Proton disorder in cubic ice: Effect on the electronic and optical properties,The Journal of Chemical Physics

当前位置： X-MOL 学术 › J. Chem. Phys. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Proton disorder in cubic ice: Effect on the electronic and optical properties
The Journal of Chemical Physics ( IF 3.1 ) Pub Date : 2015-08-27 13:27:25 , DOI: 10.1063/1.4929468
Viviana Garbuio ₁ , Michele Cascella ₂ , Igor Kupchak ₃ , Olivia Pulci ₁ , Ari Paavo Seitsonen _{4,

5}

Affiliation

The proton disorder in ice has a key role in several properties such as the growth mode, thermodynamical properties, and ferroelectricity. While structural phase transitions from proton disordered to proton ordered ices have been extensively studied, much less is known about their electronic and optical properties. Here, we present ab initio many body perturbation theory-based calculations of the electronic and optical properties of cubic ice at different levels of proton disorder. We compare our results with those from liquid water, that acts as an example of a fully (proton- and oxygen-)disordered system. We find that by increasing the proton disorder, a shrinking of the electronic gap occurs in ice, and it is smallest in the liquid water. Simultaneously, the excitonic binding energy decreases, so that the final optical gaps result to be almost independent on the degree of proton disorder. We explain these findings as an interplay between the local dipolar disorder and the electronic correlation.

中文翻译：

立方冰中的质子紊乱：对电子和光学性质的影响

冰中的质子紊乱在多种性质（例如生长模式，热力学性质和铁电性质）中具有关键作用。虽然已经广泛研究了从无序质子到质子有序冰的结构相变，但对它们的电子和光学性质知之甚少。在这里，我们介绍从头开始在质子紊乱的不同水平下，许多基于人体扰动理论的立方冰电子和光学性质的计算。我们将我们的结果与液态水的结果进行比较，液态水是一个完全（质子和氧）无序系统的例子。我们发现，通过增加质子紊乱，冰中的电子间隙会缩小，而液态水中的电子间隙会缩小。同时，激子结合能降低，因此最终的光学间隙几乎与质子紊乱的程度无关。我们将这些发现解释为局部躁郁症和电子相关性之间的相互作用。

更新日期：2015-08-28

点击分享查看原文

点击收藏

公开下载

阅读更多本刊新发论文