CoChat
Sign Up
Cited by 5Quantum Mechanics and ApplicationsSpectroscopy and Quantum Chemical StudiesAdvanced Thermodynamics and Statistical Mechanics

Decoherence dynamics in molecular qubits: Exponential, gaussian and beyond

Open access
Gustin, Ignacio, Chen, Xinxian, Franco, Ignacio·2025·The Journal of Chemical Physics
DOI 10.1063/5.0246970
Open this paper in CoChat — free accountOpen PDF

Abstract

In this work, we examine how the structure of system-bath interactions can determine commonly encountered temporal decoherence patterns, such as Gaussian and exponential decay, in molecular and other qubits coupled to a thermal bosonic bath. The analysis, based on a pure dephasing picture that admits analytical treatment, shows that decoherence, in general, is neither purely Gaussian nor exponential but rather the exponential of oscillatory functions, with periods determined by the bath's frequencies. For initially unentangled qubit-bath states, Gaussian decay is always present at early times. It becomes increasingly dominant with increasing temperature, qubit-bath interaction strength, and bath correlation time. Initial system-bath entanglement that arises due to displacement in the position of the bath states preserves the Gaussian decay. By contrast, strict exponential decay arises only in very specific models that we isolate. However, it becomes dominant for times longer than the bath correlation time or for early times when there is initial entanglement due to momentum displacement of the bath states. For molecular electronic decoherence, the long-time exponential regime plays a limited role as it emerges after most coherence is lost. Thus, the Gaussian decay provides a more suitable (albeit imperfect) model of such decoherence. Furthermore, we discuss the connection between electronic decoherence dynamics and electronic spectroscopic line shape theory, where Gaussian spectral peaks correspond to Gaussian coherence decay and Lorentzian peaks correspond to exponential coherence decay. We find that Gaussian spectral peaks, usually associated with inhomogeneous broadening, can emerge from the entangling unitary system-bath dynamics even when there is no inhomogeneity in the initial conditions.

The claims and statistics of this paper haven’t been checked yet.

Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.

A few free checks a day · papers already verified open instantly · results are public

Integrity signals

Registry

Crossref · 10.1063/5.0246970

Cites

72 of 72 references verified0 citation errors · 0 not checkable

Statistics

Claims the paper makes

The claims and statistics of this paper haven’t been checked yet.

Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.

A few free checks a day · papers already verified open instantly · results are public

Claims other papers make about this one

Each is checked against this paper’s own text: does it say what the citing paper says it does?

Self-check

Percentages, sums and reported differences re-computed from the paper’s own numbers.

The self-check needs the paper’s full text.

Cites

Flagged first, then by citations

Research works printed but not linked: 11

  1. M. Shapiro and P. Brumer, Quantum Control of Molec- ular Processes ((Wiley-VCH, Hoboken, NJ, 2012).
  2. S. Rice and M. Zhao, Optical Control of Molecular Dy- namics (Wiley, 2000).
  3. M. Schlosshauer, Decoherence And the Quantum-To- Classical Transition, The Frontiers Collection (Springer, 2007).
  4. H. Breuer and F. Petruccione, The Theory of Open Quan- tum Systems (Oxford University Press, 2002).
  5. S. Mukamel, Principles of Nonlinear Optical Spec- troscopy (Oxford University Press, 1995).
  6. L. Wang, M. A. Allodi, and G. S. Engel, Quantum co- herences reveal excited-state dynamics in biophysical sys- tems, Nat. Rev. Chem. 3, 477 (2019).
  7. A. Nitzan, Chemical Dynamics in Condensed Phases: Relaxation, Transfer and Reactions in Condensed Molec- ular Systems (Oxford University Press, 2006).
  8. J.-P. Hansen and I. R. McDonald, Theory of simple liq- uids: with applications to soft matter (Academic press, 2013).
  9. J. Von Neumann, Mathematical foundations of quantum mechanics: New edition, Vol. 53 (Princeton university press, 2018).
  10. M. Schlosshauer. Decoherence: And the Quantum-To-Classical Transition, The Frontiers Collection (Springer, 2007)
  11. Minhaeng Cho. Chem. Phys. Rev. 4, 021311 (2023)

Cited by

Sorted by citations

Related

Authors
Gustin, I., Chen, X., & Franco, I.
Affiliations
  • Department of Chemistry, University of Rochester 1 , Rochester, New York 14627,
  • University of Rochester (US)
Corresponding author
Franco, Ignacio
ORCID
Venue
The Journal of Chemical Physics
Publisher
AIP Publishing
Published
2025-02-10
Volume
162
Issue
6
ISSN
  • 0021-9606 (ISSN-L)
  • 1089-7690
DOI
10.1063/5.0246970
OpenAlex
W4407294752
Cited by
5
References
72
Citations by year
2026: 3 · 2025: 2
FWCI
1.83
Type
journal article
Language
en
Open access
Locations
  • The Journal of Chemical Physics (publishedVersion)
  • PubMed (publishedVersion)
  • arXiv (Cornell University) (submittedVersion)
  • arXiv (Cornell University)
Funders
U.S. Department of Energy (DE-SC0025334)
Topics
  • Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Quantum Mechanics and Applications
  • Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
  • Physical Sciences › Physics and Astronomy › Statistical and Nonlinear Physics › Advanced Thermodynamics and Statistical Mechanics
Keywords
decoherence dynamics, molecular qubits, Gaussian decay, exponential decay, system-bath interaction, pure dephasing, electronic decoherence, inhomogeneous broadening

About these checks

Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.

Statistics and arithmetic are recomputed, not judged.

Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.

What counts as a claim ›How we measure confidence ›How we check this ›

Are you an author, or do you see a problem with this page? Request a review