Collaborative Research: Unravelling many-body correlations in two-dimensional hybrid semiconductors

合作研究：揭示二维混合半导体中的多体相关性

基本信息

批准号：
1903785
负责人：
Eric Bittner
金额：
$ 39.83万
依托单位：
University of Houston
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2019
资助国家：
美国
起止时间：
2019-08-01 至 2023-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1903785&HistoricalAwards=false
关键词：
Collaborative Research Unravelling many body

项目摘要

Non-technical Abstract:This project addresses the properties of a promising kind of semiconductor material, called hybrid organic-inorganic perovskites, upon interaction with light, in the context of a variety of envisioned technologies such as solar cells, light-emitting diodes, and lasers. The atoms that constitute these materials produce substantially "shaky" crystal lattices, in which at ambient conditions the motion of interconnected atoms is vigorous. In spite of this highly dynamic environment, particles that arise from interaction with light, so-called excitons, interact amongst each other strongly and are stable. An analogy would be that of a perfectly choreographed set of multiple dancers in perfect choreography during a high-magnitude earthquake. The details on how and for how long these particles interact is of central importance in this project. To study these details, researchers at Georgia Tech will develop experimental methods based on lasers producing very short bursts of light (femtoseconds, shorter than amillionth of a billionth of a second) to study selectively their mutual interactions as a function of time. In parallel, researchers at the University of Houston will develop theoretical techniques to model the experiments. These collaborative activities will result in new understanding of the fundamental materials physics of these exciton semiconductors, which will facilitate the next significant breakthroughs in optoelectronic devices for solid-state lighting and lasers.Technical Abstract:This collaborative project will develop a coherent two-dimensional (2D) photoexcitation spectroscopy optimized to probe multi-particle correlations in semiconductor materials implemented in functional optoelectronic devices. The technique is based on phase modulation of a sequence of four variably delayed ultrashort laser pulses, and phase-sensitive detection of the photocurrent induced by that pulse sequence. This permits acquisition of 2D coherent spectra by isolating specific nonlinear contributions to the photocurrent excitation signal. This methodology has been previously implemented by several researchers. Recently it was demonstrated that an incoherent contribution to the measured line shape, arising from nonlinear population dynamics over the entire photoexcitation lifetime, generates a similar line shape to the expected 2D coherent spectra in many condensed-phase systems, in which photoexcitations are sufficiently mobile such that inter-particle interactions are important on any time scale, including those long compared with the 2D coherent experiment. The co-investigators propose a heterodyne detection scheme that surmounts this limitation, and will exploit the technique to study multi-particle correlations involving excitons and charge-carriers in two-dimensional, quantum-well-like hybrid organic-inorganic metal-halide perovskites. The specific objectives are (i) to develop a heterodyne detection protocol for photocurrent-detected 2D coherent multiexcitation spectroscopy and to demonstrate it in a highly efficient GaAs photodetector, in an optimized methylammonium lead-iodide perovskite solar cell, and in a phenylethylammonium lead-iodide 2D perovskite light-emitting diode; (ii) to develop a multiquantum 2D variant based on the same detection scheme and to study multi-excitons and trions in the 2D perovskite device above, and (iii) to develop an accessible, general modeling protocol for the photocurrent-detected 2D coherent excitation spectra based on parametrized lattice Hamiltonians, which connects early-time non-Markovian dynamics with the time-integrated response.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

非技术摘要：该项目在与光线相互作用后，在各种设想的技术（例如太阳能电池，照明二极管二极管和激光）的背景下，在与光线相互作用后，介绍了一种有希望的半导体材料的特性，称为混合有机无机钙钛矿。构成这些材料的原子产生了基本的“摇晃”晶体晶格，在这种环境条件下，互连原子的运动是剧烈的。尽管存在这种高度动态的环境，但由于与光，所谓的激子相互作用而产生的颗粒相互互动，并且稳定稳定。一个比喻是在高磁性地震期间完美编舞的一组完美编排的多个舞者。这些粒子相互作用的时间和多长时间的细节在该项目中至关重要。为了研究这些细节，佐治亚理工学院的研究人员将基于激光器产生非常短的光爆发（飞秒，比十亿分之一的四分之一的光爆发）开发实验方法，以选择性地研究它们的相互作用作为时间的函数。同时，休斯顿大学的研究人员将开发理论技术来对实验进行建模。这些协作活动将对这些激子半导体的基本材料物理学有了新的了解，这将促进用于固态照明和激光器的光电设备中的下一个重大突破。功能光电设备。该技术基于四个可变延迟的超短激光脉冲的序列的相位调制，以及该脉冲序列诱导的光电流的相位敏感检测。这可以通过将特定的非线性贡献对光电流激发信号分离，从而允许采集2D相干光谱。此方法先前已由几位研究人员实施。最近证明，在整个光激发寿命中非线性种群动态产生的对线形状的不一致贡献，在许多凝聚相相系统中产生与预期的2D相干光谱的线形状，在许多凝聚相cip仪中，光陈述足够可移动，其中与任何时间尺度相比，与2D相比，互相互作用很重要。共同投资者提出了一个杂尼检测方案，该方案可以克服这一限制，并将利用该技术来研究涉及二维，类似量子的混合有机甲甲基金属金属 - 甲状腺肿的多粒子相关性。 The specific objectives are (i) to develop a heterodyne detection protocol for photocurrent-detected 2D coherent multiexcitation spectroscopy and to demonstrate it in a highly efficient GaAs photodetector, in an optimized methylammonium lead-iodide perovskite solar cell, and in a phenylethylammonium lead-iodide 2D perovskite light-emitting diode; （ii）基于相同的检测方案开发多功能2D变体，并在上面的2D perovskite设备中研究多脱子和TRIONS，以及（iii）为基于与参数的Lattice Hamiltonians Nonemints的响应resptrients resplients resprients tirnersints，与光电频道检测的2D相干性激励的访问，通用建模方案开发可访问的一般建模协议，该协议，该协议，该协议是连接的，该方案是连接的。 NSF的法定使命，并使用基金会的知识分子优点和更广泛的影响审查标准来评估值得支持。

项目成果

期刊论文数量（9）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Electron–Phonon Couplings Inherent in Polarons Drive Exciton Dynamics in Two-Dimensional Metal-Halide Perovskites

DOI：
10.1021/acs.chemmater.9b02267
发表时间：
2019-06
期刊：
Chemistry of Materials
影响因子：
8.6
作者：
F. Thouin;A. R. Srimath Kandada;David A. Valverde-Ch'avez;D. Cortecchia;I. Bargigia;A. Petrozza;Xunmo Yang;E. Bittner;Carlos Silva
通讯作者：
F. Thouin;A. R. Srimath Kandada;David A. Valverde-Ch'avez;D. Cortecchia;I. Bargigia;A. Petrozza;Xunmo Yang;E. Bittner;Carlos Silva

QuDPy: A Python-based tool for computing ultrafast non-linear optical responses

QuDPy：基于 Python 的工具，用于计算超快非线性光学响应