Non-adiabatic quantum electrodynamic effects on electron–nucleus–photon systems: Single photonic mode vs infinite photonic modes.
| Title: | Non-adiabatic quantum electrodynamic effects on electron–nucleus–photon systems: Single photonic mode vs infinite photonic modes. |
|---|---|
| Authors: | Shen, Chih-En1,2 (AUTHOR), Tsai, Hung-Sheng1,2 (AUTHOR), Hsu, Liang-Yan1,2,3 (AUTHOR) lyhsu@gate.sinica.edu.tw |
| Source: | Journal of Chemical Physics. 1/21/2025, Vol. 162 Issue 3, p1-13. 13p. |
| Subject Terms: | *DENSITY of states |
| Abstract: | The quantum-electrodynamic non-adiabatic emission (QED-NAE) is a type of radiatively assisted vibronic de-excitation due to electromagnetic vacuum fluctuations on non-adiabatic processes. Building on our previous work [Tsai et al., J. Phys. Chem. Lett. 14, 5924 (2023)], we extend the theory of the QED-NAE rate from a single cavity photonic mode to infinite photonic modes and calculate the QED-NAE rates of 9-cyanoanthracene at the first-principles level. To avoid the confusion, the quantum electrodynamic internal conversion process is renamed as "QED-NAE" in our present work. According to our theory, we identify three key factors influencing the QED-NAE processes: light–matter coupling strength (mode volume), mass-weighted orientation factor, and photonic density of states. The mode volume is the primary factor causing rate differences between the two scenarios. In a single cavity with a small mode volume, strong light–matter coupling strength boosts QED-NAE rates. In contrast, in free space with infinite photonic modes, weak coupling strength significantly reduces these rates. From a single cavity photonic mode to infinite photonic modes, the mass-weighted orientation factor only causes an 8π/3-fold increase in the QED-NAE rate. In free space, the photonic density of state exhibits a flat and quadratic distribution, which slightly reduces the QED-NAE rate. Our study shows that cavities can significantly enhance non-adiabatic QED effects while providing a robust analysis demonstrating that QED vibronic effects can be safely ignored in free space. [ABSTRACT FROM AUTHOR] |
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| Items | – Name: Title Label: Title Group: Ti Data: Non-adiabatic quantum electrodynamic effects on electron–nucleus–photon systems: Single photonic mode vs infinite photonic modes. – Name: Author Label: Authors Group: Au Data: <searchLink fieldCode="AR" term="%22Shen%2C+Chih-En%22">Shen, Chih-En</searchLink><relatesTo>1,2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Tsai%2C+Hung-Sheng%22">Tsai, Hung-Sheng</searchLink><relatesTo>1,2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Hsu%2C+Liang-Yan%22">Hsu, Liang-Yan</searchLink><relatesTo>1,2,3</relatesTo> (AUTHOR)<i> lyhsu@gate.sinica.edu.tw</i> – Name: TitleSource Label: Source Group: Src Data: <searchLink fieldCode="JN" term="%22Journal+of+Chemical+Physics%22">Journal of Chemical Physics</searchLink>. 1/21/2025, Vol. 162 Issue 3, p1-13. 13p. – Name: Subject Label: Subject Terms Group: Su Data: *<searchLink fieldCode="DE" term="%22DENSITY+of+states%22">DENSITY of states</searchLink> – Name: Abstract Label: Abstract Group: Ab Data: The quantum-electrodynamic non-adiabatic emission (QED-NAE) is a type of radiatively assisted vibronic de-excitation due to electromagnetic vacuum fluctuations on non-adiabatic processes. Building on our previous work [Tsai et al., J. Phys. Chem. Lett. 14, 5924 (2023)], we extend the theory of the QED-NAE rate from a single cavity photonic mode to infinite photonic modes and calculate the QED-NAE rates of 9-cyanoanthracene at the first-principles level. To avoid the confusion, the quantum electrodynamic internal conversion process is renamed as "QED-NAE" in our present work. According to our theory, we identify three key factors influencing the QED-NAE processes: light–matter coupling strength (mode volume), mass-weighted orientation factor, and photonic density of states. The mode volume is the primary factor causing rate differences between the two scenarios. In a single cavity with a small mode volume, strong light–matter coupling strength boosts QED-NAE rates. In contrast, in free space with infinite photonic modes, weak coupling strength significantly reduces these rates. From a single cavity photonic mode to infinite photonic modes, the mass-weighted orientation factor only causes an 8π/3-fold increase in the QED-NAE rate. In free space, the photonic density of state exhibits a flat and quadratic distribution, which slightly reduces the QED-NAE rate. Our study shows that cavities can significantly enhance non-adiabatic QED effects while providing a robust analysis demonstrating that QED vibronic effects can be safely ignored in free space. [ABSTRACT FROM AUTHOR] – Name: AbstractSuppliedCopyright Label: Group: Ab Data: <i>Copyright of Journal of Chemical Physics is the property of American Institute of Physics and its content may not be copied or emailed to multiple sites or posted to a listserv without the copyright holder's express written permission. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.) |
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| RecordInfo | BibRecord: BibEntity: Identifiers: – Type: doi Value: 10.1063/5.0238657 Languages: – Code: eng Text: English PhysicalDescription: Pagination: PageCount: 13 StartPage: 1 Subjects: – SubjectFull: DENSITY of states Type: general Titles: – TitleFull: Non-adiabatic quantum electrodynamic effects on electron–nucleus–photon systems: Single photonic mode vs infinite photonic modes. Type: main BibRelationships: HasContributorRelationships: – PersonEntity: Name: NameFull: Shen, Chih-En – PersonEntity: Name: NameFull: Tsai, Hung-Sheng – PersonEntity: Name: NameFull: Hsu, Liang-Yan IsPartOfRelationships: – BibEntity: Dates: – D: 21 M: 01 Text: 1/21/2025 Type: published Y: 2025 Identifiers: – Type: issn-print Value: 00219606 Numbering: – Type: volume Value: 162 – Type: issue Value: 3 Titles: – TitleFull: Journal of Chemical Physics Type: main |
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