Molecular-frame photoelectron angular distributions
Bibliographic record
Abstract
Angle-resolved photoelectron measurements in molecular ionization continue to grow in importance due to their sensitivity to molecular dynamics combined with their avoidance of deleterious averaging over molecular orientation. This special issue contains only regularly refereed articles and provides an account of current experimental and theoretical studies of such molecular-frame photoelectron angular distributions (MFPADs). Recent experimental activity in this field has been stimulated by advances in light sources such as x-ray free electron lasers, attosecond XUV laser pulses and phase-stable ultrashort strong laser fields. This effort is further amplified by recent developments in coincidence detection and molecular-frame alignment/orientation techniques. Beyond perturbative light–matter interactions, strong field processes such as tunnel ionization, above threshold ionization and rescattering phenomena such as high harmonic generation and laser-induced electron diffraction are beginning to probe molecular-frame photoelectron-molecule scattering dynamics. Theoretical developments are playing an equally important role in furthering molecular-frame photoelectron science. This issue contains several purely theoretical papers that aim to provide insight into possible schemes for using MFPADs in the study of molecular dynamics. Because the details of the electron-molecule scattering dynamics are important to the interpretation of experimental data, significant progress is made by a close collaboration between theory and experiment. There are a number of such contributions in this issue that combine theory and experiment to obtain a detailed understanding of the observed processes. One recurring theme is the use of measured MFPADs as probes of the molecular state and to uncover information about the dynamics of molecular systems. Contributions in this issue consider using MFPADs to investigate molecular geometry or the rotational, vibrational or electronic state of a molecule. As discussed in several contributions, the advent of short pulse ionization sources will enable the use of MFPADs in pump–probe experiments to investigate the time dependence of dynamical processes in molecular systems. In the studies presented here, the most common approach for measuring MFPADs is through ionization to dissociative ion states with the subsequent coincidence detection of photoelectron and photofragments. However, there is one contribution that considers the use of impulsively aligned molecules and the high harmonic generation process to extract the MFPAD from ionization to non-dissociating ion states. Contributions consider MFPADs from single photon ionization and from high-field tunnel ionization. Furthermore, single-photon studies consider both core and valence ionization processes.
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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 | 0.001 | 0.008 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.001 | 0.000 |
| Bibliometrics | 0.001 | 0.001 |
| Science and technology studies | 0.001 | 0.000 |
| Scholarly communication | 0.002 | 0.001 |
| Open science | 0.001 | 0.001 |
| Research integrity | 0.002 | 0.001 |
| Insufficient payload (model declined to judge) | 0.135 | 0.057 |
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".