First-principles investigations of As-doped tetragonal boron nitride nanosheets for toxic gas sensing applications.

Abstract

Pristine and arsenic-doped tetragonal boron nitride nanosheets (BNNS and As-BNNS) have been reported as potential candidates for toxic gas sensing applications. We have investigated the adsorption behavior of BNNS and As-BNNS for CO2, H2S, and SO3 gas molecules using first-principles density functional theory (DFT). Both BNNS and As-BNNS possess negative cohesive energies of -8.47 and -8.22 eV, respectively, which indicates that both sheets are energetically stable. Successful adsorption is inferred from the negative adsorption energy and structural deformation in the vicinity of the adsorbent and adsorbate. As-doping results in a significant increase in adsorption energies from -0.094, -0.175, and -0.462 eV to -2.748, -2.637, and 3.057 eV for CO2, H2S and SO3 gases, respectively. Due to gas adsorption, the electronic bandgap in As-BNNS varies by approximately 32% compared to a maximum of 24% in BNNS. A notable fluctuation in the energy gap and electrical conductivity is seen, with ambient temperature being the point of maximal sensitivity. For SO3, the maximum charge transfer during adsorption in BNNS and As-BNNS is determined to be 0.08|e| and 0.25|e|, respectively. Due to the interaction with gases, all structures exhibit an extremely high absorption coefficient on the order of 104 cm-1 with minimal peak shifting. Additionally, doping an As atom on BNNS' surface remarkably improved its ability to sense CO2, H2S, and SO3 gasses.