First-Principles Design of Charged Defects for Two-dimensional Quantum Technologies

二维量子技术带电缺陷的第一性原理设计

• 批准号: 1760260
• 负责人: Yuan Ping
• 金额: $ 35.31万
• 依托单位: University of California-Santa Cruz
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-08-15 至 2022-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1760260&HistoricalAwards=false
• 关键词: First; Principles; Design; Charged; Defects

NONTECHNICAL SUMMARYThis award supports research and education to develop computational methodologies aimed to investigate properties of defects, a kind of imperfection in solid materials. The PI will focus on defects in extremely thin materials, so thin that they are called 2D materials, and layered materials made from stacking them. Computational methods based on advanced theories can be used to help design defects in these materials so that they can be used to emit a single-quantum of light or photon. These single photon emitters can be the heart of building blocks for a new generation of information technology devices. Two-dimensional materials have major advantages over more traditional bulk materials, allowing, for example, easier production and integration into solid-state devices. Computational methods play a key role in designing 2D materials with defects for advanced sensing, computing, information, modeling and communications technologies. This project is aligned with NSF's Quantum Leap Big Idea.This project includes educational activities aimed to increase participation and representation of women in science, technology, engineering, and math (STEM) disciplines, especially in the physical sciences. Efforts in this project are planned to fill a significant gap in the physical and materials chemistry educational curriculum at University of California, Santa Cruz and build up theoretical/computational materials research on the campus under the umbrella of the Materials Science & Engineering Initiative. The activities include developing new computational materials courses for upper-division undergraduate and graduate students, providing undergraduate research opportunities through various existing programs and organizing workshops and seminars that offer career planning advices, especially for women students.TECHNICAL SUMMARYThis award supports theoretical and computational research to develop computational methods and to investigate materials with potential application to quantum information technology. Defects in two-dimensional (2D) materials, such as ultrathin hexagonal Boron Nitride, have been found to be promising single-photon emitters with polarized and ultrabright single-photon emission at room temperature. This discovery opens new possibilities for emerging applications in nanophotonics and quantum information, with potentially much better scalability than the long-studied nitrogen vacancy center (NV-) in diamond. Despite the promising properties that have been experimentally demonstrated to date, accurate first-principles prediction of defect properties in 2D materials remains challenging. Difficulties arise mainly because of the highly anisotropic dielectric screening in 2D materials and the presence of strong many-body interactions, including electron-hole, electron-phonon, and defect-exciton interactions, which are not included in standard density functional theory computer codes. The plans to develop efficient computational methods to accurately determine defect charge transition levels and excited state lifetimes of defects in ultrathin 2D materials and heterojunctions, and then to use them to design complex defects with ideal properties for quantum emitters and quantum computation applications based on first-principles calculations.This research can contribute to resolving long-standing issues of simulating charged defects in 2D materials from first-principles, which necessitates proper treatment of electrostatic potentials of charges near a 2D plane and of the screened Coulomb interaction in many-body perturbation theory. Accurate electronic structure methods developed through this project can be used for determining defect charge transition levels, radiative exciton recombination lifetimes, and phonon-assisted non-radiative lifetimes in defective 2D monolayer and heterojunctions. They will also enable the rational design of quantum defects in 2D materials.This project includes educational activities aimed to increase participation and representation of women in STEM disciplines, especially in the physical sciences. Efforts in this project will fill a significant gap in the physical and materials chemistry educational curriculum at University of California, Santa Cruz (UCSC) and build up theoretical and computational materials research on the campus. Students from physics, chemistry, and engineering departments can join in the research and gain first-hand experience in computational materials research in the PI's group. The PI aims to recruit women and minority students to participate in these experiences. This project will also strengthen the research infrastructure at UCSC, a Hispanic Serving Institution.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.

非技术总结该奖项支持研究和教育，以开发旨在调查缺陷（固体材料中的一种缺陷）特性的计算方法。PI将专注于极薄材料中的缺陷，薄到被称为2D材料，以及由堆叠它们制成的分层材料。基于先进理论的计算方法可以用来帮助设计这些材料中的缺陷，以便它们可以用来发射单量子光或光子。这些单光子发射器可以成为新一代信息技术设备的核心。二维材料比传统的块状材料具有更大的优势，例如更容易生产和集成到固态器件中。计算方法在设计具有缺陷的2D材料方面发挥着关键作用，用于先进的传感，计算，信息，建模和通信技术。该项目与美国国家科学基金会的“量子飞跃大构想”保持一致，包括旨在增加妇女在科学、技术、工程和数学学科，特别是在物理科学领域的参与和代表性的教育活动。该项目旨在填补加州大学（圣克鲁斯）物理和材料化学教育课程的空白，并在材料科学工程倡议的保护下，在校园内建立理论/计算材料研究。这些活动包括为高年级本科生和研究生开发新的计算材料课程，通过各种现有项目提供本科生研究机会，并组织提供职业规划建议的讲习班和研讨会，特别是对女学生。技术总结该奖项支持理论和计算研究，以开发计算方法，并调查材料与量子信息的潜在应用技术.二维（2D）材料中的缺陷，如六方氮化硼，已被发现是有前途的单光子发射体，在室温下具有偏振和超亮单光子发射。这一发现为纳米光子学和量子信息的新兴应用开辟了新的可能性，其可扩展性可能比长期研究的金刚石中的氮空位中心（NV-）更好。尽管到目前为止已经通过实验证明了这些有希望的性质，但准确预测2D材料中缺陷性质的第一性原理仍然具有挑战性。困难的出现主要是因为在2D材料中的高度各向异性的介电屏蔽和强的多体相互作用的存在，包括电子-空穴，电子-声子，和缺陷-激子相互作用，这是不包括在标准的密度泛函理论的计算机代码。该计划开发有效的计算方法，以准确地确定缺陷电荷跃迁能级和激发态寿命的缺陷在二维材料和异质结，然后利用它们设计具有理想性质的复杂缺陷，用于量子发射体和基于第一性原理计算的量子计算应用。从第一性原理出发模拟二维材料中的带电缺陷是一个长期存在的问题，这就需要正确处理二维平面附近电荷的静电势和多体微扰理论中的屏蔽库仑相互作用。通过该项目开发的精确电子结构方法可用于确定缺陷电荷跃迁能级、辐射激子复合寿命和缺陷2D单层和异质结中的声子辅助非辐射寿命。该项目包括旨在提高妇女在STEM学科，特别是在物理科学领域的参与和代表性的教育活动。该项目的努力将填补加州大学圣克鲁斯分校（UCSC）物理和材料化学教育课程中的一个重大空白，并在校园内建立理论和计算材料研究。来自物理、化学和工程系的学生可以参加研究，并在PI小组中获得计算材料研究的第一手经验。PI旨在招募妇女和少数民族学生参加这些体验。该项目还将加强UCSC的研究基础设施，这是一个西班牙裔服务机构。该奖项反映了NSF的法定使命，并被认为是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的支持。

项目成果

Spin-phonon relaxation from a universal ab initio density-matrix approach

• DOI: 10.1038/s41467-020-16063-5
• 发表时间: 2020-06
• 期刊: Nature Communications
• 影响因子: 16.6
• 作者: Junqing Xu;A. Habib;Sushant Kumar;Feng Wu;R. Sundararaman;Y. Ping

Carrier recombination mechanism at defects in wide band gap two-dimensional materials from first principles

• DOI: 10.1103/physrevb.100.081407
• 发表时间: 2019-06
• 期刊: Physical Review B
• 影响因子: 3.7
• 作者: Feng Wu;T. Smart;Junqing Xu;Y. Ping

Fundamental principles for calculating charged defect ionization energies in ultrathin two-dimensional materials

• DOI: 10.1103/physrevmaterials.2.124002
• 发表时间: 2018-08
• 期刊: Physical Review Materials
• 影响因子: 3.4
• 作者: T. Smart;Feng Wu;M. Govoni;Y. Ping

Optical absorption induced by small polaron formation in transition metal oxides: The case of Co3O4

• DOI: 10.1103/physrevmaterials.3.102401
• 发表时间: 2019-09
• 期刊: Physical Review Materials
• 影响因子: 3.4
• 作者: T. Smart;T. Pham;Y. Ping;T. Ogitsu

Dimensionality and anisotropicity dependence of radiative recombination in nanostructured phosphorene

• DOI: 10.1039/c9tc02214g
• 发表时间: 2019-03
• 期刊: Journal of Materials Chemistry C
• 影响因子: 6.4
• 作者: Feng Wu;D. Rocca;Y. Ping