Using Photoexcited Core/Shell Quantum Dots to Spin Polarize Appended Radical Qubits

Jacob H. Olshansky; Samantha M. Harvey; Makenna L. Pennel; Matthew D. Krzyaniak; Richard D. Schaller; Michael R. Wasielewski

doi:10.1021/jacs.0c06073

Using Photoexcited Core/Shell Quantum Dots to Spin Polarize Appended Radical Qubits

Jacob H. Olshansky, Samantha M. Harvey, Makenna L. Pennel, Matthew D. Krzyaniak, Richard D. Schaller, Michael R. Wasielewski^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

16 Scopus citations

Abstract

The synthetic tunability, flexibility, and rich spin physics of semiconductor quantum dots (QDs) make them promising candidates for quantum information science applications. However, the rapid spin relaxation observed in colloidal quantum dots limits their functionality. In the current work, we demonstrate a method to harness photoexcited spin states in QDs to produce long-lived spin polarization on an appended organic ligand molecule. We present a system composed of CdSe/CdS core/shell QDs, covalently linked to naphthalenediimide (NDI) electron-accepting molecules. The electron transfer dynamics from photoexcited QDs to the appended NDI ligands is explored as a function of both shell thickness and number of NDIs per QD. Transient EPR spectroscopy shows that the photoexcited QDs strongly spin polarize the NDI radical anion, which is interpreted in the context of both the radical pair and the triplet mechanisms of spin polarization. This work serves as an initial step toward using photoexcited QDs to strongly spin polarize organic radicals having long spin relaxation times to serve as spin qubits in quantum information science applications.

Original language	English (US)
Pages (from-to)	13590-13597
Number of pages	8
Journal	Journal of the American Chemical Society
Volume	142
Issue number	31
DOIs	https://doi.org/10.1021/jacs.0c06073
State	Published - Aug 5 2020

ASJC Scopus subject areas

Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry

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@article{9ed8a58a5fbb4097b2e4985071e3b965,

title = "Using Photoexcited Core/Shell Quantum Dots to Spin Polarize Appended Radical Qubits",

abstract = "The synthetic tunability, flexibility, and rich spin physics of semiconductor quantum dots (QDs) make them promising candidates for quantum information science applications. However, the rapid spin relaxation observed in colloidal quantum dots limits their functionality. In the current work, we demonstrate a method to harness photoexcited spin states in QDs to produce long-lived spin polarization on an appended organic ligand molecule. We present a system composed of CdSe/CdS core/shell QDs, covalently linked to naphthalenediimide (NDI) electron-accepting molecules. The electron transfer dynamics from photoexcited QDs to the appended NDI ligands is explored as a function of both shell thickness and number of NDIs per QD. Transient EPR spectroscopy shows that the photoexcited QDs strongly spin polarize the NDI radical anion, which is interpreted in the context of both the radical pair and the triplet mechanisms of spin polarization. This work serves as an initial step toward using photoexcited QDs to strongly spin polarize organic radicals having long spin relaxation times to serve as spin qubits in quantum information science applications.",

author = "Olshansky, {Jacob H.} and Harvey, {Samantha M.} and Pennel, {Makenna L.} and Krzyaniak, {Matthew D.} and Schaller, {Richard D.} and Wasielewski, {Michael R.}",

note = "Funding Information: This work was supported by the Department of Energy, Office of Science, Office of Basic Energy Sciences Award DE-SC0020168 (M.R.W.) S.M.H was supported by the National Science Foundation Graduate Research Fellowship Program under Grant No. DGE-1324585. M.P. would like to acknowledge the International Institute of Nanotechnology summer undergraduate research experience. This material is based upon work supported by the National Science Foundation (NSF) under Grant Number EEC-1757618. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the NSF. This work was performed, in part, at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. This work also made use of the EPIC facility of Northwestern University{\textquoteright}s NU ANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205), the MRSEC program (NSF DMR-1720139) at the Materials Research Center, the International Institute for Nanotechnology (IIN), the Keck Foundation, and the State of Illinois, through the IIN. Publisher Copyright: Copyright {\textcopyright} 2020 American Chemical Society.",

year = "2020",

month = aug,

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doi = "10.1021/jacs.0c06073",

language = "English (US)",

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T1 - Using Photoexcited Core/Shell Quantum Dots to Spin Polarize Appended Radical Qubits

AU - Olshansky, Jacob H.

AU - Harvey, Samantha M.

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AU - Krzyaniak, Matthew D.

AU - Schaller, Richard D.

AU - Wasielewski, Michael R.

N1 - Funding Information: This work was supported by the Department of Energy, Office of Science, Office of Basic Energy Sciences Award DE-SC0020168 (M.R.W.) S.M.H was supported by the National Science Foundation Graduate Research Fellowship Program under Grant No. DGE-1324585. M.P. would like to acknowledge the International Institute of Nanotechnology summer undergraduate research experience. This material is based upon work supported by the National Science Foundation (NSF) under Grant Number EEC-1757618. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the NSF. This work was performed, in part, at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. This work also made use of the EPIC facility of Northwestern University’s NU ANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205), the MRSEC program (NSF DMR-1720139) at the Materials Research Center, the International Institute for Nanotechnology (IIN), the Keck Foundation, and the State of Illinois, through the IIN. Publisher Copyright: Copyright © 2020 American Chemical Society.

PY - 2020/8/5

Y1 - 2020/8/5

N2 - The synthetic tunability, flexibility, and rich spin physics of semiconductor quantum dots (QDs) make them promising candidates for quantum information science applications. However, the rapid spin relaxation observed in colloidal quantum dots limits their functionality. In the current work, we demonstrate a method to harness photoexcited spin states in QDs to produce long-lived spin polarization on an appended organic ligand molecule. We present a system composed of CdSe/CdS core/shell QDs, covalently linked to naphthalenediimide (NDI) electron-accepting molecules. The electron transfer dynamics from photoexcited QDs to the appended NDI ligands is explored as a function of both shell thickness and number of NDIs per QD. Transient EPR spectroscopy shows that the photoexcited QDs strongly spin polarize the NDI radical anion, which is interpreted in the context of both the radical pair and the triplet mechanisms of spin polarization. This work serves as an initial step toward using photoexcited QDs to strongly spin polarize organic radicals having long spin relaxation times to serve as spin qubits in quantum information science applications.

AB - The synthetic tunability, flexibility, and rich spin physics of semiconductor quantum dots (QDs) make them promising candidates for quantum information science applications. However, the rapid spin relaxation observed in colloidal quantum dots limits their functionality. In the current work, we demonstrate a method to harness photoexcited spin states in QDs to produce long-lived spin polarization on an appended organic ligand molecule. We present a system composed of CdSe/CdS core/shell QDs, covalently linked to naphthalenediimide (NDI) electron-accepting molecules. The electron transfer dynamics from photoexcited QDs to the appended NDI ligands is explored as a function of both shell thickness and number of NDIs per QD. Transient EPR spectroscopy shows that the photoexcited QDs strongly spin polarize the NDI radical anion, which is interpreted in the context of both the radical pair and the triplet mechanisms of spin polarization. This work serves as an initial step toward using photoexcited QDs to strongly spin polarize organic radicals having long spin relaxation times to serve as spin qubits in quantum information science applications.

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Using Photoexcited Core/Shell Quantum Dots to Spin Polarize Appended Radical Qubits

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