Rahul Soni, Nathan S. Nichols, Sutirtha Paul, Garfield Warren, Paul Sokol and Adrian Del Maestro
Atomic-scale modification of mesopore interfaces provides a route to tune the confinement experienced by adsorbed fluids, but how a specific interface preparation translates into the resulting microscopic confinement potential remains unclear. Here, we show that preplating MCM-41 with an argon monolayer modifies the effective pore interface by occupying strongly attractive regions of the heterogeneous silica surface and screening its atomic-scale corrugation. Grand-canonical Monte Carlo simulations of argon adsorption, low-temperature molecular dynamics, and helium test-particle insertion are combined with adsorption isotherms and neutron-scattering measurements to characterize the preplated pore at the atomic scale. Helium test-particle insertion calculations show that the modified interface shifts the helium adsorption minimum to an annular region inside the pore and produces a confinement landscape dominated by a smooth radial component. The resulting radial confinement potential can be described by a continuum cylindrical model, providing microscopic support for the effective potential used in earlier quantum Monte Carlo studies. Residual corrugation persists over multiple spatial scales and is accurately captured by a Gaussian process surrogate. These results demonstrate how atomic preplating can tailor nanopore confinement and provide an experimentally constrained microscopic potential for predictive studies of confined quantum fluids.
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This work was performed with support from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award Number DE-SC0024333. Nathan S. Nichols was supported by the Office of Science, U.S. Department of Energy, under contract DE-AC02-06CH11357.
