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Record W3165838807 · doi:10.1002/mas.21701

Toward ICP‐SIFT mass spectrometry and atomic cation ligation as a probe of relativistic effects—A personal journey

2021· review· en· W3165838807 on OpenAlex
Diethard K. Böhme

Why this work is in the frame

A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.

Bibliographic record

VenueMass Spectrometry Reviews · 2021
Typereview
Languageen
FieldPhysics and Astronomy
TopicX-ray Spectroscopy and Fluorescence Analysis
Canadian institutionsYork University
Fundersnot available
KeywordsChemistryMass spectrometryInductively coupled plasma mass spectrometryAnalytical Chemistry (journal)Environmental chemistryChromatography

Abstract

fetched live from OpenAlex

Abstract The ICP–SIFT mass spectrometer at York University, a derivative of flowing afterglow (FA) and selected‐ion flow tube (SIFT) mass spectrometers, has provided a powerful technique to measure the chemistry and kinetics of atomic cation–molecule reactions. Here, I focus on periodic trends in the kinetics of ligation reactions of atomic ions with small molecules. I examine trends in ammonia ligation kinetics across the first two rows of the atomic transition metal cations and their correlation with ligand bond enthalpies and ligand field stabilization energies. Also explored are trends down Groups 1 and 2 in the kinetics of noncovalent electrostatic ligand bonding and the tendency for s electron solvation of the atomic alkaline‐earth cations with ammonia. Finally, I briefly review trends observed with 12 different ligands in the ligation rate down the periodic table with Group 9–12 transition atomic metal cations. These trends provide a compelling probe for the presence of relativistic effects that influence the strengths of the metal‐ion ligand bonds that are formed. There is a clear third‐row rate enhancement with Ir + , Pt + , Au + , and Hg + , the extent of which depends on the nature of the ligand. This large set of kinetic data provides an unprecedented broad perspective of relativistic effects in ligand bonding. With CS 2 as a ligand, the third‐row relativistic effect is apparent in the formation of both the first and the second ligand bond with the Groups 10 and 11 atomic cations as predicted by our quantum chemical calculations of ligation energies.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

Full frame distilled prediction

Teacher imitation

Not 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.

metaresearch head score (Codex)0.001
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow), Insufficient payload (model declined to judge)
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Not applicable · Consensus signal: none
GenreCandidate signal: Review · Consensus signal: Review
Teacher disagreement score0.852
Threshold uncertainty score0.999

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.000
Meta-epidemiology (narrow)0.0010.001
Meta-epidemiology (broad)0.0050.002
Bibliometrics0.0010.003
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0010.000
Research integrity0.0000.001
Insufficient payload (model declined to judge)0.0020.000

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.

Opus teacher head0.032
GPT teacher head0.318
Teacher spread0.286 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it