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CsPbI2Br epitaxial shell for efficient PbS quantum dot solar cells 高效PbS量子点太阳能电池用CsPbI2Br外延壳
IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-12 DOI: 10.1007/s12274-024-6988-4
Sami Ur Rahman, Yong-Hui Song, Zhen-Yu Ma, Xiao-Lin Tai, Bai-Sheng Zhu, Yi-Chen Yin, Li-Zhe Feng, Jing-Ming Hao, Guan-Jie Ding, Kuang-Hui Song, Ya-Lan Hu, Tieqiang Li, Jixian Xu, Hong-Bin Yao

Lead sulfide quantum dots (PbS QDs) are promising candidates for high-performance solar cells due to their tunable bandgaps and low-cost solution processing. However, low carrier mobility and numerous surface defects restrict the performance of the fabricated solar cells. Herein, we report the synthesis of novel PbS-perovskite core-shell QDs to solve the low carrier mobility problem of PbS QDs via a facile hot injection method. CsPbI2Br shell enabled strain-free epitaxial growth on the surface of PbS QDs because of 98% lattice match. Our results demonstrate a significant improvement in the photoluminescence and stability of the synthesized PbS-CsPbI2Br QDs upon shell formation, attributed to the effective suppression of surface defects by the epitaxial shell of CsPbI2Br. As a result, the obtained solar cell based on PbS-CsPbI2Br core-shell QD exhibits a power conversion efficiency (PCE) of 8.43%, two times higher than that of pristine PbS QDs. Overall, the construction of PbS-CsPbI2Br core-shell structures represent a promising strategy for advancing the performance of PbS QDs-based optoelectronic devices.

硫化铅量子点(PbS QDs)由于其可调谐的带隙和低成本的溶液处理而成为高性能太阳能电池的有希望的候选者。然而,低载流子迁移率和大量的表面缺陷限制了制备的太阳能电池的性能。本文报道了一种新型PbS-钙钛矿核壳量子点的合成方法,以解决PbS量子点载流子迁移率低的问题。CsPbI2Br壳层在PbS量子点表面实现了98%的晶格匹配,实现了无应变外延生长。我们的研究结果表明,由于CsPbI2Br外延壳有效地抑制了表面缺陷,合成的bs -CsPbI2Br量子点在形成壳后的光致发光和稳定性有了显著改善。结果表明,所制备的基于PbS- cspbi2br核壳量子点的太阳能电池的功率转换效率(PCE)为8.43%,是原始PbS量子点的2倍。总体而言,构建PbS- cspbi2br核壳结构是提高基于PbS qds的光电器件性能的一种很有前途的策略。
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引用次数: 0
Single-particle photoluminescence connects thermal processing with heterogeneity in the trap distribution of cesium lead bromide nanocrystals 单粒子光致发光将热处理与铯-溴化铅纳米晶体阱分布的非均质性联系起来
IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-11 DOI: 10.1007/s12274-024-6989-3
Dong Wang, Jie Chen, Dongyan Zhang, Dariusz M. Niedzwiedzki, Richard A. Loomis, Bryce Sadtler

Understanding the mechanisms of degradation in lead halide perovskite nanocrystals is critical for their future application in optoelectronic devices. We report single-particle measurements of the photoluminescence from cesium lead bromide nanocrystals coated with a silica shell (CsPbBr3@SiO2). Through correlative imaging, we quantified changes in the fluorescence intensity trajectories of the same nanocrystals before and after annealing them at different temperatures. We observe that nearly equal numbers of CsPbBr3@SiO2 nanocrystals exhibit an increase versus decrease in the amount of time they spend in an emissive state after annealing at temperatures of 70 and 100 °C. On the other hand, annealing at 120 °C produces a decrease in the on-fraction for most nanocrystals and, correspondingly, a substantial decrease in the photoluminescence intensity for a thin film annealed at this temperature. We attribute the differences in behavior among individual nanocrystals to heterogeneity in the distribution of trap states that are initially present. X-ray photoelectron, time-resolved photoluminescence, and transient absorption spectroscopies performed on thin films of CsPbBr3@SiO2 nanocrystals indicate that thermal annealing heals electron traps by passivating surface Pb ions and simultaneously creates hole traps through the formation of Pb and Cs vacancies. The relative rates of these parallel processes depend on the annealing temperature, which are important to account for when developing passivation strategies for lead halide perovskite nanocrystals in optoelectronic devices that will operate at elevated temperatures.

了解卤化铅钙钛矿纳米晶体的降解机制对其未来在光电器件中的应用至关重要。我们报告了单粒子测量的光致发光铯-溴化铅纳米晶体包覆二氧化硅外壳(CsPbBr3@SiO2)。通过相关成像,我们量化了相同纳米晶体在不同温度下退火前后荧光强度轨迹的变化。我们观察到,在70°C和100°C退火后,几乎相同数量的CsPbBr3@SiO2纳米晶体在发射状态下花费的时间增加而减少。另一方面,在120℃下退火会使大多数纳米晶体的导通分数降低,相应地,在该温度下退火的薄膜的光致发光强度也会大幅降低。我们将单个纳米晶体之间的行为差异归因于最初存在的陷阱态分布的异质性。对CsPbBr3@SiO2纳米晶体薄膜进行的x射线光电子、时间分辨光致发光和瞬态吸收光谱分析表明,热退火通过钝化表面Pb离子来修复电子陷阱,同时通过形成Pb和Cs空位来产生空穴陷阱。这些平行过程的相对速率取决于退火温度,这对于在高温下工作的光电器件中开发卤化铅钙钛矿纳米晶体的钝化策略非常重要。
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引用次数: 0
Real-time fluorescent detection of food spoilage with doped quantum dots-anchored hydrogel sensor 掺杂量子点锚定水凝胶传感器实时荧光检测食品腐败
IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-11 DOI: 10.1007/s12274-024-6957-y
Chenying Li, Jianzhong Li, Lei Ji, Yibin Zhu, Jiajia Liu, Jiatao Zhang

Spermine assumes a pivotal role in assessing food safety due to its potential to induce a spectrum of diseases upon excessive consumption. However, contemporary spermine detection methodologies, exemplified by high-performance liquid chromatography (HPLC), demand costly instrumentation and the expertise of skilled technicians. To address this challenge, the study introduces a portable fluorescence sensing platform. Ratiometric fluorescent probes were realized through the utilization of CdS quantum dots deeply doped with Ag+ (CdS:Ag QDs) and nitrogen-doped carbon quantum dots (N-CQDs). Hydrogen bonds formed between CdS:Ag QDs and spermine result in the formation of the assembly and the decreasing of the fluorescence intensity. In an effort to broaden the applicative scope and streamline deployment processes, fluorescent sensing hydrogels were meticulously engineered, capitalizing on the swelling properties inherent in polyvinyl alcohol (PVA) hydrogels. The systematic delineation of the correlation between 1 − R/B and spermine concentration facilitates the quantitative determination of spermine concentration. The incorporation of this composite construct serves to alleviate environmental influences on the probes, thereby augmenting their precision. The portable fluorescent sensing platform proves pivotal in expeditiously measuring spermine concentration within the fluorescent sensing hydrogel, enabling a quantitative assessment of pork freshness. The utilization of this platform for food freshness evaluation imparts the benefits of convenience, cost-effectiveness, and intuitive operation.

精胺在评估食品安全方面发挥着关键作用,因为它有可能在过量食用后诱发一系列疾病。然而,以高效液相色谱(HPLC)为例的当代精胺检测方法需要昂贵的仪器和熟练的技术人员的专业知识。为了解决这一挑战,该研究引入了一种便携式荧光传感平台。利用深度掺杂Ag+的CdS量子点(CdS:Ag量子点)和氮掺杂的碳量子点(N-CQDs)实现了比例荧光探针。在CdS:Ag量子点和精胺之间形成氢键,导致组装体的形成和荧光强度的降低。为了扩大应用范围和简化部署过程,荧光传感水凝胶经过精心设计,充分利用聚乙烯醇(PVA)水凝胶固有的膨胀特性。系统地描述了1 - R/B与精胺浓度之间的关系,有助于精胺浓度的定量测定。这种复合结构的结合有助于减轻环境对探针的影响,从而提高其精度。便携式荧光传感平台在荧光传感水凝胶中快速测量精胺浓度,实现猪肉新鲜度的定量评估方面发挥了关键作用。利用该平台进行食品新鲜度评价具有方便、性价比高、操作直观等优点。
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引用次数: 0
Unveiling multimodal hot carrier excitation in plasmonic bimetallic Au@Ag nanostars for photochemistry and SERS sensing 揭示多模态热载子激发等离子体双金属Au@Ag纳米星光化学和SERS传感
IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-26 DOI: 10.1007/s12274-024-6950-5
Yoel Negrín-Montecelo, Amir Elsaidy, Jesús Giráldez-Martínez, Enrique Carbó-Argibay, Zhiming Wang, Alexander O. Govorov, Ramon A. Alvarez-Puebla, Miguel A. Correa-Duarte, Lucas V. Besteiro

Plasmonic nanostructures stand at the forefront of nanophotonics research, particularly in sensing and energy conversion applications. Their unique ability to confine light energy at the nanoscale makes them indispensable for a wide array of technological advancements. The study of these structures often makes use of different materials and, even more extensively, explores new shapes and configurations to extend our common repertoire of useful nanophotonics tools. Exploring the creation of bimetallic plasmonic nanostructures combines these two dimensions determining the space of possible plasmonic resonators and opens the possibility of tailoring systems with behavior unavailable to single-metal plasmonic structures. In this paper, we delve into the exploration of bimetallic systems employing plasmonic nanostars. These structures have demonstrated remarkable capabilities for surface-enhanced Raman scattering (SERS) spectroscopy and photochemistry, due to the strong plasmonic response of their peaks, whose disposition following a spherical symmetry makes them largely polarization- and orientation-insensitive. Herein, we report the colloidal synthesis of two different water-stable Au@Ag nanostars, explore their performance as photocatalysts and SERS substrates, and provide an in-depth account of their non-trivial physical response.

等离子体纳米结构站在纳米光子学研究的前沿,特别是在传感和能量转换应用方面。它们将光能限制在纳米尺度上的独特能力,使它们成为广泛的技术进步所不可或缺的。对这些结构的研究通常使用不同的材料,甚至更广泛地探索新的形状和配置,以扩展我们常用的有用的纳米光子学工具。探索双金属等离子体纳米结构的创造结合了这两个维度,确定了可能的等离子体谐振器的空间,并打开了定制系统的可能性,这些系统的行为是单金属等离子体结构所无法实现的。在本文中,我们深入探讨了利用等离子体纳米星的双金属系统的探索。这些结构在表面增强拉曼散射(SERS)光谱和光化学方面表现出了显著的能力,由于它们的峰具有强烈的等离子体响应,其沿球面对称的分布使得它们在很大程度上对极化和取向不敏感。在此,我们报道了两种不同的水稳定性Au@Ag纳米星的胶体合成,探索了它们作为光催化剂和SERS底物的性能,并深入介绍了它们的非平凡物理响应。
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引用次数: 0
Alkali metal carboxylates as non-polar-facet ligands for the synthesis of colloidal quantum dots 碱金属羧酸盐作为非极性面配体用于胶体量子点的合成
IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-21 DOI: 10.1007/s12274-024-6987-5
Li Luo, Xiaolan Zhou, Xiaozhi Xu, Zhuo Zhao, Chaodan Pu

The impact of alkali metal carboxylates on the synthesis of colloidal quantum dots (CQDs) was investigated. Through a ligand removal experiment, we demonstrated that due to its high hydrophilic nature, sodium oleate dispersed in n-octadecene (ODE) with the formation of micelles with the help of other polar molecules, which resulted in reduced concentration of oleic acid and cadmium oleate both in the solution and on the surface of CQDs. These effects allow for control the size of CdSe CQDs in a wide range when synthesizing them by solely changing the amount of sodium oleate, under either cation-rich or anion-rich conditions. Additionally, enhanced ligand dynamics promote morphology transformation and suppress size deviation caused by different morphologies’ existence in CQDs synthesis. Alkali metal oleate not only stabilized anion-rich CdSe CQDs but also results in highly crystallized wurtzite structure of CdSe CQDs when synthesizing them with excess anions. Furthermore, under anion-rich synthetic condition, anisotropic growth can be realized, leading to nanorods and nanoplatelets based on the alkali metal ions used. Given their outstanding effects and widely applicable synthetic conditions, alkali metal carboxylates offer new possibilities for designing efficient methods for synthesizing CQDs.

研究了碱金属羧酸盐对胶体量子点合成的影响。通过配体去除实验,我们证明了由于油酸钠的高亲水性,在其他极性分子的帮助下,油酸钠通过形成胶束分散在正十八烯(ODE)中,从而导致油酸和油酸镉在溶液中和CQDs表面的浓度降低。这些效应允许在合成CdSe CQDs时,通过单独改变油酸钠的量,在富含阳离子或阴离子的条件下,在很大范围内控制它们的大小。此外,配体动力学的增强促进了CQDs合成过程中形态的转变,抑制了由于不同形态的存在而导致的尺寸偏差。碱金属油酸盐不仅稳定了富含阴离子的CdSe CQDs,而且当过量的阴离子合成CdSe CQDs时,使得CdSe CQDs具有高结晶的纤锌矿结构。此外,在富含阴离子的合成条件下,可以实现各向异性生长,从而产生基于碱金属离子的纳米棒和纳米片。碱金属羧酸酯具有优异的效果和广泛适用的合成条件,为设计高效的CQDs合成方法提供了新的可能性。
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引用次数: 0
Emergent quantum properties from low-dimensional building blocks and their superlattices 低维积木及其超晶格的涌现量子特性
IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-21 DOI: 10.1007/s12274-024-6984-8
Ken Seungmin Hong, Ou Chen, Yusong Bai

Low-dimensional materials, with highly tunable electronic structures depending on their sizes and shapes, can be exploited as fundamental building blocks to construct higher-order structures with tailored emergent properties. This is akin to molecules or crystals that are assembled by atoms with diverse symmetries and interactions. Prominent low-dimensional materials developed in recent decades include zero-dimensional (0D) quantum dots, one-dimensional (1D) carbon nanotubes, and two-dimensional (2D) van der Waals materials. These materials enclose a vast diversity of electronic structures ranging from metals and semimetals to semiconductors and insulators. Moreover, low-dimensional materials can be assembled into higher-order architectures known as superlattices, wherein collective electronic and optical behaviors emerge that are absent in the individual building blocks alone. Superlattices composed of interacting low-dimensional entities thus define an ultra-manipulatable materials platform for realizing artificial structures with customizable functionalities. Here, we review significant milestones and recent progress in the field of low-dimensional materials and their superlattices. We survey recently observed exotic emergent electronic and optical properties in these materials and delve into the underlying mechanisms driving these phenomena. Additionally, we hint the future opportunities and remaining challenges in advancing this exciting area of research.

低维材料具有高度可调的电子结构,这取决于它们的大小和形状,可以作为构建具有定制紧急特性的高阶结构的基本构建模块。这类似于由具有不同对称性和相互作用的原子组成的分子或晶体。近几十年来发展起来的突出的低维材料包括零维(0D)量子点、一维(1D)碳纳米管和二维(2D)范德华材料。这些材料包含了各种各样的电子结构,从金属和半金属到半导体和绝缘体。此外,低维材料可以组装成称为超晶格的高阶结构,其中集体电子和光学行为出现,而这些行为单独存在于单个构建块中。因此,由相互作用的低维实体组成的超晶格定义了一个超可操作的材料平台,用于实现具有可定制功能的人工结构。在这里,我们回顾了低维材料及其超晶格领域的重要里程碑和最新进展。我们调查了最近在这些材料中观察到的奇异的新兴电子和光学性质,并深入研究了驱动这些现象的潜在机制。此外,我们暗示了未来的机会和仍然存在的挑战,以推进这一令人兴奋的研究领域。
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引用次数: 0
Advancement in QDs for optoelectronic applications and beyond 光电应用及其他领域的量子点研究进展
IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-02 DOI: 10.1007/s12274-024-6982-x
Memoona Qammar, Max J. H. Tan, Pengbo Ding, Jianchao Ge, Yinthai Chan, Jonathan E. Halpert

This review focuses on the history and current state of the art optoelectronic applications of quantum dots involving light emission. We focus mainly on three areas of commercial, or potential commercial interest, including quantum dot light emitting devices (QLEDs, sometimes called QD-LEDs), lasing applications, and quantum computing applications. The main connection between these areas is the development of the science and engineering needed to achieve electrical excitation of the quantum dot in an optoelectronic device in order to achieve emission with characteristics particularly suited to the application in question. Due to the special physics of quantum dots, these materials are particularly well suited for both existing commercial applications, and potentially for future applications, such as single photon sources, spin cubits, or polarized emission. We conclude with an analysis of the future prospects for these exciting materials. Given 30 years of progress since the Nobel Prize winning work on monodisperse samples of QDs, our goal is to highlight the current start of the art, discuss the current issues for each technology, and suggest future goals for the next 30 years for quantum dot research.

本文综述了涉及光发射的量子点光电应用的历史和现状。我们主要关注商业或潜在商业利益的三个领域,包括量子点发光器件(qled,有时称为qd - led),激光应用和量子计算应用。这些领域之间的主要联系是实现光电器件中量子点的电激发所需的科学和工程的发展,以便实现具有特别适合于所讨论的应用的特性的发射。由于量子点的特殊物理特性,这些材料特别适合于现有的商业应用,以及潜在的未来应用,如单光子源、自旋腕尺或偏振发射。最后,我们对这些令人兴奋的材料的未来前景进行了分析。自从获得诺贝尔奖以来,量子点的单分散样本已经取得了30年的进展,我们的目标是突出当前艺术的开端,讨论每种技术的当前问题,并建议未来30年量子点研究的未来目标。
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引用次数: 0
NIR-II silver-based quantum dots: Synthesis and applications NIR-II银基量子点:合成与应用
IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-28 DOI: 10.1007/s12274-024-6977-7
Ziyan Zhang, Hongchao Yang, Mingzhe Wang, Yejun Zhang, Jiang Jiang, Qiangbin Wang

Silver-based quantum dots (QDs) such as Ag2S, Ag2Se, and Ag2Te, which emit in the second near-infrared window (NIR-II, 900–1700 nm), have attracted great research interest due to their prominent optical properties and eco-friendly compositions. Over the past decade, the controllable synthesis, bandgap modulation, and fluorescence improvement of NIR-II Ag-based QDs have greatly promoted their practical applications. In this review, we summarize the development process and latest achievements of NIR-II Ag-based QDs, covering major synthesis techniques for fabricating NIR-II Ag-based QDs, general methods for improving their fluorescence properties and recent advances in the applications of NIR-II Ag-based QDs from bioimaging to optoelectronic devices. Finally, we discuss the challenges and prospects of NIR-II Ag-based QDs in their optical properties and applications. This review aims to present synthesis and modification strategies and future application prospects for NIR-II Ag-based QDs, providing guidance for the design and integration of fluorescent probes in NIR-II window.

银基量子点(QDs)如Ag2S、Ag2Se和Ag2Te,在第二个近红外窗口(NIR-II, 900-1700 nm)中发射,由于其突出的光学特性和环保成分而引起了人们的极大兴趣。近十年来,NIR-II ag基量子点的可控合成、带隙调制和荧光性能的提高极大地促进了它们的实际应用。本文综述了NIR-II ag基量子点的发展历程和最新成果,包括制备NIR-II ag基量子点的主要合成技术、提高其荧光特性的一般方法以及NIR-II ag基量子点从生物成像到光电器件的最新应用进展。最后,我们讨论了NIR-II ag基量子点在光学性质和应用方面面临的挑战和前景。本文综述了NIR-II ag基量子点的合成、修饰策略及未来应用前景,为NIR-II窗口荧光探针的设计和集成提供指导。
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引用次数: 0
Instability of colloidal lead halide perovskite nanocrystals: Causes, improvement, and evaluation 胶体卤化铅钙钛矿纳米晶体的不稳定性:原因、改进和评价
IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-28 DOI: 10.1007/s12274-024-6975-9
Thi Kim Tran Tran, Hawi N. Nyiera, Jing Zhao

The instability of colloidal lead halide perovskite nanocrystals (NCs) presents a significant challenge for their application in optoelectronic devices. This review examines the primary causes of instability in these NCs and the proposed mechanisms of degradation. It also introduces the recently developed synthesis and surface passivation methods to address the instability issue of colloidal perovskite NCs. Specifically, we focus on the various types of ligands and precursors introduced during NC synthesis or post-treatment and how they impact the structural and optical properties of the perovskite NCs. This review also proposes a systematic approach to evaluating stability enhancement strategies by establishing key parameters and ranking them based on working and processing conditions. Finally, we discuss the issues that need to be addressed in future research to achieve practical application of lead halide perovskite NCs in advanced optoelectronic systems.

胶体卤化铅钙钛矿纳米晶体(NCs)的不稳定性对其在光电器件中的应用提出了重大挑战。这篇综述探讨了这些NCs不稳定的主要原因和提出的降解机制。介绍了最近发展的合成方法和表面钝化方法,以解决胶体钙钛矿纳米碳的不稳定性问题。具体来说,我们关注在NC合成或后处理过程中引入的各种类型的配体和前体,以及它们如何影响钙钛矿NC的结构和光学性质。本文还提出了通过建立关键参数并根据工作和加工条件对其进行排序来评估稳定性增强策略的系统方法。最后,我们讨论了卤化铅钙钛矿NCs在先进光电系统中实现实际应用需要解决的问题。
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引用次数: 0
Machine learning force field study of carboxylate ligands on the surface of zinc-blende CdSe quantum dots 混合锌镉硒量子点表面羧酸配体的机器学习力场研究
IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-27 DOI: 10.1007/s12274-024-6983-9
Haibing Zhang, Bichuan Cao, Lei Huang, Xiaogang Peng, Linjun Wang

In colloidal quantum dots (QDs), the geometries of surface ligands may play significant roles in tuning the electronic structure, optical spectra and exciton dynamics. We here propose an effective approach to build a diverse dataset of small QDs, based on which the machine learning force field (MLFF) can be obtained based on the DeePMD framework and the energy of each atom is expressed based on the local atomic structure. Using the obtained QD force field (QDFF), molecular dynamics simulation of large zinc-blende CdSe QDs passivated by carboxylate ligands is successfully carried out, and the complex surface structure is extensively studied. We find that bridging, tilted, chelating and claw geometries are the major geometries of carboxylate ligands in CdSe QDs, and the alkyl chain length of ligands plays a significant role. The Markov state model is utilized to reveal the detailed geometry transformation channels. Due to the high performance of QDFF, the present approach is promising for systematic studies of large QDs with different kinds of ligands that can be synthesized in experiment.

在胶体量子点(QDs)中,表面配体的几何形状可能对电子结构、光谱和激子动力学的调节起重要作用。在此,我们提出了一种有效的方法来构建多样化的小量子点数据集,在此基础上,可以基于DeePMD框架获得机器学习力场(MLFF),并根据局部原子结构表示每个原子的能量。利用得到的量子点力场(QDFF),成功地进行了羧酸盐配体钝化大型锌-闪锌矿CdSe量子点的分子动力学模拟,并对其复杂的表面结构进行了广泛的研究。我们发现桥接、倾斜、螯合和爪形几何是CdSe量子点中羧酸盐配体的主要几何形状,而配体的烷基链长度起着重要的作用。利用马尔可夫状态模型揭示了详细的几何变换通道。由于QDFF的高性能,该方法有望用于系统研究具有不同类型配体的大量子点,这些配体可以在实验中合成。
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引用次数: 0
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Nano Research
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