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Record W4307302306 · doi:10.1002/smll.202204578

Tuning Structural and Optical Properties of Porphyrin‐based Hydrogen‐Bonded Organic Frameworks by Metal Insertion

2022· article· en· W4307302306 on OpenAlexaff
Patrik Tholen, Craig A. Peeples, Mehmet Menaf Ayhan, Lukas Wagner, Heidi Thomas, Paulius Imbrasas, Yunus Zorlu, Clemens Baretzky, Sebastian Reineke, Gabriel Hanna, Gündoğ Yücesan

Bibliographic record

VenueSmall · 2022
Typearticle
Languageen
FieldChemistry
TopicMetal-Organic Frameworks: Synthesis and Applications
Canadian institutionsUniversity of Alberta
Fundersnot available
KeywordsPorphyrinMaterials scienceAtomic orbitalPhotoluminescenceBand gapMetalHydrogen bondMoleculeCrystallographyPhotochemistryChemistryOptoelectronicsOrganic chemistryPhysics

Abstract

fetched live from OpenAlex

Abstract Herein, a simple way of tuning the optical and structural properties of porphyrin‐based hydrogen‐bonded organic frameworks (HOFs) is reported. By inserting transition metal ions into the porphyrin cores of GTUB‐5 ( p ‐H 8 ‐TPPA (5,10,15,20‐Tetrakis[p‐phenylphosphonic acid] HOF), the authors show that it is possible to generate HOFs with different band gaps, photoluminescence (PL) life times, and textural properties. The band gaps of the resulting HOFs (viz., Cu‐, Ni‐, Pd‐, and Zn‐GTUB‐5) are measured by diffuse reflectance and PL spectroscopy, as well as calculated via DFT, and the PL lifetimes are measured. Across the series, the band gaps vary over a narrow range from 1.37 to 1.62 eV, while the PL lifetimes vary over a wide range from 2.3 to 83 ns. These differences ultimately arise from metal‐induced structural changes, viz., changes in the metal‐to‐nitrogen distances, number of hydrogen bonds, and pore volumes. DFT reveals that the band gaps of Cu‐, Zn‐, and Pd‐ GTUB‐5 are governed by highest occupied/lowest unoccupied crystal orbitals (HOCO/LUCO) composed of π‐ orbitals on the porphyrin linkers, while that of Ni‐GTUB‐5 is governed by a HOCO and LUCO composed of Ni dorbitals. Overall, our findings show that metal‐insertion can be used to optimize HOFs for optoelectronics and small‐molecule capture applications.

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 categoriesInsufficient payload (model declined to judge)
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 score0.005
Threshold uncertainty score0.997

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)0.0030.000

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 head0.017
GPT teacher head0.211
Teacher spread0.194 · 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.

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

Citations30
Published2022
Admission routes1
Has abstractyes

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