By appending a 'pump-refocus' block to an arbitrary pulse sequence it is possible to simultaneously measure both in-and anti-phase coherences, and by repeating the experiment with the pump and detection frequencies switched the expectation values of all eight single-quantum coherences can be observed (Table ). This can be further extended to perform quantum state tomography by the addition of the pairs of operations outlined above, resulting in the proposed DEER Assisted Tomography (DEERATom) procedure (Figure ). Note that by moving the pump pulse through the refocussing period the in-and anti-phase coherences become effectively 'phase-labelled', a technique earlier used to facilitate the quantum state tomography of a hybrid electron-nuclear system. 9