论文标题

IRFEL选择性辐照无定形固体水:从悬挂到散装模式

IRFEL Selective Irradiation of Amorphous Solid Water: from Dangling to Bulk Modes

论文作者

Coussan, S., Noble, J. A., Cuppen, H. M., Redlich, B., Ioppolo, S.

论文摘要

无定形固体水(ASW)是研究最广泛的固相系统之一。然而,对ASW中分子间和分子内部力的性质的更好理解仍然需要正确解释ASW在太阳系对象的冰冷表面,在星际冰冷的尘埃谷物上,甚至可能在地球上层的层层上,在诸如太阳系对象的冰上表面,诸如太阳系对象的冰冷表面的环境中的催化作用。在这项工作中,我们在荷兰的HFML-Felix设施上系统地将多孔ASW(PASW)系统暴露于中红外辐射,以研究振动能量注射到PASW的表面和散装模式的效果。在同一冰斑的多个顺序辐照过程中,我们观察到表面和大部分冰的选择性效应。尽管PASW中状态的密度应允许通过H键网络进行快速的振动弛豫,但在进行傅立叶变换红外光谱镜头反射模式中,一部分注入的能量被转化为结构冰的变化。未来的研究将包括通过系统地研究冰厚,冰形和冰组成来量化此类效应。

Amorphous solid water (ASW) is one of the most widely studied solid phase systems. A better understanding of the nature of inter- and intramolecular forces in ASW is, however, still required to correctly interpret the catalytic role of ASW in the formation and preservation of molecular species in environments such as the icy surfaces of Solar System objects, on interstellar icy dust grains and potentially even in the upper layers of the Earth's atmosphere. In this work, we have systematically exposed porous ASW (pASW) to mid-infrared radiation generated by a free-electron laser at the HFML-FELIX facility in the Netherlands to study the effect of vibrational energy injection into the surface and bulk modes of pASW. During multiple sequential irradiations on the same ice spot, we observed selective effects both at the surface and in the bulk of the ice. Although the density of states in pASW should allow for a fast vibrational relaxation through the H-bonded network, part of the injected energy is converted into structural ice changes as illustrated by the observation of spectral modifications when performing Fourier transform infrared spectroscopy in reflection-absorption mode. Future studies will include the quantification of such effects by systematically investigating ice thickness, ice morphology, and ice composition.

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