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Register a new userMechanism of Indirect Photon-induced Desorption at the Water Ice Surface
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Electronic excitations near the surface of water ice lead to the desorption of adsorbed molecules, through a so far debated mechanism. A systematic study of photon-induced indirect desorption, revealed by the spectral dependence of the desorption (7 to 13 eV), is conducted for Ar, Kr, N2, and CO adsorbed on H2O or D2O amorphous ices. The mass and isotopic dependence and the increase of intrinsic desorption efficiency with photon energy all point to a mechanism of desorption induced by collisions between adsorbates and energetic H or D atoms, produced by photodissociation of water. This constitutes a direct and unambiguous experimental demonstration of the mechanism of indirect desorption of weakly adsorbed species on water ice, and sheds new light on the possibility of this mechanism in other systems. It also has implications for the description of photon-induced desorption in astrochemical models.
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We report an investigation of X-ray induced desorption of neutrals, cations and anions from CO ice. The desorption of neutral CO, by far the most abundant, is quantified and discussed within the context of its application to astrochemistry. The desorption of many different cations, including large cations up to the mass limit of the spectrometer, are observed. In contrast, the only desorbing anions detected are O$^-$ and C$^-$. The desorption mechanisms of all these species are discussed with the aid of their photodesorption spectrum. The evolution of the X-ray absorption spectrum shows significant chemical modifications of the ice upon irradiation, which along with the desorption of large cations gives a new insight into X-ray induced photochemistry in CO ice.
We made near infrared multicolor imaging observations of a disk around Herbig Be star HD100546 using Gemini/NICI. K (2.2,$mu$m), H$_2$O ice (3.06,$mu$m), and L(3.8,$mu$m) disk images were obtained and we found the 3.1,$mu$m absorption feature in the scattered light spectrum, likely due to water ice grains at the disk surface. We compared the observed depth of the ice absorption feature with the disk model based on cite{Oka2012} including water ice photodesorption effect by stellar UV photons. The observed absorption depth can be explained by the both disk models with/without photodesorption effect within the measurement accuracy, but slightly favors the model with photodesorption effects, implying that the UV photons play an important role on the survival/destruction of ice grains at the Herbig Ae/Be disk surface. Further improvement on the accuracy of the observations of the water ice absorption depth is needed to constrain the disk models.
The ultraviolet (UV) photodissociation of amorphous water ice at different ice temperatures is investigated using molecular dynamics (MD) simulations and analytical potentials. Previous MD calculations of UV photodissociation of amorphous and crystalline water ice at 10 K [S. Andersson et al., J. Chem. Phys. 124, 064715 (2006)] revealed -for both types of ice- that H atom, OH, and H2O desorption are the most important processes after photoexcitation in the uppermost layers of the ice. Water desorption takes place either by direct desorption of recombined water, or when, after dissociation, an H atom transfers part of its kinetic energy to one of the surrounding water molecules which is thereby kicked out from the ice. We present results of MD simulations of UV photodissociation of amorphous ice at 10, 20, 30, and 90 K in order to analyze the effect of ice temperature on UV photodissociation processes. Desorption and trapping probabilities are calculated for photoexcitation of H2O in the top four monolayers and the main conclusions are in agreement with the 10 K results: desorption dominates in the top layers, while trapping occurs deeper in the ice. The hydrogen atom photodesorption probability does not depend on ice temperature, but OH and H2O photodesorption probabilities tend to increase slightly (~30%) with ice temperature. We have compared the total photodesorption probability (OH+H2O) with the experimental total photodesorption yield, and in both cases the probabilities rise smoothly with ice temperature. The experimental yield is on average 3.8 times larger than our theoretical results, which can be explained by the different time scales studied and the approximations in our model.
We study the initial stages of homogeneous melting of a hexagonal ice crystal at coexistence and at moderate superheating. Our trajectory-based computer simulation approach provides a comprehensive picture of the events that lead to melting; from the initial accumulation of 5+7 defects, via the formation of L-D and interstitial-vacancy pairs, to the formation of a liquid nucleus. Of the different types of defects that we observe to be involved in melting, a particular kind of 5+7 type defect (type 5) plays a prominent role as it often forms prior to the formation of the initial liquid nucleus and close to the site where the nucleus forms. Hence, like other solids, ice homogeneously melts via the prior accumulation of defects.
The inter oxygen repulsion opposes compression minimizing the compressibility. Polarization enlarges the bandgap and the dielectric permittivity of water ice by raising the nonbonding states above the Fermi energy. Progress evidences the efficiency and essentiality of the coupled hydrogen bonding and electronic dynamics in revealing the core physics and chemistry of water ice, which could extend to other molecular crystals such as energetic materials.
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