TY - JOUR
T1 - Spin-Polarized Molecular Triplet States as Qubits
T2 - Phosphorus Hyperfine Coupling in the Triplet State of Benzoisophosphinoline
AU - Christensen, Joseph A.
AU - Zhou, Jiawang
AU - Tcyrulnikov, Nikolai A.
AU - Krzyaniak, Matthew 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 under Award DE-SC0020168 (M.R.W.). The authors thank Dr. Brian T. Phelan and Prof. Ryan M. Young for assistance with the fsTA experiments and for helpful discussions. The authors also thank Prof. Marek B. Majewski for helpful discussions regarding the synthetic procedures.
PY - 2020/9/17
Y1 - 2020/9/17
N2 - Advances in quantum information science (QIS) require the development of new molecular materials to serve as microwave addressable qubits that can be read out optically. Laser photoexcitation of organic π-conjugated molecules often results in spin-polarized phosphorescent triplet states that can be readily observed and manipulated using time-resolved electron paramagnetic resonance (EPR) techniques. Photoexcitation of N-mesityl-1,8-naphthalimide (M-NMI) and its phosphorus analogues, 2-mesitylbenzoisophosphinoline (M-BIPD) and 2-mesitylbenzoisophosphinoline oxide (M-BIPDO) results in ultrafast spin-orbit charge-transfer intersystem crossing to form the corresponding phosphorescent triplet states M-3NMI, M-3BIPD and M-3BIPDO. The ultrafast triplet formation dynamics, phosphorescence, and spin-polarized EPR spectra of these triplet states were examined. The most promising qubit candidate, M-3BIPD, was examined using pulse-EPR to measure its spin relaxation times, and pulse electron-nuclear double resonance spectroscopy to perform a two-qubit CNOT gate using the phosphorus nuclear spin.
AB - Advances in quantum information science (QIS) require the development of new molecular materials to serve as microwave addressable qubits that can be read out optically. Laser photoexcitation of organic π-conjugated molecules often results in spin-polarized phosphorescent triplet states that can be readily observed and manipulated using time-resolved electron paramagnetic resonance (EPR) techniques. Photoexcitation of N-mesityl-1,8-naphthalimide (M-NMI) and its phosphorus analogues, 2-mesitylbenzoisophosphinoline (M-BIPD) and 2-mesitylbenzoisophosphinoline oxide (M-BIPDO) results in ultrafast spin-orbit charge-transfer intersystem crossing to form the corresponding phosphorescent triplet states M-3NMI, M-3BIPD and M-3BIPDO. The ultrafast triplet formation dynamics, phosphorescence, and spin-polarized EPR spectra of these triplet states were examined. The most promising qubit candidate, M-3BIPD, was examined using pulse-EPR to measure its spin relaxation times, and pulse electron-nuclear double resonance spectroscopy to perform a two-qubit CNOT gate using the phosphorus nuclear spin.
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U2 - 10.1021/acs.jpclett.0c01912
DO - 10.1021/acs.jpclett.0c01912
M3 - Article
C2 - 32812766
AN - SCOPUS:85091191450
VL - 11
SP - 7569
EP - 7574
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
SN - 1948-7185
IS - 18
ER -