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Molecular Design for Optically Induced Magnetization: Targeting Excited State Orbital Degeneracy in Tungsten(V)
Ian E Ramsier1, Alysia Mandato1, Sunil Saxena1
1Department of Chemistry, University of Pittsburgh, Pittsburgh, Pennsylvania 15213, United States.
Abstract:
The rise of quantum information science has spurred chemists to prepare new molecules that serve as useful building blocks in quantum technologies of the future. Implementation of molecular spin-based qubits requires new methods to induce high spin polarization of samples. Herein, we report design criteria to develop axially symmetric spin-1/2 molecules amenable to optically induced magnetization (OIM), a technique using circularly polarized (CP) excitation to deliver spin polarization. We apply these criteria to develop a series of tungsten(V) chalcogenide complexes that are demonstrated to have large spin-sensitive responses to CP light using magnetic circular dichroism (MCD) that could allow up to ∼20% spin polarization through OIM. Pulsed electron paramagnetic resonance (EPR) spectra reveal these systems have improved relaxation times over molecules like K2IrCl6, a species recently investigated by OIM, and field-swept electron spin-echo (FS-ESE) experiments show they have a remarkable lack of anisotropy in their phase-memory Tm times. The design criteria are general and point toward future ways to improve OIM-initializable qubits.
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