Theoretical Insights into Gas Migration Within Ice on Earth and Icy Celestial Bodies

IF 2.9 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Yoo Soo Yi*,  and , Yeongcheol Han*, 
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Abstract

Atmospheric gases trapped in icy environments, such as Earth’s polar regions and Jupiter’s moon Europa, offer a unique opportunity to explore paleoclimate and astrogeological history. While previous studies have addressed the diffusive behaviors of these gases and their implications for paleoclimatological and geochronological reconstructions, the underlying mechanisms of gas migration in ice remain largely unexplored. Achieving an atomistic-level understanding of gas migration is therefore essential for improving our knowledge of the long-term behavior of gases in icy environments. In this study, we investigated the migration of noble gases encapsulated in isolated air bubbles within bulk ice using density functional theory calculations. We focused on both the dissolution at the gas–ice interface and the subsequent molecular diffusion through the ice lattice. Our results show that energy barriers for dissolution and molecular diffusion increase almost linearly with atomic size, leading to nonlinear, exponential-like decreases in solubility and diffusivity, due to their Arrhenius behavior in relation to the corresponding energy barriers. These energy barriers primarily arise from the structural distortions in the ice lattice, as it accommodates noble gas atoms. Additionally, our findings indicate that dissolution is energetically both more demanding and slower than molecular diffusion, making it the rate-limiting step in gas migration through ice. These findings provide valuable insights into gas migration and fractionation mechanisms in Earth’s polar ice, highlighting the importance of incorporating atomic-level interactions into geochronological models. By deepening our fundamental understanding of gas mobility, this work not only advances methodologies for analyzing Earth’s ice but also broadens our perspective on extraterrestrial icy environments, with potential implications for the search for life-supporting conditions beyond Earth.

Abstract Image

地球和冰冷天体冰内气体迁移的理论见解
被困在冰冷环境中的大气气体,如地球极地和木星的卫星木卫二,为探索古气候和天体地质历史提供了一个独特的机会。虽然以前的研究已经解决了这些气体的扩散行为及其对古气候学和地质年代学重建的影响,但冰中气体迁移的潜在机制仍然很大程度上未被探索。因此,实现对气体迁移的原子级理解对于提高我们对冰环境中气体长期行为的认识至关重要。在这项研究中,我们使用密度泛函理论计算研究了包裹在大块冰内孤立气泡中的惰性气体的迁移。我们关注了气体-冰界面的溶解和随后的分子通过冰格的扩散。我们的研究结果表明,溶解和分子扩散的能量势垒几乎随着原子尺寸的增加而线性增加,导致溶解度和扩散率的非线性指数下降,这是由于它们与相应的能量势垒相关的Arrhenius行为。这些能量障碍主要来自于冰格的结构扭曲,因为它容纳了稀有气体原子。此外,我们的研究结果表明,溶解在能量上比分子扩散要求更高,速度更慢,使其成为气体通过冰迁移的限速步骤。这些发现为地球极地冰的气体迁移和分馏机制提供了有价值的见解,强调了将原子水平的相互作用纳入地质年代学模型的重要性。通过加深我们对气体流动性的基本理解,这项工作不仅推进了分析地球冰的方法,而且拓宽了我们对地外冰环境的看法,对寻找地球以外的生命支持条件具有潜在的意义。
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来源期刊
ACS Earth and Space Chemistry
ACS Earth and Space Chemistry Earth and Planetary Sciences-Geochemistry and Petrology
CiteScore
5.30
自引率
11.80%
发文量
249
期刊介绍: The scope of ACS Earth and Space Chemistry includes the application of analytical, experimental and theoretical chemistry to investigate research questions relevant to the Earth and Space. The journal encompasses the highly interdisciplinary nature of research in this area, while emphasizing chemistry and chemical research tools as the unifying theme. The journal publishes broadly in the domains of high- and low-temperature geochemistry, atmospheric chemistry, marine chemistry, planetary chemistry, astrochemistry, and analytical geochemistry. ACS Earth and Space Chemistry publishes Articles, Letters, Reviews, and Features to provide flexible formats to readily communicate all aspects of research in these fields.
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