Interplay of exciton annihilation and transport in fifth order electronic spectroscopy

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F20%3A10406480" target="_blank" >RIV/00216208:11320/20:10406480 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=0~3m5dHczU" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=0~3m5dHczU</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1016/j.chemphys.2019.110433" target="_blank" >10.1016/j.chemphys.2019.110433</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Interplay of exciton annihilation and transport in fifth order electronic spectroscopy

Popis výsledku v původním jazyce

Multidimensional fifth order spectroscopy is a sophisticated and specialized tool for probing bi-exciton dynamics. The complexity of the signals emitted into +/- 2 (K) over right arrow (1) -/+ 2 (K) over right arrow (2) + (K) over right arrow3 directions calls for a detailed theoretical treatment of 2D line shapes, including both exciton-exciton annihilation and intraband relaxation dynamics. Based on a master equation formalism, we discuss the signal&apos;s temporal evolution and clearly distinguish between intraband transport within first and second exciton manifolds. We prove analytically that signatures of single exciton transport vanish from spectrally integrated signals of parallel homo-aggregates of arbitrary length, while transport within the second manifold accounts for the diffusion limitations of annihilation. In an effort to model fifth order electronic spectra of tractably small systems, we develop a dynamical model for molecular dimers and trimers. We show that fifth order two-dimensional spectroscopy allows to track and pinpoint population transfer- and annihilation dynamics of bi-excitons, without the need to perform and analyse intensity dependent experiments.

Název v anglickém jazyce

Interplay of exciton annihilation and transport in fifth order electronic spectroscopy

Popis výsledku anglicky

Multidimensional fifth order spectroscopy is a sophisticated and specialized tool for probing bi-exciton dynamics. The complexity of the signals emitted into +/- 2 (K) over right arrow (1) -/+ 2 (K) over right arrow (2) + (K) over right arrow3 directions calls for a detailed theoretical treatment of 2D line shapes, including both exciton-exciton annihilation and intraband relaxation dynamics. Based on a master equation formalism, we discuss the signal&apos;s temporal evolution and clearly distinguish between intraband transport within first and second exciton manifolds. We prove analytically that signatures of single exciton transport vanish from spectrally integrated signals of parallel homo-aggregates of arbitrary length, while transport within the second manifold accounts for the diffusion limitations of annihilation. In an effort to model fifth order electronic spectra of tractably small systems, we develop a dynamical model for molecular dimers and trimers. We show that fifth order two-dimensional spectroscopy allows to track and pinpoint population transfer- and annihilation dynamics of bi-excitons, without the need to perform and analyse intensity dependent experiments.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10300 - Physical sciences

Projekt

Výsledek vznikl pri realizaci vícero projektů. Více informací v záložce Projekty.

Návaznosti

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

Rok uplatnění

2020

Kód důvěrnosti údajů

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

Název periodika

Chemical Physics

ISSN

0301-0104

e-ISSN

—

Svazek periodika

528

Číslo periodika v rámci svazku

1

Stát vydavatele periodika

NL - Nizozemsko

Počet stran výsledku

11

Strana od-do

110433

Kód UT WoS článku

000490758300009

EID výsledku v databázi Scopus

2-s2.0-85072304988