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Record W4396905747 · doi:10.1021/jacs.3c14801

An Unexpected Decrease in Vibrational Entropy of Multicomponent Rutile Oxides

2024· article· en· W4396905747 on OpenAlexaff
Yaowen Wang, Xinbo Li, Jipeng Luo, Brian F. Woodfield, Xiyang Wang, Tao Feng, Nan Yin, Quan Shi, Liping Li

Bibliographic record

VenueJournal of the American Chemical Society · 2024
Typearticle
Languageen
FieldEngineering
TopicHigh Entropy Alloys Studies
Canadian institutionsUniversity of Waterloo
FundersHefei Science Center, Chinese Academy of SciencesDepartment of Science and Technology of Jilin ProvinceNational Natural Science Foundation of China
KeywordsRutileChemistryThermodynamicsEntropy (arrow of time)Configuration entropyNon-equilibrium thermodynamicsHeat capacityOxideMolecular vibrationChemical physicsMoleculePhysicsOrganic chemistry

Abstract

fetched live from OpenAlex

High-entropy oxides (HEOs), featuring infinite chemical composition and exceptional physicochemical properties, are attracting much attention. The configurational entropy caused by a component disorder of HEOs is popularly believed to be the main driving force for thermal stability, while the role of vibrational entropy in the thermodynamic landscape has been neglected. In this study, we systematically investigated the vibrational entropy of multicomponent rutile oxides (including Fe 0.5 Ta 0.5 O 2, Fe 0.333 Ti 0.333 Ta 0.333 O 2, Fe 0.25 Ti 0.25 Ta 0.25 Sn 0.25 O 2, and Fe 0.21 Ti 0.21 Ta 0.21 Sn 0.21 Ge 0.16 O 2 ) by precise heat capacity measurements. It is found that vibrational entropy gradually decreases with increasing component disorder, beyond what one could expect from an equilibrium thermodynamics perspective. Moreover, all multicomponent rutile oxides exhibit a positive excess vibrational entropy at 298.15 K. Upon examinations of configuration disorder, size mismatch, phase transition, and polyhedral distortions, we demonstrate that the excess vibrational entropy plays a pivotal role in lowering the crystallization temperature of multicomponent rutile oxides. These findings represent the first experimental confirmation of the role of lattice vibrations in the thermodynamic landscape of rutile HEOs. In particular, vibrational entropy could serve as a novel descriptor to guide the predictive design of multicomponent oxide materials.

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 score0.127
Threshold uncertainty score0.293

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 integrity0.0000.000
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 head0.007
GPT teacher head0.238
Teacher spread0.231 · 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

Citations12
Published2024
Admission routes1
Has abstractyes

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Same venueJournal of the American Chemical SocietySame topicHigh Entropy Alloys StudiesFrench-language works237,207