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 -mesityl-1,8-naphthalimide () and its phosphorus analogues, 2-mesitylbenzoisophosphinoline () and 2-mesitylbenzoisophosphinoline oxide () results in ultrafast spin-orbit charge-transfer intersystem crossing to form the corresponding phosphorescent triplet states , and . The ultrafast triplet formation dynamics, phosphorescence, and spin-polarized EPR spectra of these triplet states were examined. The most promising qubit candidate, , 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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