Excited-State Vibration-Polariton Transitions and Dynamics in Nitroprusside Article Swipe
Andrea B. Grafton
,
Adam D. Dunkelberger
,
Blake S. Simpkins
,
Johan F. Triana
,
Federico J. Hernández
,
Felipe Herrera
,
Jeffrey C. Owrutsky
·
YOU?
·
· 2020
· Open Access
·
· DOI: https://doi.org/10.26434/chemrxiv.12518555
YOU?
·
· 2020
· Open Access
·
· DOI: https://doi.org/10.26434/chemrxiv.12518555
Strong cavity coupling to molecular vibrations creates vibration-polaritons capable of modifying chemical reaction kinetics, product branching ratios, and charge transfer equilibria. However, the mechanisms impacting these molecular processes remain elusive. Furthermore, even basic elements determining the spectral properties of polaritons, such as selection rules, transition moments, and lifetimes, are poorly understood. Here, we use two-dimensional infrared and filtered pump–probe spectroscopy to report clear spectroscopic signatures and relaxation dynamics of excited vibration-polaritons formed from the cavity- coupled NO band of nitroprusside. We apply a multi-level quantum Rabi model that predicts transition frequencies and strengths that agree very well with our experiment. Notably, the polariton features decay ~3-4 times slower than the polariton dephasing time, indicating that they support incoherent population, a consequence of their partial matter character. Understanding the factors determining polariton population and dephasing lifetimes will impact polariton-modified energy transfer, photophysics, and chemistry.
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- Type
- preprint
- Language
- en
- Landing Page
- https://doi.org/10.26434/chemrxiv.12518555
- OA Status
- gold
- Cited By
- 1
- Related Works
- 10
- OpenAlex ID
- https://openalex.org/W4249836112
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Raw OpenAlex JSON
- OpenAlex ID
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https://openalex.org/W4249836112Canonical identifier for this work in OpenAlex
- DOI
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https://doi.org/10.26434/chemrxiv.12518555Digital Object Identifier
- Title
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Excited-State Vibration-Polariton Transitions and Dynamics in NitroprussideWork title
- Type
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preprintOpenAlex work type
- Language
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enPrimary language
- Publication year
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2020Year of publication
- Publication date
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2020-06-23Full publication date if available
- Authors
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Andrea B. Grafton, Adam D. Dunkelberger, Blake S. Simpkins, Johan F. Triana, Federico J. Hernández, Felipe Herrera, Jeffrey C. OwrutskyList of authors in order
- Landing page
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https://doi.org/10.26434/chemrxiv.12518555Publisher landing page
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YesWhether a free full text is available
- OA status
-
goldOpen access status per OpenAlex
- OA URL
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https://doi.org/10.26434/chemrxiv.12518555Direct OA link when available
- Concepts
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Polariton, Dephasing, Excited state, Rabi cycle, Population, Chemistry, Excitation, Relaxation (psychology), Atomic physics, Physics, Molecular physics, Chemical physics, Condensed matter physics, Quantum, Quantum mechanics, Sociology, Demography, Social psychology, PsychologyTop concepts (fields/topics) attached by OpenAlex
- Cited by
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1Total citation count in OpenAlex
- Citations by year (recent)
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2020: 1Per-year citation counts (last 5 years)
- Related works (count)
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10Other works algorithmically related by OpenAlex
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| abstract_inverted_index.consequence | 123 |
| abstract_inverted_index.determining | 37, 132 |
| abstract_inverted_index.equilibria. | 23 |
| abstract_inverted_index.experiment. | 102 |
| abstract_inverted_index.frequencies | 93 |
| abstract_inverted_index.multi-level | 86 |
| abstract_inverted_index.polaritons, | 42 |
| abstract_inverted_index.population, | 121 |
| abstract_inverted_index.understood. | 53 |
| abstract_inverted_index.</div> | 147, 148, 149 |
| abstract_inverted_index.Furthermore, | 33 |
| abstract_inverted_index.pump–probe | 61 |
| abstract_inverted_index.spectroscopy | 62 |
| abstract_inverted_index.Understanding | 129 |
| abstract_inverted_index.photophysics, | 143 |
| abstract_inverted_index.spectroscopic | 66 |
| abstract_inverted_index.nitroprusside. | 82 |
| abstract_inverted_index.<p>Strong | 3 |
| abstract_inverted_index.two-dimensional | 57 |
| abstract_inverted_index.polariton-modified | 140 |
| abstract_inverted_index.vibration-polaritons | 10, 73 |
| cited_by_percentile_year.max | 94 |
| cited_by_percentile_year.min | 89 |
| countries_distinct_count | 1 |
| institutions_distinct_count | 7 |
| sustainable_development_goals[0].id | https://metadata.un.org/sdg/7 |
| sustainable_development_goals[0].score | 0.8600000143051147 |
| sustainable_development_goals[0].display_name | Affordable and clean energy |
| citation_normalized_percentile.value | 0.58131821 |
| citation_normalized_percentile.is_in_top_1_percent | False |
| citation_normalized_percentile.is_in_top_10_percent | False |