Separating single- from multi-particle dynamics in nonlinear spectroscopy
The result's identifiers
Result code in 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>
Result on the web
<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>
Alternative languages
Result language
angličtina
Original language name
Separating single- from multi-particle dynamics in nonlinear spectroscopy
Original language description
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).
Czech name
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Czech description
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Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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OECD FORD branch
10301 - Atomic, molecular and chemical physics (physics of atoms and molecules including collision, interaction with radiation, magnetic resonances, Mössbauer effect)
Result continuities
Project
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Continuities
I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace
Others
Publication year
2023
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
Nature
ISSN
0028-0836
e-ISSN
1476-4687
Volume of the periodical
616
Issue of the periodical within the volume
7956
Country of publishing house
GB - UNITED KINGDOM
Number of pages
13
Pages from-to
280-292
UT code for WoS article
000960436400001
EID of the result in the Scopus database
2-s2.0-85150909628