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Vibrational response functions for multidimensional electronic spectroscopy in non-adiabatic models
Quantum Physics · Submitted 3 Oct 2022
abstract compiled · 2026-09-23 · no language-model review
The authors' main claim Here, we report analytical expressions for the response functions corresponding to a class of model systems.
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The abstract, sentence by sentence
The interplay of nuclear and electronic dynamics characterizes the multi-dimensional electronic spectra of various molecular and solid-state systems. Theoretically, the observable effect of such interplay can be accounted for by response functions. Here, we report analytical expressions for the response functions corresponding to a class of model systems. These are characterized by the coupling between the diabatic electronic states and the vibrational degrees of freedom resulting in linear displacements of the corresponding harmonic oscillators, and by nonadiabatic couplings between pairs of diabatic states. In order to derive the linear response functions, we first perform the Dyson expansion of the relevant propagators with respect to the nonadiabatic component of the Hamiltonian, then derive and expand with respect to the displacements the propagators at given interaction times, and finally provide analytical expressions for the time integrals that lead to the different contributions to the linear response function. The approach is then applied to the derivation of third-order response functions describing different physical processes: ground state bleaching, stimulated emission, excited state absorption and double quantum coherence. Comparisons between the results obtained up to sixth order in the Dyson expansion and independent numerical calculation of the response functions provide an evidence of the series convergence in a few representative cases.
background contribution method result interpretation main claim
| # | sentence | role | the authors' own work | states the main conclusion | strength |
|---|---|---|---|---|---|
| s0 | The interplay of nuclear and electronic dynamics characterizes the multi-dimensional electronic spectra of various molecular and solid-state systems. | background 1.00 | 0.06 | 0.03 | asserted 1.00 |
| s1 | Theoretically, the observable effect of such interplay can be accounted for by response functions. | background 1.00 | 0.06 | 0.04 | asserted 0.63 |
| s2 | Here, we report analytical expressions for the response functions corresponding to a class of model systems. | contribution 1.00 | 0.95 | 0.44 | asserted 1.00 |
| s3 | These are characterized by the coupling between the diabatic electronic states and the vibrational degrees of freedom resulting in linear displacements of the corresponding harmonic oscillators, and by nonadiabatic couplings between pairs of diabatic states. | method 0.51 | 0.21 | 0.07 | asserted 0.99 |
| s4 | In order to derive the linear response functions, we first perform the Dyson expansion of the relevant propagators with respect to the nonadiabatic component of the Hamiltonian, then derive and expand with respect to the displacements the propagators at given interaction times, and finally provide analytical expressions for the time integrals that lead to the different contributions to the linear response function. | method 1.00 | 0.96 | 0.07 | asserted 0.98 |
| s5 | The approach is then applied to the derivation of third-order response functions describing different physical processes: ground state bleaching, stimulated emission, excited state absorption and double quantum coherence. | contribution 0.75 | 0.95 | 0.15 | asserted 1.00 |
| s6 | Comparisons between the results obtained up to sixth order in the Dyson expansion and independent numerical calculation of the response functions provide an evidence of the series convergence in a few representative cases. | result 0.92 | 0.94 | 0.23 | asserted 0.75 |
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Original abstract
The interplay of nuclear and electronic dynamics characterizes the multi-dimensional electronic spectra of various molecular and solid-state systems. Theoretically, the observable effect of such interplay can be accounted for by response functions. Here, we report analytical expressions for the response functions corresponding to a class of model systems. These are characterized by the coupling between the diabatic electronic states and the vibrational degrees of freedom resulting in linear displacements of the corresponding harmonic oscillators, and by nonadiabatic couplings between pairs of diabatic states. In order to derive the linear response functions, we first perform the Dyson expansion of the relevant propagators with respect to the nonadiabatic component of the Hamiltonian, then derive and expand with respect to the displacements the propagators at given interaction times, and finally provide analytical expressions for the time integrals that lead to the different contributions to the linear response function. The approach is then applied to the derivation of third-order response functions describing different physical processes: ground state bleaching, stimulated emission, excited state absorption and double quantum coherence. Comparisons between the results obtained up to sixth order in the Dyson expansion and independent numerical calculation of the response functions provide an evidence of the series convergence in a few representative cases.
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