Separating single- from multi-particle dynamics in nonlinear spectroscopy

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F23%3A10476119" target="_blank" >RIV/00216208:11320/23:10476119 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=gyBy98zTGG" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=gyBy98zTGG</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1038/s41586-023-05846-7" target="_blank" >10.1038/s41586-023-05846-7</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Separating single- from multi-particle dynamics in nonlinear spectroscopy

Popis výsledku v původním jazyce

Quantum states depend on the coordinates of all their constituent particles, with essential multi-particle correlations. Time-resolved laser spectroscopy(1) is widely used to probe the energies and dynamics of excited particles and quasiparticles such as electrons and holes(2,3), excitons(4-6), plasmons(7), polaritons(8) or phonons(9). However, nonlinear signals from single- and multiple-particle excitations are all present simultaneously and cannot be disentangled without a priori knowledge of the system(4,10). Here, we show that transient absorption-the most commonly used nonlinear spectroscopy-with N prescribed excitation intensities allows separation of the dynamics into N increasingly nonlinear contributions; in systems well-described by discrete excitations, these N contributions systematically report on zero to N excitations. We obtain clean single-particle dynamics even at high excitation intensities and can systematically increase the number of interacting particles, infer their interaction energies and reconstruct their dynamics, which are not measurable via conventional means. We extract single- and multiple-exciton dynamics in squaraine polymers(11,12) and, contrary to common assumption(6,13), we find that the excitons, on average, meet several times before annihilating. This surprising ability of excitons to survive encounters is important for efficient organic photovoltaics(14,15). As we demonstrate on five diverse systems, our procedure is general, independent of the measured system or type of observed (quasi)particle and straightforward to implement. We envision future applicability in the probing of (quasi)particle interactions in such diverse areas as plasmonics(7), Auger recombination(2) and exciton correlations in quantum dots(5,16,17), singlet fission(18), exciton interactions in two-dimensional materials(19) and in molecules(20,21), carrier multiplication(22), multiphonon scattering(9) or polariton-polariton interaction(8).

Název v anglickém jazyce

Separating single- from multi-particle dynamics in nonlinear spectroscopy

Popis výsledku anglicky

Quantum states depend on the coordinates of all their constituent particles, with essential multi-particle correlations. Time-resolved laser spectroscopy(1) is widely used to probe the energies and dynamics of excited particles and quasiparticles such as electrons and holes(2,3), excitons(4-6), plasmons(7), polaritons(8) or phonons(9). However, nonlinear signals from single- and multiple-particle excitations are all present simultaneously and cannot be disentangled without a priori knowledge of the system(4,10). Here, we show that transient absorption-the most commonly used nonlinear spectroscopy-with N prescribed excitation intensities allows separation of the dynamics into N increasingly nonlinear contributions; in systems well-described by discrete excitations, these N contributions systematically report on zero to N excitations. We obtain clean single-particle dynamics even at high excitation intensities and can systematically increase the number of interacting particles, infer their interaction energies and reconstruct their dynamics, which are not measurable via conventional means. We extract single- and multiple-exciton dynamics in squaraine polymers(11,12) and, contrary to common assumption(6,13), we find that the excitons, on average, meet several times before annihilating. This surprising ability of excitons to survive encounters is important for efficient organic photovoltaics(14,15). As we demonstrate on five diverse systems, our procedure is general, independent of the measured system or type of observed (quasi)particle and straightforward to implement. We envision future applicability in the probing of (quasi)particle interactions in such diverse areas as plasmonics(7), Auger recombination(2) and exciton correlations in quantum dots(5,16,17), singlet fission(18), exciton interactions in two-dimensional materials(19) and in molecules(20,21), carrier multiplication(22), multiphonon scattering(9) or polariton-polariton interaction(8).

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

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2023

Kód důvěrnosti údajů

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

Název periodika

Nature

ISSN

0028-0836

e-ISSN

1476-4687

Svazek periodika

616

Číslo periodika v rámci svazku

7956

Stát vydavatele periodika

GB - Spojené království Velké Británie a Severního Irska

Počet stran výsledku

13

Strana od-do

280-292

Kód UT WoS článku

000960436400001

EID výsledku v databázi Scopus

2-s2.0-85150909628