Understanding and Enhancing Electronic Coupling Between Metal Halide Perovskite Quantum Dots Through Surface Molecular Engineering

通过表面分子工程了解和增强金属卤化物钙钛矿量子点之间的电子耦合

• 批准号: 1904547
• 负责人: Jin Zhang
• 金额: $ 45万
• 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: 2019
• 资助国家: 美国
• 起止时间: 2019-07-01 至 2023-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1904547&HistoricalAwards=false
• 关键词: Understanding; Enhancing; Electronic; Coupling; Between

Nanoparticles are extremely small crystals. They can be just a few nanometers in size, or about 100,000 thinner than a sheet of paper, and they can be formed from many different types of materials, including semiconductors. When the electrons are squeezed into very small semiconductor nanocrystals, they become quantum-confined and new properties emerge, which can be harnessed for use in new technologies. Before proceeding to applications, researchers must learn how to pack the quantum dots (QDs) together into solids so that one nanoparticle can share its electrons with another. With support from the Macromolecular, Supramolecular and Nanochemistry Program in the Division of Chemistry, Professors Jin Z. Zhang and Yuan Ping from University of California Santa Cruz (UCSC) are studying QD solids formed from a new class of semiconductors called perovskites. Unlike traditional semiconductors, such as silicon, perovskites are a mixture of inorganic components and organic molecules and this gives rise to unusual properties. Working with their students, Professors Zhang and Pin are developing ways to create stable QD solids where the electrons are easily shared. Their discoveries could impact applications ranging from quantum computing to solar cells. The project also provides training opportunities for future scientists in advanced experimental and computational techniques. Through their "The Sun, Spectroscopy, and Santa Cruz" events held each summer, the research groups are introducing the project to local high school students and teachers to enhance public awareness about science. The research team is developing novel semiconductor QD solids based on metal halide (MH) perovskites. This research addressws the challenge that charge transport properties of QD solids are often limited due to weak coupling between QDs, hindering device applications in emerging technologies. The project is systematically studying the fundamental factors, such as size, shape and surface, that determine the electronic coupling between perovskite QDs (PQDs) by developing designer ligands that enhance both the coupling between the PQDs and their stability. The coupling between PDQs and interaction between ligands are characterized using a combination of time-resolved photoluminescence, transmission electron microscopy, infrared spectroscopy, and ultrafast pump-probe methods. Unique conductive or aromatic ligand molecules are expected to both stabilize the QDs and enhance their electronic coupling so that the QD solids will exhibit strong charge transport while maintaining the novel properties of the QDs. Computational studies based on state-of-the-art quantum mechanical methods are exploring the ligand-PQD interaction and inter-PQD coupling to guide and corroborate experimental studies.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.

纳米颗粒是非常小的晶体。它们可能只有几个纳米大小，或者说大约比一张纸薄10万，它们可以由包括半导体在内的许多不同类型的材料形成。当电子被挤压成非常小的半导体纳米晶体时，它们就会变成量子受限的，新的性质就会出现，这些新的性质可以用在新技术中。在开始应用之前，研究人员必须学习如何将量子点(QD)包装成固体，以便一个纳米粒子可以与另一个纳米粒子共享电子。在化学系大分子、超分子和纳米化学项目的支持下，加州大学圣克鲁斯分校(UCSC)的张金展和袁平教授正在研究由一种名为钙钛矿的新型半导体形成的量子点固体。与硅等传统半导体不同，钙钛矿是无机成分和有机分子的混合物，这导致了不寻常的性质。张教授和平教授正在与他们的学生合作，开发出创造稳定的量子点固体的方法，在这种固体中，电子很容易共享。他们的发现可能会影响从量子计算到太阳能电池的各种应用。该项目还为未来的科学家提供了先进实验和计算技术方面的培训机会。通过每年夏天举行的“太阳、光谱和圣克鲁兹”活动，研究小组向当地高中生和教师介绍该项目，以提高公众对科学的认识。该研究小组正在开发基于金属卤化物(MH)钙钛矿的新型半导体量子点固体。这项研究解决的挑战是，由于量子点之间的弱耦合，量子点固体的电荷传输特性往往受到限制，阻碍了器件在新兴技术中的应用。该项目正在系统地研究决定钙钛矿量子点(PQD)之间电子耦合的基本因素，如尺寸、形状和表面，通过开发设计的配体来增强PQD之间的耦合及其稳定性。用时间分辨光致发光、透射电子显微镜、红外光谱和超快泵浦探测等方法表征了PDQs之间的耦合和配体之间的相互作用。独特的导电或芳香族配体分子有望既稳定量子点又增强其电子耦合，从而使量子点固体在保持量子点新颖性质的同时表现出强大的电荷传输能力。基于最先进的量子力学方法的计算研究正在探索配体-PQD相互作用和PQD间的耦合，以指导和证实实验研究。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Complex Dependence of Optoelectronic Properties of Metal Halide Perovskite Thin Films on Quantum Dot Decoration Layers

• DOI: 10.1021/acs.jpcc.3c03832
• 发表时间: 2023-08-29
• 期刊: JOURNAL OF PHYSICAL CHEMISTRY C
• 影响因子: 3.7
• 作者: Arteaga, Jorge;Cherrette, Vivien;Ghosh, Sayantani
• 通讯作者: Ghosh, Sayantani

Doping Bottleneck in Hematite: Multipole Clustering by Small Polarons

• DOI: 10.1021/acs.chemmater.1c00304
• 发表时间: 2021-06
• 期刊: Chemistry of Materials
• 影响因子: 8.6
• 作者: T. Smart;Valentin Urena Baltazar;Mingpeng Chen;Bin Yao;Kiley Mayford;F. Bridges;Yat Li;Y. Ping-Y.-P

Enhancing Charge Carrier Delocalization in Perovskite Quantum Dot Solids with Energetically Aligned Conjugated Capping Ligands

• DOI: 10.1021/acsenergylett.0c00093
• 发表时间: 2020-03-13
• 期刊: ACS ENERGY LETTERS
• 影响因子: 22
• 作者: Vickers, Evan T.;Enlow, Emily E.;Zhang, Jin Z.
• 通讯作者: Zhang, Jin Z.

Organically Capped Iridium Nanoparticles as High-Performance Bifunctional Electrocatalysts for Full Water Splitting in Both Acidic and Alkaline Media: Impacts of Metal–Ligand Interfacial Interactions

• DOI: 10.1021/acscatal.0c03747
• 发表时间: 2021-01
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Yi Peng;Qiming Liu;Bingzhang Lu;T. He;Forrest Nichols;Xiao Hu;Tiffanie Huang;Grace Huang

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