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In the quest to understand the formation of the building blocks of life,amorphous solid water (ASW) is one of the most widely studied molecularsystems. Indeed, ASW is ubiquitous in the cold interstellar medium (ISM), whereASW-coated dust grains provide a catalytic surface for solid phase chemistry,and is believed to be present in the Earth's atmosphere at high altitudes. Ithas been shown that the ice surface adsorbs small molecules such as CO, N$_2$,or CH$_4$, most likely at OH groups dangling from the surface. Our studypresents completely new insights concerning the behaviour of ASW upon selectiveinfrared (IR) irradiation of its dangling modes. When irradiated, these surfaceH$_2$O molecules reorganise, predominantly forming a stabilised monomer-likewater mode on the ice surface. We show that we systematically provoke"hole-burning" effects (or net loss of oscillators) at the wavelength ofirradiation and reproduce the same absorbed water monomer on the ASW surface.Our study suggests that all dangling modes share one common channel ofvibrational relaxation; the ice remains amorphous but with a reduced range ofbinding sites, and thus an altered catalytic capacity.

Unveiling the Surface Structure of Amorphous Solid Water via Selective Infrared Irradiation of OH Stretching Modes