Designing robust molecular spins for quantum technologies with theoretical chemistry

Quantum Physics arXiv:2608.13744 (quant-ph) [Submitted on 13 Aug 2026] Title:Designing robust molecular spins for quantum technologies with theoretical chemistry Authors:Timothy J. Krogmeier, Pranay Venkatesh, Mikayla Z. Fahrenbruch, Anthony W. Schlimgen, Andres Montoya-Castillo, Kade Head-Marsden View a PDF of the paper titled Designing robust molecular spins for quantum technologies with theoretical chemistry, by Timothy J. Krogmeier and 5 other authors View PDF HTML (experimental) Abstract:Molecular spins represent a versatile platform for quantum information science, with the potential to offer chemically tunable, addressable qubits. However, achieving this requires understanding and mitigating quantum decoherence. This Chapter provides a theoretical overview of current state-of-the-art chemical theory connecting ab initio electronic structure with open quantum system dynamics to guide the rational design of long-lived molecular qubits. Beginning at the electronic level, multi-reference and relativistic electronic structure methods to parameterize effective spin Hamiltonians are discussed, with a primary focus on accurately capturing $g$-tensors, zero-field splitting, and hyperfine interactions. These parameters feed into models of spin-phonon and spin-spin coupling to quantify $T_1$ and $T_2$ relaxation across various environmental regimes. This Chapter evaluates a hierarchy of dynamical methods, ranging from factorization to matrix product state approaches, balancing computational cost against accuracy and generalizability. Ultimately, mapping these theoretical models to molecular architecture can establish design principles, such as isotopic substitution and spatial spin delocalization, to understand and extend coherence lifetimes. Subjects: Quantum Physics (quant-ph) Cite as: arXiv:2608.13744 [quant-ph] (or arXiv:2608.13744v1 [quant-ph] for this version) https://doi.org/10.48550/arXiv.2608.13744 Focus to learn more arXiv-issued DOI via DataCite (pending registration) Submission history From: Kade Head-Marsden [view email] [v1] Thu, 13 Aug 2026 19:58:05 UTC (8,729 KB) Full-text links: Access Paper: View a PDF of the paper titled Designing robust molecular spins for quantum technologies with theoretical chemistry, by Timothy J. Krogmeier and 5 other authorsView PDFHTML (experimental)TeX Source view license Current browse context: quant-ph new | recent | 2026-08 References & Citations INSPIRE HEP NASA ADSGoogle Scholar Semantic Scholar export BibTeX citation Loading... BibTeX formatted citation × loading... Data provided by: Bookmark Bibliographic Tools Bibliographic and Citation Tools Bibliographic Explorer Toggle Bibliographic Explorer (What is the Explorer?) Connected Papers Toggle Connected Papers (What is Connected Papers?) Litmaps Toggle Litmaps (What is Litmaps?) scite.ai Toggle scite Smart Citations (What are Smart Citations?) Code, Data, Media Code, Data and Media Associated with this Article alphaXiv Toggle alphaXiv (What is alphaXiv?) Links to Code Toggle CatalyzeX Code Finder for Papers (What is CatalyzeX?) DagsHub Toggle DagsHub (What is DagsHub?) GotitPub Toggle Gotit.pub (What is GotitPub?) Huggingface Toggle Hugging Face (What is Huggingface?) ScienceCast Toggle ScienceCast (What is ScienceCast?) Demos Demos Replicate Toggle Replicate (What is Replicate?) Spaces Toggle Hugging Face Spaces (What is Spaces?) Spaces Toggle TXYZ.AI (What is TXYZ.AI?) Related Papers Recommenders and Search Tools Link to Influence Flower Influence Flower (What are Influence Flowers?) Core recommender toggle CORE Recommender (What is CORE?) Author Venue Institution Topic About arXivLabs arXivLabs: experimental projects with community collaborators arXivLabs is a framework that allows collaborators to develop and share new arXiv features directly on our website. Both individuals and organizations that work with arXivLabs have embraced and accepted our values of openness, community, excellence, and user data privacy. arXiv is committed to these values and only works with partners that adhere to them. Have an idea for a project that will add value for arXiv's community? Learn more about arXivLabs. Which authors of this paper are endorsers? | Disable MathJax (What is MathJax?)