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The Impact of Ligand Field Symmetry on Molecular Qubit Coherence

Kazmierczak, Nathanael P. and Mirzoyan, Ruben and Hadt, Ryan G. (2021) The Impact of Ligand Field Symmetry on Molecular Qubit Coherence. Journal of the American Chemical Society, 143 (42). pp. 17305-17315. ISSN 0002-7863. doi:10.1021/jacs.1c04605. https://resolver.caltech.edu/CaltechAUTHORS:20210513-100749414

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Abstract

Developing quantum bits (qubits) exhibiting room temperature electron spin coherence is a key goal of molecular quantum information science. At high temperatures, coherence is often limited by electron spin relaxation, measured by T₁. Here we develop a simple and powerful model for predicting relative T₁ relaxation times in transition metal complexes from dynamic ligand field principles. By considering the excited state origins of ground state spin-phonon coupling, we derive group theory selection rules governing which vibrational symmetries can induce decoherence. Thermal weighting of the coupling terms produces surprisingly good predictions of experimental T₁ trends as a function of temperature and explains previously confounding features in spin–lattice relaxation data. We use this model to evaluate experimental relaxation rates across S = 1/2 transition metal qubit candidates with diverse structures, gaining new insights into the interplay between spin-phonon coupling and molecular symmetry. This methodology elucidates the specific vibrational modes giving rise to decoherence, providing insight into the origin of room temperature coherence in transition metal complexes. We discuss the outlook of symmetry-based modeling and design strategies for understanding molecular coherence.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/jacs.1c04605DOIArticle
https://doi.org/10.26434/chemrxiv.14531694.v1DOIDiscussion Paper
ORCID:
AuthorORCID
Kazmierczak, Nathanael P.0000-0002-7822-6769
Mirzoyan, Ruben0000-0002-2334-4012
Hadt, Ryan G.0000-0001-6026-1358
Additional Information:© 2021 American Chemical Society. Received: May 3, 2021; Published: October 7, 2021. The authors thank Dr. Alec Follmer for helpful discussions. N.P.K. acknowledges support by the National Science Foundation Graduate Research Fellowship under Grant No. DGE-1745301. This paper’s computational modeling was supported in part by National Science Foundation MRI-Grant 1726260 based at Calvin University in Grand Rapids, MI, USA. The computations presented here were also conducted in part in the Resnick High Performance Computing Center, a facility supported by Resnick Sustainability Institute at the California Institute of Technology. Financial support from Caltech and the Dow Next Generation Educator Fund is gratefully acknowledged. The authors declare no competing financial interest.
Group:Resnick Sustainability Institute
Funders:
Funding AgencyGrant Number
NSF Graduate Research FellowshipDGE-1745301
NSFOAC-1726260
Resnick Sustainability InstituteUNSPECIFIED
CaltechUNSPECIFIED
Dow Next Generation Educator FundUNSPECIFIED
Subject Keywords:Group theory, Quantum mechanics, Molecular modeling, Excited states, Oscillation
Issue or Number:42
DOI:10.1021/jacs.1c04605
Record Number:CaltechAUTHORS:20210513-100749414
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210513-100749414
Official Citation:The Impact of Ligand Field Symmetry on Molecular Qubit Coherence. Nathanael P. Kazmierczak, Ruben Mirzoyan, and Ryan G. Hadt. Journal of the American Chemical Society 2021 143 (42), 17305-17315; DOI: 10.1021/jacs.1c04605
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:109111
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:13 May 2021 17:55
Last Modified:08 Nov 2021 21:44

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