Quantum Dot–Organic Molecule Conjugates as Hosts for Photogenerated Spin Qubit Pairs

Lee, Autumn Y.; Colleran, Troy A.; Jain, Amisha; Niklas, Jens; Rugg, Brandon K.; Mani, Tomoyasu; Poluektov, Oleg G.; Olshansky, Jacob H.

doi:10.1021/jacs.2c11952

Title: Quantum Dot–Organic Molecule Conjugates as Hosts for Photogenerated Spin Qubit Pairs

Journal Article · Wed Feb 08 00:00:00 UTC 2023 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.2c11952 · OSTI ID:1959944

Lee, Autumn Y. ^[1]; Colleran, Troy A. ^[1];

^[1];

^[2]; Rugg, Brandon K. ^[3];

^[4];

^[2];

^[1]

Amherst College, MA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
University of Connecticut, Storrs, CT (United States)

The inherent spin polarization present in photogenerated spin-correlated radical pairs makes them promising candidates for quantum computing and quantum sensing applications. The spin states of these systems can be probed and manipulated with microwave pulses using electron paramagnetic resonance spectrometers. However, to date, there are no reports on magnetic resonance-based spin measurements of photogenerated spin-correlated radical pairs hosted on quantum dots. In the current work, we prepare dye molecule-inorganic quantum dot conjugates and show that they can produce photogenerated spin-polarized states. The dye molecule, D131, is chosen for its ability to undergo efficient charge separation, and the nanoparticle materials, ZnO quantum dots, are chosen for their promising spin properties. Transient and steady state optical spectroscopy performed on ZnO quantum dot-D131 conjugates shows that reversible photogenerated charge separation is occurring. Transient and pulsed electron paramagnetic resonance experiments are then performed on the photogenerated radical pair, which demonstrate that (1) the radical pair is polarized at moderate temperatures and well modeled by existing theories and (2) the spin states can be accessed and manipulated with microwave pulses. In conclusion, this work opens the door to a new class of promising qubit materials that can be photogenerated in polarized states and hosted by highly tailorable inorganic nanoparticles.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-06CH11357; AC36-08GO28308

OSTI ID:: 1959944

Report Number(s):: NREL/JA--5900-84464; MainId:85237; UUID:99607881-7ac9-4e6d-b6b6-1e2405307839; MainAdminID:68618

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 8 Vol. 145; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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