Pub Date : 2026-10-14Epub Date: 2026-10-01DOI: 10.1021/acs.nanolett.6c03636
Pengpeng Teng, Haifeng Zhao, Wenbin Wang, Dongqin Yuan, Xingjiao Feng, Yatao Zou, Xiyu Luo, Zhongcheng Yuan, Tiankai Zhang, Lian Duan, Tao Yu, Chunxiong Bao, Weidong Xu, Jie Yang, Sai Bai, Xiaodong Shen
Perovskitelight-emitting diodes (LEDs) have attracted significantattention owing to their rapidly increasing external quantum efficiencies(EQEs). However, achieving bright and operationally stable perovskiteLEDs remains a great challenge. Here, we reveal that the most commonlyused surface modifier of zinc-oxide (ZnO) electron-transport layer,polyethylenimine ethoxylate (PEIE), inhibits the perovskite nucleationby inducing in situ chemical reactions of perovskite precursor components,forming thermally unstable interfacial species and reducing long-termoperational stability of resultant devices. We develop a surface-engineeringstrategy by using an ether-based polymer modifier to regulate perovskitecrystallization kinetics and simultaneously suppress ZnO-induced deprotonationduring long-term device operation. As a result, the optimized near-infrared(NIR) perovskite LEDs exhibit a maximum EQE of 24% and a peak radianceof 539 W sr–1 m–2, along withsignificantly enhanced operational stability. Furthermore, partialsubstitution of FA with Cs confirms the generality of this strategy,yielding bright NIR devices with an operational half-lifetime of 561h at 20 mA cm–2.
钙钛矿发光二极管(led)由于其快速提高的外量子效率(EQEs)而引起了人们的广泛关注。然而,实现明亮且运行稳定的钙钛矿led仍然是一个巨大的挑战。本文揭示了氧化锌(ZnO)电子传递层最常用的表面改性剂聚乙烯亚胺乙氧基酸酯(PEIE)通过诱导钙钛矿前驱体组分的原位化学反应抑制钙钛矿成核,形成热不稳定的界面物质并降低所合成器件的长期操作稳定性。我们开发了一种表面工程策略,通过使用醚基聚合物改性剂来调节钙钛矿结晶动力学,同时在设备长期运行期间抑制zno诱导的去质子化。结果表明,优化后的近红外(NIR)钙钛矿led的最大EQE为24%,峰值亮度为539 W sr-1 m-2,同时显著增强了工作稳定性。此外,用Cs部分取代FA证实了这一策略的普遍性,产生了在20 mA cm-2下工作半衰期为561 h的明亮近红外器件。
{"title":"Manipulating Crystallization and Deprotonation Reaction through Surface Engineering of ZnO for Bright and Stable Near-Infrared Perovskite LEDs","authors":"Pengpeng Teng, Haifeng Zhao, Wenbin Wang, Dongqin Yuan, Xingjiao Feng, Yatao Zou, Xiyu Luo, Zhongcheng Yuan, Tiankai Zhang, Lian Duan, Tao Yu, Chunxiong Bao, Weidong Xu, Jie Yang, Sai Bai, Xiaodong Shen","doi":"10.1021/acs.nanolett.6c03636","DOIUrl":"10.1021/acs.nanolett.6c03636","url":null,"abstract":"<p>Perovskitelight-emitting diodes (LEDs) have attracted significantattention owing to their rapidly increasing external quantum efficiencies(EQEs). However, achieving bright and operationally stable perovskiteLEDs remains a great challenge. Here, we reveal that the most commonlyused surface modifier of zinc-oxide (ZnO) electron-transport layer,polyethylenimine ethoxylate (PEIE), inhibits the perovskite nucleationby inducing in situ chemical reactions of perovskite precursor components,forming thermally unstable interfacial species and reducing long-termoperational stability of resultant devices. We develop a surface-engineeringstrategy by using an ether-based polymer modifier to regulate perovskitecrystallization kinetics and simultaneously suppress ZnO-induced deprotonationduring long-term device operation. As a result, the optimized near-infrared(NIR) perovskite LEDs exhibit a maximum EQE of 24% and a peak radianceof 539 W sr<sup>–1</sup> m<sup>–2</sup>, along withsignificantly enhanced operational stability. Furthermore, partialsubstitution of FA with Cs confirms the generality of this strategy,yielding bright NIR devices with an operational half-lifetime of 561h at 20 mA cm<sup>–2</sup>.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"26 40","pages":"13979–13986"},"PeriodicalIF":9.1,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149088201","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-10-14Epub Date: 2026-10-05DOI: 10.1021/acs.nanolett.6c03019
Yuanyuan Qiu, Bin Hua, Zhenping Wang, Fei Hu, Dong Zhang, Yang Lu, Marvin L. Cohen, Alex Zettl, Kecheng Cao, Cong Su, Young Woo Choi, Qingqing Ji
Theatomic thickness of two-dimensional (2D) semiconductorsmakesconventional postgrowth substitutional doping highly challenging.Instead, such atomic substitution can be more effectively achieved in situ through chemical vapor deposition synthesis. However,the mechanistic details governing this growth process have remainedpoorly understood. Using V-doped monolayer MoS2 as a modelsystem, this work elucidates its growth mechanism and doping tunabilityfacilitated by a potassium iodide (KI) promoter. A Raman spectroscopicprobe, established through correlation with scanning transmissionelectron microscopy, was developed to quantify the V dopant concentrationand distribution uniformity. Systematic growth experiments and detailedcharacterizations revealed that doping saturation levels were significantlybelow the precursor feeding ratio. This saturation phenomenon couldbe modulated by KI dosage following a Boltzmann sigmoid function,indicative of an iodide-activated doping mechanism compatible withthe edge passivation substitution (EPS) model. Our findings advancethe doping theory in low-dimensional systems and provide essentialinsights into achieving controlled heteroatom substitution in 2D semiconductors.
{"title":"Boltzmann Sigmoidal Modulation of Vanadium Doping in Monolayer MoS2 by Potassium Iodide","authors":"Yuanyuan Qiu, Bin Hua, Zhenping Wang, Fei Hu, Dong Zhang, Yang Lu, Marvin L. Cohen, Alex Zettl, Kecheng Cao, Cong Su, Young Woo Choi, Qingqing Ji","doi":"10.1021/acs.nanolett.6c03019","DOIUrl":"10.1021/acs.nanolett.6c03019","url":null,"abstract":"<p>Theatomic thickness of two-dimensional (2D) semiconductorsmakesconventional postgrowth substitutional doping highly challenging.Instead, such atomic substitution can be more effectively achieved <em>in situ</em> through chemical vapor deposition synthesis. However,the mechanistic details governing this growth process have remainedpoorly understood. Using V-doped monolayer MoS<sub>2</sub> as a modelsystem, this work elucidates its growth mechanism and doping tunabilityfacilitated by a potassium iodide (KI) promoter. A Raman spectroscopicprobe, established through correlation with scanning transmissionelectron microscopy, was developed to quantify the V dopant concentrationand distribution uniformity. Systematic growth experiments and detailedcharacterizations revealed that doping saturation levels were significantlybelow the precursor feeding ratio. This saturation phenomenon couldbe modulated by KI dosage following a Boltzmann sigmoid function,indicative of an iodide-activated doping mechanism compatible withthe edge passivation substitution (EPS) model. Our findings advancethe doping theory in low-dimensional systems and provide essentialinsights into achieving controlled heteroatom substitution in 2D semiconductors.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"26 40","pages":"13836–13842"},"PeriodicalIF":9.1,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092230","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-10-14DOI: 10.1021/acs.nanolett.6c02284
Zijian Zhou,Chun-Chih Tseng,Wenjun Zheng,Heng Wang,Heze Zhao,Christopher C. Homes,G. L. Carr,D. N. Basov,Yinming Shao,Matthew Yankowitz,Mengkun Liu,Lukas Wehmeier
Abstract Interfacial charge transfer in van der Waals heterostructures provides a powerful, contact-free mechanism to activate two-dimensional plasmons. Chromium iodide (CrI3), a layered ferromagnetic insulator, induces significant doping in adjacent graphene, yet its nanoscale polaritonic response and the optical manifestation of this charge transfer remain unexplored. Here, we report the direct real-space observation of propagating graphene surface plasmon polaritons (SPPs) sustained entirely by spontaneous interfacial charge transfer at the graphene/CrI3 interface. Interestingly, a distinct polaritonic anticrossing near 214 cm–1 (6.4 THz) between the charge-transfer-induced graphene SPP and the CrI3 phonon is identified, suggesting this hybrid system lies within the strong-coupling regime. Our work is enabled by the recent advances in broadband synchrotron near-field nanospectroscopy and suggests intriguing opportunities for magnetically switchable polaritonics in the hybrid charge-transfer heterostructures.
{"title":"Broadband Near-Field\u0000Imaging of Strong Polariton Coupling\u0000in Graphene/CrI3 Heterostructures","authors":"Zijian Zhou,Chun-Chih Tseng,Wenjun Zheng,Heng Wang,Heze Zhao,Christopher C. Homes,G. L. Carr,D. N. Basov,Yinming Shao,Matthew Yankowitz,Mengkun Liu,Lukas Wehmeier","doi":"10.1021/acs.nanolett.6c02284","DOIUrl":"https://doi.org/10.1021/acs.nanolett.6c02284","url":null,"abstract":"Abstract Interfacial charge transfer in van der Waals heterostructures provides a powerful, contact-free mechanism to activate two-dimensional plasmons. Chromium iodide (CrI3), a layered ferromagnetic insulator, induces significant doping in adjacent graphene, yet its nanoscale polaritonic response and the optical manifestation of this charge transfer remain unexplored. Here, we report the direct real-space observation of propagating graphene surface plasmon polaritons (SPPs) sustained entirely by spontaneous interfacial charge transfer at the graphene/CrI3 interface. Interestingly, a distinct polaritonic anticrossing near 214 cm–1 (6.4 THz) between the charge-transfer-induced graphene SPP and the CrI3 phonon is identified, suggesting this hybrid system lies within the strong-coupling regime. Our work is enabled by the recent advances in broadband synchrotron near-field nanospectroscopy and suggests intriguing opportunities for magnetically switchable polaritonics in the hybrid charge-transfer heterostructures.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"42 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209321","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}