Spin counting is an experimental NMR technique where Multiple Quantum Coherences (MQCOs) are created between dipolar or J-coupled nuclear spins. In such experiments, a coherence is defined as a multiple spin transition (forbidden but made allowable by spinspin coupling) from different ground states to the same excited state at the same time and with the same phase . The number of neighboring nuclei, the distances between them and the uniformity of their spatial arrangements determine the number of MQCOs one can detect ? , along with the mode of MQCO excitation ? . While traditional MQ-NMR employs standard phase cycling to select each coherence order in a separate experiment, MQ-SC experiments increment the phase of either the excitation or reconversion block, allowing for different coherence evolution in a single experiment ? (Figure ). MQ-NMR spin counting still requires multiple experiments to extract the individual frequencies of each coherence order, which is either done via a 2D experiment with time-proportional phase incrementation, in which the excitation pulse phase increment is proportional to the t 1 evolution or via a pseudo 2D experiment with the excitation pulse phase incremented and directly detected in the t 2 dimension 33? . MQ-SC has been performed on crystals 26? -31 , liquid crystals , minerals , catalysts/zeolites , glasses , molecules , amorphous semiconductors , hybrid materials 50 , thin films/polymers , diamond surfaces ? , and peptides/proteins , all under static or varying MAS rates with various nuclear spins (S=1/2 and 3/2 ) and employing zero quantum, single quantum, double quantum (DQ), or triple quantum (TQ) propagators. The aforementioned extensive history of successful spin counting experiments demonstrates it as a reliable technique, however MQ-SC under DNP conditions of solution species vitrified in a frozen matrix has never been performed by any study reported to date to our knowledge. Our critical case study provides an avenue for future studies of solution intermediate states, showing the feasibility of quickly analyzing these otherwise indistinguishable spectroscopic signatures, even when suffering from low sensitivity.