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Multidimensional Attosecond Resonant X-Ray Spectroscopy of Molecules: Lessons from the Optical Regime
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New free-electron laser and high-harmonic generation X-ray light sources are capable of supplying pulses short and intense enough to perform resonant nonlinear time-resolved experiments in molecules. Valence-electron motions can be triggered impulsively by core excitations and monitored with high temporal and spatial resolution. We discuss possible experiments that employ attosecond X-ray pulses to probe the quantum coherence and correlations of valence electrons and holes, rather than the charge density alone, building on the analogy with existing studies of vibrational motions using femtosecond techniques in the visible regime.
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“Multidimensional spectroscopies [223] remain an important goal of the field to peer beneath broadened and obscured spectral features with coherent methods.”
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Metadata
- Authors
- Mukamel, S., Healion, D., Zhang, Y., & Biggs, J. D.
- Affiliations
- University of California, Irvine (US)
- Venue
- Annual Review of Physical Chemistry
- Publisher
- Annual Reviews
- Published
- 2013-04-01
- Volume
- 64
- Issue
- 1
- Pages
- 101-127
- ISSN
- 0066-426X (ISSN-L)
- 1545-1593
- PMC
- PMC3721744
- OpenAlex
- W2122020953
- Cited by
- 200
- References
- 162
- Citations by year
- 2026: 7 · 2025: 8 · 2024: 14 · 2023: 13 · 2022: 20 · 2021: 19 · 2020: 24 · 2019: 16 · 2018: 15 · 2017: 14 · 2016: 16 · 2015: 9 · 2014: 17 · 2013: 8
- FWCI
- 0.84
- Type
- journal article
- Language
- en
- Open access
- green
- www.ncbi.nlm.nih.gov
- Locations
- Annual Review of Physical Chemistry (publishedVersion)
- PubMed (publishedVersion)
- Europe PMC (PubMed Central) (acceptedVersion)
- PubMed Central (acceptedVersion)
- Funders
- National Science Foundation
- National Institute of General Medical Sciences (GM059230, R01GM059230)
- Topics
- 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
- Physical Sciences › Physics and Astronomy › Radiation › Advanced X-ray Imaging Techniques
- Keywords
- valence electron dynamics, core-excited states, quantum coherence, electron-hole correlation, free-electron laser, high harmonic generation, molecular dynamics
- MeSH terms
- Algorithms, Spectrometry, X-Ray Emission, Spectrum Analysis, Spectrum Analysis, Raman, X-Rays
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