Tunable Cr 4+ Molecular Color Centers
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 applica...
| Main Authors: | , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Article |
| Language: | English |
| Published: |
American Chemical Society (ACS)
2022
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| Online Access: | https://hdl.handle.net/1721.1/146760 |
| _version_ | 1826215366623232000 |
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| author | 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 Berkelbach, Timothy C Freedman, Danna E |
| author2 | Massachusetts Institute of Technology. Department of Chemistry |
| author_facet | Massachusetts Institute of Technology. Department of Chemistry 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 Berkelbach, Timothy C Freedman, Danna E |
| author_sort | Laorenza, Daniel W |
| collection | MIT |
| description | 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. |
| first_indexed | 2024-09-23T16:25:59Z |
| format | Article |
| id | mit-1721.1/146760 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T16:25:59Z |
| publishDate | 2022 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1467602023-07-05T20:26:50Z Tunable Cr 4+ Molecular Color Centers 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 Berkelbach, Timothy C Freedman, Danna E Massachusetts Institute of Technology. Department of Chemistry 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. 2022-12-05T19:15:48Z 2022-12-05T19:15:48Z 2021 2022-12-05T19:12:19Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/146760 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). en 10.1021/JACS.1C10145 Journal of the American Chemical Society Creative Commons Attribution-Noncommercial-Share Alike http://creativecommons.org/licenses/by-nc-sa/4.0/ application/pdf American Chemical Society (ACS) DOE repository |
| spellingShingle | 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 Berkelbach, Timothy C Freedman, Danna E Tunable Cr 4+ Molecular Color Centers |
| title | Tunable Cr 4+ Molecular Color Centers |
| title_full | Tunable Cr 4+ Molecular Color Centers |
| title_fullStr | Tunable Cr 4+ Molecular Color Centers |
| title_full_unstemmed | Tunable Cr 4+ Molecular Color Centers |
| title_short | Tunable Cr 4+ Molecular Color Centers |
| title_sort | tunable cr 4 molecular color centers |
| url | https://hdl.handle.net/1721.1/146760 |
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