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Record W4282830363 · doi:10.1038/s41467-022-31008-w

Direct observation of ultrafast exciton localization in an organic semiconductor with soft X-ray transient absorption spectroscopy

2022· article· en· W4282830363 on OpenAlexfundno aff
Douglas Garratt, Lukas Misiekis, David Wood, Esben W. Larsen, Mary Matthews, Oliver Alexander, Peng Ye, Sebastian Jarosch, Clément Ferchaud, Christian Strüber, Allan S. Johnson, Artem A. Bakulin, Thomas J. Penfold, J. P. Marangos

Bibliographic record

VenueNature Communications · 2022
Typearticle
Languageen
FieldEngineering
TopicOrganic Electronics and Photovoltaics
Canadian institutionsnot available
FundersNatural Sciences and Engineering Research Council of CanadaEngineering and Physical Sciences Research CouncilLeverhulme TrustDefence Science and Technology LaboratoryResearch Councils UKMultidisciplinary University Research InitiativeRoyal SocietyAstex Pharmaceuticals
KeywordsExcitonDelocalized electronUltrafast laser spectroscopySpectroscopyPolaronMaterials scienceOrganic semiconductorUltrashort pulseSemiconductorAttosecondAbsorption (acoustics)Molecular physicsAbsorption spectroscopyOrganic solar cellOptoelectronicsAtomic physicsChemical physicsPolymerChemistryPhysicsOpticsCondensed matter physicsElectronLaser

Abstract

fetched live from OpenAlex

Abstract The localization dynamics of excitons in organic semiconductors influence the efficiency of charge transfer and separation in these materials. Here we apply time-resolved X-ray absorption spectroscopy to track photoinduced dynamics of a paradigmatic crystalline conjugated polymer: poly(3-hexylthiophene) (P3HT) commonly used in solar cell devices. The π→π * transition, the first step of solar energy conversion, is pumped with a 15 fs optical pulse and the dynamics are probed by an attosecond soft X-ray pulse at the carbon K-edge. We observe X-ray spectroscopic signatures of the initially hot excitonic state, indicating that it is delocalized over multiple polymer chains. This undergoes a rapid evolution on a sub 50 fs timescale which can be directly associated with cooling and localization to form either a localized exciton or polaron pair.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

How this classification was reachedexpand

Full frame distilled prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.186
Threshold uncertainty score0.522

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.001
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.001
Insufficient payload (model declined to judge)0.0000.000

Machine scores (provisional)

The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

Opus teacher head0.012
GPT teacher head0.231
Teacher spread0.220 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it

Classification

machine, unvalidated

Machine predicted; a candidate call from one teacher head, not a consensus.

The models applied no category: nothing in the taxonomy fit this work.
Study designBench or experimental
Domainnot available
GenreEmpirical

How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".

Quick stats

Citations41
Published2022
Admission routes1
Has abstractyes

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