Nuclear double resonance between statistical spin polarizations

We demonstrate nuclear double resonance for nanometer-scale volumes of spins where random fluctuations rather than Boltzmann polarization dominate. When the Hartmann-Hahn condition is met in a cross-polarization experiment, flip-flops occur between two species of spins and their fluctuations become coupled. We use magnetic resonance force microscopy to measure this effect between H1 and C13 spins in C13-enriched stearic acid. The development of a cross-polarization technique for statistical ensembles adds an important tool for generating chemical contrast in nanometer-scale magnetic resonance. © 2009 The American Physical Society.