从第一原理看碘化甲铵铅的超快电荷载流子动力学

IF 2.9 Q3 CHEMISTRY, PHYSICAL Electronic Structure Pub Date : 2024-07-04 DOI:10.1088/2516-1075/ad5b40
Ariel M Cabrera, Michele Guerrini, Henry P Pinto and Caterina Cocchi
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引用次数: 0

摘要

甲基碘化铵铅(MAPbI3)是过去十年来光伏研究的重点。这种材料的结构特性和电子特性之间的独特相互作用造就了其令人兴奋的光学特性,尤其是在超快激光脉冲的作用下。实时时变密度泛函理论(RT-TDDFT)等第一性原理方法可以在不借助经验参数的情况下进行相应的模拟:所获得的知识可用于未来对其他复杂材料的研究。在这项工作中,我们研究了间隙上方谐振脉冲激发的 MAPbI3 的超快电荷载流子动力学和非线性光学响应。首先,我们研究了静态下的电子和光学特性。接着,我们用不同强度的飞秒场冲击该系统,并跟踪光激发载流子密度的演变。我们观察到了明显的强度依赖性响应,表现为高次谐波产生以及激发电子数和激发能量的非线性趋势。我们的研究结果为 MAPbI3 在强相干辐射下的行为提供了相关指示,并证实 RT-TDDFT 是从第一原理模拟复杂材料光诱导动力学的可行工具。
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Ultrafast charge carrier dynamics of methylammonium lead iodide from first principles
Methylammonium lead iodide (MAPbI3) has been a major focus of photovoltaic research for the last decade. The unique interplay between the structural and electronic properties of this material contributes to its exciting optical properties especially under the action of an ultrafast laser pulse. First-principles methods like real-time time-dependent density functional theory (RT-TDDFT) enable performing corresponding simulations without the aid of empirical parameters: the gained knowledge can be applied to future studies of other complex materials. In this work, we investigate the ultrafast charge-carrier dynamics and the nonlinear optical response of MAPbI3 excited by a resonant pulse above the gap. First, we examine the electronic and optical properties in the static regime. Next, we impinge the system with a femtosecond field of varying intensity and follow the evolution of the photoexcited carrier density. A pronounced intensity-dependent response is observed, manifested by high-harmonic generation and nonlinear trends in the number of excited electrons and excitation energy. Our results provide relevant indications about the behavior of MAPbI3 under strong and coherent radiation and confirm that RT-TDDFT is a viable tool to simulate the photo-induced dynamics of complex materials from first principles.
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来源期刊
CiteScore
3.70
自引率
11.50%
发文量
46
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