Illuminating mechanochemical reactions by combining real-time fluorescence emission monitoring and periodic time-dependent density-functional calculations
Bibliographic record
Abstract
We provide a proof-of-principle demonstration of the first dual-spectroscopic method for direct and real-time observation of mechanochemical reactions by ball milling, supported by high-level molecular and periodic density-functional theory (DFT) calculations, including periodic time-dependent (TD-DFT) calculations to model solid-state fluorescence spectra. By combining standard Raman and fluorescence benchtop spectrometers in a single readily accessible tandem monitoring technique, we simultaneously observe changes to the supramolecular structure during mechanochemical polymorph transformation and cocrystallization of the model pharmaceutical system indometacin. The observed time-resolved in situ spectroscopic data is supported by ex situ X-ray diffraction and solid-state nuclear magnetic resonance spectroscopy measurements. First principles calculations facilitate the interpretation of both real-time spectroscopic and ex situ data by demonstrating how changes in crystalline environment affect vibrational and electronic excited states.
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How this classification was reachedexpand
Full frame distilled prediction
Teacher imitationNot 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.
Codex and Gemma teacher scores by category
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.001 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.001 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.001 |
| Research integrity | 0.001 | 0.001 |
| Insufficient payload (model declined to judge) | 0.001 | 0.000 |
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.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one teacher head, not a consensus.
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".