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The surface of hydrogen-terminated diamond (H-terminated diamond) supports a p-type surface conductivity when interfaced with high electron-affinity surface acceptors through the surface transfer doping process. High electron-affinity transition metal oxides (TMOs), such as MoO3, have been regarded as superior candidates in surface transfer doping of diamond, holding great promise for enabling practical diamond electronic devices. In this work, a simple, solution-processed method is demonstrated to deposit a molybdenum trioxide (MoO3) layer on H-terminated diamond surface to achieve surface transfer doping of diamond. The surface of diamond following the deposition of solution-processed MoO3 (sp-MoO3) experienced significant reduction in sheet resistivity, corresponding to an increase in hole density, compared with the pristine air-doped diamond. This hole accumulation layer induced by sp-MoO3 is thermally stable up to 450 °C, and demonstrates metallic conductivity down to 250 mK with a strong spin-orbit interaction (SOI) in the induced two-dimensional (2D) surface conducting layer. Our study demonstrates that sp-MoO3 is comparable with thermally-evaporated MoO3 in doping performance but with great advantage as a simple, inexpensive and highly flexible fabrication method for developing diamond electronics.

Hydrogen-terminated (H-terminated) diamond, when surface transfer doped, can support a sub-surface two-dimensional (2D) hole band that possesses a strong Rashba-type spin–orbit interaction. By incorporating a V2O5/Al2O3 bilayer gate dielectric in a diamond-based metal–oxide–semiconductor architecture, metallic surface conductivity can be maintained at low temperature, avoiding the carrier freeze out exhibited by devices with an Al2O3 gate dielectric alone. Hole densities of up to 2.5 × 1013 cm−2 are achieved by the electrostatic gating of the device, and the spin–orbit interaction strength can be tuned from 3.5 ± 0.5 meV to 8.4 ± 0.5 meV, with a concurrent reduction in the spin coherence length from 40 ± 1 nm to 27 ± 1 nm. The demonstration of a gated device architecture on the H-terminated that avoids the need to cycle the temperature, as is required for ionic liquid gating protocols, opens a pathway to engineering practical devices for the study and application of spin transport in diamond.

Surface transfer doping of diamond using high electron affinity transition metal oxides (TMOs), such as MoO3, has emerged as a key enabling technology for the development of diamond-based surface two-dimensional (2D) electronics. However, the omission of a critical pre-annealing step in the device fabrication process to remove atmospheric adsorbates prior to TMO deposition, as seen in numerous studies, makes the role of TMOs ambiguous in light of air-induced surface conductivity, preventing a full understanding of the intrinsic surface transfer doping behavior of TMO-based surface acceptors. Here, using in-situ four-probe electrical measurements we explicitly show the insulating-to-conducting transition in diamond surface driven by MoO3 induced surface transfer doping. Variable-temperature Hall-effect measurements reveal weak temperature-dependence down to 250 mK, evidencing the 2D Fermi liquid nature of the resulting surface conducting channel on diamond. Using first-principles calculations, we confirm the interfacial charge exchange upon MoO3 adsorption leading to a degenerate hole conducting layer on diamond. This work provides significant insights into understanding the surface transfer doping of diamond induced by TMOs, and paves the way for the investigations of many interesting quantum transport properties in the resulting 2D hole conducting layer, such as phase-coherent magnetotransport, on diamond surface.