Electron Correlation Effects on the Photophysics and Device Physics of Pi-conjugated Polymers

该基金由DMR材料理论项目和CHE理论与计算化学项目共同资助，支持p共轭聚合物基础科学和器件物理的理论和计算研究。本研究有三个重点：（1)PI的目标是建立一个完整的光致发光p共轭聚合物（如聚对苯乙烯）（PPV）和聚对苯乙烯（PPP））的激发态吸收理论，以及对苯乙烯分子晶体。这将包括理解在超快光谱中看到的双光子态的性质及其弛豫机制。(2)该工作的目标是开发一个概念框架，用于设计在红外发射的光致发光p共轭聚合物。计划鉴定具有小光学间隙但仍具有有利于光致发光的激发态有序的真实材料。(3) PI计划开发一种通用理论技术，用于计算有机发光二极管（oled）和光伏器件分子组分之间竞争性电荷转移反应的相对横截面。目的是达到oled中单线态和三重态激发产率的定量理论，并了解光诱导电荷转移过程效率的材料依赖性。为了描述这些材料中的电子态，PI将从低聚物和分子系统的parier - parr - people p-电子哈密顿量开始，并使用PI开发的多参考双组态相互作用（MRDCI）和图解激子基价键方法进行计算。MRDCI允许基态的适当截断，而激子基给出了相关特征态的图像描述，这反过来又导致光物理的机械描述。在oled和光伏过程中发生的分子间或链间电荷转移反应的计算将在时间依赖的schr0101659mazumdar1中进行。该资助由DMR材料理论计划和CHE理论与计算化学计划共同资助，支持pi共轭聚合物基础科学和器件物理的理论和计算研究。本研究有三个重点：(1)PI旨在建立一个完整的光致发光PI共轭聚合物（如聚对苯基乙烯（PPV）和聚对苯基乙烯（PPP））和丙烯酸分子晶体的激发态吸收理论。这将包括理解在超快光谱中看到的双光子态的性质及其弛豫机制。(2)该工作的目标是开发一个概念框架，用于设计在红外中发射的光致发光π共轭聚合物。计划鉴定具有小光学间隙但仍具有有利于光致发光的激发态有序的真实材料。(3) PI计划开发一种通用理论技术，用于计算有机发光二极管（oled）和光伏器件分子组分之间竞争性电荷转移反应的相对横截面。目的是达到oled中单线态和三重态激发产率的定量理论，并了解光诱导电荷转移过程效率的材料依赖性。为了描述这些材料中的电子态，PI将从低聚物和分子系统的parier - parr - people PI -电子哈密顿量开始，并使用PI开发的多参考双组态相互作用（MRDCI）和图解激子基价键方法进行计算。MRDCI允许基态的适当截断，而激子基给出了相关特征态的图像描述，这反过来又导致光物理的机械描述。在oled和光伏过程中发生的分子间或链间电荷转移反应的计算将在一个时间依赖的薛定谔公式中进行，该公式允许监测竞争电荷转移相互作用的相对产率。该基金由DMR材料理论项目和CHE理论与计算化学项目共同资助，支持π共轭聚合物的基础化学、光物理和器件物理的理论和计算研究。PI将研究涉及或干扰PI共轭聚合物中光的吸收和发射的基本物理过程。量子化学技术和PI开发的方法将用于包括电子相关效应在内的定量计算。这项工作将有助于寻找用于红外激光器的新型光致发光材料，并且对oled的研究有望预测电致发光效率与材料特性的依赖关系。该项目将为pi共轭聚合物的化学、物理和光学方面的培训提供研究生水平和更高的学习环境。***丁格公式，允许监测竞争电荷转移相互作用的相对产量。该基金由DMR的材料理论项目和CHE的理论和计算化学项目共同资助，支持p共轭聚合物的基础化学、光物理和器件物理的理论和计算研究。PI将研究p共轭聚合物中涉及或干扰光的吸收和发射的基本物理过程。量子化学技术和PI开发的方法将用于包括电子相关效应在内的定量计算。这项工作将有助于寻找用于红外激光器的新型光致发光材料，并且对oled的研究有望预测电致发光效率与材料特性的依赖关系。该项目将为p共轭聚合物的化学、物理和光学方面的培训提供研究生水平和更高的学习环境

0101659MazumdarThis grant, jointly funded by the Materials Theory Program in DMR and the Theoretical and Computational Chemistry Program in CHE, supports theoretical and computational research on the fundamental science and device physics of p-conjugated polymers. The research has three foci: (1) The PI aims to develop a complete theory of excited state absorption in photoluminescent p-conjugated polymers like poly(para-phenylenvinylene) (PPV) and poly(paraphenylene) (PPP), and of acene molecular crystals. This will involve understanding the nature of two-photon states seen in ultrafast spectroscopy and their relaxation mechanisms. (2) A goal of the work is to develop a conceptual framework for designing photoluminescent p-conjugated polymers that emit in the infrared. Identification of real materials that have small optical gaps, but nevertheless, posses the excited state ordering conducive to photoluminescence is planned. (3) The PI plans to develop a general theoretical technique for calculating the relative cross-sections of competing charge-transfer reactions between molecular components of organic light emitting diodes (OLEDs) and photovoltaic devices. The aim is to reach a quantitative theory of the yields of singlet verses triplet excitations in OLEDs and to understand the material dependence of the efficiencies of photoinduced charge transfer processes. To describe the electronic states in these materials, the PI will begin from the Pariser-Parr-Pople p-electron Hamiltonian for oligomers and molecular systems and perform calculations using the multiple-reference doubles configuration interaction (MRDCI) and a diagrammatic exciton basis valance bond method developed by the PI. The MRDCI allows proper truncation of basis states, while the exciton basis gives pictorial descriptions of correlated eigenstates, which in turn lead to mechanistic descriptions of the photophysics. Calculations of the intermolecular or interchain charge transfer reactions that occur in OLEDs and photovoltaic processes will be performed within a time-dependent Schr0101659MazumdarThis grant, jointly funded by the Materials Theory Program in DMR and the Theoretical and Computational Chemistry Program in CHE, supports theoretical and computational research on the fundamental science and device physics of pi-conjugated polymers. The research has three foci: (1) The PI aims to develop a complete theory of excited state absorption in photoluminescent pi-conjugated polymers like poly(para-phenylenvinylene) (PPV) and poly(paraphenylene) (PPP), and of acene molecular crystals. This will involve understanding the nature of two-photon states seen in ultrafast spectroscopy and their relaxation mechanisms. (2) A goal of the work is to develop a conceptual framework for designing photoluminescent pi-conjugated polymers that emit in the infrared. Identification of real materials that have small optical gaps, but nevertheless, posses the excited state ordering conducive to photoluminescence is planned. (3) The PI plans to develop a general theoretical technique for calculating the relative cross-sections of competing charge-transfer reactions between molecular components of organic light emitting diodes (OLEDs) and photovoltaic devices. The aim is to reach a quantitative theory of the yields of singlet verses triplet excitations in OLEDs and to understand the material dependence of the efficiencies of photoinduced charge transfer processes. To describe the electronic states in these materials, the PI will begin from the Pariser-Parr-Pople pi-electron Hamiltonian for oligomers and molecular systems and perform calculations using the multiple-reference doubles configuration interaction (MRDCI) and a diagrammatic exciton basis valance bond method developed by the PI. The MRDCI allows proper truncation of basis states, while the exciton basis gives pictorial descriptions of correlated eigenstates, which in turn lead to mechanistic descriptions of the photophysics. Calculations of the intermolecular or interchain charge transfer reactions that occur in OLEDs and photovoltaic processes will be performed within a time-dependent Schrodinger formulation that allows the monitoring of relative yields of competing charge transfer interactions. %%%This grant, jointly funded by the Materials Theory Program in DMR and the Theoretical and Computational Chemistry Program in CHE, supports theoretical and computational research on the fundamental chemical, photophysics, and device physics of pi-conjugated polymers. The PI will study the fundamental physical processes involved in, or that interfere with, the absorption and emission of light in pi-conjugated polymers. Quantum chemical techniques together with methods developed by the PI will be used to perform quantitative calculations that include the effects of electronic correlations. The work will contribute to the search for novel photoluminescent materials that are candidates for use in infrared lasers and research on the OLEDs is expected to predict dependencies of electroluminescence efficiency on materials properties. This project will provide a graduate level and higher learning environment for training in the chemistry, physics, and optics of pi-conjugated polymers.***dinger formulation that allows the monitoring of relative yields of competing charge transfer interactions. %%%This grant, jointly funded by the Materials Theory Program in DMR and the Theoretical and Computational Chemistry Program in CHE, supports theoretical and computational research on the fundamental chemical, photophysics, and device physics of p-conjugated polymers. The PI will study the fundamental physical processes involved in, or that interfere with, the absorption and emission of light in p-conjugated polymers. Quantum chemical techniques together with methods developed by the PI will be used to perform quantitative calculations that include the effects of electronic correlations. The work will contribute to the search for novel photoluminescent materials that are candidates for use in infrared lasers and research on the OLEDs is expected to predict dependencies of electroluminescence efficiency on materials properties. This project will provide a graduate level and higher learning environment for training in the chemistry, physics, and optics of p-conjugated polymers.***