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Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules
Jie Yang, Markus Guehr, Xiaozhe Shen, Renkai Li, Theodore Vecchione, Ryan Coffee, Jeff Corbett, Alan Fry, Nick Hartmann, Carsten Hast, Kareem Hegazy, Keith Jobe, Igor Makasyuk, Joseph Robinson, Matthew S. Robinson, Sharon Vetter, Stephen Weathersby, Charles Yoneda, Xijie Wang, and Martin Centurion
Phys. Rev. Lett. 117, 153002 – Published 3 October 2016
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Abstract
Observing the motion of the nuclear wave packets during a molecular reaction, in both space and time, is crucial for understanding and controlling the outcome of photoinduced chemical reactions. We have imaged the motion of a vibrational wave packet in isolated iodine molecules using ultrafast electron diffraction with relativistic electrons. The time-varying interatomic distance was measured with a precision 0.07Å and temporal resolution of 230fs full width at half maximum. The method is not only sensitive to the position but also the shape of the nuclear wave packet.
- Received 19 March 2016
DOI:https://doi.org/10.1103/PhysRevLett.117.153002
© 2016 American Physical Society
Physics Subject Headings (PhySH)
- Research Areas
Chemical reactions
- Physical Systems
Molecules
Atomic, Molecular & Optical
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Showtime for Molecular Movies
Published 3 October 2016
Molecular movies of vibrating iodine molecules have been recorded in time-resolved x-ray and electron diffraction experiments.
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Authors & Affiliations
Jie Yang1, Markus Guehr2,3,*, Xiaozhe Shen4, Renkai Li4, Theodore Vecchione4, Ryan Coffee4, Jeff Corbett4, Alan Fry4, Nick Hartmann4, Carsten Hast4, Kareem Hegazy4, Keith Jobe4, Igor Makasyuk4, Joseph Robinson4, Matthew S. Robinson1, Sharon Vetter4, Stephen Weathersby4, Charles Yoneda4, Xijie Wang4,†, and Martin Centurion1,‡
- 1University of Nebraska-Lincoln, 855 N 16th Street, Lincoln, Nebraska 68588, USA
- 2PULSE, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA
- 3Physics and Astronomy, Potsdam University, 14476 Potsdam, Germany
- 4SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA
- *Corresponding author.mguehr@uni-potsdam.de
- †Corresponding author.wangxj@slac.stanford.edu
- ‡Corresponding author.martin.centurion@unl.edu
See Also
Self-Referenced Coherent Diffraction X-Ray Movie of Ångstrom- and Femtosecond-Scale Atomic Motion
J. M. Glownia, A. Natan, J. P. Cryan, R. Hartsock, M. Kozina, M. P. Minitti, S. Nelson, J. Robinson, T. Sato, T. van Driel, G. Welch, C. Weninger, D. Zhu, and P. H. Bucksbaum
Phys. Rev. Lett. 117, 153003 (2016)
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Issue
Vol. 117, Iss. 15 — 7 October 2016
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Images
Figure 1
(a)Diagram of the experimental setup showing the laser beam (green), electron beam (blue), and gas jet (gray). (b)Potential energy surfaces of ground state (dashed blue line) and the excited state (dashed red line), along with the ground and excited state wave packets (solid lines). The blue and red colors represent ground and the excited states, respectively. (c)Simulated dynamics of the nuclear wave packet of in the state, after excitation by a 530nm laser pulse. The figure displays the amplitude of the wave function as a function of time, in arbitrary units.
Figure 2
(a)Experimental difference diffraction pattern averaged over to 550fs. (b)Simulated difference diffraction pattern averaged over to 550fs. The color scales are in arbitrary units. (c)through (f): experimental difference diffraction patterns at , , , and , respectively.
Figure 3
(a),(b)The experimental (a) and simulated (b)time-resolved modified scattering intensity difference . (c), (d)The experimental (c) and simulated (d)time-resolved modified scattering intensity of the excited state . The pattern in (c)was generated by adding the known contribution from ground state to the experimental pattern in (a). The pattern in (d)was generated by adding the known contribution from ground state to the simulated pattern in (b). The experiment misses values between 0 and (area underneath the white dashed line in each pattern) due to a hole in the detector that serves to transmit the main electron beam.
Figure 4
(a)Time-resolved experimental (blue circles with error bars) and simulated (red dashed line) bond lengths from a single sine fit of . (b)The experimental (left panel) and simulated (right panel) time-resolved probability density function of the wave packet, , calculated using Eq.(5). The dashed red line is the results of the theoretical calculation with the same spatial resolution as the experiment, and the solid green line includes also averaging due to the temporal resolution (230fs). The black dotted line indicates the baseline for each curve.
