“…Hydrogenated amorphous silicon (a‐Si:H) and related thin films have been implemented in device applications, including absorbers in thin film solar cells, [ 11–21 ] passivation layers in wafer silicon photovoltaics, [ 22–28 ] and imaging layers in uncooled infrared (IR) sensing microbolometers. [ 29–37 ] The a‐Si:H network varies in terms of incorporated hydrogen content and bonding configuration, [ 23,26,38–41 ] the presence of nanoscale voids and vacancy structures, [ 38,39 ] and film stress [ 42 ] as deduced from experimental measurements. The formation of short and long filamentary structures, bond length distributions, and bond angle distributions has been identified through advanced computational modeling.…”