Alternant Hydrocarbon Diradicals as Optically Addressable Molecular Qubits

Poh, Yong Rui; Morozov, Dmitry; Kazmierczak, Nathanael P.; Hadt, Ryan G.; Groenhof, Gerrit; Yuen-Zhou, Joel

doi:10.1021/jacs.4c04360

Alternant Hydrocarbon Diradicals as Optically Addressable Molecular Qubits

Journal Article · Mon May 27 04:00:00 EDT 2024 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.4c04360· OSTI ID:2999598

Poh, Yong Rui ^[1]; ^[2]; ^[3]; ^[3]; Groenhof, Gerrit ^[4]; ^[1]

University of California San Diego, La Jolla, CA (United States)
Terra Quantum AG (Switzerland)
California Institute of Technology, Pasadena, CA (United States)
University of Jyväskylä (Finland)

High-spin molecules allow for bottom-up qubit design and are promising platforms for magnetic sensing and quantum information science. Optical addressability of molecular electron spins has also been proposed in first-row transition-metal complexes via optically detected magnetic resonance (ODMR) mechanisms analogous to the diamond-nitrogen-vacancy color center. However, significantly less progress has been made on the front of metal-free molecules, which can deliver lower costs and milder environmental impacts. At present, most luminescent open-shell organic molecules are π-diradicals, but such systems often suffer from poor ground-state open-shell characters necessary to realize a stable ground-state molecular qubit. In this work, we use alternancy symmetry to selectively minimize radical–radical interactions in the ground state, generating π-systems with high diradical characters. We call them m-dimers, referencing the need to covalently link two benzylic radicals at their meta carbon atoms for the desired symmetry. Through a detailed electronic structure analysis, we find that the excited states of alternant hydrocarbon m-diradicals contain important symmetries that can be used to construct ODMR mechanisms leading to ground-state spin polarization. Furthermore, the molecular parameters are set in the context of a tris(2,4,6-trichlorophenyl)methyl (TTM) radical dimer covalently tethered at the meta position, demonstrating the feasibility of alternant m-diradicals as molecular color centers.

View Accepted Manuscript (DOE)

Research Organization:: California Institute of Technology, Pasadena, CA (United States)

Sponsoring Organization:: USDOE; Academy of Finland; National Science Foundation Graduate Research Fellowship Program

Grant/Contract Number:: SC0022089

OSTI ID:: 2999598

Alternate ID(s):: OSTI ID: 2577887

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 22 Vol. 146; ISSN 0002-7863; ISSN 1520-5126

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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