Unraveling the competition between charge and energy transfer in 0D/2D nanographene-graphene heterojunctions

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989100%3A27740%2F25%3A10256592" target="_blank" >RIV/61989100:27740/25:10256592 - isvavai.cz</a>

Výsledek na webu

<a href="https://link.springer.com/article/10.1007/s00214-024-03166-1" target="_blank" >https://link.springer.com/article/10.1007/s00214-024-03166-1</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1007/s00214-024-03166-1" target="_blank" >10.1007/s00214-024-03166-1</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Unraveling the competition between charge and energy transfer in 0D/2D nanographene-graphene heterojunctions

Popis výsledku v původním jazyce

The charge and energy transfer processes in photoexcited 0D/2D donor/graphene heterojunctions occur through multiple different pathways. A donor deexcitation event occurring in the most prevalent Förster energy transfer mechanism (strongly favored over Dexter transfer in van der Waals heterojunctions) prevents charge transfer from taking place, thus creating a competition between the two processes. By applying a robust computational approach, we describe the two processes from first principles and quantify their rates using Förster and Marcus theories. We consider nanojunctions where the donor are nanographenes with varying size and symmetry, and discern important trends, e.g., the symmetry-induced quenching, or the enhancement due to increased size. We observe that heterojunctions where nanographenes do not have a center of symmetry show decreased photoinduced hole and energy transfer rates, which can then be recovered by increasing the delocalization length, whereas for centrosymmetric nanographenes both hole and energy transfer processes are enhanced. Nevertheless, the hole transfer rate dominates over the energy transfer process, providing a new computation-driven design principle for obtaining a high-charge transfer junction with minimized contribution of the competing energy transfer. © The Author(s) 2024.

Název v anglickém jazyce

Unraveling the competition between charge and energy transfer in 0D/2D nanographene-graphene heterojunctions

Popis výsledku anglicky

The charge and energy transfer processes in photoexcited 0D/2D donor/graphene heterojunctions occur through multiple different pathways. A donor deexcitation event occurring in the most prevalent Förster energy transfer mechanism (strongly favored over Dexter transfer in van der Waals heterojunctions) prevents charge transfer from taking place, thus creating a competition between the two processes. By applying a robust computational approach, we describe the two processes from first principles and quantify their rates using Förster and Marcus theories. We consider nanojunctions where the donor are nanographenes with varying size and symmetry, and discern important trends, e.g., the symmetry-induced quenching, or the enhancement due to increased size. We observe that heterojunctions where nanographenes do not have a center of symmetry show decreased photoinduced hole and energy transfer rates, which can then be recovered by increasing the delocalization length, whereas for centrosymmetric nanographenes both hole and energy transfer processes are enhanced. Nevertheless, the hole transfer rate dominates over the energy transfer process, providing a new computation-driven design principle for obtaining a high-charge transfer junction with minimized contribution of the competing energy transfer. © The Author(s) 2024.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

—

Návaznosti

O - Projekt operacniho programu

Rok uplatnění

2025

Kód důvěrnosti údajů

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

Název periodika

Theoretical Chemistry Accounts

ISSN

1432-881X

e-ISSN

1432-2234

Svazek periodika

144

Číslo periodika v rámci svazku

1

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

10

Strana od-do

14

Kód UT WoS článku

001385148100001

EID výsledku v databázi Scopus

2-s2.0-85213261328