Tunable Cr 4+ Molecular Color Centers
Name
1840978.pdf
Description
Accepted version
Size
3.43 MB
Format
Adobe PDF
Checksum (MD5)
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Author(s)
Laorenza, Daniel W
Kairalapova, Arailym
Bayliss, Sam L
Goldzak, Tamar
Greene, Samuel M
Weiss, Leah R
Deb, Pratiti
Mintun, Peter J
Collins, Kelsey A
Awschalom, David D
Date Issued
2021
Journal
Journal of the American Chemical Society
Publisher
American Chemical Society (ACS)
Citation
Laorenza, Daniel W, Kairalapova, Arailym, Bayliss, Sam L, Goldzak, Tamar, Greene, Samuel M et al. 2021. "Tunable Cr 4+ Molecular Color Centers." Journal of the American Chemical Society, 143 (50).
Version
Author's final manuscript
Abstract
The inherent atomistic precision of synthetic chemistry enables bottom-up structural control over quantum bits, or qubits, for quantum technologies. Tuning paramagnetic molecular qubits that feature optical-spin initialization and readout is a crucial step toward designing bespoke qubits for applications in quantum sensing, networking, and computing. Here, we demonstrate that the electronic structure that enables optical-spin initialization and readout for S = 1, Cr(aryl)4, where aryl = 2,4-dimethylphenyl (1), o-tolyl (2), and 2,3-dimethylphenyl (3), is readily translated into Cr(alkyl)4 compounds, where alkyl = 2,2,2-triphenylethyl (4), (trimethylsilyl)methyl (5), and cyclohexyl (6). The small ground state zero field splitting values (<5 GHz) for 1-6 allowed for coherent spin manipulation at X-band microwave frequency, enabling temperature-, concentration-, and orientation-dependent investigations of the spin dynamics. Electronic absorption and emission spectroscopy confirmed the desired electronic structures for 4-6, which exhibit photoluminescence from 897 to 923 nm, while theoretical calculations elucidated the varied bonding interactions of the aryl and alkyl Cr4+ compounds. The combined experimental and theoretical comparison of Cr(aryl)4 and Cr(alkyl)4 systems illustrates the impact of the ligand field on both the ground state spin structure and excited state manifold, laying the groundwork for the design of structurally precise optically addressable molecular qubits.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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DOI of Published Version
https://doi.org/10.1021/JACS.1C10145
