Identifying Sources of Entanglement Loss in Photodriven Molecular Electron Spin Teleportation

Yuheng Huang; Yunfan Qiu; Ryan M. Young; George C. Schatz; Matthew D. Krzyaniak; Michael R. Wasielewski

doi:10.1021/jacs.4c04393

Identifying Sources of Entanglement Loss in Photodriven Molecular Electron Spin Teleportation

Yuheng Huang, Yunfan Qiu, Ryan M. Young, George C. Schatz^*, Matthew D. Krzyaniak^*, Michael R. Wasielewski^*

^*Corresponding author for this work

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

Abstract

We report on an electron donor-electron acceptor-stable radical (D-A-R^•) molecule in which an electron spin state first prepared on R^• is followed by photogeneration of an entangled singlet ¹[D^•+-A^•−] spin pair to produce D^•+-A^•−-R^•. Since the A^•− and R^• spins within D^•+-A^•−-R^• are uncorrelated, spin teleportation from R^• to D^•+ occurs with a maximal 25% efficiency only for the singlet pair ¹(A^•−-R^•) by spin-allowed electron transfer from A^•− to R^•. However, since ¹[D^•+-A^•−] is sufficiently long-lived, coherent spin mixing involving the unreactive ³(A^•−-R^•) population affects entanglement and teleportation within D^•+-A^•−-R^•. Pulse electron paramagnetic resonance experiments show a direct correlation between electron spin flip-flops and entanglement loss, providing information for designing molecular materials to serve as nanoscale quantum device interconnects.

Original language	English (US)
Pages (from-to)	20133-20140
Number of pages	8
Journal	Journal of the American Chemical Society
Volume	146
Issue number	29
DOIs	https://doi.org/10.1021/jacs.4c04393
State	Published - Jul 24 2024

Funding

This work was supported by the National Science Foundation under Award No. CHE-2154627 (M.R.W., synthesis, transient optical and EPR measurements). This research was also supported as part of the Center for Molecular Quantum Transduction, an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Award DE-SC0021314 (R.M.Y., transient optical measurements, G.C.S., theory, and M.D.K., EPR data analysis). H nuclear magnetic resonance (NMR) spectroscopy, and mass spectrometry are conducted in IMSERC facilities at Northwestern University, which have received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-2025633), NSF CHE-1048773, Northwestern University, the State of Illinois, and the International Institute for Nanotechnology (IIN).

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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title = "Identifying Sources of Entanglement Loss in Photodriven Molecular Electron Spin Teleportation",

abstract = "We report on an electron donor-electron acceptor-stable radical (D-A-R•) molecule in which an electron spin state first prepared on R• is followed by photogeneration of an entangled singlet 1[D•+-A•−] spin pair to produce D•+-A•−-R•. Since the A•− and R• spins within D•+-A•−-R• are uncorrelated, spin teleportation from R• to D•+ occurs with a maximal 25% efficiency only for the singlet pair 1(A•−-R•) by spin-allowed electron transfer from A•− to R•. However, since 1[D•+-A•−] is sufficiently long-lived, coherent spin mixing involving the unreactive 3(A•−-R•) population affects entanglement and teleportation within D•+-A•−-R•. Pulse electron paramagnetic resonance experiments show a direct correlation between electron spin flip-flops and entanglement loss, providing information for designing molecular materials to serve as nanoscale quantum device interconnects.",

author = "Yuheng Huang and Yunfan Qiu and Young, {Ryan M.} and Schatz, {George C.} and Krzyaniak, {Matthew D.} and Wasielewski, {Michael R.}",

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doi = "10.1021/jacs.4c04393",

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AU - Huang, Yuheng

AU - Qiu, Yunfan

AU - Young, Ryan M.

AU - Schatz, George C.

AU - Krzyaniak, Matthew D.

AU - Wasielewski, Michael R.

PY - 2024/7/24

Y1 - 2024/7/24

N2 - We report on an electron donor-electron acceptor-stable radical (D-A-R•) molecule in which an electron spin state first prepared on R• is followed by photogeneration of an entangled singlet 1[D•+-A•−] spin pair to produce D•+-A•−-R•. Since the A•− and R• spins within D•+-A•−-R• are uncorrelated, spin teleportation from R• to D•+ occurs with a maximal 25% efficiency only for the singlet pair 1(A•−-R•) by spin-allowed electron transfer from A•− to R•. However, since 1[D•+-A•−] is sufficiently long-lived, coherent spin mixing involving the unreactive 3(A•−-R•) population affects entanglement and teleportation within D•+-A•−-R•. Pulse electron paramagnetic resonance experiments show a direct correlation between electron spin flip-flops and entanglement loss, providing information for designing molecular materials to serve as nanoscale quantum device interconnects.

AB - We report on an electron donor-electron acceptor-stable radical (D-A-R•) molecule in which an electron spin state first prepared on R• is followed by photogeneration of an entangled singlet 1[D•+-A•−] spin pair to produce D•+-A•−-R•. Since the A•− and R• spins within D•+-A•−-R• are uncorrelated, spin teleportation from R• to D•+ occurs with a maximal 25% efficiency only for the singlet pair 1(A•−-R•) by spin-allowed electron transfer from A•− to R•. However, since 1[D•+-A•−] is sufficiently long-lived, coherent spin mixing involving the unreactive 3(A•−-R•) population affects entanglement and teleportation within D•+-A•−-R•. Pulse electron paramagnetic resonance experiments show a direct correlation between electron spin flip-flops and entanglement loss, providing information for designing molecular materials to serve as nanoscale quantum device interconnects.

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Identifying Sources of Entanglement Loss in Photodriven Molecular Electron Spin Teleportation

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