Here, we present novel 31 P NMR spin counting studies of both powdered and vitrified phosphate-containing samples, for which we have extracted the minimum number of dipolar coupled spins via the creation of multiple even and odd quantum coherence orders 62 using the SR2 8 pulse sequence (see Figure and Listing 2, Supporting Information) , where the overall phase of the excitation block is incremented in a pseudo 2D mode to extract the MQCOs. The SR2 pulse sequence is an R-symmetry based double quantum recoupling sequence which works with a low radio frequency power requirement equal to half the spinning frequency, hence permitting longer recoupling times. The SR2 pulse sequence is a non-gamma encoded sequence and is a super cycled version of R2 , described as π/2-pulsesandwiched R2 1 8 R2 -1 8 pulse sequence which has a duration of 16 rotor periods as shown in Figure . Longer recoupling times are required to generate the higher multiple quantum coherences. We also present a novel method for analyzing MQ-SC data, for which we extract individual frequencies of the spin transitions using knowledge based fitting with n (integer) multiple of cosine waves, allowing for more physically meaningful extraction of the minimum bound of coupled nuclear spins when compared to the traditional Fourier transform which can generate nonphysical frequencies.