Abstract
The combination of structural precision and reproducibility of synthetic chemistry is perfectly suited for the creation of chemical qubits, the core units of a quantum information science (QIS) system. By exploiting the atomistic control inherent to synthetic chemistry, we address a fundamental question of how the spin-spin distance between two qubits impacts electronic spin coherence. To achieve this goal, we designed a series of molecules featuring two spectrally distinct qubits, an early transition metal, Ti3+, and a late transition metal, Cu2+ with increasing separation between the two metals. Crucially, we also synthesized the monometallic congeners to serve as controls. The spectral separation between the two metals enables us to probe each metal individually in the bimetallic species and compare it with the monometallic control samples. Across a range of 1.2-2.5 nm, we find that electron spins have a negligible effect on coherence times, a finding we attribute to the distinct resonance frequencies. Coherence times are governed, instead, by the distance to nuclear spins on the other qubit's ligand framework. This finding offers guidance for the design of spectrally addressable molecular qubits.
Original language | English (US) |
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Pages (from-to) | 8069-8077 |
Number of pages | 9 |
Journal | Journal of the American Chemical Society |
Volume | 143 |
Issue number | 21 |
DOIs | |
State | Published - Jun 2 2021 |
Funding
We thank Dr. Lei Sun and Dr. Tijana Rajh for help with preliminary EPR experiments, Mr. Saman Shafaie for high resolution mass spectrometry, and Dr. Chung-Jui Yu for expert assistance with data visualization. This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under award DE-SC0019356. S.v.K. also acknowledges support from the Arnold and Mabel Beckman Foundation through a Postdoctoral Fellowship in the Chemical Sciences. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Mass spectrometry, NMR spectroscopy, and X-ray crystallography made use of the IMSERC at Northwestern University, which has received support from the NSF (CHE-1048773), Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205), the State of Illinois and International Institute for Nanotechnology (IIN).
ASJC Scopus subject areas
- General Chemistry
- Biochemistry
- Catalysis
- Colloid and Surface Chemistry
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CCDC 2063308: Experimental Crystal Structure Determination
Von Kugelgen, S. (Contributor), Krzyaniak, M. D. (Contributor), Gu, M. (Contributor), Puggioni, D. (Contributor), Rondinelli, J. M. (Contributor), Wasielewski, M. R. (Contributor) & Freedman, D. E. (Contributor), Cambridge Crystallographic Data Centre, 2021
DOI: 10.5517/ccdc.csd.cc2781bx, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.5517/ccdc.csd.cc2781bx&sid=DataCite
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CCDC 2063311: Experimental Crystal Structure Determination
Von Kugelgen, S. (Contributor), Krzyaniak, M. D. (Contributor), Gu, M. (Contributor), Puggioni, D. (Contributor), Rondinelli, J. M. (Contributor), Wasielewski, M. R. (Contributor) & Freedman, D. E. (Contributor), Cambridge Crystallographic Data Centre, 2021
DOI: 10.5517/ccdc.csd.cc2781f0, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.5517/ccdc.csd.cc2781f0&sid=DataCite
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CCDC 2063319: Experimental Crystal Structure Determination
Von Kugelgen, S. (Contributor), Krzyaniak, M. D. (Contributor), Gu, M. (Contributor), Puggioni, D. (Contributor), Rondinelli, J. M. (Contributor), Wasielewski, M. R. (Contributor) & Freedman, D. E. (Contributor), Cambridge Crystallographic Data Centre, 2021
DOI: 10.5517/ccdc.csd.cc2781p8, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.5517/ccdc.csd.cc2781p8&sid=DataCite
Dataset