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Record W4414701048 · doi:10.1063/5.0278659

Spin decoherence in molecular crystals: Nuclear vs electronic spin baths

2025· article· en· W4414701048 on OpenAlexaff
C. E. Ryan, Valerio Briganti, Caitlin M. Hogan, Mark L. O’Neill, Alessandro Lunghi

Bibliographic record

VenueThe Journal of Chemical Physics · 2025
Typearticle
Languageen
FieldPhysics and Astronomy
TopicSpectroscopy and Quantum Chemical Studies
Canadian institutionsTrinity College
FundersHORIZON EUROPE European Research CouncilIrish Research Council
KeywordsQuantum decoherenceSpinsCoherence (philosophical gambling strategy)QubitSpin engineeringSpin (aerodynamics)Coherence timeQuantum

Abstract

fetched live from OpenAlex

The loss of information about the relative phase between two quantum states, known as decoherence, strongly limits resolution in electron paramagnetic spectroscopy and hampers the use of molecules for quantum information processing. At low temperatures, the decoherence of an electronic molecular spin can be driven by its interaction with either other electron spins or nuclear spins. Many experimental techniques have been used to prolong the coherence time of molecular qubits, but these efforts have been hampered by the uncertainty about which of the two mechanisms is effectively limiting coherence in different experimental conditions. Here, we use the cluster-correlation expansion to simulate the decoherence of two prototypical molecular qubits and quantitatively demonstrate that nuclear spins become the leading source of decoherence only when the electron spin concentration is below ∼1 mM. Moreover, we show that deuterated samples, much easier to achieve than fully spin-free environments, could achieve record coherence times of ∼0.1 ms for an electron spin concentration of ∼0.1 mM. Alternatively, hydrogen-rich molecular crystals with electron spin concentrations below 1 mM can still achieve coherence times of 10 ms through dynamical decoupling, showing that the potential of molecular spins for quantum technologies is still untapped.

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.

How this classification was reachedexpand

Full frame machine prediction

Teacher imitation

Not 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.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.001
Version: metacan-v3-hybrid-931329e0061cValidation status: machine_predicted_unvalidated
Candidate categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: none
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.008
Threshold uncertainty score0.016

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.001
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0010.001
Scholarly communication0.0010.001
Open science0.0000.001
Research integrity0.0000.001
Insufficient payload (model declined to judge)0.0010.000

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 head0.006
GPT teacher head0.267
Teacher spread0.262 · 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

Classification

machine, unvalidated

Machine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.

The models applied no category: nothing in the taxonomy fit this work.
Study designBench or experimental
Domainnot available
GenreEmpirical

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".

Quick stats

Citations5
Published2025
Admission routes1
Has abstractyes

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