{"title":"Optoelectronic Properties of PbS Nanocrystals Preserved through L-Type Ligand Surface Reactivity","authors":"Christian Y. Dones Lassalle, Jillian L. Dempsey","doi":"10.1021/acs.chemmater.4c01287","DOIUrl":null,"url":null,"abstract":"In this work, <sup>1</sup>H NMR and photoluminescence spectroscopies have been leveraged to identify how amine-terminated molecules react with the surface of oleate-capped PbS nanocrystals (NCs) and impact their optical properties. The alkyl amine undec-10-ene-1-amine binds weakly to the NC surface and promotes the displacement of the native Z-type ligand Pb(oleate)<sub>2</sub>. Through systematic experiments, we deconvolute the parallel reaction mechanisms that drive this reactivity. The binding and displacement reactivity results in a net-zero change in the NC emission, attributed to preservation of the electronic structure of PbS NCs through surface restructuring. The photoluminescence of PbS NCs remains robust even when exposed to bulky chelating diamines that exclusively promote displacement of Z-type ligands, reactivity that slightly quenches NC emission by exposing undercoordinated chalcogenides and forming trap states. This work improves fundamental understanding of NC surface reactivity with L-type ligands and their potential impact in developing improved NCs.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":null,"pages":null},"PeriodicalIF":7.2000,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemistry of Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acs.chemmater.4c01287","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
In this work, 1H NMR and photoluminescence spectroscopies have been leveraged to identify how amine-terminated molecules react with the surface of oleate-capped PbS nanocrystals (NCs) and impact their optical properties. The alkyl amine undec-10-ene-1-amine binds weakly to the NC surface and promotes the displacement of the native Z-type ligand Pb(oleate)2. Through systematic experiments, we deconvolute the parallel reaction mechanisms that drive this reactivity. The binding and displacement reactivity results in a net-zero change in the NC emission, attributed to preservation of the electronic structure of PbS NCs through surface restructuring. The photoluminescence of PbS NCs remains robust even when exposed to bulky chelating diamines that exclusively promote displacement of Z-type ligands, reactivity that slightly quenches NC emission by exposing undercoordinated chalcogenides and forming trap states. This work improves fundamental understanding of NC surface reactivity with L-type ligands and their potential impact in developing improved NCs.
期刊介绍:
The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.