Figure : a. Simulated frequency domain EPR spectrum of compound 1 at 342.9 mT (black) and corresponding sub-spectra corresponding to the nuclear spin states (grey), overlayed with simulated excitation profiles of 80 ns 180° pulses at 𝜈 " (9.54 GHz, blue) and 𝜈 # (9.69 GHz, orange). b. Orientations of the nitroxide spin excited by pulses at 80 ns 180° pulses at 𝜈 " (top) and 𝜈 # (bottom). Simulation parameters and echo-detected field-swept spectra are included in Figure . All simulations were performed using the Matlab toolbox Easyspin. If the pulses used were capable of exciting all electron spins within these nuclear spin manifolds, then one third of the spin centres would be detected as the three nuclear spin states are approximately equally populated. Of these detected spins, the pump pulse would invert one third of their coupled partners, and so one ninth of the molecules in the sample would contribute an oscillatory component to the recorded trace. In reality the pulses only excite a fraction of the spins in each manifold, and so the inter-spin interactions recorded represent an even smaller proportion of molecules corresponding to specific orientations of the nitroxide spin centres with respect to the external magnetic field (Figure ). The background corrected results of the 3P-DEER experiment detected at 𝜈 ) and 𝜈 * are almost identical (Figure , raw data in Figure ), and from these it can be determined that the twoqubit gate time, i.e. the first minimum in the time trace, is 250 ns. Despite being in frozen solution, compound 1 exhibits a narrow distribution of coupling frequencies centred at 2 MHz (Figure , right). This likely a result of the rigidity of the alkyne and phenyl groups connecting the two nitroxide spins, which will limit the distribution of conformations adopted in solution.