Trigonal Bipyramidal V3+Complex as an Optically Addressable Molecular Qubit Candidate

Majed S. Fataftah, Sam L. Bayliss, Daniel W. Laorenza, Xiaoling Wang, Brian T. Phelan, C. Blake Wilson, Peter J. Mintun, Berk D. Kovos, Michael R. Wasielewski*, Songi Han, Mark S. Sherwin, David D. Awschalom, Danna E. Freedman

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

4 Scopus citations

Abstract

Synthetic chemistry enables a bottom-up approach to quantum information science, where atoms can be deterministically positioned in a quantum bit or qubit. Two key requirements to realize quantum technologies are qubit initialization and read-out. By imbuing molecular spins with optical initialization and readout mechanisms, analogous to solid-state defects, molecules could be integrated into existing quantum infrastructure. To mimic the electronic structure of optically addressable defect sites, we designed the spin-triplet, V3+ complex, (C6F5)3trenVCNtBu (1). We measured the static spin properties as well as the spin coherence time of 1 demonstrating coherent control of this spin qubit with a 240 GHz electron paramagnetic resonance spectrometer powered by a free electron laser. We found that 1 exhibited narrow, near-infrared photoluminescence (PL) from a spin-singlet excited state. Using variable magnetic field PL spectroscopy, we resolved emission into each of the ground-state spin sublevels, a crucial component for spin-selective optical initialization and readout. This work demonstrates that trigonally symmetric, heteroleptic V3+ complexes are candidates for optical spin addressability.

Original languageEnglish (US)
Pages (from-to)20400-20408
Number of pages9
JournalJournal of the American Chemical Society
Volume142
Issue number48
DOIs
StatePublished - Dec 2 2020

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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