Tunable Spin Qubit Pairs in Quantum Dot–Molecule Conjugates

Lee, Autumn Y.; Teferi, Mandefro; Hernandez, Frida S.; Jain, Amisha; Tran, Tiffany; Wang, Kefu; Mani, Tomoyasu; Schwartzberg, Adam M.; Tang, Ming Lee; Niklas, Jens; Poluektov, Oleg G.; Olshansky, Jacob H.

doi:10.1021/acsnano.5c00288

Title: Tunable Spin Qubit Pairs in Quantum Dot–Molecule Conjugates

Journal Article · 19 March 2025 · ACS Nano

DOI: https://doi.org/10.1021/acsnano.5c00288 · OSTI ID:2532480

^[1]; Teferi, Mandefro ^[2]; Hernandez, Frida S. ^[1];

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^[4]; Schwartzberg, Adam M. ^[5];

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Amherst College, MA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
University of Utah, Salt Lake City, UT (United States)
University of Connecticut, Storrs, CT (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Organic molecules and quantum dots (QDs) have both shown promise as materials that can host quantum bits (qubits). This is in part because of their synthetic tunability. The current work employs a combination of both materials to demonstrate a series of tunable quantum dot–organic molecule conjugates that can both host photogenerated spin-based qubit pairs (SQPs) and sensitize molecular triplet states. The photogenerated qubit pairs, composed of a spin-correlated radical pair (SCRP), are particularly intriguing since they can be initialized in well-defined, nonthermally populated, quantum states. Additionally, the radical pair enables charge recombination to a polarized molecular triplet state, also in a well-defined quantum state. The materials underlying this system are an organic molecular chromophore and electron donor, 9,10-bis(phenylethynyl)anthracene, and a quantum dot acceptor composed of ZnO. We prepare a series of quantum dot–molecule conjugates that possess variable quantum dot size and two different linker lengths connecting the two moieties. Optical spectroscopy revealed that the QD–molecule conjugates undergo photoexcited charge separation to generate long-lived charge-separated radical pairs. The resulting spin states are probed using light-induced time-resolved electron paramagnetic resonance (TR-EPR) spectroscopy, revealing the presence of singlet-generated SCRPs and molecular triplet states. Notably, the EPR spectra of the radical pairs are dependent on the geometry of this highly tunable system. The g value of the ZnO QD anion is size tunable, and the line widths are influenced by radical pair separation. Overall, this work demonstrates the power of synthetic tunability in adjusting the spin specific addressability, satisfying a key requirement of functional qubit systems.

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Research Organization:: Amherst College, MA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: Air Force of Scientific Research (AFOSR); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357

OSTI ID:: 2532480

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 12 Vol. 19; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Tunable Spin Qubit Pairs in Quantum Dot–Molecule Conjugates

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