Abstract
We introduce chiral rotational spectroscopy: a new technique that enables the determination of the orientated optical activity pseudotensor components $B_{XX}$, $B_{YY}$ and $B_{ZZ}$ of chiral molecules, in a manner that reveals the enantiomeric constitution of a sample and provides an incisive signal even for a racemate. Chiral rotational spectroscopy could find particular use in the analysis of molecules that are chiral solely by virtue of their isotopic constitution and molecules with multiple chiral centres. The principles that underpin chiral rotational spectroscopy could be exploited moreover in the search for molecular chirality in space, which, if found, might add weight to hypotheses that biological homochirality and indeed life itself are of cosmic origin. A basic design for a chiral rotational spectrometer together with a model of its functionality is given. Our proposed technique offers the more familiar polarisability components $\alpha_{XX}$, $\alpha_{YY}$ and $\alpha_{ZZ}$ as by-products, which could see it find use even for achiral molecules.
Highlights
Chirality pervades the natural world and is of particular importance to life, as the molecules that comprise living things are chiral and their chirality is crucial to their biological function [1,2,3,4]
We elucidate the basic premise of chiral rotational spectroscopy: chiral molecules illuminated by circularly polarized light yield orientated chiroptical information via their rotational spectrum
Let us emphasize that chiral rotational spectroscopy is quite distinct from these techniques, including chiral microwave three-wave mixing, and that it offers fundamentally different information about molecular chirality
Summary
Chirality pervades the natural world and is of particular importance to life, as the molecules that comprise living things are chiral and their chirality is crucial to their biological function [1,2,3,4]. (iv) distinguish clearly and in a chirally sensitive manner between subtly different molecular forms, making it useful for molecules with multiple chiral centers, the analysis of which using traditional techniques represents a serious challenge; Chiral rotational spectroscopy is distinct from another class of techniques introduced recently, in which the phase of a microwave signal is used to discriminate between opposite enantiomers [23,24,25,26,27,28,29,30,31,32] We refer to these collectively as “chiral microwave three-wave mixing.”.
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