Non-adiabatic quantum electrodynamic effects on electron–nucleus–photon systems: Single photonic mode vs infinite photonic modes DOI
Chih‐En Shen, Hung-Sheng Tsai, Liang‐Yan Hsu

et al.

The Journal of Chemical Physics, Journal Year: 2025, Volume and Issue: 162(3)

Published: Jan. 15, 2025

The quantum-electrodynamic non-adiabatic emission (QED-NAE) is a type of radiatively assisted vibronic de-excitation due to electromagnetic vacuum fluctuations on processes. Building our previous work [Tsai et al., J. Phys. Chem. Lett. 14, 5924 (2023)], we extend the theory QED-NAE rate from single cavity photonic mode infinite modes and calculate rates 9-cyanoanthracene at first-principles level. To avoid confusion, quantum electrodynamic internal conversion process renamed as "QED-NAE" in present work. According theory, identify three key factors influencing processes: light-matter coupling strength (mode volume), mass-weighted orientation factor, density states. volume primary factor causing differences between two scenarios. In with small volume, strong boosts rates. contrast, free space modes, weak significantly reduces these From only causes an 8π/3-fold increase rate. space, state exhibits flat quadratic distribution, which slightly Our study shows that cavities can enhance QED effects while providing robust analysis demonstrating be safely ignored space.

Language: Английский

Non-adiabatic quantum electrodynamic effects on electron–nucleus–photon systems: Single photonic mode vs infinite photonic modes DOI
Chih‐En Shen, Hung-Sheng Tsai, Liang‐Yan Hsu

et al.

The Journal of Chemical Physics, Journal Year: 2025, Volume and Issue: 162(3)

Published: Jan. 15, 2025

The quantum-electrodynamic non-adiabatic emission (QED-NAE) is a type of radiatively assisted vibronic de-excitation due to electromagnetic vacuum fluctuations on processes. Building our previous work [Tsai et al., J. Phys. Chem. Lett. 14, 5924 (2023)], we extend the theory QED-NAE rate from single cavity photonic mode infinite modes and calculate rates 9-cyanoanthracene at first-principles level. To avoid confusion, quantum electrodynamic internal conversion process renamed as "QED-NAE" in present work. According theory, identify three key factors influencing processes: light-matter coupling strength (mode volume), mass-weighted orientation factor, density states. volume primary factor causing differences between two scenarios. In with small volume, strong boosts rates. contrast, free space modes, weak significantly reduces these From only causes an 8π/3-fold increase rate. space, state exhibits flat quadratic distribution, which slightly Our study shows that cavities can enhance QED effects while providing robust analysis demonstrating be safely ignored space.

Language: Английский

Citations

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