Polarization-resolved core exciton dynamics in LiF using attosecond transient absorption spectroscopy Article Swipe
Kylie Gannan
,
Lorenz Drescher
,
Rafael Quintero‐Bermudez
,
Navdeep Rana
,
Chengye Huang
,
Kenneth J. Schäfer
,
Mette B. Gaarde
,
Stephen R. Leone
·
YOU?
·
· 2025
· Open Access
·
· DOI: https://doi.org/10.1103/physrevb.111.134306
YOU?
·
· 2025
· Open Access
·
· DOI: https://doi.org/10.1103/physrevb.111.134306
The ability to control absorption by modifying the polarization of light presents an exciting opportunity to experimentally determine the orbital alignment of absorption features. Here, attosecond extreme ultraviolet (XUV) transient absorption spectroscopy is used to investigate the polarization dependence of core exciton dynamics in LiF thin films at the Li+K edge. XUV pulses excite electrons from the Li 1s core level into the conduction band, allowing for the formation of a p-orbital-like core exciton, aligned along the XUV light polarization axis. A sub-5 fs near-infrared (NIR) probe pulse then arrives at variable time delays, perturbing the XUV-excited states and allowing the coherence decay of the core exciton to be mapped. The coherence lifetimes are found to be ≈2.4±0.4fs, which is attributed to a phonon-mediated dephasing mechanism as in previous core exciton studies. The differential absorption features are also shown to be sensitive to the relative polarization of the XUV and NIR fields. The parallel NIR probe induces couplings between the initial XUV-excited p-like bright exciton and s-like dark excitons. When crossed pump and probe polarizations are used, the coupling between the bright and dark states is no longer dipole-allowed, and the transient absorption signal associated with the coupling is suppressed by approximately 90%. This interpretation is supported by simulations of a few-level model system, as well as analysis of the calculated band structure. The results indicate that laser polarization can serve as a powerful experimental tool for exploring the orbital alignment of core excitonic states in solid-state materials.
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- Type
- article
- Language
- en
- Landing Page
- https://doi.org/10.1103/physrevb.111.134306
- OA Status
- gold
- Cited By
- 2
- References
- 77
- Related Works
- 10
- OpenAlex ID
- https://openalex.org/W4409870543
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Raw OpenAlex JSON
- OpenAlex ID
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https://openalex.org/W4409870543Canonical identifier for this work in OpenAlex
- DOI
-
https://doi.org/10.1103/physrevb.111.134306Digital Object Identifier
- Title
-
Polarization-resolved core exciton dynamics in LiF using attosecond transient absorption spectroscopyWork title
- Type
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articleOpenAlex work type
- Language
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enPrimary language
- Publication year
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2025Year of publication
- Publication date
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2025-04-28Full publication date if available
- Authors
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Kylie Gannan, Lorenz Drescher, Rafael Quintero‐Bermudez, Navdeep Rana, Chengye Huang, Kenneth J. Schäfer, Mette B. Gaarde, Stephen R. LeoneList of authors in order
- Landing page
-
https://doi.org/10.1103/physrevb.111.134306Publisher landing page
- Open access
-
YesWhether a free full text is available
- OA status
-
goldOpen access status per OpenAlex
- OA URL
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https://escholarship.org/uc/item/2ds948prDirect OA link when available
- Concepts
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Attosecond, Polarization (electrochemistry), Ultrafast laser spectroscopy, Exciton, Spectroscopy, Atomic physics, Absorption spectroscopy, Materials science, Physics, Molecular physics, Optics, Ultrashort pulse, Chemistry, Condensed matter physics, Laser, Quantum mechanics, Physical chemistryTop concepts (fields/topics) attached by OpenAlex
- Cited by
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2Total citation count in OpenAlex
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2025: 2Per-year citation counts (last 5 years)
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77Number of works referenced by this work
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10Other works algorithmically related by OpenAlex
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