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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. . (Unpublished)

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Developing quantum bits (qubits) exhibiting room temperature electron spin coherence is a key goal of molecular quantum information science. Here we develop a simple and powerful model for predicting relative T1 coherence 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 = ½ 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, suggesting symmetry-based design strategies and providing insight into the origin of room temperature coherence in transition metal complexes.

Item Type:Report or Paper (Discussion Paper)
Related URLs:
URLURL TypeDescription Paper
Mirzoyan, Ruben0000-0002-2334-4012
Hadt, Ryan G.0000-0001-6026-1358
Additional Information:License: CC BY-NC-ND 4.0. Preprint submitted on 03.05.2021, 21:34 and posted on 05.05.2021. NPK 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. Financial support from Caltech and the Dow Next Generation Educator Fund is gratefully acknowledged. No conflict of interest.
Funding AgencyGrant Number
NSF Graduate Research FellowshipDGE-1745301
Dow Next Generation Educator FundUNSPECIFIED
Subject Keywords:qubit candidates; group theory; ligand field theory; spin-lattice relaxation rates; coherence; spin-phonon coupling
Record Number:CaltechAUTHORS:20210513-100749414
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:109111
Deposited By: Tony Diaz
Deposited On:13 May 2021 17:55
Last Modified:25 Jun 2021 19:40

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