{"title":"球旋转算法和离散高斯曲率:弯曲纳米石墨烯圆偏振发光光谱模拟的直接方法","authors":"Giovanni Bella, Giuseppe Bruno, Antonio Santoro","doi":"10.1016/j.flatc.2023.100567","DOIUrl":null,"url":null,"abstract":"<div><p>Theoretical innovations for constructing robust computational protocols are of fundamental significance for a variety of advanced chiroptical spectroscopies. The new generation of chiral curved nanographenes offered us the opportunity to study the chiral emission phenomena in the nanometers scale. Herein we reported a distinctive method that combines topological aspects and the density functional theory in order to reach a coherent description of calculated circularly polarized luminescence spectra of negatively curved nanographenes. Our computational plan was defined as a multi-sequence strategy, paying the attention on the relationship between the molecular curvature and the relative spectroscopic properties: 1) the Ball Pivoting Algorithm for the nanographene surface reconstruction; 2) the atom by atom discrete gaussian curvature analysis to establish which DFT functional better approximates the shape of nanographenes backbones; 3) molecular dynamics in the first excited state for accounting the thermal effect; 4) TDDFT benchmark to scrutinize which functional provides the most reliable excitation energies and rotatory strengths for an accurate CPL spectral simulation. The direct merging of the previous steps celebrated the B3LYP (coupled with the 6-311G(d,p) basis set) as the most precise exchange–correlation functional in duplicating exquisitely the CPL profiles of a heterogeneous set of functionalized nanographene.</p></div>","PeriodicalId":316,"journal":{"name":"FlatChem","volume":null,"pages":null},"PeriodicalIF":5.9000,"publicationDate":"2023-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Ball Pivoting Algorithm and discrete gaussian curvature: A direct way to curved nanographene circularly polarized luminescence spectral simulation\",\"authors\":\"Giovanni Bella, Giuseppe Bruno, Antonio Santoro\",\"doi\":\"10.1016/j.flatc.2023.100567\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Theoretical innovations for constructing robust computational protocols are of fundamental significance for a variety of advanced chiroptical spectroscopies. The new generation of chiral curved nanographenes offered us the opportunity to study the chiral emission phenomena in the nanometers scale. Herein we reported a distinctive method that combines topological aspects and the density functional theory in order to reach a coherent description of calculated circularly polarized luminescence spectra of negatively curved nanographenes. Our computational plan was defined as a multi-sequence strategy, paying the attention on the relationship between the molecular curvature and the relative spectroscopic properties: 1) the Ball Pivoting Algorithm for the nanographene surface reconstruction; 2) the atom by atom discrete gaussian curvature analysis to establish which DFT functional better approximates the shape of nanographenes backbones; 3) molecular dynamics in the first excited state for accounting the thermal effect; 4) TDDFT benchmark to scrutinize which functional provides the most reliable excitation energies and rotatory strengths for an accurate CPL spectral simulation. The direct merging of the previous steps celebrated the B3LYP (coupled with the 6-311G(d,p) basis set) as the most precise exchange–correlation functional in duplicating exquisitely the CPL profiles of a heterogeneous set of functionalized nanographene.</p></div>\",\"PeriodicalId\":316,\"journal\":{\"name\":\"FlatChem\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.9000,\"publicationDate\":\"2023-11-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"FlatChem\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2452262723000995\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"FlatChem","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2452262723000995","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Ball Pivoting Algorithm and discrete gaussian curvature: A direct way to curved nanographene circularly polarized luminescence spectral simulation
Theoretical innovations for constructing robust computational protocols are of fundamental significance for a variety of advanced chiroptical spectroscopies. The new generation of chiral curved nanographenes offered us the opportunity to study the chiral emission phenomena in the nanometers scale. Herein we reported a distinctive method that combines topological aspects and the density functional theory in order to reach a coherent description of calculated circularly polarized luminescence spectra of negatively curved nanographenes. Our computational plan was defined as a multi-sequence strategy, paying the attention on the relationship between the molecular curvature and the relative spectroscopic properties: 1) the Ball Pivoting Algorithm for the nanographene surface reconstruction; 2) the atom by atom discrete gaussian curvature analysis to establish which DFT functional better approximates the shape of nanographenes backbones; 3) molecular dynamics in the first excited state for accounting the thermal effect; 4) TDDFT benchmark to scrutinize which functional provides the most reliable excitation energies and rotatory strengths for an accurate CPL spectral simulation. The direct merging of the previous steps celebrated the B3LYP (coupled with the 6-311G(d,p) basis set) as the most precise exchange–correlation functional in duplicating exquisitely the CPL profiles of a heterogeneous set of functionalized nanographene.
期刊介绍:
FlatChem - Chemistry of Flat Materials, a new voice in the community, publishes original and significant, cutting-edge research related to the chemistry of graphene and related 2D & layered materials. The overall aim of the journal is to combine the chemistry and applications of these materials, where the submission of communications, full papers, and concepts should contain chemistry in a materials context, which can be both experimental and/or theoretical. In addition to original research articles, FlatChem also offers reviews, minireviews, highlights and perspectives on the future of this research area with the scientific leaders in fields related to Flat Materials. Topics of interest include, but are not limited to, the following: -Design, synthesis, applications and investigation of graphene, graphene related materials and other 2D & layered materials (for example Silicene, Germanene, Phosphorene, MXenes, Boron nitride, Transition metal dichalcogenides) -Characterization of these materials using all forms of spectroscopy and microscopy techniques -Chemical modification or functionalization and dispersion of these materials, as well as interactions with other materials -Exploring the surface chemistry of these materials for applications in: Sensors or detectors in electrochemical/Lab on a Chip devices, Composite materials, Membranes, Environment technology, Catalysis for energy storage and conversion (for example fuel cells, supercapacitors, batteries, hydrogen storage), Biomedical technology (drug delivery, biosensing, bioimaging)