Haibing Zhang, Bichuan Cao, Lei Huang, Xiaogang Peng, Linjun Wang
{"title":"Machine learning force field study of carboxylate ligands on the surface of zinc-blende CdSe quantum dots","authors":"Haibing Zhang, Bichuan Cao, Lei Huang, Xiaogang Peng, Linjun Wang","doi":"10.1007/s12274-024-6983-9","DOIUrl":null,"url":null,"abstract":"<div><p>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.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":713,"journal":{"name":"Nano Research","volume":"17 :","pages":"10685 - 10693"},"PeriodicalIF":9.0000,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nano Research","FirstCategoryId":"88","ListUrlMain":"https://link.springer.com/article/10.1007/s12274-024-6983-9","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
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.
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.