Using Time-Resolved Experiments and Coherent Control to Determine the Phase of Transition Dipole Moments between Individual Energy Eigenstates
Bibliographic record
Abstract
We develop an imaging method which uses bichromatic coherent control (BCC) in conjunction with time-resolved fluorescence to extract the complex amplitudes of individual transition dipole matrix elements (TDMs) as well as the amplitude of time-evolving wave packets. The method relies on determining the phase relation between the BCC fields, which look to deplete the population of different pairs of excited energy eigenstates, through the computation of a Fourier integral of the time-resolved fluorescence at the beat frequencies of these pairs of states. We illustrate our procedure by determining the amplitudes of the TDM’s linking the vibrational states of the A 1 ∑ u + and those of the X 1 ∑ u + electronic states of Na 2 . Furthermore, we demonstrate its broad applicability by extracting the expansion coefficients of a wave packet in the basis of vibrational energy eigenstates in the strong spin–orbit coupling potentials in RbCs. The approach, which is found to be quite robust against errors can be readily generalized to the imaging of wave packets of polyatomic molecules.
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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 | 0.001 | 0.001 |
| Open science | 0.001 | 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 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".