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 1H and 13C spins in 13C-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.