Energy Transfer and Restructuring in Amorphous Solid Water upon Consecutive Irradiation.
Energy Transfer and Restructuring in Amorphous Solid Water upon Consecutive Irradiation.
复制标题
连续辐照下无定形固体水中的能量转移和重构。
DOI：
10.1021/acs.jpca.2c06314
复制
发表时间：
2022-12-01
影响因子：
2.9
通讯作者：
Ioppolo, Sergio
中科院分区：
文献类型：
--
作者：
Cuppen, Herma M.;Noble, Jennifer A.;Coussan, Stephane;Redlich, Britta;Ioppolo, Sergio
星际冰和彗星冰在年轻恒星周围行星系统的形成中起着重要作用。其主要成分是无定形固体水（ASW）。尽管对ASW的研究非常广泛，但对振动能量耗散和振动激发引起的结构变化却知之甚少。氢键网络可能是其中的关键组成部分。在这里，我们展示了在荷兰奈梅亨大学的hml - felix设施中，FELIX-2光束线的强、近单色中红外自由电子激光（FEL）辐射诱导ASW中氢键变化的实验结果。反射-吸收红外光谱法可以监测冰的结构变化，这取决于冰的辐照历史。实验表明，FEL辐照能引起受激分子的局部邻域因能量转移而发生变化。分子动力学模拟证实了这一观点：振动激发的分子可以在不破坏现有氢键的情况下重新定向，形成更理想的四面体。振动能量可以通过氢键网络传递给具有相同振动频率的水分子。因此，我们预计由于振动频率的不均匀性以及特定氢键缺陷位点的存在，非晶材料相对于晶体材料的能量耗散会减少，这也会阻碍能量传递。
Interstellar and cometary ices play an important role in the formation of planetary systems around young stars. Their main constituent is amorphous solid water (ASW). Although ASW is widely studied, vibrational energy dissipation and structural changes due to vibrational excitation are less well understood. The hydrogen-bonding network is likely a crucial component in this. Here, we present experimental results on hydrogen-bonding changes in ASW induced by the intense, nearly monochromatic mid-IR free-electron laser (FEL) radiation of the FELIX-2 beamline at the HFML-FELIX facility at the Radboud University in Nijmegen, The Netherlands. Structural changes in ASW are monitored by reflection–absorption infrared spectroscopy and depend on the irradiation history of the ice. The experiments show that FEL irradiation can induce changes in the local neighborhood of the excited molecules due to energy transfer. Molecular dynamics simulations confirm this picture: vibrationally excited molecules can reorient for a more optimal tetrahedral surrounding without breaking existing hydrogen bonds. The vibrational energy can transfer through the hydrogen-bonding network to water molecules that have the same vibrational frequency. We hence expect a reduced energy dissipation in amorphous material with respect to crystalline material due to the inhomogeneity in vibrational frequencies as well as the presence of specific hydrogen-bonding defect sites, which can also hamper the energy transfer.
登录
查看更多内容
影响因子：
4.9
作者：
Ioppolo, S.;Cuppen, H. M.;Linnartz, H.
通讯作者：
Linnartz, H.
影响因子：
44.1
作者：
Bartels-Rausch, Thorsten;Bergeron, Vance;Uras-Aytemiz, Nevin
通讯作者：
Uras-Aytemiz, Nevin
影响因子：
4.4
作者：
Lambros, Eleftherios;Paesani, Francesco
通讯作者：
Paesani, Francesco
影响因子：
3.3
作者：
Accolla, Mario;Congiu, Emanuele;Pirronello, Valerio
通讯作者：
Pirronello, Valerio
影响因子：
15
作者：
Sudera, Prerna;Cyran, Jenee D.;Bonn, Mischa
通讯作者：
Bonn, Mischa