Quantum Dot-Organic Molecule Conjugates as Hosts for Photogenerated Spin Qubit Pairs

Autumn Lee, Troy Colleran, Amisha Jain, Jens Niklas, Brandon Rugg, Tomoyasu Mani, Oleg Poluektov, Jacob Olshansky

Research output: Contribution to journalArticlepeer-review

3 Scopus Citations


The inherent spin polarization present in photogenerated spin-correlated radical pairs makes them promising candidates for quantum computing and quantum sensing applications. The spin states of these systems can be probed and manipulated with microwave pulses using electron paramagnetic resonance spectrometers. However, to date, there are no reports on magnetic resonance-based spin measurements of photogenerated spin-correlated radical pairs hosted on quantum dots. In the current work, we prepare dye molecule-inorganic quantum dot conjugates and show that they can produce photogenerated spin-polarized states. The dye molecule, D131, is chosen for its ability to undergo efficient charge separation, and the nanoparticle materials, ZnO quantum dots, are chosen for their promising spin properties. Transient and steady state optical spectroscopy performed on ZnO quantum dot-D131 conjugates shows that reversible photogenerated charge separation is occurring. Transient and pulsed electron paramagnetic resonance experiments are then performed on the photogenerated radical pair, which demonstrate that (1) the radical pair is polarized at moderate temperatures and well modeled by existing theories and (2) the spin states can be accessed and manipulated with microwave pulses. This work opens the door to a new class of promising qubit materials that can be photogenerated in polarized states and hosted by highly tailorable inorganic nanoparticles.
Original languageAmerican English
Pages (from-to)4372-4377
Number of pages6
JournalJournal of the American Chemical Society
Issue number8
StatePublished - 2023

NREL Publication Number

  • NREL/JA-5900-84464


  • electron paramagnetic resonance spectroscopy
  • electron spin
  • electron transfer
  • photochemistry
  • quantum dot
  • quantum information


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