Quantum Diamonds at the Beach: Chemical Insights into Silica Growth on Nanoscale Diamond using Multimodal Characterization and Simulation

IF 4.8 Q2 NANOSCIENCE & NANOTECHNOLOGY ACS Nanoscience Au Pub Date : 2023-09-15 DOI:10.1021/acsnanoscienceau.3c00033
Perla J. Sandoval, Karen Lopez, Andres Arreola, Anida Len, Nedah Basravi, Pomaikaimaikalani Yamaguchi, Rina Kawamura, Camron X. Stokes, Cynthia Melendrez, Davida Simpson, Sang-Jun Lee, Charles James Titus, Virginia Altoe, Sami Sainio, Dennis Nordlund, Kent Irwin and Abraham Wolcott*, 
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Abstract

Surface chemistry of materials that host quantum bits such as diamond is an important avenue of exploration as quantum computation and quantum sensing platforms mature. Interfacing diamond in general and nanoscale diamond (ND) in particular with silica is a potential route to integrate room temperature quantum bits into photonic devices, fiber optics, cells, or tissues with flexible functionalization chemistry. While silica growth on ND cores has been used successfully for quantum sensing and biolabeling, the surface mechanism to initiate growth was unknown. This report describes the surface chemistry responsible for silica bond formation on diamond and uses X-ray absorption spectroscopy (XAS) to probe the diamond surface chemistry and its electronic structure with increasing silica thickness. A modified Stöber (Cigler) method was used to synthesize 2–35 nm thick shells of SiO2 onto carboxylic acid-rich ND cores. The diamond morphology, surface, and electronic structure were characterized by overlapping techniques including electron microscopy. Importantly, we discovered that SiO2 growth on carboxylated NDs eliminates the presence of carboxylic acids and that basic ethanolic solutions convert the ND surface to an alcohol-rich surface prior to silica growth. The data supports a mechanism that alcohols on the ND surface generate silyl–ether (ND–O–Si–(OH)3) bonds due to rehydroxylation by ammonium hydroxide in ethanol. The suppression of the diamond electronic structure as a function of SiO2 thickness was observed for the first time, and a maximum probing depth of ∼14 nm was calculated. XAS spectra based on the Auger electron escape depth was modeled using the NIST database for the Simulation of Electron Spectra for Surface Analysis (SESSA) to support our experimental results. Additionally, resonant inelastic X-ray scattering (RIXS) maps produced by the transition edge sensor reinforces the chemical analysis provided by XAS. Researchers using diamond or high-pressure high temperature (HPHT) NDs and other exotic materials (e.g., silicon carbide or cubic-boron nitride) for quantum sensing applications may exploit these results to design new layered or core–shell quantum sensors by forming covalent bonds via surface alcohol groups.

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海滩上的量子钻石:利用多模态表征和模拟揭示纳米级金刚石上二氧化硅生长的化学原理
随着量子计算和量子传感平台的成熟,对承载量子比特(如金刚石)的材料进行表面化学处理是一条重要的探索途径。将一般金刚石,特别是纳米级金刚石(ND)与二氧化硅相接,是将室温量子比特集成到光子设备、光纤、细胞或组织中的一条潜在途径,其功能化化学反应非常灵活。虽然二氧化硅在 ND 内核上的生长已成功用于量子传感和生物标记,但启动生长的表面机制尚不清楚。本报告描述了在金刚石上形成二氧化硅键的表面化学机制,并利用 X 射线吸收光谱 (XAS) 技术探测了随着二氧化硅厚度的增加而产生的金刚石表面化学及其电子结构。采用改良斯托伯(Cigler)法在富含羧酸的玖龙核心上合成了 2-35 纳米厚的二氧化硅外壳。通过电子显微镜等重叠技术对金刚石的形态、表面和电子结构进行了表征。重要的是,我们发现二氧化硅在羧基 ND 上的生长消除了羧酸的存在,碱性乙醇溶液在二氧化硅生长之前将 ND 表面转化为富含醇的表面。这些数据支持一种机制,即 ND 表面的醇在乙醇中通过氢氧化铵的再羟化作用生成硅烷醚(ND-O-Si-(OH)3)键。首次观察到金刚石电子结构的抑制与 SiO2 厚度的函数关系,并计算出最大探测深度为 14 nm。为了支持我们的实验结果,我们利用美国国家标准与技术研究院的表面分析电子能谱模拟(SESSA)数据库建立了基于奥杰电子逸出深度的 XAS 光谱模型。此外,过渡边缘传感器产生的共振非弹性 X 射线散射 (RIXS) 图加强了 XAS 提供的化学分析。将金刚石或高压高温(HPHT)ND 及其他特殊材料(如碳化硅或立方氮化硼)用于量子传感应用的研究人员可以利用这些结果,通过表面醇基形成共价键来设计新的层状或核壳量子传感器。
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来源期刊
ACS Nanoscience Au
ACS Nanoscience Au 材料科学、纳米科学-
CiteScore
4.20
自引率
0.00%
发文量
0
期刊介绍: ACS Nanoscience Au is an open access journal that publishes original fundamental and applied research on nanoscience and nanotechnology research at the interfaces of chemistry biology medicine materials science physics and engineering.The journal publishes short letters comprehensive articles reviews and perspectives on all aspects of nanoscience and nanotechnology:synthesis assembly characterization theory modeling and simulation of nanostructures nanomaterials and nanoscale devicesdesign fabrication and applications of organic inorganic polymer hybrid and biological nanostructuresexperimental and theoretical studies of nanoscale chemical physical and biological phenomenamethods and tools for nanoscience and nanotechnologyself- and directed-assemblyzero- one- and two-dimensional materialsnanostructures and nano-engineered devices with advanced performancenanobiotechnologynanomedicine and nanotoxicologyACS Nanoscience Au also publishes original experimental and theoretical research of an applied nature that integrates knowledge in the areas of materials engineering physics bioscience and chemistry into important applications of nanomaterials.
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