Long-lived selective spin echoes in dipolar solids under periodic and aperiodic pi-pulse trains

The application of Carr-Purcell-Meiboom-Gill (CPMG) π-trains for dynamically decoupling a system from its environment has been extensively studied in a variety of physical systems. When applied to dipolar solids, recent experiments have demonstrated that CPMG pulse trains can generate long-lived spin echoes. While there still remains some controversy as to the origins of these long-lived spin echoes under the CPMG sequence, there is a general agreement that pulse errors during the π-pulses are a necessary requirement. In this work, we develop a theory to describe the spin dynamics in dipolar coupled spin-1/2 system under a CPMG$φ₁,φ₂$ pulse train, where φ₁ and φ₂ are the phases of the π-pulses. From our theoretical framework, the propagator for the CPMG$φ₁,φ₂$ pulse train is equivalent to an effective "pulsed" spin-locking of single-quantum coherences with phase pmfrac{φ₂-3φ₁}{2}, which generates a periodic quasiequilibrium that corresponds to the long-lived echoes. Numerical simulations, along with experiments on both magnetically dilute, random spin networks found in C₆₀ and C₇₀ and in non-dilute spin systems found in adamantane and ferrocene, were performed and confirm the predictions from the proposed theory.