Lisanne M. Einhaus, Xiao Zhang, Jeroen P. Korterik, Guido Mul, Johan E. ten Elshof, Annemarie Huijser
Quasi-2D lead-halide perovskites consist of conducting inorganic layers with tunable thickness (n) separated by large organic spacer cations. Typically, domains with different n and bandgaps are formed within a single film. Here, the crystallization of the films is tuned by mixing Dion-Jacobson (DJ) with Ruddlesden-Popper (RP) spacer cations. Compared to the quasi-2D perovskite film based on solely the DJ type spacer 1,4-phenylenedimethylammonium (PDMA), a film with less defects and more vertically aligned crystallization is achieved by addition of the RP type spacer propylammonium (PA). As the film structure plays an important role in the photophysics, time-resolved photoluminescence (TRPL) and femtosecond transient absorption (TA) are used to investigate the impact of mixing these spacer cations on the dynamics of hot carrier cooling, the occurrence and directionality of energy or electron transfer between the different domains, and the exciton and charge carrier dynamics. Exciton transfer from low-n to high-n domains occurs at a favorable faster rate for the PDMA-based film (0.0640 ps−1) compared to the PA-based film (0.0365 ps−1), while the mixed spacer film demonstrates intermediate behavior (0.0473 ps−1). This study facilitates the design of advanced materials with optimized photophysical characteristics for a next generation of optoelectronic devices.
准二维卤化铅包晶石由厚度(n)可调的导电无机层组成,这些无机层被大的有机间隔阳离子隔开。通常,在单层薄膜中会形成具有不同 n 和带隙的畴。在这里,通过混合 Dion-Jacobson (DJ) 和 Ruddlesden-Popper (RP) 间距阳离子来调整薄膜的结晶。与仅基于 DJ 型间隔物 1,4-亚苯基二甲基铵(PDMA)的准二维包光体薄膜相比,加入 RP 型间隔物丙基铵(PA)后,薄膜的缺陷更少,结晶的垂直排列更整齐。由于薄膜结构在光物理中起着重要作用,因此我们使用时间分辨光致发光(TRPL)和飞秒瞬态吸收(TA)来研究混合这些间隔阳离子对热载流子冷却动力学、不同畴之间能量或电子转移的发生和方向性以及激子和电荷载流子动力学的影响。与基于 PA 的薄膜(0.0365ps-1)相比,基于 PDMA 的薄膜的激子从低 n 域向高 n 域转移的速度更快(0.0640ps-1),而混合间隔物薄膜则表现出中间行为(0.0473ps-1)。这项研究有助于为下一代光电设备设计具有优化光物理特性的先进材料。
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When decorated with plasmonic nanoparticles, pulled optical nanofibers are compatible with plasmonic techniques enabling the ability to probe microenvironments with high spatial and temporal resolution. Although the nanofibers exhibit excellent compatibility for biological samples including cells and tissues, the underlying interactions between the dielectric fiber, plasmonic nanoparticles, and the incident light have been minimally explored. It is shown that the complex coupling of optical and plasmonic properties within the nanofiber strongly influences both the surface‐enhanced Raman scattering (SERS) and photothermal capabilities. Through a combination of experimental results and simulated electric field distributions and spectra it is demonstrated that, although the nanofibers may be homogeneously decorated with gold nanoparticles, the optical effects spatially differ. Specifically, the SERS performance varies periodically based on the diameter of the nanofiber, which is associated with ring resonator modes, while the photothermal effects are more homogeneous over the same diameters, highlighting differences in optoplasmonic properties at this length scale. Through understanding these effects, it may become possible to control temperatures and SERS properties to evaluate processes with micrometric spatial resolution, such as the analytes secreted during temperature‐induced death of single cells.
{"title":"Surface‐Enhanced Raman Scattering and Photothermal Effects on Optoplasmonic Nanofibers","authors":"Gregory Q. Wallace, Emilie Ringe, Karen Faulds, Duncan Graham, Jean‐François Masson","doi":"10.1002/adom.202401640","DOIUrl":"https://doi.org/10.1002/adom.202401640","url":null,"abstract":"When decorated with plasmonic nanoparticles, pulled optical nanofibers are compatible with plasmonic techniques enabling the ability to probe microenvironments with high spatial and temporal resolution. Although the nanofibers exhibit excellent compatibility for biological samples including cells and tissues, the underlying interactions between the dielectric fiber, plasmonic nanoparticles, and the incident light have been minimally explored. It is shown that the complex coupling of optical and plasmonic properties within the nanofiber strongly influences both the surface‐enhanced Raman scattering (SERS) and photothermal capabilities. Through a combination of experimental results and simulated electric field distributions and spectra it is demonstrated that, although the nanofibers may be homogeneously decorated with gold nanoparticles, the optical effects spatially differ. Specifically, the SERS performance varies periodically based on the diameter of the nanofiber, which is associated with ring resonator modes, while the photothermal effects are more homogeneous over the same diameters, highlighting differences in optoplasmonic properties at this length scale. Through understanding these effects, it may become possible to control temperatures and SERS properties to evaluate processes with micrometric spatial resolution, such as the analytes secreted during temperature‐induced death of single cells.","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"12 1","pages":""},"PeriodicalIF":9.0,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142183910","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nithesh Kumar, Estevao Marques Dos Santos, Tahmid H. Talukdar, Judson D. Ryckman
Quantitative Dynamic Structural Color
In article number 2401152 Nithesh Kumar, Judson D. Ryckman, and co-workers demonstrate an approach to overcome the limited sensitivity and often qualitative nature of structural-color-based sensors and indicators in a scheme referred to as ‘quantitative dynamic structural color’. As illustrated in this cover image, their scheme relies on a spectrally engineered mesoporous metamaterial combined with dichromatic laser illumination. The sensors achieve a well-defined and strongly enhanced color response toward refractometric stimuli including small molecules, vapors, and aerosols.