Exploring Photogenerated Molecular Quartet States as Spin Qubits and Qudits

Maximilian Mayländer; Su Chen; Emmaline R. Lorenzo; Michael R. Wasielewski; Sabine Richert

doi:10.1021/jacs.1c01620

Exploring Photogenerated Molecular Quartet States as Spin Qubits and Qudits

Maximilian Mayländer, Su Chen, Emmaline R. Lorenzo, Michael R. Wasielewski^*, Sabine Richert

^*Corresponding author for this work

Chemistry

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

52 Scopus citations

Abstract

Photogenerated molecular spin systems hold great promise for applications in quantum information science because they can be prepared in well-defined spin states at modest temperatures, they often exhibit long coherence times, and their properties can be tuned by chemical synthesis. Here, we investigate a molecular spin system composed of a 1,6,7,12-tetra(4-tert-butylphenoxy)perylene-3,4:9,10-bis(dicarboximide) (PDI) chromophore covalently linked to a stable nitroxide radical (TEMPO) by optical and electron paramagnetic resonance (EPR) techniques. Upon photoexcitation of the spin system, a quartet state is formed as confirmed by transient nutation experiments. This quartet state has spin polarization lifetimes longer than 0.1 ms and is characterized by relatively long coherence times of ∼1.8 μs even at 80 K. Rabi oscillation experiments reveal that more than 60 single-qubit logic operations can be performed with this system at 80 K. The large magnitude of the nitroxide 14N hyperfine coupling in the quartet state of PDI-TEMPO is resolved in the transient EPR spectra and leads to a further splitting of the quartet state electron spin sublevels. We discuss the properties of this photogenerated multilevel system, comprising 12 electron-nuclear spin states, in the context of its viability as a qubit for applications in quantum information science.

Original language	English (US)
Pages (from-to)	7050-7058
Number of pages	9
Journal	Journal of the American Chemical Society
Volume	143
Issue number	18
DOIs	https://doi.org/10.1021/jacs.1c01620
State	Published - May 12 2021

Funding

This work was supported by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) Project number 417643975 (S.R.). S.R. expresses her gratitude to Prof. S. Weber (University of Freiburg, Germany) for providing her access to his EPR instrumentation and equipment. Work at Northwestern University was supported by the Center for Molecular Quantum Transduction and the Energy Frontier Research Center funded by DOE, Office of Science, BES under Award DE-SC0021314. E.R.L. was supported by a U.S. National Science Foundation Graduate Research Fellowship (DGE-1842165).

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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10.1021/jacs.1c01620

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title = "Exploring Photogenerated Molecular Quartet States as Spin Qubits and Qudits",

abstract = "Photogenerated molecular spin systems hold great promise for applications in quantum information science because they can be prepared in well-defined spin states at modest temperatures, they often exhibit long coherence times, and their properties can be tuned by chemical synthesis. Here, we investigate a molecular spin system composed of a 1,6,7,12-tetra(4-tert-butylphenoxy)perylene-3,4:9,10-bis(dicarboximide) (PDI) chromophore covalently linked to a stable nitroxide radical (TEMPO) by optical and electron paramagnetic resonance (EPR) techniques. Upon photoexcitation of the spin system, a quartet state is formed as confirmed by transient nutation experiments. This quartet state has spin polarization lifetimes longer than 0.1 ms and is characterized by relatively long coherence times of ∼1.8 μs even at 80 K. Rabi oscillation experiments reveal that more than 60 single-qubit logic operations can be performed with this system at 80 K. The large magnitude of the nitroxide 14N hyperfine coupling in the quartet state of PDI-TEMPO is resolved in the transient EPR spectra and leads to a further splitting of the quartet state electron spin sublevels. We discuss the properties of this photogenerated multilevel system, comprising 12 electron-nuclear spin states, in the context of its viability as a qubit for applications in quantum information science.",

author = "Maximilian Mayl{\"a}nder and Su Chen and Lorenzo, {Emmaline R.} and Wasielewski, {Michael R.} and Sabine Richert",

note = "Funding Information: This work was supported by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) Project number 417643975 (S.R.). S.R. expresses her gratitude to Prof. S. Weber (University of Freiburg, Germany) for providing her access to his EPR instrumentation and equipment. Work at Northwestern University was supported by the Center for Molecular Quantum Transduction and the Energy Frontier Research Center funded by DOE, Office of Science, BES under Award DE-SC0021314. E.R.L. was supported by a U.S. National Science Foundation Graduate Research Fellowship (DGE-1842165). Publisher Copyright: {\textcopyright} 2021 American Chemical Society. All rights reserved.",

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N1 - Funding Information: This work was supported by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) Project number 417643975 (S.R.). S.R. expresses her gratitude to Prof. S. Weber (University of Freiburg, Germany) for providing her access to his EPR instrumentation and equipment. Work at Northwestern University was supported by the Center for Molecular Quantum Transduction and the Energy Frontier Research Center funded by DOE, Office of Science, BES under Award DE-SC0021314. E.R.L. was supported by a U.S. National Science Foundation Graduate Research Fellowship (DGE-1842165). Publisher Copyright: © 2021 American Chemical Society. All rights reserved.

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N2 - Photogenerated molecular spin systems hold great promise for applications in quantum information science because they can be prepared in well-defined spin states at modest temperatures, they often exhibit long coherence times, and their properties can be tuned by chemical synthesis. Here, we investigate a molecular spin system composed of a 1,6,7,12-tetra(4-tert-butylphenoxy)perylene-3,4:9,10-bis(dicarboximide) (PDI) chromophore covalently linked to a stable nitroxide radical (TEMPO) by optical and electron paramagnetic resonance (EPR) techniques. Upon photoexcitation of the spin system, a quartet state is formed as confirmed by transient nutation experiments. This quartet state has spin polarization lifetimes longer than 0.1 ms and is characterized by relatively long coherence times of ∼1.8 μs even at 80 K. Rabi oscillation experiments reveal that more than 60 single-qubit logic operations can be performed with this system at 80 K. The large magnitude of the nitroxide 14N hyperfine coupling in the quartet state of PDI-TEMPO is resolved in the transient EPR spectra and leads to a further splitting of the quartet state electron spin sublevels. We discuss the properties of this photogenerated multilevel system, comprising 12 electron-nuclear spin states, in the context of its viability as a qubit for applications in quantum information science.

AB - Photogenerated molecular spin systems hold great promise for applications in quantum information science because they can be prepared in well-defined spin states at modest temperatures, they often exhibit long coherence times, and their properties can be tuned by chemical synthesis. Here, we investigate a molecular spin system composed of a 1,6,7,12-tetra(4-tert-butylphenoxy)perylene-3,4:9,10-bis(dicarboximide) (PDI) chromophore covalently linked to a stable nitroxide radical (TEMPO) by optical and electron paramagnetic resonance (EPR) techniques. Upon photoexcitation of the spin system, a quartet state is formed as confirmed by transient nutation experiments. This quartet state has spin polarization lifetimes longer than 0.1 ms and is characterized by relatively long coherence times of ∼1.8 μs even at 80 K. Rabi oscillation experiments reveal that more than 60 single-qubit logic operations can be performed with this system at 80 K. The large magnitude of the nitroxide 14N hyperfine coupling in the quartet state of PDI-TEMPO is resolved in the transient EPR spectra and leads to a further splitting of the quartet state electron spin sublevels. We discuss the properties of this photogenerated multilevel system, comprising 12 electron-nuclear spin states, in the context of its viability as a qubit for applications in quantum information science.

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Exploring Photogenerated Molecular Quartet States as Spin Qubits and Qudits

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