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 remain an important goal of the field to peer beneath broadened and obscured spectral features with coherent methods.
“Multidimensional spectroscopies [223] remain an important goal of the field to peer beneath broadened and obscured spectral features with coherent methods.”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [223]
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Molecular Chirality and Its Monitoring by Ultrafast X-ray Pulses
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Self-citationControllable X-Ray Pulse Trains from Enhanced Self-Amplified Spontaneous Emission
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Excited-state vibronic wave-packet dynamics in H 2 probed by XUV transient four-wave mixing
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Zhang, Y. A., Hua, W., Bennett, K., & Mukamel, S. (2014) · Topics in current chemistry · doi:10.1007/128_2014_618 · Cited by 42 · see citing works
Self-citationX-ray Raman scattering: a building block for nonlinear spectroscopy
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Nonlinear XUV signal generation probed by transient grating spectroscopy with attosecond pulses
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Time-, frequency-, and wavevector-resolved x-ray diffraction from single molecules
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Self-citationMultidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses
Bennett, K., Zhang, Y. A., Kowalewski, M., Hua, W., & Mukamel, S. (2016) · Physica Scripta · doi:10.1088/0031-8949/t169/1/014002 · Cited by 34 · see citing works
Self-citationTowards X-ray transient grating spectroscopy
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Two-Dimensional Impulsively Stimulated Resonant Raman Spectroscopy of Molecular Excited States
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Self-citationPhoton-recoil imaging: Expanding the view of nonlinear x-ray physics
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Free-Electron Laser Design for Four-Wave Mixing Experiments with Soft-X-Ray Pulses
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Attosecond science in atomic, molecular, and condensed matter physics
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Multidimensional high harmonic spectroscopy
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Ultrafast population transfer to excited valence levels of a molecule driven by x-ray pulses
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Attosecond single-cycle undulator light: a review
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Multidimensional x-ray spectroscopy of valence and core excitations in cysteine
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Self-citationLoe, C. M., Liekhus-Schmaltz, C. E., Govind, N., & Khalil, M. (2021) · The Journal of Physical Chemistry Letters · doi:10.1021/acs.jpclett.1c02483 · Cited by 24 · see citing works
Bidimensional electronic spectroscopy on indole in gas phase and in water from first principles
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Self-citationA Polarization Propagator for Nonlinear X-ray Spectroscopies
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Four-wave-mixing experiments with seeded free electron lasers
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Time-resolved experiments on gas-phase atoms and molecules with XUV and X-ray free-electron lasers
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Observation of site-selective chemical bond changes via ultrafast chemical shifts
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Self-citationNonlinear XUV-optical transient grating spectroscopy at the Si L2,3–edge
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Manipulating Core Excitations in Molecules by X-Ray Cavities
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Self-citationDetecting electronic coherence by multidimensional broadband stimulated x-ray Raman signals
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- 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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