DMREF: Metallic-type transport in polymers: Establishing materials design criteria and predicting structure/property interrelations

DMREF：聚合物中的金属型传输：建立材料设计标准并预测结构/性能相互关系

• 批准号: 1729737
• 负责人: Natalie Stingelin
• 金额: $ 150万
• 依托单位: Georgia Tech Research Corporation
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-10-01 至 2022-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1729737&HistoricalAwards=false
• 关键词: DMREF; Metallic; type; transport; polymers

Non-technical Description: A materials design framework is proposed that will provide quantitative insights into what determines charge transport properties in organic semiconductors, and will provide verifiable hypotheses towards accelerated materials discovery. The motivation is partly that, although the multibillion dollar organic electronic industry is based on a unique combination of performance and processability of organic semiconductors, solubility/processability, intermolecular interactions, and other factors impacting delocalization of charge carriers, which determines transport properties, are still not fully understood for these materials. Critical properties can depend subtly on chemical structure and processing conditions and, often, changes in properties and processing parameters are intertwined in non-obvious ways. This creates a daunting task to establish comprehensive structure/processing/property interrelations, often reducing materials discovery to heuristic time-consuming, expensive studies. To unravel the complex interaction of structure/processing and transport properties, a multidisciplinary team of materials chemists, materials engineers, ultrafast spectroscopists, and theorists from Georgia Tech (GT), University of Massachusetts Amherst (UMass), and Los Alamos National Laboratory (LANL), has been assembled. This research will provide critical insights that will enable the quantitative design of materials that optimize both mobility and conductivity. It will also make available to a broad community an extensive database that can be mined to advance materials science discovery platforms, and that will be used in education. We will develop theoretical tools with improved parameterization, allowing the modeling of a broader set of materials. The target materials will be employed in a variety of applications including, amongst others, electrodes, thermoelectric materials, and charge-extraction layers. The highly diverse team will reach out to under-served communities, by recruiting female and under-represented scientists and engineers to carry out research in its shared program, but also through extensive interactions with high schools and the public through a variety of engagement programs and public outreach events.Technical Description: The research addresses fundamental questions of how charge-carrier coherence length and transport properties correlate with specific structural features in doped organic materials. Optical spectroscopies (absorption, photoinduced absorption, photoluminescence, photoluminescence excitation, and two-dimensional coherent excitation spectra), along with thermal analysis and X-ray diffraction data, will be used to construct a database on doped polymers, oligomers and small molecules, utilizing a variety of dopants. Key spectral observables will be modeled with existing theoretical tools at LANL, using first-principle calculations with atomistic approaches, nonadiabatic molecular dynamics simulations, and parameterized Holstein lattice models to simulate quantum dynamics of charges, focusing on spatial coherence lengths of charge carriers in materials. Nonlinear spectroscopies will be used to refine the details of the quantum dynamics models, as they provide details of not only population but also temporal and spatial coherence dynamics. In particular, these measurements can isolate the homogeneous excitation linewidth from the total spectral lineshape, thereby providing a very sensitive probe of spatial coherence, limited by the quantum dynamics that lead to carrier localization. The PIs also plan to release the DMREF Polymeric Semiconductor Toolbox and Database as open source and build a user community around the language by ensuring that interested researchers are able to contribute to the DMREF Polymeric Semiconductor Toolbox and Database codebase. This will allow a wider growth of the project. This aspect is of special interest to the software cluster in the Office of Advanced Cyberinfrastructure, which has provided co-funding for this award.

非技术描述：提出了一种材料设计框架，将提供定量的见解是什么决定有机半导体中的电荷传输特性，并将提供可验证的假设加速材料的发现。其动机部分在于，尽管数十亿美元的有机电子工业是基于有机半导体的性能和可加工性的独特组合，但溶解性/可加工性、分子间相互作用和影响电荷载流子离域的其他因素（其决定了传输特性）对于这些材料仍然没有完全理解。关键性能可能微妙地取决于化学结构和加工条件，并且通常，性能和加工参数的变化以不明显的方式交织在一起。这就产生了一个艰巨的任务，建立全面的结构/加工/性能的相互关系，往往减少材料的发现启发式耗时，昂贵的研究。为了解开结构/加工和输运性质的复杂相互作用，来自格鲁吉亚理工学院（GT）、马萨诸塞州阿默斯特大学（UMass）和洛斯阿拉莫斯国家实验室（LANL）的材料化学家、材料工程师、超快光谱学家和理论家组成了一个多学科团队。这项研究将提供关键的见解，使材料的定量设计，优化流动性和导电性。它还将向广大社区提供一个广泛的数据库，可以挖掘以推进材料科学发现平台，并将用于教育。我们将开发具有改进的参数化的理论工具，允许对更广泛的材料进行建模。靶材料将用于各种应用中，包括电极、热电材料和电荷提取层等。这个高度多元化的团队将通过招募女性和代表性不足的科学家和工程师在其共享计划中开展研究，并通过各种参与计划和公共宣传活动与高中和公众进行广泛的互动，来接触服务不足的社区。技术描述：该研究解决了电荷载流子相干长度和传输特性如何与掺杂有机材料中的特定结构特征相关的基本问题。光学光谱（吸收，光致吸收，光致发光，光致发光激发，和二维相干激发光谱），沿着热分析和X射线衍射数据，将用于构建一个数据库的掺杂聚合物，低聚物和小分子，利用各种掺杂剂。关键的光谱观测量将与现有的理论工具在LANL建模，使用第一原理计算与原子的方法，非绝热分子动力学模拟和参数化的Holstein晶格模型来模拟电荷的量子动力学，重点是材料中电荷载流子的空间相干长度。非线性光谱学将被用来细化量子动力学模型的细节，因为它们不仅提供了人口的细节，而且还提供了时间和空间相干动力学的细节。特别是，这些测量可以隔离的均匀激发线宽从总的光谱线型，从而提供了一个非常敏感的空间相干性的探针，有限的量子动力学，导致载流子本地化。 PI还计划将DMREF聚合物半导体测试和数据库作为开源发布，并通过确保感兴趣的研究人员能够为DMREF聚合物半导体测试和数据库代码库做出贡献，围绕该语言建立一个用户社区。这将使该项目得到更广泛的发展。高级网络基础设施办公室的软件集群对此特别感兴趣，该办公室为该奖项提供了共同资助。

项目成果

Enhanced Thermoelectric Power Factor of Tensile Drawn Poly(3-hexylthiophene)

• DOI: 10.1021/acsmacrolett.8b00820
• 发表时间: 2019-01-01
• 期刊: ACS MACRO LETTERS
• 影响因子: 7.015
• 作者: Hynynen, Jonna;Jarsvall, Emmy;Mueller, Christian
• 通讯作者: Mueller, Christian

Electron transport in a sequentially doped naphthalene diimide polymer

• DOI: 10.1039/d0ma00406e
• 发表时间: 2020-09-01
• 期刊: MATERIALS ADVANCES
• 影响因子: 5
• 作者: Al Kurdi, Khaled;Gregory, Shawn A.;Marder, Seth R.
• 通讯作者: Marder, Seth R.

Disentangling Bulk and Interface Phenomena in a Molecularly Doped Polymer Semiconductor

• DOI: 10.1002/adom.202002039
• 发表时间: 2021-02-02
• 期刊: ADVANCED OPTICAL MATERIALS
• 影响因子: 9
• 作者: Lungwitz, Dominique;Schultz, Thorsten;Koch, Norbert
• 通讯作者: Koch, Norbert

Toward Fast Screening of Organic Solar Cell Blends

• DOI: 10.1002/advs.202000960
• 发表时间: 2020-06
• 期刊: Advanced Science
• 影响因子: 15.1
• 作者: Artem Levitsky;G. Matrone;Aditi Khirbat;I. Bargigia;Xiaolei Chu;Oded Nahor;T. Segal‐Peretz;A. Moulé;L. Richter;Carlos Silva;N. Stingelin;G. Frey

High-density polyethylene—an inert additive with stabilizing effects on organic field-effect transistors

高密度聚乙烯——一种对有机场效应晶体管具有稳定作用的惰性添加剂

• DOI: 10.1039/d0tc03173a
• 发表时间: 2020
• 期刊: Journal of Materials Chemistry C
• 影响因子: 6.4
• 作者: Scaccabarozzi, Alberto D.;Basham, James I.;Yu, Liyang;Westacott, Paul;Zhang, Weimin;Amassian, Aram;McCulloch, Iain;Caironi, Mario;Gundlach, David J.;Stingelin, Natalie
• 通讯作者: Stingelin, Natalie