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Molecular qubits are an emerging platform in quantum information science (QIS) due to the unmatched structural control that chemical design and synthesis provide compared to other leading qubit technologies. This theoretical study investigates pulse sequence protocols for spin-correlated radical pairs (SCRPs), which are important molecular spin qubit pair (SQP) candidates. Here, we introduce improved microwave pulse protocols for enhancing the execution times of quantum logic gates based on SQPs. Significantly, this study demonstrates that the proposed pulse sequences selectively remove certain contributions from nuclear spin effects on spin dynamics, which are a common source of decoherence. Additionally, we have analyzed the factors that control the fidelity of the SQP spin state following application of the CNOT gate. It was found that higher magnetic fields introduce a high frequency oscillation in the fidelity. Thereupon, it is suggested that further research should be geared towards executing quantum gates at lower magnetic field values. In addition, an absolute bound of the fidelity outcome due to decoherence is determined, which clearly identifies the important factors that control gate execution. Finally, examples of the application of these pulse sequences to SQPs are described. 

Molecular spins are promising building blocks of future quantum technologies thanks to the unparalleled flexibility provided by chemistry, which allows the design of complex structures targeted for specific applications. However, their weak interaction with external stimuli makes it difficult to access their state at the single-molecule level, a fundamental tool for their use, for example, in quantum computing and sensing. Here, an innovative solution exploiting the interplay between chirality and magnetism using the chirality-induced spin selectivity effect on electron transfer processes is foreseen. It is envisioned to use a spin-to-charge conversion mechanism that can be realized by connecting a molecular spin qubit to a dyad where an electron donor and an electron acceptor are linked by a chiral bridge. By numerical simulations based on realistic parameters, it is shown that the chirality-induced spin selectivity effect could enable initialization, manipulation, and single-spin readout of molecular qubits and qudits even at relatively high temperatures. 

Organic trisradicals featuring three-fold symmetry have attracted significant interest because of their unique magnetic properties associated with spin frustration. Herein, we describe the synthesis and characterization of a triangular prism-shaped organic cage for which we have coined the name PrismCage6+ and its trisradical trication—TR3(•+). PrismCage6+ is composed of three 4,4'-bipyridinium dications and two 1,3,5-phenylene units bridged by six methylene groups. In the solid state, PrismCage6+ adopts a highly twisted conformation with close to C3 symmetry as a result of encapsulating one PF6− anion as a guest. PrismCage6+ undergoes stepwise reduction to its mono-, di- and trisradical cations in MeCN on account of strong electronic communication between its 4,4'-bipyridinium units. TR3(•+), which is obtained by reduction of PrismCage6+ employing CoCp2, adopts a triangular prism-shaped conformation with close to C2v symmetry in the solid state. Temperature-dependent continuous-wave and nutation frequency-selective EPR spectra of TR3(•+) in frozen N,N-dimethylformamide indicate its doublet ground state. The doublet-quartet energy gap of TR3(•+) is estimated to be −0.06 kcal mol−1 and the critical temperature of spin-state conversion is found to be ca. 50 K, suggesting that it displays pronounced spin-frustration at the molecular level. To the best of our knowledge, this example is the first organic radical cage to exhibit spin frustration. The trisradical trication of PrismCage6+ opens up new possibilities for fundamental investigations and potential applications in the fields of both organic cages and spin chemistry.