• 主题
高级搜索  >
历史搜索 清空历史
首页> 美国卫生研究院文献>Frontiers in Chemistry >Electronic Structure and Band Alignments of Various Phases of Titania Using the Self-Consistent Hybrid Density Functional and DFT+U Methods
【2h】

Electronic Structure and Band Alignments of Various Phases of Titania Using the Self-Consistent Hybrid Density Functional and DFT+U Methods

机译：使用自洽混合密度泛函和DFT + U方法研究二氧化钛各相的电子结构和能带排列

代理获取
本网站仅为用户提供外文OA文献查询和代理获取服务，本网站没有原文。下单后我们将采用程序或人工为您竭诚获取高质量的原文，但由于OA文献来源多样且变更频繁，仍可能出现获取不到、文献不完整或与标题不符等情况，如果获取不到我们将提供退款服务。请知悉。
页面导航
  • 摘要
  • 著录项
  • 相似文献
  • 相关主题

摘要

To understand, and thereby rationally optimize photoactive interfaces, it is of great importance to elucidate the electronic structures and band alignments of these interfaces. For the first-principles investigation of these properties, conventional density functional theory (DFT) requires a solution to mitigate its well-known bandgap underestimation problem. Hybrid functional and Hubbard U correction are computationally efficient methods to overcome this limitation, however, the results are largely dependent on the choice of parameters. In this study, we employed recently developed self-consistent approaches, which enable non-empirical determination of the parameters, to investigate TiO2 interfacial systems—the most prototypical photocatalytic systems. We investigated the structural, electronic, and optical properties of rutile and anatase phases of TiO2. We found that the self-consistent hybrid functional method predicts the most reliable structural and electronic properties that are comparable to the experimental and high-level GW results. Using the validated self-consistent hybrid functional method, we further investigated the band edge positions between rutile and anatase surfaces in a vacuum and electrolyte medium, by coupling it with the Poisson-Boltzmann theory. This suggests the possibility of a transition from the straddling-type to the staggered-type band alignment between rutile and anatase phases in the electrolyte medium, manifested by the formation of a Stern-like layer at the interfaces. Our study not only confirms the efficacy of the self-consistent hybrid functional method by reliably predicting the electronic structure of photoactive interfaces, but also elucidates a potentially dramatic change in the band edge positions of TiO2 in aqueous electrolyte medium which can extensively affect its photophysical properties.
机译：为了理解并由此合理地优化光敏界面，阐明这些界面的电子结构和能带对准非常重要。对于这些性质的第一性原理研究，常规密度泛函理论（DFT）需要一种解决方案来缓解其众所周知的带隙低估问题。混合函数和Hubbard U校正是克服此限制的有效计算方法，但是，结果很大程度上取决于参数的选择。在这项研究中，我们采用了最近开发的自洽方法，该方法可以非经验地确定参数，以研究TiO2界面系统，这是最典型的光催化系统。我们研究了TiO2的金红石相和锐钛矿相的结构，电子和光学性质。我们发现，自洽混合函数方法可预测出最可靠的结构和电子特性，可与实验和高级GW结果媲美。使用经过验证的自洽混合函数方法，我们将其与Poisson-Boltzmann理论耦合，进一步研究了真空和电解质介质中金红石和锐钛矿表面之间的能带边缘位置。这表明在电解质介质中金红石相和锐钛矿相之间从跨越型跃迁到交错型能带排列的可能性，这在界面处形成了斯特恩样层。我们的研究不仅通过可靠地预测光敏界面的电子结构来确认自洽混合功能方法的功效，而且阐明了TiO2在水性电解质介质中的能带边缘位置可能发生的显着变化，这可能会广泛影响其光物理性质。

著录项

相似文献

  • 外文文献
  • 中文文献
  • 专利
代理获取

客服邮箱：kefu@zhangqiaokeyan.com

京公网安备：11010802029741号 ICP备案号：京ICP备15016152号-6 六维联合信息科技 (北京) 有限公司©版权所有

  • 客服微信

  • 服务号