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Imaging ultrafast molecular dynamics with laser-induced electron diffraction

Abstract

Establishing the structure of molecules and solids has always had an essential role in physics, chemistry and biology. The methods of choice are X-ray and electron diffraction, which are routinely used to determine atomic positions with sub-ångström spatial resolution. Although both methods are currently limited to probing dynamics on timescales longer than a picosecond, the recent development of femtosecond sources of X-ray pulses and electron beams suggests that they might soon be capable of taking ultrafast snapshots of biological molecules1,2 and condensed-phase systems3,4,5,6 undergoing structural changes. The past decade has also witnessed the emergence of an alternative imaging approach based on laser-ionized bursts of coherent electron wave packets that self-interrogate the parent molecular structure7,8,9,10,11. Here we show that this phenomenon can indeed be exploited for laser-induced electron diffraction10 (LIED), to image molecular structures with sub-ångström precision and exposure times of a few femtoseconds. We apply the method to oxygen and nitrogen molecules, which on strong-field ionization at three mid-infrared wavelengths (1.7, 2.0 and 2.3 μm) emit photoelectrons with a momentum distribution from which we extract diffraction patterns. The long wavelength is essential for achieving atomic-scale spatial resolution, and the wavelength variation is equivalent to taking snapshots at different times. We show that the method has the sensitivity to measure a 0.1 Å displacement in the oxygen bond length occurring in a time interval of 5 fs, which establishes LIED as a promising approach for the imaging of gas-phase molecules with unprecedented spatio-temporal resolution.

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Figure 1: The principle of laser-induced electron diffraction.
Figure 2: LIED for unaligned N 2 and O 2 molecules.

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Acknowledgements

The work at The Ohio State University and Kansas State University was performed under DOE/BES contracts DE-FG02-06ER15833 and DE-FG02-06ER15832, respectively. L.F.D. acknowledges support from the Hagenlocker chair.

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Authors

Contributions

C.I.B. and J.X. designed the experiment and performed the data analysis. C.I.B., A.D.D., E.S. and K.Z. performed the experiment. J.X. and C.D.L. performed the theoretical analysis. C.I.B., J.X., A.D.D., P.A., T.A.M., L.F.D. and C.D.L. interpreted the results and prepared the manuscript.

Corresponding author

Correspondence to Cosmin I. Blaga.

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The authors declare no competing financial interests.

Supplementary information

Supplementary Information

This file contains Supplementary Methods and Data comprising: (i) elastic differential scattering cross section retrieval from the experiment; (ii) the independent atom model used to extract internuclear distances; and (iii) an account for all the factors that could limit the femtosecond temporal resolution. This file also contains Supplementary Figures 1-4 and additional references. (PDF 1290 kb)

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Blaga, C., Xu, J., DiChiara, A. et al. Imaging ultrafast molecular dynamics with laser-induced electron diffraction. Nature 483, 194–197 (2012). https://doi.org/10.1038/nature10820

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