Computer modelling of novel perovskite halides for next-generation solar cells

用于下一代太阳能电池的新型钙钛矿卤化物的计算机建模

• 批准号: 2886759
• 金额: --
• 依托单位: University of Oxford
• 依托单位国家: 英国
• 项目类别: Studentship
• 财政年份: 2023
• 资助国家: 英国
• 起止时间: 2023 至 无数据
• 项目状态: 未结题
• 来源: https://gtr.ukri.org/projects?ref=studentship-2886759
• 关键词: Computer; modelling; novel; perovskite; halides

a) Brief description of the context of the researchMetal halide perovskites are generating enormous excitement for their use in low-cost, high-performance and scalable photovoltaic (PV) devices. These materials have the general ABX3 structure, where A is a mono-cation (methylammonium, MA; formamidinium, FA; and/or cesium, Cs), B is a di-cation (typically Pb), and X is an anion (typically I or an I/Br mixture). In contrast to crystalline silicon, perovskites offer low-temperature processability and band gap tunability through modifications of the chemical composition. Within 10 years, there has been an unprecedented rise in the power conversion efficiency (PCE) of perovskite solar cells from 3% to over 25%. However, there are significant stability issues and a full understanding of the underpinning defect, ion transport and interfacial properties is incomplete. Hence, we have yet to unlock the full performance potential of these materials.b) Aims and objectivesThis project will address critical challenges of this extraordinary class of material through a multi-faceted computational approach led by Prof Saiful Islam (SI) with the following key objectives: (i) To elucidate the activation energies and diffusion coefficients for ion migration across multiple compositions (partial A-cation substitution vs mixed I/Br) with comparison to the best-in-class perovskite (FA,Cs)PbI3 as an appropriate reference system.(ii) To compare and contrast how ion accumulation at the interfaces influence current transport and device stability. (iii) To elucidate how A-site cation doping and 2D structures can mitigate ion migration and surface reactions, and to formulate design guidelines for optimum compositions, enabling industrial relevance.c) Novelty of the research methodologyParticular strengths of this project will be (i) the ability to harness a range of density functional theory (DFT) and molecular dynamics (MD) methods (e.g. VASP, LAMMPS codes), (ii) the effective exploitation of high-performance supercomputers (e.g. Archer-2), and (iii) the close synergistic relationship with experimental work in Oxford Physics. In addition, there will be the novel use of emerging artificial intelligence (AI) and machine learning techniques which offer innovative capabilities for studying new PV materials, promising quantum-mechanical accuracy and predictive power, whilst being many orders of magnitude faster than conventional methods. For such materials modelling work, Oxford has excellent in-house computational facilities and SI has extensive access to the national Archer-2 supercomputer through the HPC Materials Chemistry Consortium (SI is Co-I).d) Alignment to EPSRC's strategies and research areas This project falls within the EPSRC 'Energy and Decarbonation' theme and the research areas: 'Solar Technology' and 'Materials for Energy Applications'. Hence, this project aligns well with EPSRC strategic objectives indicating the 'utilisation of new materials' and that 'significant advances in solar technology have arisen from underpinning materials sciences'. e) Any companies or collaborators involvedThis project will have links to complementary experimental studies on perovskite solar cells in the groups of Prof Henry Snaith FRS and Prof Laura Herz (both nearby in Oxford Physics). There will also be industry interactions with Oxford-PV, which was founded in 2010 as a spinout from the University of Oxford to commercialise hybrid photovoltaics and have developed a perovskite-on-silicon tandem efficiency of > 29%, exceeding that of the record performance of silicon.

a）研究背景简介金属卤化物钙钛矿因其在低成本、高性能和可扩展的光伏（PV）器件中的应用而引起巨大的兴奋。这些材料具有一般的ABX 3结构，其中A是单阳离子（甲基铵，MA;甲脒鎓，FA;和/或铯，Cs），B是双阳离子（通常是Pb），并且X是阴离子（通常是I或I/Br混合物）。与晶体硅相比，钙钛矿通过化学组成的改变提供低温可加工性和带隙可调谐性。在10年内，钙钛矿太阳能电池的功率转换效率（PCE）从3%上升到25%以上。然而，存在显著的稳定性问题，并且对支撑缺陷、离子传输和界面性质的充分理解是不完整的。B）目的和目标本项目将通过由Saiful Islam教授（SI）领导的多方面计算方法解决这类特殊材料的关键挑战，主要目标如下：（i）阐明离子在多种组合物中迁移的活化能和扩散系数（部分A-阳离子取代相对于混合I/Br），并与作为适当参比系统的同类最佳钙钛矿（FA，Cs）PbI 3进行比较。(ii)比较和对比界面处离子积累如何影响电流输运和器件稳定性。(iii)阐明A位阳离子掺杂和二维结构如何减轻离子迁移和表面反应，并制定最佳组合物的设计指南，使其具有工业相关性。c）研究方法的新奇本项目的特别优势将是（i）能够利用一系列密度泛函理论（DFT）和分子动力学（MD）方法（例如VASP，LAMMPS代码），（ii）高性能超级计算机（例如Archer-2）的有效利用，以及（iii）与牛津物理实验工作的密切协同关系。此外，新兴的人工智能（AI）和机器学习技术将得到新的应用，这些技术为研究新的光伏材料提供了创新能力，有望实现量子力学精度和预测能力，同时比传统方法快许多数量级。对于这种材料建模工作，牛津大学拥有出色的内部计算设施，SI通过HPC材料化学联盟（SI是Co-I）广泛使用国家Archer-2超级计算机。d）与EPSRC的战略和研究领域保持一致该项目福尔斯属于EPSRC的“能源和脱碳”主题和研究领域：“太阳能技术”和“能源应用材料”。因此，该项目符合EPSRC的战略目标，即“利用新材料”和“太阳能技术的重大进步源于基础材料科学”。e）任何参与的公司或合作者这个项目将与亨利斯奈斯FRS教授和劳拉赫兹教授（都在牛津物理附近）的小组对钙钛矿太阳能电池的补充实验研究有联系。还将与Oxford-PV进行行业互动，Oxford-PV成立于2010年，是牛津大学的一个分支，旨在将混合光电子学商业化，并开发出了> 29%的硅上钙钛矿串联效率，超过了硅的创纪录性能。