Coherent spin-control of S = 1 vanadium and molybdenum complexes
The burgeoning field of quantum sensing hinges on the creation and control of quantum bits. To date, the most well-studied quantum sensors are optically active, paramagnetic defects residing in crystalline hosts. We previously developed analogous optically addressable molecules featuring a ground-st...
| Main Authors: | , , , , , , , |
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| Format: | Article |
| Language: | English |
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Royal Society of Chemistry
2024
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| Online Access: | https://hdl.handle.net/1721.1/157463 |
| _version_ | 1824457884938797056 |
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| author | Laorenza, Daniel W Mullin, Kathleen R Weiss, Leah R Bayliss, Sam L Deb, Pratiti Awschalom, David D Rondinelli, James M Freedman, Danna E |
| author2 | Massachusetts Institute of Technology. Department of Chemistry |
| author_facet | Massachusetts Institute of Technology. Department of Chemistry Laorenza, Daniel W Mullin, Kathleen R Weiss, Leah R Bayliss, Sam L Deb, Pratiti Awschalom, David D Rondinelli, James M Freedman, Danna E |
| author_sort | Laorenza, Daniel W |
| collection | MIT |
| description | The burgeoning field of quantum sensing hinges on the creation and control of quantum bits. To date, the most well-studied quantum sensors are optically active, paramagnetic defects residing in crystalline hosts. We previously developed analogous optically addressable molecules featuring a ground-state spin-triplet centered on a Cr4+ ion with an optical-spin interface. In this work, we evaluate isovalent V3+ and Mo4+ congeners, which offer unique advantages, such as an intrinsic nuclear spin for V3+ or larger spin–orbit coupling for Mo4+, as optically addressable spin systems. We assess the ground-state spin structure and dynamics for each complex, illustrating that all of these spin-triplet species can be coherently controlled. However, unlike the Cr4+ derivatives, these pseudo-tetrahedral V3+ and Mo4+ complexes exhibit no measurable emission. Coupling absorption spectroscopy with computational predictions, we investigate why these complexes exhibit no detectable photoluminescence. These cumulative results suggest that design of future V3+ complexes should target pseudo-tetrahedral symmetries using bidentate or tridentate ligand scaffolds, ideally with deuterated or fluorinated ligand environments. We also suggest that spin-triplet Mo4+, and by extension W4+, complexes may not be suitable candidate optically addressable qubit systems due to their low energy spin-singlet states. By understanding the failures and successes of these systems, we outline additional design features for optically addressable V- or Mo-based molecules to expand the library of tailor-made quantum sensors. |
| first_indexed | 2025-02-19T04:17:06Z |
| format | Article |
| id | mit-1721.1/157463 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2025-02-19T04:17:06Z |
| publishDate | 2024 |
| publisher | Royal Society of Chemistry |
| record_format | dspace |
| spelling | mit-1721.1/1574632024-12-23T06:21:29Z Coherent spin-control of S = 1 vanadium and molybdenum complexes Laorenza, Daniel W Mullin, Kathleen R Weiss, Leah R Bayliss, Sam L Deb, Pratiti Awschalom, David D Rondinelli, James M Freedman, Danna E Massachusetts Institute of Technology. Department of Chemistry The burgeoning field of quantum sensing hinges on the creation and control of quantum bits. To date, the most well-studied quantum sensors are optically active, paramagnetic defects residing in crystalline hosts. We previously developed analogous optically addressable molecules featuring a ground-state spin-triplet centered on a Cr4+ ion with an optical-spin interface. In this work, we evaluate isovalent V3+ and Mo4+ congeners, which offer unique advantages, such as an intrinsic nuclear spin for V3+ or larger spin–orbit coupling for Mo4+, as optically addressable spin systems. We assess the ground-state spin structure and dynamics for each complex, illustrating that all of these spin-triplet species can be coherently controlled. However, unlike the Cr4+ derivatives, these pseudo-tetrahedral V3+ and Mo4+ complexes exhibit no measurable emission. Coupling absorption spectroscopy with computational predictions, we investigate why these complexes exhibit no detectable photoluminescence. These cumulative results suggest that design of future V3+ complexes should target pseudo-tetrahedral symmetries using bidentate or tridentate ligand scaffolds, ideally with deuterated or fluorinated ligand environments. We also suggest that spin-triplet Mo4+, and by extension W4+, complexes may not be suitable candidate optically addressable qubit systems due to their low energy spin-singlet states. By understanding the failures and successes of these systems, we outline additional design features for optically addressable V- or Mo-based molecules to expand the library of tailor-made quantum sensors. 2024-11-01T20:30:37Z 2024-11-01T20:30:37Z 2024-08-05 2024-11-01T20:15:57Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/157463 Laorenza, Daniel W, Mullin, Kathleen R, Weiss, Leah R, Bayliss, Sam L, Deb, Pratiti et al. 2024. "Coherent spin-control of S = 1 vanadium and molybdenum complexes." Chemical Science, 15 (34). en 10.1039/d4sc03107e Chemical Science Creative Commons Attribution https://creativecommons.org/licenses/by/3.0/ application/pdf Royal Society of Chemistry Royal Society of Chemistry |
| spellingShingle | Laorenza, Daniel W Mullin, Kathleen R Weiss, Leah R Bayliss, Sam L Deb, Pratiti Awschalom, David D Rondinelli, James M Freedman, Danna E Coherent spin-control of S = 1 vanadium and molybdenum complexes |
| title | Coherent spin-control of S = 1 vanadium and molybdenum complexes |
| title_full | Coherent spin-control of S = 1 vanadium and molybdenum complexes |
| title_fullStr | Coherent spin-control of S = 1 vanadium and molybdenum complexes |
| title_full_unstemmed | Coherent spin-control of S = 1 vanadium and molybdenum complexes |
| title_short | Coherent spin-control of S = 1 vanadium and molybdenum complexes |
| title_sort | coherent spin control of s 1 vanadium and molybdenum complexes |
| url | https://hdl.handle.net/1721.1/157463 |
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