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Record W4281752390 · doi:10.1021/acs.jpclett.2c01395

Parallel versus Twisted Pentacenes: Conformational Impact on Singlet Fission

2022· article· en· W4281752390 on OpenAlexafffund
Ilias Papadopoulos, S. Rajagopala Reddy, Pedro B. Coto, Dan Lehnherr, Dominik Thiel, Michael Thoss, Rik R. Tykwinski, Dirk M. Guldi

Bibliographic record

VenueThe Journal of Physical Chemistry Letters · 2022
Typearticle
Languageen
FieldPhysics and Astronomy
TopicAdvanced Chemical Physics Studies
Canadian institutionsUniversity of Alberta
FundersNatural Sciences and Engineering Research Council of CanadaCanada Foundation for InnovationUniversity Grants CommissionBayerisches Staatsministerium für Wissenschaft und KunstDeutsche ForschungsgemeinschaftMinisterio de Ciencia, Innovación y Universidades
KeywordsPhotoexcitationSinglet fissionDelocalized electronDiacetyleneSinglet stateChemistryAbsorption (acoustics)PhotochemistryChemical physicsMolecular physicsMaterials scienceAtomic physicsExcited stateMonomerPhysicsPolymer

Abstract

fetched live from OpenAlex

We placed two pentacene chromophores at the termini of a diacetylene linker to investigate the impact of excitation wavelength, conformational flexibility, and vibronic coupling on singlet fission. Photoexcitation of the low-energy absorption results in a superposed mixture of states, which transform on an ultrafast time-scale into a spin-correlated and vibronically coupled/hot delocalized triplet pair 1(T1T1)deloc. Regardless of temperature, the lifetime for 1(T1T1)deloc is less than 2 ps. In contrast, photoexcitation of the high-energy absorption results in the formation of 1(T1T1)deloc lasting 1.0 ps, which then decays at room temperature within 4 ps via triplet–triplet annihilation. Lowering the temperature enables 1(T1T1)deloc to delocalize and vibronically decouple, in turn affording 1(T1T1)loc. In addition, our results suggest that the quasi-free rotation at the diacetylene spacer may lead to twisted conformations with very low SF quantum yields, highlighting the need of controlling this structural aspect in the design of new singlet fission active molecules.

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 score0.163
Threshold uncertainty score0.473

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
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 head0.013
GPT teacher head0.274
Teacher spread0.261 · 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

Citations18
Published2022
Admission routes2
Has abstractyes

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