Abstract
Chiral molecules that are non-superimposable mirror images of each other, known as enantiomers, have identical chemical and physical properties unless they interact with another chiral entity, such as chiral light. Chiroptical1 effects arising from such interactions are used to detect enantiomers in mixtures and to induce enantioselective synthesis and catalysis. Chiroptical effects often arise from the interplay between light-induced electric- and magnetic-dipole transitions in a molecule and evolve on ultrafast electronic timescales. Here we use high-harmonic generation2,3 from a randomly oriented gas of molecules subjected to an intense laser field, to probe chiral interactions on these sub-femtosecond timescales. We show that a slight disparity in the laser-driven electron dynamics in the two enantiomers is recorded and amplified by several orders of magnitude in the harmonic spectra. Our work shows that chiroptical detection can go beyond detecting chiral structure4,5,6,7 to resolving and controlling chiral dynamics on electronic timescales.
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Acknowledgements
Experiments on epoxypropane were performed at Advanced Laser Light Source in Montreal. We thank A. Laramée and F. Poitras for their technical expertise. Experiments on fenchone were performed at CELIA, Université de Bordeaux, Talence. We thank E. Constant, E. Cormier and E. Mével for providing key apparatus used in the experiment. We thank M. Y. Ivanov, L. Nahon and M. Spanner for fruitful discussions. We acknowledge financial support from Natural Science and Engineering Research Council of Canada, Canadian Foundation for Innovation, Canada Research Chairs, FRQNT, MDEIE, CIPI, CFI, ANR (ANR-08-JCJC-0029 HarMoDyn), the Conseil Regional d’Aquitaine (20091304003 ATTOMOL and 2.1.3-09010502 COLA2), the European Union (Laserlab), the European COST Action CM1204 XLIC, the EU Marie Curie ITN network CORINF, Grant Agreement No. 264951, and the support of Einstein foundation project A-211-55 Attosecond Electron Dynamics.
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R.C. and A.E.B. contributed equally to the experimental work. A.E.B. and V.R.B. designed experiments on epoxypropane and analysed the data; A.E.B., M.C.H.W. and A.F.A., in collaboration with B.E.S., N.T. and F.L., performed experiments on epoxypropane at ALLS. R.C., B.F., A.F., J.H., H.R., N.T., V.B. and Y.M. designed, conducted and analysed the fenchone measurements. D.D. and S.Petit operated the laser system at CELIA. J.S. and B.P. performed the TDSE calculations for the model chiral molecules and analysed the type-I mechanism of cHHG. S.Patchkovskii proposed and analysed the type-I mechanism of cHHG and performed quantum chemical calculations for epoxypropane and fenchone. O.S. proposed and analysed the type-II mechanism of cHHG and the reconstruction of the time-dependent chiral response. All authors contributed to writingthe manuscript.
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Cireasa, R., Boguslavskiy, A., Pons, B. et al. Probing molecular chirality on a sub-femtosecond timescale. Nature Phys 11, 654–658 (2015). https://doi.org/10.1038/nphys3369
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DOI: https://doi.org/10.1038/nphys3369
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