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

Research output: Contribution to journalArticlepeer-review

30 Scopus citations


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 languageEnglish (US)
Pages (from-to)7050-7058
Number of pages9
JournalJournal of the American Chemical Society
Issue number18
StatePublished - May 12 2021

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry
  • Biochemistry
  • Colloid and Surface Chemistry


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