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Decoupled molecular and inorganic framework dynamics in <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:msub><mml:mi>CH</mml:mi><mml:mn>3</mml:mn></mml:msub><mml:msub><mml:mi>NH</mml:mi><mml:mn>3</mml:mn></mml:msub><mml:msub><mml:mi>PbCl</mml:mi><mml:mn>3</mml:mn></mml:msub></mml:mrow></mml:math>

2019· article· lv· W2996096047 on OpenAlex
M. Songvilay, Zitian Wang, Victoria García Sakai, T. Guidi, M. Bari, Zuo‐Guang Ye, Guangyong Xu, Kevin L. Brown, P. M. Gehring, Christian Stock

Why this work is in the frame

A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.
fundA Canadian funder is recorded on the work.

Bibliographic record

VenuePhysical Review Materials · 2019
Typearticle
Languagelv
FieldEngineering
TopicPerovskite Materials and Applications
Canadian institutionsSimon Fraser University
FundersOffice of Naval ResearchScience and Technology Facilities CouncilEngineering and Physical Sciences Research CouncilNatural Sciences and Engineering Research Council of Canada
KeywordsTetragonal crystal systemHalideMaterials scienceOrthorhombic crystal systemHydrogen bondNeutron diffractionMolecular dynamicsHalogenSpectroscopyMoleculeNeutron spectroscopyCrystallographyPhysical chemistryNeutronComputational chemistryPhysicsCrystal structureChemistryInorganic chemistryNeutron scatteringOrganic chemistry

Abstract

fetched live from OpenAlex

The organic-inorganic lead-halide perovskites are composed of organic molecules imbedded in an inorganic framework. The compounds with general formula ${\mathrm{CH}}_{3}{\mathrm{NH}}_{3}\mathrm{Pb}{X}_{3}$ ($\mathrm{MAPb}{X}_{3}$) display large photovoltaic efficiencies for halogens $X=\mathrm{Cl}$, Br, and I in a wide variety of sample geometries and preparation methods. The organic cation and inorganic framework are bound by hydrogen bonds that tether the molecules to the halide anions, and this has been suggested to be important to the optoelectronic properties. We have studied the effects of this bonding using time-of-flight neutron spectroscopy to measure the molecular dynamics in ${\mathrm{CH}}_{3}{\mathrm{NH}}_{3}{\mathrm{PbCl}}_{3}$ (${\mathrm{MAPbCl}}_{3}$). Low-energy/high-resolution neutron backscattering reveals thermally activated molecular dynamics with a characteristic temperature of $\ensuremath{\sim}95$ K. At this same temperature, higher-energy neutron spectroscopy indicates the presence of an anomalous broadening in energy (reduced lifetime) associated with the molecular vibrations. By contrast, neutron powder diffraction shows that a spatially long-range structural phase transitions occurs at 178 K (cubic $\ensuremath{\rightarrow}$ tetragonal) and 173 K (tetragonal $\ensuremath{\rightarrow}$ orthorhombic). The large difference between these two temperature scales suggests that the molecular and inorganic lattice dynamics in ${\mathrm{MAPbCl}}_{3}$ are actually decoupled. With the assumption that underlying physical mechanisms do not change with differing halogens in the organic-inorganic perovskites, we speculate that the energy scale most relevant to the photovoltaic properties of the lead-halogen perovskites is set by the lead-halide bond, not by the hydrogen bond.

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.

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)0.005
metaresearch head score (Gemma)0.004
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow), Science and technology studies, Scholarly communication, Research integrity, Insufficient payload (model declined to judge)
Consensus categoriesMeta-epidemiology (narrow), Research integrity, Insufficient payload (model declined to judge)
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: none
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.883
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0050.004
Meta-epidemiology (narrow)0.0030.005
Meta-epidemiology (broad)0.0020.004
Bibliometrics0.0010.003
Science and technology studies0.0030.003
Scholarly communication0.0040.003
Open science0.0050.005
Research integrity0.0050.004
Insufficient payload (model declined to judge)0.6410.008

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 head0.245
Teacher spread0.232 · 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