Estimation of electron absorption spectra and lifetime of the two lowest singlet excited states of pyrimidine nucleobases and their derivatives

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F22%3A10438871" target="_blank" >RIV/00216208:11320/22:10438871 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=tLpjZ58CEh" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=tLpjZ58CEh</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1016/j.molstruc.2021.131863" target="_blank" >10.1016/j.molstruc.2021.131863</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Estimation of electron absorption spectra and lifetime of the two lowest singlet excited states of pyrimidine nucleobases and their derivatives

Popis výsledku v původním jazyce

Vertical absorption spectra of selected molecules (pyrimidine nucleobases and 5-azacytosin, 2-amino-1,3,5-triazine, 2,4-diamino-1,3,5-triazine, 2,4,6-triamino-1,3,5-triazine, and s-triazine) were performed using TD-DFT, post-HF, and semiempirical OM2/MNDO methods. From comparing a relatively large set of functionals from the different rungs of Jacob&apos;s DFT ladder, the important role of the exact exchange interaction is demonstrated. TD-DFT results with the omega B2GP-PLYP functional (and a few others) are comparable with the post-HF methods. An important finding is also a good accuracy of the semiempirical OM2 approximation, which is used for estimations of lifetimes of the excited states for the same set of molecules. The lifetimes&apos; determination is based on a stochastical treatment of a swarm of MD trajectories. The time-dependent Schrodinger equation is solved for the electronic degrees of freedom while the dynamics of nuclei is treated classically in each trajectory step applying Tully&apos;s fewest switch algorithm. The probability of individual states in time is determined and compared with both experimental and computational studies. Our results are in fair accord with available experiments. The nucleobases relatively quickly deactivate - all the relaxation times are below 0.5 ps (in very good accord with measured values). Much longer lifetimes (a few hundred ps) were obtained for other molecules: 5-azacytosin, 2,4-diamino-1,3,5-triazine, and 2,4,6-triamino-1,3,5-triazine. Also, in agreement with experimental data, 2-amino-1,3,5-triazine returns to the ground state on a nanosecond scale. (C) 2021 Elsevier B.V. All rights reserved.

Název v anglickém jazyce

Estimation of electron absorption spectra and lifetime of the two lowest singlet excited states of pyrimidine nucleobases and their derivatives

Popis výsledku anglicky

Vertical absorption spectra of selected molecules (pyrimidine nucleobases and 5-azacytosin, 2-amino-1,3,5-triazine, 2,4-diamino-1,3,5-triazine, 2,4,6-triamino-1,3,5-triazine, and s-triazine) were performed using TD-DFT, post-HF, and semiempirical OM2/MNDO methods. From comparing a relatively large set of functionals from the different rungs of Jacob&apos;s DFT ladder, the important role of the exact exchange interaction is demonstrated. TD-DFT results with the omega B2GP-PLYP functional (and a few others) are comparable with the post-HF methods. An important finding is also a good accuracy of the semiempirical OM2 approximation, which is used for estimations of lifetimes of the excited states for the same set of molecules. The lifetimes&apos; determination is based on a stochastical treatment of a swarm of MD trajectories. The time-dependent Schrodinger equation is solved for the electronic degrees of freedom while the dynamics of nuclei is treated classically in each trajectory step applying Tully&apos;s fewest switch algorithm. The probability of individual states in time is determined and compared with both experimental and computational studies. Our results are in fair accord with available experiments. The nucleobases relatively quickly deactivate - all the relaxation times are below 0.5 ps (in very good accord with measured values). Much longer lifetimes (a few hundred ps) were obtained for other molecules: 5-azacytosin, 2,4-diamino-1,3,5-triazine, and 2,4,6-triamino-1,3,5-triazine. Also, in agreement with experimental data, 2-amino-1,3,5-triazine returns to the ground state on a nanosecond scale. (C) 2021 Elsevier B.V. All rights reserved.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10301 - Atomic, molecular and chemical physics (physics of atoms and molecules including collision, interaction with radiation, magnetic resonances, Mössbauer effect)

Projekt

<a href="/cs/project/GAP208%2F12%2F0622" target="_blank" >GAP208/12/0622: Interakce organokovových protinádorových komplexů s nukleovými kyselinami a proteiny: studium sekvenční a substrátové selektivity</a><br>

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Rok uplatnění

2022

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Journal of Molecular Structure

ISSN

0022-2860

e-ISSN

1872-8014

Svazek periodika

1250

Číslo periodika v rámci svazku

2

Stát vydavatele periodika

NL - Nizozemsko

Počet stran výsledku

13

Strana od-do

131863

Kód UT WoS článku

000744651100005

EID výsledku v databázi Scopus

2-s2.0-85120329190