Laser-Limited Signatures of Quantum Coherence
Bibliographic record
Abstract
Quantum coherence is proclaimed to promote efficient energy collection by light-harvesting complexes and prototype organic photovoltaics. However, supporting spectroscopic studies are hindered by the problem of distinguishing between the excited state and ground state origin of coherent spectral transients. Coherence amplitude maps, which systematically represent quantum beats observable in two-dimensional (2D) spectroscopy, are currently the prevalent tool for making this distinction. In this article, we present coherence amplitude maps of a molecular dimer, which have become significantly distorted as a result of the finite laser bandwidth used to record the 2D spectra. We argue that under standard spectroscopic conditions similar distortions are to be expected for compounds absorbing over a spectral range similar to, or exceeding, that of the dimer. These include virtually all photovoltaic polymers and certain photosynthetic complexes. With the distortion of coherence amplitude maps, alternative ways to identify quantum coherence are called for. Here, we use numerical simulations that reproduce the essential photophysics of the dimer to unambiguously determine the excited state origin of prominent quantum beats observed in the 2D spectral measurements. This approach is proposed as a dependable method for coherence identification.
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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".