Rydberg Exciton in Atomically Thin Semiconductor for On-chip Quantum Optoelectronics

里德伯原子是指一种高能量原子，其尺寸比最低能量状态的原子大得多。里德伯原子的大尺寸使它们之间的强相互作用成为可能，可以用于量子信息科学。半导体的光激发可以产生结合在一起的正电荷和负电荷，称为激子。处于高能态的紧密束缚激子，称为里德伯激子，是里德伯原子的类似物，并且具有许多上级性质，例如强相互作用。传统半导体中的里德伯激子要么不够稳定，要么难以图案化和控制。然而，被称为过渡金属二硫属化物（TMDC）的原子薄半导体拥有强大的激子，并在二维（2D）中操纵里德伯激子的令人兴奋的平台。TMDCs中的里德伯激子也有一个新的量子自由度。我们最近开发了一种新的测量技术，具有高灵敏度，以探测有史以来报道的最大的二维里德伯激子。在这个提议中，我们将图案化原子级薄的半导体，这样我们就可以控制面内电场，并研究它与2D里德伯激子的相互作用。我们还将探索里德伯激子之间的强相互作用，这将为量子信息科学的新平台铺平道路。综合教育部分通过研究机会，课程开发和推广活动，为半导体，纳米技术，光学科学和工程培养下一代劳动力，特别强调教育和招聘代表性不足的群体。伦斯勒理工学院现有的项目和新开发的推广项目都将被用来鼓励K-12学生在量子信息科学和工程领域学习。技术说明：里德伯原子是指外层电子占据高激发态，主量子数n很大的原子。里德伯原子之间的强相互作用导致了里德伯封锁等非线性效应，为量子计算和模拟提供了一条有前途的途径。里德伯激子是光激发电子-空穴对的激发态，是里德伯原子的凝聚态类似物，由于成熟的半导体制造和控制技术，可以直接用于光电器件。虽然高阶里德伯激子在Cu_2O晶体中已被广泛研究，但在体半导体中很难对其进行图案化和控制。原子薄的半导体拥有强大的激子，具有大的结合能，也可以有效地静电控制，从而为量子光电子学打开了令人兴奋的机会之门。在这里，我们建议构建高品质的单层过渡金属二硫属化物（TMDCs）的设备中，我们制造的芯片上的p-n结。我们还建议通过我们最近开发的光电流光谱技术来探测和控制里德伯激子，我们已经在单层WSe 2中显示了前所未有的高阶里德伯激子，n = 11。我们将研究里德伯激子对外电场和磁场的敏感响应。我们还将探索非线性效应，并试图首次证明2D里德伯激子封锁。该提案不仅将直接展示基于2D Rydberg激子的量子传感设备的原型，而且还为开创性的平台铺平了道路，以操纵高度可调谐的2D Rydberg激子用于量子信息科学和工程。 紧密结合的研究和教育部分为研究生，本科生和K-12学生提供先进的光学光谱学，纳米器件制造和量子材料的培训机会，特别强调招募代表性不足的群体。该奖项反映了NSF的法定使命，并被认为值得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来支持。

Rydberg atom refers to a high energy atom with a size much larger than the atom at its lowest energy state. The large size of the Rydberg atoms enables strong interactions among themselves that can be exploited for quantum information science. Light excitation of semiconductors can generate positive and negative charges bound together, known as excitons. The tightly bound exciton at the high energy state, known as Rydberg exciton, is an analogue to the Rydberg atom and shares many superior properties, such as the strong interaction. Rydberg excitons in traditional semiconductors are either not stable enough or difficult to be patterned and controlled. The atomically thin semiconductors known as transitional metal dichalcogenides (TMDCs), however, host robust excitons and usher in an exciting platform of manipulating Rydberg excitons in two-dimension (2D). The Rydberg exciton in TMDCs also has a new quantum degree of freedom. We have recently developed a new measurement technique with high sensitivity to probe the largest 2D Rydberg exciton ever reported. In this proposal, we will pattern the atomically thin semiconductor so that we can control the in-plane electric field and study its interaction with the 2D Rydberg excitons. We will also probe the strong interaction between Rydberg excitons, which will pave the way for a new platform for quantum information science. The integrated education components train the next generation workforce for semiconductors, nanoscale technology, optical science and engineering through research opportunities, curriculum development, and outreach activities, with a particular emphasis on educating and recruiting under-represented groups. Both existing programs at Rensselaer Polytechnic Institute and newly developed outreach programs will be utilized to encourage K-12 students to study in the field of quantum information science and engineering.Technical Description: Rydberg atoms refer to the atoms with the outer electron occupying the highly excited state with a very large principal quantum number n. The strong interaction between Rydberg atoms leads to nonlinear effects such as the Rydberg blockade, providing a promising route for quantum computing and simulation. Rydberg exciton, an excited state of the optically excited electron-hole pair, is a condensed matter analogue of the Rydberg atom and can be directly used for optoelectronic devices thanks to mature fabrication and control technologies of semiconductors. Although high-order Rydberg excitons have been extensively studied in Cu2O crystals, it is difficult to pattern and control the Rydberg exciton in bulk semiconductors. Atomically thin semiconductors host robust exciton with large binding energy, which can also be efficiently controlled electrostatically, thereby opening doors to exciting opportunities for quantum optoelectronics. Here we propose to construct high-quality monolayer transitional metal dichalcogenides (TMDCs) devices in which we fabricate an on-chip p-n junction. We also propose to probe and control the Rydberg excitons through our recently developed photocurrent spectroscopy techniques, with which we have shown unprecedented high order Rydberg excitons in monolayer WSe2 with n = 11. We will investigate the Rydberg exciton’s sensitive response to the external electric and magnetic fields. We will also explore nonlinear effects and try to demonstrate the 2D Rydberg exciton blockade for the first time. This proposal will not only directly demonstrate a prototype of a quantum sensing device based on 2D Rydberg excitons but also paves the way for a ground-breaking platform to manipulate highly tunable 2D Rydberg excitons for quantum information science and engineering. The closely integrated research and education components provide training opportunities for graduate, undergraduate, and K-12 students on advanced optical spectroscopy, nanoscale device fabrication, and quantum materials, with special emphasis on recruiting under-represented groups. This proposal also includes outreach programs for K-12 students, such as working with Troy Boys and Girls Club.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.