Vibrationally excited ultrafast thermodynamic phase transitions at the water/air interface
Bibliographic record
Abstract
The extraordinary ability of the hydrogen-bond network of water in the condensed phase to thermalize vibrational excitations within several picoseconds, even under supercritical conditions, offers the possibility of creating highly excited thermodynamic states at water surfaces on ultrafast time scales using vibrationally resonant short infrared laser pulses. We experimentally and numerically studied such states created by depositing ~100 ps long pulses tuned to the 3400 cm(-1) O–H stretch vibration at the water/air interface using time-resolved dark-field imaging and time-resolved optical reflectivity. The results are reasonably well described by using a hydrodynamic ablation model under the assumption of impulsive heat deposition. The large thermoelastic stress amplitudes on the order of 1 GPa created within 100 ps by depositing laser pulses with ~1 J cm(-2) fluence were inferred from the numerical simulations. Stresses of this magnitude drive the excited water layer into a very fast expansion resulting in rapid adiabatic cooling and thorough vaporization within a few nanoseconds. The spatial and temporal lengths scales of the ablation plume are nearly ideal for ejecting molecules into the gas phase with minimum perturbation for applications ranging from mass spectrometry and laser surgery to the development of extremely high pressure molecular beams.
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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 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.001 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 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".