13C Spin–Lattice Relaxation in Natural Diamond: Zeeman Relaxation at 4.7 T and 300 K Due to Fixed Paramagnetic Nitrogen Defects

Abstract 13 C spin–lattice relaxation times in the laboratory frame, ranging from 1.4 to 36 h, have been measured on a suite of five natural type Ia and Ib diamonds at 4.7 T and 300 K. Each of the diamonds contains two types of fixed paramagnetic centers with overlapping inhomogeneous electron paramagnetic resonance (EPR) lines. EPR techniques have been employed to identify these defects and to determine their concentrations and relaxation times at X-band. Spin–lattice relaxation behavior of 13 C in diamonds containing paramagnetic P1, P2, N2, and N3 centers are discussed. Depending on the paramagnetic impurity types and concentrations present in each diamond, three different nuclear spin–lattice relaxation (SLR) paths exist, namely that due to electron SLR mechanisms and two types of three-spin processes (TSPs). The one three-spin process (TSP1) involves a simultaneous transition of two electron spins belonging to the same hyperfine EPR line and a flip of a 13 C spin, while the other process (TSP2) involves two electron spins belonging to different hyperfine EPR lines and a 13 C spin. It is shown that the thermal contact between the 13 C nuclear Zeeman and electron dipole–dipole interaction reservoirs is field dependent, thus forming a bottleneck in the 13 C relaxation path due to TSP1 at high magnetic fields.