High-field Overhauser DNP in silicon below the metal-insulator transition

TL;DR

This study demonstrates hyperpolarization of silicon-29 nuclei in n-doped silicon via an Overhauser mechanism within exchange-coupled donor clusters, achieving significant polarization enhancement at low temperatures.

Contribution

It reveals the Overhauser mechanism as the dominant DNP process in silicon with specific doping levels, highlighting the role of exchange interactions and spin diffusion.

Findings

Achieved a silicon-29 polarization of about 10% after two hours.

Observed a DNP enhancement factor of approximately 244.

Identified exchange-coupled donor clusters as key to the Overhauser mechanism.

Abstract

Single crystal silicon is an excellent system in which to explore dynamic nuclear polarization (DNP), as it exhibits a continuum of properties from metallic to insulating as a function of doping concentration and temperature. At low doping concentrations DNP has been observed to occur via the solid effect, while at very high doping concentrations an Overhauser mechanism is responsible. Here we report the hyperpolarization of 29Si in n-doped silicon crystals, with doping concentrations in the range of 1-3 x 10^17 /cc. In this regime exchange interactions between donors become extremely important. The sign of the enhancement in our experiments and its frequency dependence suggest that the 29Si spins are directly polarized by donor electrons via an Overhauser mechanism within exchange-coupled donor clusters. The exchange interaction between donors only needs to be larger than the silicon hyperfine interaction (typically much smaller than the donor hyperfine coupling) to enable this Overhauser mechanism. Nuclear polarization enhancement is observed for a range of donor clusters in which the exchange energy is comparable to the donor hyperfine interaction. The DNP dynamics are characterized by a single exponential time constant that depends on the microwave power, indicating that the Overhauser mechanism is the rate-limiting step. Since only about 2 % of the silicon nuclei are located within one Bohr radius of the donor electron, nuclear spin diffusion is important in transferring the polarization to all the spins. However, the spin-diffusion time is much shorter than the Overhauser time due to the relatively weak silicon hyperfine coupling strength. In a 2.35 T magnetic field at 1.1 K, we observed a DNP enhancement of $244 +/- 84 resulting in a silicon polarization of $10.4 +/- 3.4 % following two hours of microwave irradiation.