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.

Author information

Affiliations

  1. LCAR, Université de Toulouse, 31062, Toulouse Cedex 09, France

    • R. Cireasa
    • , N. Thiré
    •  & V. Blanchet
  2. Institut des Sciences Moléculaires d’Orsay, Université Paris Sud, 91405 Orsay Cedex, France

    • R. Cireasa
  3. University of Ottawa, 150 Louis Pasteur, Ottawa, K1N 6N5, Canada

    • A. E. Boguslavskiy
    • , M. C. H. Wong
    • , A. F. Alharbi
    •  & V. R. Bhardwaj
  4. NRC Canada, 100 Sussex Drive, Ottawa, K1A 0R6, Canada

    • A. E. Boguslavskiy
    •  & S. Patchkovskii
  5. Department of Physics, Queen’s University, 99 University Avenue Kingston, Ontario K7L 3N6, Canada

    • A. E. Boguslavskiy
  6. CELIA, Université de Bordeaux - CNRS - CEA, F33405 Talence, France

    • B. Pons
    • , D. Descamps
    • , S. Petit
    • , H. Ruf
    • , A. Ferré
    • , J. Higuet
    • , V. Blanchet
    • , B. Fabre
    •  & Y. Mairesse
  7. INRS-EMT, Advanced Laser Light Source, 1650 Lionel-Boulet Bvd, Varennes, J3X1S2, Canada

    • N. Thiré
    • , B. E. Schmidt
    •  & F. Légaré
  8. Departamento de Química, Universidad Autónoma de Madrid, E-28049 Madrid, Spain

    • J. Suarez
  9. King Abdulaziz City for Science and Technology (KACST), PO Box 6086, Riyadh 11442, Saudi Arabia

    • A. F. Alharbi
  10. Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, Max-Born-Straße 2A, 12489 Berlin, Germany

    • S. Patchkovskii
    •  & O. Smirnova

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Contributions

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.

Competing interests

The authors declare no competing financial interests.

Corresponding authors

Correspondence to O. Smirnova or Y. Mairesse or V. R. Bhardwaj.

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DOI

https://doi.org/10.1038/nphys3369

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