Nonadiabatic transition probabilities for quantum systems in electromagnetic fields : Dephasing and population relaxation due to contact with a bath
© 2023 Author(s). Published under an exclusive license by AIP Publishing..
We contrast Dirac's theory of transition probabilities and the theory of nonadiabatic transition probabilities, applied to a perturbed system that is coupled to a bath. In Dirac's analysis, the presence of an excited state |k0⟩ in the time-dependent wave function constitutes a transition. In the nonadiabatic theory, a transition occurs when the wave function develops a term that is not adiabatically connected to the initial state. Landau and Lifshitz separated Dirac's excited-state coefficients into a term that follows the adiabatic theorem of Born and Fock and a nonadiabatic term that represents excitation across an energy gap. If the system remains coherent, the two approaches are equivalent. However, differences between the two approaches arise when coupling to a bath causes dephasing, a situation that was not treated by Dirac. For two-level model systems in static electric fields, we add relaxation terms to the Liouville equation for the time derivative of the density matrix. We contrast the results obtained from the two theories. In the analysis based on Dirac's transition probabilities, the steady state of the system is not an equilibrium state; also, the steady-state population ρkk,s increases with increasing strength of the perturbation and its value depends on the dephasing time T2. In the nonadiabatic theory, the system evolves to the thermal equilibrium with the bath. The difference is not simply due to the choice of basis because the difference remains when the results are transformed to a common basis.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2023 |
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| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:158 |
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| Enthalten in: |
The Journal of chemical physics - 158(2023), 16 vom: 28. Apr. |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Jovanovski, Sara D [VerfasserIn] |
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Date Completed 27.04.2023 Date Revised 27.04.2023 published: Print Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1063/5.0138817 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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NLM356024083 |
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| 100 | 1 | |a Jovanovski, Sara D |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a Nonadiabatic transition probabilities for quantum systems in electromagnetic fields |b Dephasing and population relaxation due to contact with a bath |
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| 500 | |a Date Revised 27.04.2023 | ||
| 500 | |a published: Print | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a © 2023 Author(s). Published under an exclusive license by AIP Publishing. | ||
| 520 | |a We contrast Dirac's theory of transition probabilities and the theory of nonadiabatic transition probabilities, applied to a perturbed system that is coupled to a bath. In Dirac's analysis, the presence of an excited state |k0⟩ in the time-dependent wave function constitutes a transition. In the nonadiabatic theory, a transition occurs when the wave function develops a term that is not adiabatically connected to the initial state. Landau and Lifshitz separated Dirac's excited-state coefficients into a term that follows the adiabatic theorem of Born and Fock and a nonadiabatic term that represents excitation across an energy gap. If the system remains coherent, the two approaches are equivalent. However, differences between the two approaches arise when coupling to a bath causes dephasing, a situation that was not treated by Dirac. For two-level model systems in static electric fields, we add relaxation terms to the Liouville equation for the time derivative of the density matrix. We contrast the results obtained from the two theories. In the analysis based on Dirac's transition probabilities, the steady state of the system is not an equilibrium state; also, the steady-state population ρkk,s increases with increasing strength of the perturbation and its value depends on the dephasing time T2. In the nonadiabatic theory, the system evolves to the thermal equilibrium with the bath. The difference is not simply due to the choice of basis because the difference remains when the results are transformed to a common basis | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Mandal, Anirban |e verfasserin |4 aut | |
| 700 | 1 | |a Hunt, Katharine L C |e verfasserin |4 aut | |
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