahnke,H. Sann,Felix Sturm,Lothar Ph. H. Schmidt,Horst Schmidt-Böcking,Reinhard Dörner,Jürgen Stohner,Julia Kiedrowski,Michael Reggelin,Sebastian Marquardt,Alexander Schießer,Robert Berger,Markus Schöffler +16 more
TL;DR: A mass spectrometry approach is demonstrated that directly images the absolute configuration of individual molecules in the gas phase by cold target recoil ion momentum spectroscopy after laser ionization–induced Coulomb explosion.
References
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Journal ArticleDOI
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Journal ArticleDOI
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Peer Fischer,François Hache +1 more
TL;DR: In contrast to conventional natural optical activity phenomena, which depend linearly on the electric field strength of the optical field, the authors discuss how optical processes that are nonlinear (quadratic, cubic, and quartic) functions of the electromagnetic field strength may probe optically active centers and chiral vibrations.