Tailored polymers as nucleation templates for the synthesis of fluorescing nanodiamonds

定制聚合物作为合成荧光纳米金刚石的成核模板

• 批准号: 438523753
• 负责人: Professor Dr. Ulrich Ziener
• 金额: --
• 依托单位: Institut für Organische Chemie III
• 依托单位国家: 德国
• 项目类别: Research Grants
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/438523753?language=en
• 关键词: Tailored; polymers; nucleation; templates; synthesis

• The project will establish a robust protocol for the controlled synthesis of sub-10-nm fluorescing nanodiamonds (NDs) by a polymer templating process. The polymers will comprise adamantane-type diamondoid sites to facilitate efficient nucleation and growth as well as heteroatom-carrying moieties (mainly N but also Si, Ge) to achieve controlled implantation of heteroatom-vacancy defects (location, number). • The seed polymers will be applied in a high pressure high temperature (HPHT) process to grow NDs using carbon supply from “reactive hydrocarbons” (isocetane/tetracosane) as known for small molecular templates and as we used for the preliminary results on polymer templated NDs. • Vacancies will be introduced by electron beam irradiation or ion beam treatment performed in collaboration with local groups. Annealing will be done at temperatures around 800 °C in vacuum or under inert atmosphere in accordance to standard procedures. • We will analyze the obtained NDs first by electron microscopy and then by absorption and fluorescence spectra on an optical microscope to investigate the nature of the produced NV (and SiV, GeV) centers, photoluminescence quantum yield and lifetime to gain information about the concentration of defects. For the most promising samples, we will turn to autocorrelative techniques and investigate magneto-optical effects on samples with single colour centers in collaboration with the Institute for Quantum Optics. The polymeric approach allows a high local concentration of templating units with control over their location as well as precise incorporation of defects. The yield and quality of the NDs will be strongly improved compared to small molecular templates. The specific goals of this project are, increasing in complexity:1. Preparation of (hetero-)adamantyl monomers and their polymersPolymerization of seed macromolecules with defined monomodal and narrow molar mass distribution and a variety of N, Si, and Ge containing adamantyl monomers will be performed to present ideal nucleation sites for the HPHT process. 2. Production of highly fluorescing and stable NDs with multiple colour centersA controlled amount of aza-, sila- and germaadamantyl will be incorporated into the polymeric templates to steer the heteroatom-vacancy centers. For NV centers we will examine if we can control the nature of the NV center (NV0 or NV-) by controlling the electron-beam acceleration voltage and the annealing temperature. 3. Generation of small NDs with single colour centersEnd group functionalization with aza-, sila-, or germaadamantane or derivatives, respectively, will allow us to incorporate only one heteroatom species per polymeric templating unit to ultimately synthesize nanodiamonds in the range of a few nanometers with single colour centers, which are important as quantum sensors.The process shall be established as a new gold standard for the bottom-up synthesis of fluorescing nanodiamonds.

·该项目将制定一项强有力的议定书，通过聚合物模板工艺控制合成亚10纳米荧光纳米钻石(NDS)。聚合物将包括金刚烷型类金刚石中心，以促进有效的成核和生长，以及携带杂原子的部分(主要是N，但也包括Si，Ge)，以实现对杂原子-空位缺陷(位置，数目)的可控注入。·种子聚合物将应用于高压高温(HPHT)工艺，使用小分子模板已知的“活性碳氢化合物”(异辛烷/正十六烷)的碳供应生长NDS，以及我们在聚合物模板NDS的初步结果中使用的。·将通过电子束照射或与当地团体合作进行的离子束处理来引入空缺。按照标准程序，在真空或惰性气氛中在800°C左右的温度下进行退火热处理。·我们将首先用电子显微镜分析得到的NDS，然后在光学显微镜上通过吸收光谱和荧光光谱来研究产生的NV(和SIV，GeV)中心的性质，光致发光量子产率和寿命，以获得关于缺陷浓度的信息。对于最有希望的样品，我们将转向自相关技术，并与量子光学研究所合作，研究具有单一色心的样品的磁光效应。聚合体方法允许模板单元的高度局部集中，并控制其位置以及精确地结合缺陷。与小分子模板相比，NDS的产量和质量将得到极大的提高。该项目的具体目标是，增加复杂性：1.制备(杂)金刚烷基单体及其聚合物将进行具有定义的单峰和窄摩尔质量分布的种子大分子以及各种含有金刚烷基单体的N、Si和Ge的聚合，为HPHT工艺提供理想的成核位置。2.制备具有多个颜色中心的高荧光、稳定的NDS将在聚合物模板中加入受控数量的氮杂、硅铝和锗金刚烷，以引导杂原子空位中心。对于NV中心，我们将检查是否可以通过控制电子束加速电压和热处理温度来控制NV中心的性质(NV0或NV-)。3.生成具有单色中心的小NDS分别用氮杂金刚烷、硅烷或金刚烷或其衍生物进行端基官能化，将允许我们在每个聚合物模板单元中只加入一种杂原子物种，最终合成具有单一色心的纳米钻石，这是重要的量子传感器。该方法将被确立为自下而上合成荧光纳米钻石的新的金标准。