Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 138, Issue 4, Pages 1344-1348Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.5b11802
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Funding
- Northwestern University
- Institute for Sustainability and Energy at Northwestern University (ISEN) Booster Award [10031846]
- National Science Foundation for CAREER award [1455017]
- NSF [DMR-1157490]
- State of Florida
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1455017] Funding Source: National Science Foundation
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The implementation of quantum computation. (QC) would revolutionize scientific fields ranging from encryption to quantum simulation. One intuitive candidate for the smallest unit of a quantum computer, a qubit, is electronic spin. A prominent proposal for QC relies on high spin magnetic molecules, where multiple transitions between the many M-S levels are employed as qubits. Yet, over a decade after the original notion, the exploitation of multiple transitions within a single manifold for QC remains unrealized in these high-spin species due to the challenge of accessing forbidden transitions. To create a proof-of-concept system, we synthesized the novel nuclear spin-free complex ECr(C3S5)(3-) with precisely tuned zero-field splitting parameters that create two spectroscopically addressable transitions, with one being a forbidden transition. Pulsed electron paramagnetic resonance (EPR) measurements enabled the investigation of the coherent lifetimes (T-2) and quantum control (Rabi oscillations) for two transitions, one allowed and one forbidden, within the S = 3/2 spin manifold. This investigation represents a step forward in the development of high-spin species as a pathway to scalable QC systems within magnetic molecules.
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