Machine learning force field study of carboxylate ligands on the surface of zinc-blende CdSe quantum dots

IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL
Haibing Zhang, Bichuan Cao, Lei Huang, Xiaogang Peng, Linjun Wang
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Abstract

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.

混合锌镉硒量子点表面羧酸配体的机器学习力场研究
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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来源期刊
Nano Research
Nano Research 化学-材料科学:综合
CiteScore
14.30
自引率
11.10%
发文量
2574
审稿时长
1.7 months
期刊介绍: Nano Research is a peer-reviewed, international and interdisciplinary research journal that focuses on all aspects of nanoscience and nanotechnology. It solicits submissions in various topical areas, from basic aspects of nanoscale materials to practical applications. The journal publishes articles on synthesis, characterization, and manipulation of nanomaterials; nanoscale physics, electrical transport, and quantum physics; scanning probe microscopy and spectroscopy; nanofluidics; nanosensors; nanoelectronics and molecular electronics; nano-optics, nano-optoelectronics, and nano-photonics; nanomagnetics; nanobiotechnology and nanomedicine; and nanoscale modeling and simulations. Nano Research offers readers a combination of authoritative and comprehensive Reviews, original cutting-edge research in Communication and Full Paper formats. The journal also prioritizes rapid review to ensure prompt publication.
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