Observing ice structure of micron-sized vapor-deposited ice with an x-ray free-electron laser.

IF 2.3 2区物理与天体物理 Q3 CHEMISTRY, PHYSICAL Structural Dynamics-Us Pub Date : 2023-08-09 eCollection Date: 2023-07-01 DOI:10.1063/4.0000185

Seonmyeong Kim, Matlabjon Sattorov, Dongpyo Hong, Heon Kang, Jaehun Park, Jae Hyuk Lee, Rory Ma, Andrew V Martin, Carl Caleman, Jonas A Sellberg, Prasanta Kumar Datta, Sang Yoon Park, Gun-Sik Park

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Abstract

The direct observation of the structure of micrometer-sized vapor-deposited ice is performed at Pohang Accelerator Laboratory x-ray free electron laser (PAL-XFEL). The formation of micrometer-sized ice crystals and their structure is important in various fields, including atmospheric science, cryobiology, and astrophysics, but understanding the structure of micrometer-sized ice crystals remains challenging due to the lack of direct observation. Using intense x-ray diffraction from PAL-XFEL, we could observe the structure of micrometer-sized vapor-deposited ice below 150 K with a thickness of 2-50 μm grown in an ultrahigh vacuum chamber. The structure of the ice grown comprises cubic and hexagonal sequences that are randomly arranged to produce a stacking-disordered ice. We observed that ice with a high cubicity of more than 80% was transformed to partially oriented hexagonal ice when the thickness of the ice deposition grew beyond 5 μm. This suggests that precise temperature control and clean deposition conditions allow μm-thick ice films with high cubicity to be grown on hydrophilic Si₃N₄ membranes. The low influence of impurities could enable in situ diffraction experiments of ice nucleation and growth from interfacial layers to bulk ice.

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用x射线自由电子激光观测微米级气相沉积冰的冰结构。

在浦项加速器实验室x射线自由电子激光器（PAL-XFEL）对微米级气相沉积冰的结构进行了直接观测。微米大小的冰晶的形成及其结构在各个领域都很重要，包括大气科学、冷冻生物学和天体物理学，但由于缺乏直接观测，了解微米大小冰晶的结构仍然具有挑战性。利用PAL-XFEL的强x射线衍射，我们可以观察到150以下微米大小的气相沉积冰的结构厚度为2-50的K μm在超高真空室中生长。生长的冰的结构包括随机排列的立方体和六边形序列，以产生堆叠无序的冰。我们观察到，当冰沉积的厚度超过5时，立方体度超过80%的冰转变为部分取向的六边形冰 μm。这表明，精确的温度控制和清洁的沉积条件允许在亲水性Si3N4膜上生长具有高立方体度的μm厚的冰膜。杂质的低影响可以实现从界面层到大块冰的成核和生长的原位衍射实验。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Structural Dynamics-Us CHEMISTRY, PHYSICALPHYSICS, ATOMIC, MOLECU-PHYSICS, ATOMIC, MOLECULAR & CHEMICAL

CiteScore

5.50

自引率

3.60%

发文量

审稿时长

16 weeks

期刊介绍： Structural Dynamics focuses on the recent developments in experimental and theoretical methods and techniques that allow a visualization of the electronic and geometric structural changes in real time of chemical, biological, and condensed-matter systems. The community of scientists and engineers working on structural dynamics in such diverse systems often use similar instrumentation and methods. The journal welcomes articles dealing with fundamental problems of electronic and structural dynamics that are tackled by new methods, such as: Time-resolved X-ray and electron diffraction and scattering, Coherent diffractive imaging, Time-resolved X-ray spectroscopies (absorption, emission, resonant inelastic scattering, etc.), Time-resolved electron energy loss spectroscopy (EELS) and electron microscopy, Time-resolved photoelectron spectroscopies (UPS, XPS, ARPES, etc.), Multidimensional spectroscopies in the infrared, the visible and the ultraviolet, Nonlinear spectroscopies in the VUV, the soft and the hard X-ray domains, Theory and computational methods and algorithms for the analysis and description of structuraldynamics and their associated experimental signals. These new methods are enabled by new instrumentation, such as: X-ray free electron lasers, which provide flux, coherence, and time resolution, New sources of ultrashort electron pulses, New sources of ultrashort vacuum ultraviolet (VUV) to hard X-ray pulses, such as high-harmonic generation (HHG) sources or plasma-based sources, New sources of ultrashort infrared and terahertz (THz) radiation, New detectors for X-rays and electrons, New sample handling and delivery schemes, New computational capabilities.