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Record W4412686967 · doi:10.1021/acs.jpcb.5c03855

Intermolecular Interactions in Crystals Modulate Intramolecular Excited State Proton Transfer Reactions

2025· article· en· W4412686967 on OpenAlexafffund
Hyein Hwang, Alasdair Mackenzie, Michał Andrzej Kochman, Marcus Gallagher-Jones, Vandana Tiwari, Simon F. Bittmann, Friedjof Tellkamp, Stanley W. Botchway, Angus I. Kirkland, Hong-Guang Duan, R. J. Dwayne Miller, Ajay Jha

Bibliographic record

VenueThe Journal of Physical Chemistry B · 2025
Typearticle
Languageen
FieldChemistry
TopicPhotochemistry and Electron Transfer Studies
Canadian institutionsUniversity of Toronto
FundersYoung Scientists FundDeutsche ForschungsgemeinschaftMax-Planck-GesellschaftNatural Sciences and Engineering Research Council of CanadaNational Natural Science Foundation of ChinaEngineering and Physical Sciences Research Council
KeywordsIntermolecular forceIntramolecular forceHydrogen bondChemical physicsProtonChemistryMolecular dynamicsRelaxation (psychology)Excited stateCrystal structureCrystal (programming language)PhotochemistryComputational chemistryCrystallographyMoleculeOrganic chemistryAtomic physics

Abstract

fetched live from OpenAlex

Proton transfer is a fundamental process underlying chemical and biological phenomena, and its dynamics are significantly influenced by the surrounding environment. This paper studies the excited state intramolecular proton transfer (ESIPT) process, which is crucial to the photostability of hydroxyanthraquinone-based pigments through efficient energy dissipation, by investigating how crystalline packing influences photoinduced proton transfer dynamics in single crystals of dihydroxyanthraquinone (DHAQ) constitutional isomers. Comparing the proton transfer dynamics in crystalline and solution phases, we show substantial differences due to the crystalline environment, particularly in the 1,4- and 1,5-DHAQ isomers. These isomers show intermolecular hydrogen bonding within the crystal lattice, resulting in larger excitonic couplings, which significantly alters their reaction pathways compared to their behavior in solution. We show that 1,8-DHAQ, which does not form intermolecular hydrogen bonds in the crystal, shows minimal changes in dynamics between the phases. In contrast, in the case of 1,4-DHAQ, intermolecular interactions within the molecular crystal phase open up an ESIPT relaxation channel, which is not observed in the solution phase. These findings highlight the critical role of crystal packing in modulating proton transfer dynamics and offer insights into how molecular packing can be strategically manipulated to control and optimize reaction pathways in solid-state environments.

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 score0.011
Threshold uncertainty score0.788

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 head0.008
GPT teacher head0.264
Teacher spread0.256 · 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

Citations2
Published2025
Admission routes2
Has abstractyes

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