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

非技术总结材料研究部和先进网络基础设施办公室为这一职业奖项提供资金。该奖项支持一项关于开发和应用计算方法以了解非线性光学材料对光的响应的综合研究和教育努力。非线性光学材料对光的响应取决于光的强度，这导致了可以在技术应用中使用的有趣现象。例如，折射率对光强度的依赖可能会导致非线性光学材料的功能类似于透镜，从而导致光束在穿过材料时变窄或坍塌。例如，这些材料在医学、光电子器件和先进的灵敏量子力学传感器的非侵入性成像方面有应用。在微观水平上理解和准确预测强烈的光-物质相互作用将有助于为特定的应用设计具有定制的非线性光学性质的新型材料。该项目的目标是开发和应用从了解组成原子的身份开始预测特定的非线性光学材料将如何对光做出响应的方法。重点将放在新型二维材料和拓扑材料上，这些材料可以具有覆盖材料表面和边缘的具有奇异性质的金属状态。这项工作将阐明对称性、拓扑学、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。这项工作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。获得的方法和数据将通过开源分发广泛传播给科学界、行业和公众。为了将外展和教育与研究相结合，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。国际和平研究所还将把这项研究纳入本科生和研究生课程，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材料科学和工程领域的女性。从事这个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共享，以促进社区的教育和外展。技术总结材料研究司和先进网络基础设施办公室为这一职业奖项提供资金。该奖项支持一项关于开发和应用预测第一原理方法来理解材料的非线性光学响应的综合研究和教育努力。具有特殊非线性光学性质的材料和纳米结构不仅对理解、探测和最终控制纳米尺度上的光-物质相互作用具有重要意义，而且在许多应用方面也非常重要，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。最近，在二维晶体和拓扑材料中发现了二次、三次谐波等巨型非线性光学过程，这对目前的理解提出了挑战，需要在微观水平上进行基础研究。这个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。这项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途径来研究和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、因果性、电子-空穴相互作用、准粒子能量以及由载流子-载流子和载流子-声子相互作用引起的准粒子寿命将被包括在这个第一原理理论框架中。将特别强调阐明对称性、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。这些成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相结合，PI将在夏季接待和培训未被充分代表的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。国际和平研究所还将把这项研究纳入本科生和研究生课程，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开发的计算工具，并通过系列研讨会促进材料科学和工程领域的妇女。从事这个项目的研究生将在物理、材料科学和高性能计算方面获得坚实的跨学科背景。此外，该项目产生的计算方法、代码和数据将通过开源分发广泛传播给科学界、行业和公众，目的是使社区中更广泛的研究、教育和推广受益。这一奖项反映了NSF的法定使命，并通过使用基金会的智力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.