On-the-fly simulation of time-resolved fluorescence spectra and anisotropy
© 2024 Author(s). Published under an exclusive license by AIP Publishing..
We combine on-the-fly trajectory surface hopping simulations and the doorway-window representation of nonlinear optical response functions to create an efficient protocol for the evaluation of time- and frequency-resolved fluorescence (TFRF) spectra and anisotropies of the realistic polyatomic systems. This approach gives the effective description of the proper (e.g., experimental) pulse envelopes, laser field polarizations, and the proper orientational averaging of TFRF signals directly from the well-established on-the-fly nonadiabatic dynamic simulations without extra computational cost. To discuss the implementation details of the developed protocol, we chose cis-azobenzene as a prototype to simulate the time evolution of the TFRF spectra governed by its nonadiabatic dynamics. The results show that the TFRF is determined by the interplay of several key factors, i.e., decays of excited-state populations, evolution of the transition dipole moments along with the dynamic propagation, and scaling factor of the TFRF signals associated with the cube of emission frequency. This work not only provides an efficient and effective approach to simulate the TFRF and anisotropies of realistic polyatomic systems but also discusses the important relationship between the TFRF signals and the underlining nonadiabatic dynamics.
| Medienart: |
E-Artikel |
|---|
| Erscheinungsjahr: |
2024 |
|---|---|
| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:160 |
|---|---|
| Enthalten in: |
The Journal of chemical physics - 160(2024), 10 vom: 14. März |
| Sprache: |
Englisch |
|---|
| Beteiligte Personen: |
Xu, Chao [VerfasserIn] |
|---|
| Links: |
|---|
| Themen: |
|---|
| Anmerkungen: |
Date Revised 13.03.2024 published: Print Citation Status PubMed-not-MEDLINE |
|---|
| doi: |
10.1063/5.0201204 |
|---|
| funding: |
|
|---|---|
| Förderinstitution / Projekttitel: |
|
| PPN (Katalog-ID): |
NLM369670493 |
|---|
| LEADER | 01000naa a22002652 4500 | ||
|---|---|---|---|
| 001 | NLM369670493 | ||
| 003 | DE-627 | ||
| 005 | 20240313235854.0 | ||
| 007 | cr uuu---uuuuu | ||
| 008 | 240313s2024 xx |||||o 00| ||eng c | ||
| 024 | 7 | |a 10.1063/5.0201204 |2 doi | |
| 028 | 5 | 2 | |a pubmed24n1327.xml |
| 035 | |a (DE-627)NLM369670493 | ||
| 035 | |a (NLM)38477337 | ||
| 035 | |a (PII)104109 | ||
| 040 | |a DE-627 |b ger |c DE-627 |e rakwb | ||
| 041 | |a eng | ||
| 100 | 1 | |a Xu, Chao |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a On-the-fly simulation of time-resolved fluorescence spectra and anisotropy |
| 264 | 1 | |c 2024 | |
| 336 | |a Text |b txt |2 rdacontent | ||
| 337 | |a ƒaComputermedien |b c |2 rdamedia | ||
| 338 | |a ƒa Online-Ressource |b cr |2 rdacarrier | ||
| 500 | |a Date Revised 13.03.2024 | ||
| 500 | |a published: Print | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a © 2024 Author(s). Published under an exclusive license by AIP Publishing. | ||
| 520 | |a We combine on-the-fly trajectory surface hopping simulations and the doorway-window representation of nonlinear optical response functions to create an efficient protocol for the evaluation of time- and frequency-resolved fluorescence (TFRF) spectra and anisotropies of the realistic polyatomic systems. This approach gives the effective description of the proper (e.g., experimental) pulse envelopes, laser field polarizations, and the proper orientational averaging of TFRF signals directly from the well-established on-the-fly nonadiabatic dynamic simulations without extra computational cost. To discuss the implementation details of the developed protocol, we chose cis-azobenzene as a prototype to simulate the time evolution of the TFRF spectra governed by its nonadiabatic dynamics. The results show that the TFRF is determined by the interplay of several key factors, i.e., decays of excited-state populations, evolution of the transition dipole moments along with the dynamic propagation, and scaling factor of the TFRF signals associated with the cube of emission frequency. This work not only provides an efficient and effective approach to simulate the TFRF and anisotropies of realistic polyatomic systems but also discusses the important relationship between the TFRF signals and the underlining nonadiabatic dynamics | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Lin, Congru |e verfasserin |4 aut | |
| 700 | 1 | |a Peng, Jiawei |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Juanjuan |e verfasserin |4 aut | |
| 700 | 1 | |a Lin, Shichen |e verfasserin |4 aut | |
| 700 | 1 | |a Gu, Feng Long |e verfasserin |4 aut | |
| 700 | 1 | |a Gelin, Maxim F |e verfasserin |4 aut | |
| 700 | 1 | |a Lan, Zhenggang |e verfasserin |4 aut | |
| 773 | 0 | 8 | |i Enthalten in |t The Journal of chemical physics |d 1963 |g 160(2024), 10 vom: 14. März |w (DE-627)NLM042699096 |x 1089-7690 |7 nnns |
| 773 | 1 | 8 | |g volume:160 |g year:2024 |g number:10 |g day:14 |g month:03 |
| 856 | 4 | 0 | |u http://dx.doi.org/10.1063/5.0201204 |3 Volltext |
| 912 | |a GBV_USEFLAG_A | ||
| 912 | |a GBV_NLM | ||
| 951 | |a AR | ||
| 952 | |d 160 |j 2024 |e 10 |b 14 |c 03 | ||