Modulation has been understood and used to explain physical properties in solid-state materials for many years. Molecular modulated structures relatively scarce, but due to technological advances can no longer be ignored. Systematic variable temperature studies of the derivatives of Barluenga's Reagent has shed some light on why some of these salts exhibit modulation. Application of pressure allows the exploration of more of the phase diagram allowing access to new states and expanding our knowledge. A better understanding of the causes of modulation in simple molecular systems will aid our treatment of the pathological cases where solution currently eludes us.