Electronic Spin Qubit Candidates Arrayed within Layered Two-Dimensional Polymers
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Description
Accepted version
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1.8 MB
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Checksum (MD5)
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Author(s)
Oanta, Alexander K
Collins, Kelsey A
Evans, Austin M
Pratik, Saied Md
Hall, Lyndon A
Strauss, Michael J
Marder, Seth R
D’Alessandro, Deanna M
Rajh, Tijana
Freedman, Danna E
Date Issued
December 27, 2022
Journal
Journal of the American Chemical Society
Publisher
American Chemical Society
Citation
Electronic Spin Qubit Candidates Arrayed within Layered Two-Dimensional Polymers. Alexander K. Oanta, Kelsey A. Collins, Austin M. Evans, Saied Md Pratik, Lyndon A. Hall, Michael J. Strauss, Seth R. Marder, Deanna M. D’Alessandro, Tijana Rajh, Danna E. Freedman, Hong Li, Jean-Luc Brédas, Lei Sun, and William R. Dichtel. Journal of the American Chemical Society 2023 145 (1), 689-696.
Version
Author's final manuscript
Abstract
Molecular electronic spin qubits are promising candidates for quantum information science applications because they can be reliably produced and engineered via chemical design. Embedding electronic spin qubits within two-dimensional polymers (2DPs) offers the possibility to systematically engineer inter-qubit interactions while maintaining long coherence times, both of which are prerequisites to their technological utility. Here, we introduce electronic spin qubits into a diamagnetic 2DP by n-doping naphthalene diimide subunits with varying amounts of CoCp2 and analyze their spin densities by quantitative electronic paramagnetic resonance spectroscopy. Low spin densities (e.g., 6.0 × 1012 spins mm-3) enable lengthy spin-lattice (T1) and spin-spin relaxation (T2) times across a range of temperatures, ranging from T1 values of 164 ms at 10 K to 30.2 μs at 296 K and T2 values of 2.36 μs at 10 K to 0.49 μs at 296 K for the lowest spin density sample examined. Higher spin densities and temperatures were both found to diminish T1 times, which we attribute to detrimental cross-relaxation from spin-spin dipolar interactions and spin-phonon coupling, respectively. Higher spin densities decreased T2 times and modulated the T2 temperature dependence. We attribute these differences to the competition between hyperfine and dipolar interactions for electron spin decoherence, with the dominant interaction transitioning from the former to the latter as spin density and temperature increase. Overall, this investigation demonstrates that dispersing electronic spin qubits within layered 2DPs enables chemical control of their inter-qubit interactions and spin decoherence times.
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DOI of Published Version
https://doi.org/10.1021/jacs.2c11784
