On the lifetimes and physical nature of incompletely relaxed electrons in liquid water
Bibliographic record
Abstract
Despite intense study over the past two decades, the dynamics of electron solvation in water, particularly regarding the physical properties and lifetimes of non-equilibrium, incompletely relaxed electrons, remain very controversial. Both experimental and theoretical studies have reported a very diverse range, from approximately 50 to approximately 1000 fs, for the lifetime of the p-like excited state of the hydrated electron, and the nature of incompletely relaxed states remains unclear. Here, we reveal that these controversies are to a great extent due to a hidden effect, i.e., the universal existence of a coherence spike at delay time zero in pump-probe spectroscopic kinetics traces. After removing this spike effect, we show that the intrinsic lifetimes of the two incompletely relaxed states in bulk water are 180+/-30 and 545+/-30 fs, respectively. Moreover, our results using iododeoxyuridine as a molecular probe reveal that both states are electronically excited states of the hydrated electron and the second state of a 545 fs lifetime is the long-sought wet electron. These results resolve the long-standing controversies about electron hydration dynamics.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.001 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.001 |
| Scholarly communication | 0.000 | 0.001 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| 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 source (direct Gemma or distilled Codex), 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".