Floquet representation of absolute phase and pulse-shape effects on laser-driven molecular photodissociation
Bibliographic record
Abstract
Using a recent reformulation of Floquet theory [S. Gu\'erin and H. R. Jauslin, Adv. Chem. Phys. 125, 1 (2003)], we discuss the dynamical role of the absolute phase in the photofragmentation of molecules subjected to laser pulses. We show how the dependence of Floquet states on an absolute phase is related to the complexity of the dressed molecular scheme and to the multiphoton character of the molecular dynamics. The general theory is applied to the study of the photodissociation of $\mathrm{H}_{2}{}^{+}$ in a $400\text{\penalty1000-\hskip0pt}\mathrm{nm}$ periodic laser pulse, repeated with a frequency lying in the IR. The dependence of the dynamics on the phase of the pulse envelope is highlighted through an effect previously called dynamical dissociation quenching (DDQ) [F. Ch\^ateauneuf et al., J. Chem. Phys. 108, 3974 (1998)] and through photofragment kinetic energy spectra. These spectra allow us to map out the Floquet content of the dynamics---i.e., its multiphoton character both with respect to the carrier-wave frequency, which gives rise to the usual bond-softening mechanism, and with respect to the pulse modulation frequency in the IR. The synchronization of this pulse modulation with the wave packet motion governs the DDQ effect in this uv-visible pulsed excitation case.
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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 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.000 | 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".