CAREER: First-Principles Predictive Theory and Microscopic Understanding of Nonlinear Light-Matter Interactions towards Designer Nonlinear Optical Materials

材料研究部和先进网络基础设施办公室为该职业奖提供资金。该奖项支持开发和应用计算方法来理解非线性光学材料对光的响应的综合研究和教育工作。非线性光学材料对光的反应取决于光的强度，这导致了可用于技术应用的有趣现象。例如，折射率和光强的依赖关系可以使非线性光学材料像透镜一样起作用，使光束在通过该材料时变窄或坍缩。这些材料在医学、光电器件和高级敏感量子机械传感器的非侵入性成像等方面都有应用。在微观水平上理解和准确预测强光-物质相互作用将有助于为特定应用设计具有定制非线性光学特性的新型材料。该项目的目标是开发和应用从了解组成原子的身份开始的方法，以预测特定非线性光学材料对光的反应。重点将放在新颖的二维材料和拓扑材料，这些材料可以具有金属态，具有覆盖材料表面和边缘的奇异特性。这项工作将阐明对称性、拓扑、表面/边缘和自旋轨道耦合在非线性光-物质相互作用中的基本作用。从这项工作中获得的结果也将有助于产生非线性光学材料和纳米结构的设计原则。所获得的方法和数据将通过开源分发广泛传播给科学界、工业界和公众。为了将推广和教育与研究结合起来，PI将在夏季接待和培训来自代表性不足群体的高中生和中学教师进行科学计算和模拟。PI还将把研究纳入本科和研究生课程，为本科生和研究生提供多学科培训，在计算材料科学暑期学校传播计算工具，并通过系列研讨会促进妇女参与材料科学和工程。从事该项目的研究生将获得物理学、材料科学和高性能计算的跨学科背景。生成的电脑代码和数据将与公众分享，以促进社区的教育和外展。技术摘要材料研究部和先进网络基础设施办公室为该职业奖提供资金。该奖项支持开发和应用预测第一性原理方法来理解材料非线性光学响应的综合研究和教育工作。具有定制非线性光学特性的材料和纳米结构不仅对理解、探测和最终控制纳米尺度的光-物质相互作用非常重要，而且对于许多应用非常理想，例如超快非线性光学、生物传感、全光晶体管和计算机、光量子隐形传态、通信和计算。近年来，在二维晶体和拓扑材料中发现了巨大的非线性光学过程，如二次谐波和三次谐波的产生，这对现有的认识提出了挑战，需要在微观水平上进行基础研究。该项目的目标是促进对材料中非线性光物质相互作用的基本理解和理论预测。研究将集中于发展和应用基于第一性原理密度泛函的方法和方法来研究并最终预测材料的二阶和三阶非线性光学响应。自旋轨道耦合，晶体对称性，因果关系，电子-空穴相互作用，准粒子能量，准粒子寿命由于载流子-载流子和载流子-声子相互作用将包括在这个第一性原理的理论框架。特别的重点将放在阐明对称，电子拓扑，表面/边缘和自旋轨道耦合在二维材料和拓扑材料中的作用。所获得的结果将产生非线性光学过程的新知识，并为控制光-物质相互作用提供材料设计原则。为了将外展和教育与研究结合起来，PI将在夏季期间接待和培训来自代表性不足群体的高中生和中学教师进行科学计算和模拟，以激发学生对科学和工程的渴望和好奇心。PI还将把研究纳入本科和研究生课程，向本科生和研究生提供多学科培训，在计算材料科学暑期学校传播开发的计算工具，并通过系列研讨会促进妇女参与材料科学和工程。从事该项目的研究生将在物理学、材料科学和高性能计算方面获得扎实的跨学科背景。此外，本项目生成的计算方法、代码和数据将通过开源发行版广泛传播给科学界、工业界和公众，目的是使更广泛的研究、教育和社区外展受益。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

NONTECHNICAL SUMMARYThe Division of Materials Research and the Office of Advanced Cyberinfrastructure contribute funds to this CAREER award. This award supports an integrated research and education effort on developing and applying computational methods for understanding how nonlinear optical materials respond to light. How nonlinear optical materials respond to light depends on the intensity of the light which leads to interesting phenomena that can be used in technological applications. For example, the dependence of the index of refraction on light intensity can cause a nonlinear optical material to function like a lens causing a light beam to narrow or collapse as it passes through the material. These materials have applications in, for example, noninvasive imaging for medicine, optoelectronic devices, and advanced sensitive quantum mechanical sensors. Understanding and accurate prediction of strong light-matter interaction at microscopic level would help enable the design of novel materials with tailored nonlinear optical properties for specific applications.The goal of this project is to develop and apply methods that starting from knowing the identity of the constituent atoms to predict how specific nonlinear optical materials will respond to light. Emphasis will be placed on novel two-dimensional materials and topological materials which can have metallic states with exotic properties that cover surfaces and edges of the material. This work will elucidate the fundamental role of symmetry, topology, surface/edge, and spin-orbit coupling in nonlinear light-matter interactions. The results obtained from this work will also help generate design principles for nonlinear optical materials and nanostructures. The methods and data acquired will be broadly disseminated to the scientific community, industry, and the general public through open-source distributions.To integrate outreach and education with the research, the PI will host and train high-school students from under-represented groups and secondary school teachers in scientific computing and simulations during summers. The PI will also integrate the research into undergraduate and graduate curricula, provide multidisciplinary training to undergraduate and graduate students, disseminate computational tools in computational materials science summer schools, and promote women in materials science and engineering through seminar series. The graduate students working on this project will acquire an interdisciplinary background in physics, materials science, and high-performance computing. The computer codes and data generated will be shared with the public to benefit the education and outreach in the community. TECHNICAL SUMMARYThe Division of Materials Research and the Office of Advanced Cyberinfrastructure contribute funds to this CAREER award. This award supports an integrated research and education effort on developing and applying predictive first-principles methods for understanding nonlinear optical responses of materials. Materials and nanostructures with tailored nonlinear optical properties are not only important for understanding, probing, and ultimately controlling light-matter interaction at the nanoscale, but highly desirable for many applications such as ultrafast nonlinear optics, biosensing, all-optical transistor and computer, and optical quantum teleportation, communication, and computing. Recently, giant nonlinear optical processes such as second and third harmonic generation were discovered in two-dimensional crystals and topological materials, which challenges the current understanding and requires fundamental investigation at the microscopic level. The goal of this project is to advance fundamental understanding and theoretical prediction of nonlinear light-matter interaction in materials. The research will focus on developing and applying first-principles density-functional-based methods and approaches to investigate and eventually predict second and third order nonlinear optical responses of materials. Spin-orbit coupling, crystalline symmetry, causality, electron-hole interaction, quasiparticle energy, and quasiparticle lifetime due to carrier-carrier and carrier-phonon interactions will be included in this first-principles theoretical framework. Particular emphasis will be placed on elucidating the role of symmetry, electronic topology, surface/edge, and spin-orbit coupling in two-dimensional materials and topological materials. The results obtained will generate new knowledge of nonlinear optical processes and contribute materials design principles for control of light-matter interactions.To integrate outreach and education with the research, the PI will host and train high-school students from under-represented groups and secondary school teachers in scientific computing and simulations during summers to motivate the aspiration and curiosity of the students in science and engineering. The PI will also integrate the research into undergraduate and graduate curricula, provide multidisciplinary training to undergraduate and graduate students, disseminate the developed computational tools in computational materials science summer schools, and promote women in materials science and engineering through seminar series. The graduate students working on this project will acquire a solid interdisciplinary background in physics, materials science, and high-performance computing. In addition, the computational methods, codes, and data generated from this project will be broadly disseminated to the scientific community, the industry, and the general public through open-source distributions with the intent to benefit the broader research, education, and outreach in the community.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.