Self-Referenced Coherent Diffraction X-Ray Movie of Ångstrom- and Femtosecond-Scale Atomic Motion
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Time-resolved femtosecond x-ray diffraction patterns from laser-excited molecular iodine are used to create a movie of intramolecular motion with a temporal and spatial resolution of 30 fs and 0.3 Å. This high fidelity is due to interference between the nonstationary excitation and the stationary initial charge distribution. The initial state is used as the local oscillator for heterodyne amplification of the excited charge distribution to retrieve real-space movies of atomic motion on ångstrom and femtosecond scales. This x-ray interference has not been employed to image internal motion in molecules before. Coherent vibrational motion and dispersion, dissociation, and rotational dephasing are all clearly visible in the data, thereby demonstrating the stunning sensitivity of heterodyne methods.
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Rovibronic wavepackets in iodine, metal compounds in liquids and organic ring openings have all been observed with unprecedented time resolution.
“Rovibronic wavepackets in iodine, metal compounds in liquids and organic ring openings have all been observed with unprecedented time resolution [10,19,20].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [20]
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- [3]3. Extracted excited-state charge distribution vs time, for R from 2.3 to 7 ˚ A and time delays out to 2 ps. This 'movie' was extracted from β 2 ( Q,t ) (see Fig. 2) using Eqns. 1-9. Bound-state wavepacket oscillations, dissociation, and rotational dephasing are clearly visible. Letters refer to features described in the text. The scale is proportional to the excitation in the β 2 channel. Inset: Excitation path and iodine molecular potentials. A video is in Supplemental Material [21]. <!-- image --> Only the even Legendre polynomials are used because the geometry cannot break the up/down symmetry of the molecular ensemble. Contributions for n > 3 are negligible. The radial modulations in Fig. 1 are captured in the β 2 ( Q,t ) coefficient of Eq. 5, plotted in Fig. 2. This picks out scattering patterns with the symmetry of an electric dipole excitation, and contains nearly all of the timevarying portion of the total scattered signal. The largeamplitude modulations in Fig.2 are due to holographic interference between the nonstationary charge distribution of the laser-excited wavepacket and the stationary initial charge distribution. Heterodyne techniques described below allow us to deconvolve the excitation in space and plot it vs. time in Fig. 3 as a movie with femtosecond and ˚ Angstrom resolution. For time delays t < 0 the x-rays scatter from the iodine before the exciting laser arrives in the sample, and therefore the distribution is stationary and contained in the isotropic A ( Q,t ) portion of Eq.
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Roadmap of ultrafast x-ray atomic and molecular physics
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Self-citationMonitoring nonadiabatic avoided crossing dynamics in molecules by ultrafast X-ray diffraction
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- Authors
- Glownia, J. M., Natan, A., Cryan, J. P., Hartsock, R., Kozina, M., Minitti, M. P., Nelson, S., Robinson, J., Sato, T., van Driel, T., Welch, G., Weninger, C., Zhu, D., & Bucksbaum, P. H.
- Affiliations
- SLAC National Accelerator Laboratory (US)
- ORCID
- Venue
- Physical Review Letters
- Publisher
- American Physical Society (APS)
- Published
- 2016-10-03
- Volume
- 117
- Issue
- 15
- Pages
- 153003-153003
- ISSN
- 0031-9007 (ISSN-L)
- 1079-7114
- OpenAlex
- W2517509526
- Cited by
- 149
- References
- 35
- Citations by year
- 2026: 3 · 2025: 9 · 2024: 17 · 2023: 9 · 2022: 11 · 2021: 10 · 2020: 15 · 2019: 23 · 2018: 20 · 2017: 26 · 2016: 6
- FWCI
- 28.04
- Type
- journal article
- Language
- en
- Open access
- green
- arxiv.org
- Licence
- Locations
- Physical Review Letters (publishedVersion)
- PubMed (publishedVersion)
- arXiv (Cornell University) (submittedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- arXiv (Cornell University)
- Funders
- U.S. Department of Energy
- Basic Energy Sciences (DE-AC02-76SF00515)
- Office of Science
- Stanford PULSE Institute
- SLAC
- Atomic, Molecular, and Optical Science
- Linac Coherent Light Source
- Topics
- Physical Sciences › Physics and Astronomy › Radiation › Advanced X-ray Imaging Techniques
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Physics and Astronomy › Radiation › X-ray Spectroscopy and Fluorescence Analysis
- Keywords
- time-resolved X-ray diffraction, molecular iodine, intramolecular motion, X-ray interference, molecular dissociation, molecular dispersion
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