EAGER: Enabling Quantum Leap: Temperature dependence of optical nonlinearities of monolayer transition-metal dichalcogenides

该项目有助于开发一种新型光学量子计算设备，该设备使用固态薄膜材料构建，可以在室温下工作。这些新设备有可能彻底改变信息技术，其应用范围从密码破译到网络上的超安全通信。本项目研究的固态薄膜材料最令人兴奋的特点之一是，它们有可能使量子信息处理设备既不需要低温环境，也不需要高真空环境，这比以前的方法增加了大量的体积和复杂性。该项目专门解决了关于材料二硒化钼单层薄膜的室温光学特性的一系列开放性问题，这些问题的答案对于预测实际计算系统的最佳可实现性能至关重要。虽然二硒化钼的体晶体已经研究了很长时间，但最近制备和表征单层样品（只有几个原子厚）的方法的发展引发了人们对这种材料的新兴趣，因为这些薄膜的性质与体样品的性质明显不同。除了对实际量子信息技术发展的影响之外，本研究还有助于博士生的跨学科培训，以及为量子工程新兴领域的课堂教学开发最先进的教育材料。本项目主要对单层过渡金属二硫化物在4K ~ 300K温度范围内的非线性光学响应和背景光吸收进行实验和理论研究。该项目利用了激光退火技术的最新进展来制备高质量的大面积均匀二硒化钼样品，以及与束缚激子态之间跃迁相关的kerr型非线性的最新理论计算。该项目旨在扩展先前的测量和计算，以评估有限温度下激子-声子和激子-激子相互作用相关的退相干，并通过实验验证参数，在室温下获得过渡金属二硫化物量子光子器件的量子光学输入输出模型。该项目还旨在评估基于多层过渡金属二硫族化物单层堆叠构建非线性光子谐振器的可行性，并预测此类器件在量子光子信息处理中的最佳性能。该项目更广泛的影响包括研究生的跨学科培训，以及在量子光学和量子材料交叉领域为研究生水平的教学开发跨学科材料。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。

This project contributes to efforts to develop a new class of optical quantum computing devices that are constructed using solid-state thin film materials and can operate at room temperature. Such new devices have the potential to revolutionize information technology, with applications ranging from cryptographic code-breaking to ultra-secure communication over networks. One of the most exciting features of the solid-state thin film materials investigated in this project is their potential to enable quantum information processing devices that require neither cryogenic nor high-vacuum environments, which add substantial bulk and complexity to prior approaches. This project specifically addresses a set of open questions regarding the room-temperature optical properties of monolayer thin films of the material molybdenum diselenide, the answers to which are crucial for predicting the best achievable performance of practical computing systems. Although bulk crystals of molybdenum diselenide have long been studied, the recent development of methods to prepare and characterize monolayer specimens - just a few atoms thick - have sparked new interest in this material because the properties of these thin films are markedly different from those of bulk samples. Above and beyond its implications for the development of practical quantum information technology, this research contributes to the interdisciplinary training of Ph.D. students and to the development of state-of-the-art educational materials for classroom teaching in emerging areas of quantum engineering.This project focuses on experimental and theoretical studies of the nonlinear optical responses and background optical absorption of monolayer transition-metal dichalcogenides over the temperature range from 4K to 300K. The project leverages recent advances in the use of laser annealing to prepare high quality large-area homogeneous samples of molybdenum diselenide, as well as recent theoretical calculations of Kerr-type nonlinearities associated with transitions among bound exciton states. The project aims to extend prior measurements and calculations to assess decoherence associated with exciton-phonon and exciton-exciton interactions at finite temperatures, and to arrive at quantum optical input-output models of transition metal dichalcogenide-based quantum photonic devices at room temperature with experimentally validated parameters. The project also aims specifically to assess the feasibility of constructing nonlinear photonic resonators based on stacks of multiple transition metal dichalcogenide monolayers, and to predict the best possible performance of such devices for quantum photonic information processing. Broader impacts of the project include interdisciplinary training of graduate students and the development of interdisciplinary material for graduate-level teaching at the intersection of quantum optics and quantum materials.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.