University of Perugia

Whether hydrogen sulphide physisorbs or dissociates on nanoscale refractory oxide surfaces had been hard to settle because the configuration space is too large to enumerate. This work pairs unbiased automated adsorption sampling with an off-the-shelf atomistic foundation model: MACE's MPA screens candidate minima, each survivor is re-optimised with PBE-D2*(N) and HSE06 DFT, and DFT multiconfigurational infrared spectra are compared with in situ spectra at 150 K. The computed spectra reproduce the red-shift order of the H–S stretch across the three materials: silica at 2603 cm⁻¹, forsterite at 2588 cm⁻¹ and MgO at 2504 cm⁻¹.

Whether hydrogen sulphide physisorbs or dissociates on nanoscale refractory oxide surfaces had been hard to settle because the configuration space is too large to enumerate. This work pairs unbiased automated adsorption sampling with an off-the-shelf atomistic foundation model: MACE's MPA screens candidate minima, each survivor is re-optimised with PBE-D2*(N) and HSE06 DFT, and DFT multiconfigurational infrared spectra are compared with in situ spectra at 150 K. The computed spectra reproduce the red-shift order of the H–S stretch across the three materials: silica at 2603 cm⁻¹, forsterite at 2588 cm⁻¹ and MgO at 2504 cm⁻¹.