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J Phys Chem Lett. 2018 Aug 16;9(16):4539-4543. doi: 10.1021/acs.jpclett.8b01815. Epub 2018 Jul 31.

State-Specific Enrichment of Chiral Conformers with Microwave Spectroscopy.

Pérez C1,2,3, Steber AL1,4,5, Krin A1,4,5, Schnell M1,4,5.

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Deutsches Elektronen-Synchrotron DESY , Notkestraße 85 , D-22607 Hamburg , Germany.
Facultad de Ciencia y Tecnología , Universidad del País Vasco (UPV-EHU) , E-48940 Leioa , Spain.
Ikerbasque, Basque Foundation for Science, E-48013 Bilbao , Spain.
Institute of Physical Chemistry , Christian-Albrechts-Universität zu Kiel , Max-Eyth-Straße 1 , D-24118 Kiel , Germany.
The Hamburg Centre for Ultrafast Imaging at the University of Hamburg , D-22761 Hamburg , Germany.


An interesting class of molecules is that in which the molecules do not possess a stereogenic center but can become chiral because of their spatial arrangement. These molecules can be seen as chiral conformers, whose two nonsuperimposable forms can interconvert from one to another by rotations about single bonds. Here, we show that an initially racemic mixture of chiral conformers, such as a sample of cyclohexylmethanol, C7H14O, can be enantiomerically enriched by performing the enantioselective process of coherent population transfer between rotational levels. By first performing a population transfer cycle, followed by a three-wave mixing experiment, we show that an enantiomeric excess in a rotational level of choice can be achieved. This represents the first experimental demonstration of such an effect in a chiral pair of conformers, and it showcases the broad applicability of three-wave mixing not only for analytical applications but also to a wide scope of experiments of fundamental interest.

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