The authors report their initial studies of the negative resist behavior of neutral sodium atoms deposited on alkanethiol molecules during neutral atom lithographic processing. Their results show that neutral sodium atoms incident upon octadecanethiol, the longest molecule of the various alkanethiols among alkanethiol self-assembled monolayers (SAMs), formed the most robust negative resist during the patterning process and made high quality patterning profile. In order to interpret the nature of the surface interaction between neutral sodium atoms and SAMs, they examine the surface components using x-ray photoelectron spectroscopy, secondary ion mass spectroscopy, and rinse tests. Their results indicate that sodium neutral atoms do not chemically react with or physically damage the SAMs but rather accumulate on and possibly diffuse into the SAMs. (c) 2007 American Vacuum Society.