Tayla Shakespeare,Rajpinder S Seehra,Neftali Flores Rodriguez,Nkolika Atuanya,Thomas M D Sheard,Ralf Köhler,Daniel Bose,Lydia Wunderley,Philip Woodman,Barbara Ciani,Izzy Jayasinghe
Endosomes are nanoscale intracellular compartments that sort and recycle cell-surface receptors such as epidermal growth factor receptor-1 (EGFR1). Nanometer-scale interactions and coclustering of signaling proteins, cargo, and the membrane are critical to this process, yet direct 3D visualization has been hindered by the limited resolution of conventional and super-resolution microscopies. Here, we adapt expansion microscopy (ExM) to visualize and quantify nanoclusters of endosomal proteins in human retinal pigment epithelial (RPE-1) cells. We developed a 3D distortion analysis leveraging the Farneback optical-flow principle to detect anisotropies in hydrogel expansion, revealing under-expansion of cytoplasmic regions within ExM hydrogels and overestimation of size and distance measurements of small compartments such as endosomes. To calibrate ExM images of cytoplasmic regions containing endosomes, we introduced a self-assembling protein nanocage that reports the true local nanoscale expansion factor. To stimulate and visualize EGFR1 internalization and sorting, we applied a pulse-chase protocol with fluorescently tagged epidermal growth factor (EGF), fixed cells at 15 and 30 min, and subjected samples to 10-fold ExM and multiplexed 3D Airyscan microscopy to map cargo and EGFR1 relative to other endosomal proteins. A volume tracing pipeline was developed to visualize the changes in the labeled EGF and EGFR1 densities at the limiting membrane of the endosomes. These changes included enrichment of EGF and EGFR1 in the endosomal interior and accumulation of Rab5a near the limiting membrane during early endosome maturation. Together, this multiplexed 3D ExM toolkit provides a quantitative framework for visualizing and measuring small subcellular organelles at true molecular-scale resolution.
{"title":"Mapping Epidermal Growth Factor Receptor-1 Sorting Domains in Endosomes with a Calibrated Three-Dimensional Expansion Microscopy Toolkit.","authors":"Tayla Shakespeare,Rajpinder S Seehra,Neftali Flores Rodriguez,Nkolika Atuanya,Thomas M D Sheard,Ralf Köhler,Daniel Bose,Lydia Wunderley,Philip Woodman,Barbara Ciani,Izzy Jayasinghe","doi":"10.1021/acsnano.6c00277","DOIUrl":"https://doi.org/10.1021/acsnano.6c00277","url":null,"abstract":"Endosomes are nanoscale intracellular compartments that sort and recycle cell-surface receptors such as epidermal growth factor receptor-1 (EGFR1). Nanometer-scale interactions and coclustering of signaling proteins, cargo, and the membrane are critical to this process, yet direct 3D visualization has been hindered by the limited resolution of conventional and super-resolution microscopies. Here, we adapt expansion microscopy (ExM) to visualize and quantify nanoclusters of endosomal proteins in human retinal pigment epithelial (RPE-1) cells. We developed a 3D distortion analysis leveraging the Farneback optical-flow principle to detect anisotropies in hydrogel expansion, revealing under-expansion of cytoplasmic regions within ExM hydrogels and overestimation of size and distance measurements of small compartments such as endosomes. To calibrate ExM images of cytoplasmic regions containing endosomes, we introduced a self-assembling protein nanocage that reports the true local nanoscale expansion factor. To stimulate and visualize EGFR1 internalization and sorting, we applied a pulse-chase protocol with fluorescently tagged epidermal growth factor (EGF), fixed cells at 15 and 30 min, and subjected samples to 10-fold ExM and multiplexed 3D Airyscan microscopy to map cargo and EGFR1 relative to other endosomal proteins. A volume tracing pipeline was developed to visualize the changes in the labeled EGF and EGFR1 densities at the limiting membrane of the endosomes. These changes included enrichment of EGF and EGFR1 in the endosomal interior and accumulation of Rab5a near the limiting membrane during early endosome maturation. Together, this multiplexed 3D ExM toolkit provides a quantitative framework for visualizing and measuring small subcellular organelles at true molecular-scale resolution.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"11 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147464910","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}
Jonah J. Ng,Dylan M. Ladd,Akhila Mallavarapu,Keith P. White,Gary Chen,Shengsong Yang,Jun Xu,Tony Tian,Christopher B. Murray,Michael F. Toney,Cherie R. Kagan
We report all-inorganic, bicontinuous, bandgap-engineered epitaxially fused PbSe QD/CdS matrix heterostructures achieved through postdeposition sequential colloidal atomic layer deposition (c-ALD). The CdS matrix grows epitaxially on the PbSe QDs to ultimately fully infill the interstitial space between fused PbSe QD arrays in an interpenetrating fashion, resulting in bicontinuous semiconductor heterostructures. The low-energy excitonic absorbance of the epitaxially fused PbSe QD assembly is maintained, and the absorbance at energies above the CdS matrix bandgap increases. The c-ALD grown CdS matrix enhances the oxidative and thermal stability of the QD assemblies, allowing us to preserve the QD/matrix heterostructure upon annealing at 150 °C. By controlling the number of c-ALD cycles and by thermal annealing, we tailor stoichiometry and modulate carrier type, concentration, and mobility probed in the platform of field-effect transistors and the dark current density and responsivity of infrared-absorbing PbSe QD/CdS matrix heterostructure photoconductors. Photoconductors treated with c-ALD and annealed showed an increase in photocurrent modulation, enhancing infrared photoresponsivity. The bicontinuous, bandgap-engineered semiconductor QD/matrix heterostructures provide an architecture that promises the high mobility charge transport and long carrier lifetimes needed to achieve high speed and high quantum efficiency electronic and optoelectronic devices.
{"title":"All-Inorganic, Bicontinuous, Bandgap-Engineered Epitaxially-Fused PbSe Quantum Dot/CdS Matrix Heterostructures for Optoelectronic and Electronic Applications","authors":"Jonah J. Ng,Dylan M. Ladd,Akhila Mallavarapu,Keith P. White,Gary Chen,Shengsong Yang,Jun Xu,Tony Tian,Christopher B. Murray,Michael F. Toney,Cherie R. Kagan","doi":"10.1021/acsnano.6c01036","DOIUrl":"https://doi.org/10.1021/acsnano.6c01036","url":null,"abstract":"We report all-inorganic, bicontinuous, bandgap-engineered epitaxially fused PbSe QD/CdS matrix heterostructures achieved through postdeposition sequential colloidal atomic layer deposition (c-ALD). The CdS matrix grows epitaxially on the PbSe QDs to ultimately fully infill the interstitial space between fused PbSe QD arrays in an interpenetrating fashion, resulting in bicontinuous semiconductor heterostructures. The low-energy excitonic absorbance of the epitaxially fused PbSe QD assembly is maintained, and the absorbance at energies above the CdS matrix bandgap increases. The c-ALD grown CdS matrix enhances the oxidative and thermal stability of the QD assemblies, allowing us to preserve the QD/matrix heterostructure upon annealing at 150 °C. By controlling the number of c-ALD cycles and by thermal annealing, we tailor stoichiometry and modulate carrier type, concentration, and mobility probed in the platform of field-effect transistors and the dark current density and responsivity of infrared-absorbing PbSe QD/CdS matrix heterostructure photoconductors. Photoconductors treated with c-ALD and annealed showed an increase in photocurrent modulation, enhancing infrared photoresponsivity. The bicontinuous, bandgap-engineered semiconductor QD/matrix heterostructures provide an architecture that promises the high mobility charge transport and long carrier lifetimes needed to achieve high speed and high quantum efficiency electronic and optoelectronic devices.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"4 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147462217","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}
Boron neutron capture therapy (BNCT) has received significant attention due to its effectiveness in treating tumors. Preclinical and clinical studies have sought materials with a high boron content. Meanwhile, imaging-guided BNCT can not only enable the determination of the optimal neutron irradiation time and the required dose but also hold substantial significance for evaluating the therapeutic effects. Herein, iron borate (Fe2B2O5) nanobeams were synthesized via the thermal decomposition method. First, iron borate nanobeams are rich in boron, providing sufficient boron for BNCT. Second, the magnetic properties of the nanobeams enable enhancement of magnetic resonance imaging (MRI) contrast, facilitating the monitoring of the agent’s distribution. The size and morphology of the nanobeams can be tuned by varying the synthesis temperature, time, and precursor concentration. To enhance the colloidal stability and biocompatibility, the iron borate nanobeams were coated with a layer of silica (IBNBs@SiO2). The in vitro and in vivo experiments demonstrate that IBNBs@SiO2 functions as a T1 contrast agent. Furthermore, cells and mice treated with IBNBs@SiO2 followed by thermal neutron irradiation demonstrated the effective suppression of melanoma growth. Therefore, IBNBs have potential for MRI-guided BNCT.
{"title":"Iron Borate Nanobeams for Magnetic Resonance Imaging-Guided Boron Neutron Capture Therapy","authors":"Sixia Wang,Junyan Li,Yifan Liu,Ruru Zhang,Lei Chen,Zhe Yang,Jianfeng Zeng,Shuwang Wu,Mingyuan Gao","doi":"10.1021/acsnano.5c16212","DOIUrl":"https://doi.org/10.1021/acsnano.5c16212","url":null,"abstract":"Boron neutron capture therapy (BNCT) has received significant attention due to its effectiveness in treating tumors. Preclinical and clinical studies have sought materials with a high boron content. Meanwhile, imaging-guided BNCT can not only enable the determination of the optimal neutron irradiation time and the required dose but also hold substantial significance for evaluating the therapeutic effects. Herein, iron borate (Fe2B2O5) nanobeams were synthesized via the thermal decomposition method. First, iron borate nanobeams are rich in boron, providing sufficient boron for BNCT. Second, the magnetic properties of the nanobeams enable enhancement of magnetic resonance imaging (MRI) contrast, facilitating the monitoring of the agent’s distribution. The size and morphology of the nanobeams can be tuned by varying the synthesis temperature, time, and precursor concentration. To enhance the colloidal stability and biocompatibility, the iron borate nanobeams were coated with a layer of silica (IBNBs@SiO2). The in vitro and in vivo experiments demonstrate that IBNBs@SiO2 functions as a T1 contrast agent. Furthermore, cells and mice treated with IBNBs@SiO2 followed by thermal neutron irradiation demonstrated the effective suppression of melanoma growth. Therefore, IBNBs have potential for MRI-guided BNCT.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"17 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147462219","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}
Nanofluidic ion transport, traditionally governed by charge-induced electrical double layers (EDLs), has enabled diverse applications in energy conversion, sensing, and ion sieving. However, such transport is intrinsically passive as it relies on static interface charges. Inspired by biological ion channels, which utilize dynamic interface charges to drive active ion pumping in chloroplast thylakoid membranes during photosynthesis, we demonstrate a photo-induced, active bionic ion transport system. This is achieved using an ultrathin nanofluidic membrane constructed from triazine-based covalent organic frameworks (COFs). The nanofluidic membrane is fabricated via confined interface polymerization, yielding a free-standing, large-area, ultrathin (∼40 nm) structure with robust mechanical properties (Young's modulus ∼1.9 GPa). Light induces a dynamic interface charge change and a photoelectric effect that break ionic thermodynamic equilibrium, thereby stimulating active ion transport with ultrafast sensitivity (response time <1 s) and a high ion transport rate (∼6 × 106 ions/s) and achieving a nanofluidic electrokinetic energy conversion (power density >1 mW/m2). The mechanisms underlying dynamic ion transport and active ion pumping are systematically elucidated and experimentally validated. This work demonstrates the potential of COF membranes for applications in areas such as ionic photodetectors, energy conversion systems, field-effect nanofluidic devices, and desalination processes.
{"title":"Bionic Ion Pumps: Triazine-Based Covalent Organic Framework Nanofluidics for Photo-Induced Ion Transport and Nanofluidic Energy Conversion.","authors":"Yadong Wu,Yongchao Qian,Xiaofeng He,Xiang-Yu Kong,Lei Jiang,Liping Wen","doi":"10.1021/acsnano.5c22426","DOIUrl":"https://doi.org/10.1021/acsnano.5c22426","url":null,"abstract":"Nanofluidic ion transport, traditionally governed by charge-induced electrical double layers (EDLs), has enabled diverse applications in energy conversion, sensing, and ion sieving. However, such transport is intrinsically passive as it relies on static interface charges. Inspired by biological ion channels, which utilize dynamic interface charges to drive active ion pumping in chloroplast thylakoid membranes during photosynthesis, we demonstrate a photo-induced, active bionic ion transport system. This is achieved using an ultrathin nanofluidic membrane constructed from triazine-based covalent organic frameworks (COFs). The nanofluidic membrane is fabricated via confined interface polymerization, yielding a free-standing, large-area, ultrathin (∼40 nm) structure with robust mechanical properties (Young's modulus ∼1.9 GPa). Light induces a dynamic interface charge change and a photoelectric effect that break ionic thermodynamic equilibrium, thereby stimulating active ion transport with ultrafast sensitivity (response time <1 s) and a high ion transport rate (∼6 × 106 ions/s) and achieving a nanofluidic electrokinetic energy conversion (power density >1 mW/m2). The mechanisms underlying dynamic ion transport and active ion pumping are systematically elucidated and experimentally validated. This work demonstrates the potential of COF membranes for applications in areas such as ionic photodetectors, energy conversion systems, field-effect nanofluidic devices, and desalination processes.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"31 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147461657","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}
Zichen Wang,Stephanie A Buchholtz,Wooik Jang,Mike Hambsch,Stefan C B Mannsfeld,Xinglong Ren,Ian E Jacobs,Henning Sirringhaus,Hans Kleemann
Organic semiconductors offer a long-spin coherence time and diffusion length due to the weak spin-orbit and hyperfine interactions in these materials. However, in commonly used lateral field-effect transistor structures, it is challenging to define device dimensions comparable to the spin diffusion length. On the other hand, vertical structures, offering smaller device dimensions, are facing issues due to the low carrier mobilities in the vertical dimension. Here, we investigate spin relaxation in rubrene thin films with a triclinic phase, which are doped with C60F48 by coevaporation. The doping provides an efficient way to generate charge carriers, and their high out-of-plane mobility should enhance long-spin diffusion. Using electron-spin resonance, we show that the spin relaxation is governed by the interaction with the dopant counterions and estimate the spin diffusion length to be ∼200 nm. This is comparable to the film thickness, which should make such doped rubrene films an attractive system for spintronic device applications.
{"title":"Charge and Spin Transport in Doped Rubrene Thin-Film Crystals.","authors":"Zichen Wang,Stephanie A Buchholtz,Wooik Jang,Mike Hambsch,Stefan C B Mannsfeld,Xinglong Ren,Ian E Jacobs,Henning Sirringhaus,Hans Kleemann","doi":"10.1021/acsnano.6c02012","DOIUrl":"https://doi.org/10.1021/acsnano.6c02012","url":null,"abstract":"Organic semiconductors offer a long-spin coherence time and diffusion length due to the weak spin-orbit and hyperfine interactions in these materials. However, in commonly used lateral field-effect transistor structures, it is challenging to define device dimensions comparable to the spin diffusion length. On the other hand, vertical structures, offering smaller device dimensions, are facing issues due to the low carrier mobilities in the vertical dimension. Here, we investigate spin relaxation in rubrene thin films with a triclinic phase, which are doped with C60F48 by coevaporation. The doping provides an efficient way to generate charge carriers, and their high out-of-plane mobility should enhance long-spin diffusion. Using electron-spin resonance, we show that the spin relaxation is governed by the interaction with the dopant counterions and estimate the spin diffusion length to be ∼200 nm. This is comparable to the film thickness, which should make such doped rubrene films an attractive system for spintronic device applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"126 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147461745","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}
Hang Liu,Ni Yang,Jiacheng Min,Mykola Telychko,Caisheng Tang,Yi Wan,Chuanqi Zhang,Wanying Li,Lin-Yun Huang,Chengdong Yao,Hoyeon Jeon,Jiahao Liu,Zhengwei Zhang,Xiangdong Yang,George Harrison,Zhongzhe Liu,Tianchao Guo,Jing-Kai Huang,Shadi Fatayer,Kaimin Shih,Song Liu,Thomas D. Anthopoulos,Kian Ping Loh,Lain-Jong Li,Xu Lu
Two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs) exhibit exceptional electrical and optical properties, empowering their promising prospects for future nanoelectronics. Despite major advances in n-type 2D semiconductors, the field has yet to synthesize high-mobility p-type 2D TMDs, in particular WSe2, and systematically query the influence of defects. In this study, we unveil the pivotal role of substitutional impurity defects vis-à-vis the precursor used and growth method employed in defining the quality of 2D p-type WSe2. Density functional theory calculations suggest the adverse effect of Fe-, Co-, Ni- and Si-substituted W impurity defects on the mobility of WSe2, whereas defects such as O-, S-substituted Se and Mo-substituted W pose negligible impact. Guided by the theory, we pinpoint van der Waals (vdW) crystals, commonly used in mechanical exfoliation, as the optimal precursor, and develop a facile vdW crystal physical vapor deposition (PVD) method to grow high-purity monolayer 2D WSe2 film (VPVD-WSe2) that is continuous across a centimeter scale. A suite of spectroscopies confirms the markedly reduced defect density of the as-synthesized WSe2 compared to those by typical chemical vapor deposition methods, and by PVD with commercial or hydrothermal precursors. Scanning tunneling microscopy further evidence the ultralow substitutional impurity defect density of VPVD-WSe2, greatly outperforming the control samples and approaching the mechanically exfoliated counterparts. The VPVD-WSe2 based field-effect transistors exhibit notable electrical performance with record-high field-effect hole mobility up to 112 cm2 V–1s–1 at room temperature, exceeding the best-reported monolayer WSe2 synthesized by chemical vapor deposition and rivaling the mechanically exfoliated 2D WSe2 flakes.
{"title":"Growth of Low-Defect WSe2 Film via High-Purity van der Waals Crystal Precursor","authors":"Hang Liu,Ni Yang,Jiacheng Min,Mykola Telychko,Caisheng Tang,Yi Wan,Chuanqi Zhang,Wanying Li,Lin-Yun Huang,Chengdong Yao,Hoyeon Jeon,Jiahao Liu,Zhengwei Zhang,Xiangdong Yang,George Harrison,Zhongzhe Liu,Tianchao Guo,Jing-Kai Huang,Shadi Fatayer,Kaimin Shih,Song Liu,Thomas D. Anthopoulos,Kian Ping Loh,Lain-Jong Li,Xu Lu","doi":"10.1021/acsnano.5c21076","DOIUrl":"https://doi.org/10.1021/acsnano.5c21076","url":null,"abstract":"Two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs) exhibit exceptional electrical and optical properties, empowering their promising prospects for future nanoelectronics. Despite major advances in n-type 2D semiconductors, the field has yet to synthesize high-mobility p-type 2D TMDs, in particular WSe2, and systematically query the influence of defects. In this study, we unveil the pivotal role of substitutional impurity defects vis-à-vis the precursor used and growth method employed in defining the quality of 2D p-type WSe2. Density functional theory calculations suggest the adverse effect of Fe-, Co-, Ni- and Si-substituted W impurity defects on the mobility of WSe2, whereas defects such as O-, S-substituted Se and Mo-substituted W pose negligible impact. Guided by the theory, we pinpoint van der Waals (vdW) crystals, commonly used in mechanical exfoliation, as the optimal precursor, and develop a facile vdW crystal physical vapor deposition (PVD) method to grow high-purity monolayer 2D WSe2 film (VPVD-WSe2) that is continuous across a centimeter scale. A suite of spectroscopies confirms the markedly reduced defect density of the as-synthesized WSe2 compared to those by typical chemical vapor deposition methods, and by PVD with commercial or hydrothermal precursors. Scanning tunneling microscopy further evidence the ultralow substitutional impurity defect density of VPVD-WSe2, greatly outperforming the control samples and approaching the mechanically exfoliated counterparts. The VPVD-WSe2 based field-effect transistors exhibit notable electrical performance with record-high field-effect hole mobility up to 112 cm2 V–1s–1 at room temperature, exceeding the best-reported monolayer WSe2 synthesized by chemical vapor deposition and rivaling the mechanically exfoliated 2D WSe2 flakes.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"3 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147462216","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}
Exciton-plasmon polaritons, leveraging the coherent nature of their photonic component, can overcome the localization of excitations in disordered molecular solids and enable long-range transport. However, a clear understanding of how the optical cavity properties govern polariton transport is lacking. Furthermore, most studies demonstrated unidirectional propagation of polaritons. An active directional control of polariton propagation, crucial for expanding its optoelectronic functionality, remains much less explored. Here, we show enhanced and anisotropic long-range energy transport in molecular aggregates strongly coupled with surface plasmons on two-dimensional plasmonic nanoarrays. The nanoarrays exhibit in-plane angle-dependent, anisotropic, and periodically modulated plasmonic resonant properties (diffraction order, resonance energy and line width) stemming from the anisotropic dispersion of the plasmonic hexagonal lattice, leading to an anisotropic periodic modulation of the cavity-molecule coupling strength. Wavelength-resolved, momentum-selected real-space photoluminescence study reveals enhanced coherent propagation of upper and lower polaritons with ∼10 μm and large group velocities on the order of the speed of light. Crucially, an anisotropic propagation distance contrast of 90% has been achieved by tuning the dispersion and quality factor of plasmonic modes. The results provide valuable guidance for developing coherent, directional energy transport devices for photovoltaics, photocatalysis, optical routing, and organic optoelectronics applications.
{"title":"Directional Control of Strong Coupling Enables Anisotropic Propagation of Molecular Exciton-Polaritons.","authors":"Kaizhen Liu,Yueyue Wei,Jiang Hu,Juyan Tian,Peng Sun,Guangjun Zhang,Niu Xu,Weiming Song,Jin Yang,Si-Ru Shao,Jing-Jing Guo,Hao He,Jun Yi,Wenxin Wang,Bowen Liu,Jin-Hui Zhong","doi":"10.1021/acsnano.5c17969","DOIUrl":"https://doi.org/10.1021/acsnano.5c17969","url":null,"abstract":"Exciton-plasmon polaritons, leveraging the coherent nature of their photonic component, can overcome the localization of excitations in disordered molecular solids and enable long-range transport. However, a clear understanding of how the optical cavity properties govern polariton transport is lacking. Furthermore, most studies demonstrated unidirectional propagation of polaritons. An active directional control of polariton propagation, crucial for expanding its optoelectronic functionality, remains much less explored. Here, we show enhanced and anisotropic long-range energy transport in molecular aggregates strongly coupled with surface plasmons on two-dimensional plasmonic nanoarrays. The nanoarrays exhibit in-plane angle-dependent, anisotropic, and periodically modulated plasmonic resonant properties (diffraction order, resonance energy and line width) stemming from the anisotropic dispersion of the plasmonic hexagonal lattice, leading to an anisotropic periodic modulation of the cavity-molecule coupling strength. Wavelength-resolved, momentum-selected real-space photoluminescence study reveals enhanced coherent propagation of upper and lower polaritons with ∼10 μm and large group velocities on the order of the speed of light. Crucially, an anisotropic propagation distance contrast of 90% has been achieved by tuning the dispersion and quality factor of plasmonic modes. The results provide valuable guidance for developing coherent, directional energy transport devices for photovoltaics, photocatalysis, optical routing, and organic optoelectronics applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"130 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147464912","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}
Kaelyn. S. McFarlane-Connelly,Niamh L. Brown,Hua Zhu,Oliver M. Nix,Moungi G. Bawendi
Weakly confined semiconductor nanocrystals have distinct photophysical properties that arise from coherently delocalized excitons. Experimental observation of these properties has been untested for sizes well beyond those of the Bohr exciton. We produce a size series of CsPbBr3 weakly confined perovskite nanocrystals (WC-PNCs) with volumes up to ∼1000 times that of the Bohr exciton using a continuous injection procedure that controls growth at elevated temperatures. Through this reaction scheme, we are able to prepare WC-PNCs with high quantum yields and homogeneity, allowing for the observation of size-dependent optical properties. Single WC-PNCs at cryogenic temperatures exhibit excitonic emission at a radiative rate proportional to the nanocrystal volume. This dependence is consistent with coherent delocalization of the weakly confined exciton over the entire PNC volume and results in exceptionally fast radiative lifetimes (∼35 ps on average for the largest 80 nm PNCs). The properties of excitons in the weakly confined regime are well suited to the grand challenge of discovering materials for next-generation, light-based quantum technologies.
{"title":"Extending the Weakly Confined Regime of Perovskite Nanocrystals for Fast Emission at Low Temperature","authors":"Kaelyn. S. McFarlane-Connelly,Niamh L. Brown,Hua Zhu,Oliver M. Nix,Moungi G. Bawendi","doi":"10.1021/acsnano.5c18641","DOIUrl":"https://doi.org/10.1021/acsnano.5c18641","url":null,"abstract":"Weakly confined semiconductor nanocrystals have distinct photophysical properties that arise from coherently delocalized excitons. Experimental observation of these properties has been untested for sizes well beyond those of the Bohr exciton. We produce a size series of CsPbBr3 weakly confined perovskite nanocrystals (WC-PNCs) with volumes up to ∼1000 times that of the Bohr exciton using a continuous injection procedure that controls growth at elevated temperatures. Through this reaction scheme, we are able to prepare WC-PNCs with high quantum yields and homogeneity, allowing for the observation of size-dependent optical properties. Single WC-PNCs at cryogenic temperatures exhibit excitonic emission at a radiative rate proportional to the nanocrystal volume. This dependence is consistent with coherent delocalization of the weakly confined exciton over the entire PNC volume and results in exceptionally fast radiative lifetimes (∼35 ps on average for the largest 80 nm PNCs). The properties of excitons in the weakly confined regime are well suited to the grand challenge of discovering materials for next-generation, light-based quantum technologies.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"31 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147462218","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}
Aleksei V. Emelianov, Kamila K. Mentel, Amr Ghazy, Joona Pekkanen, Yu-Han Wang, Andreas Johansson, Maarit Karppinen, Mika Pettersson
Developing a controlled, defect-free, and spatially selective deposition of molecular and hybrid thin films on 2D materials remains a key challenge for their integration into multifunctional optoelectronic systems due to their surface inertness. Here, we demonstrate area-selective atomic/molecular layer deposition of europium-organic (Eu-BDC) thin films on graphene utilizing direct femtosecond laser two-photon oxidation. The laser dose defines the density of nucleation sites and precisely controls Eu-BDC film thickness and uniformity. By optimizing the deposition parameters and carefully choosing a transfer polymer, we achieve over 90% selectivity and high film homogeneity in the activated areas with submicron resolution. Upon 532 nm excitation, graphene/Eu-BDC exhibits strong emission at 612 nm with additional lines at 579, 592, and 652 nm. It also shows a green band at ∼566 nm, which is not observed on Si/SiO2. Photoluminescence quenching on graphene shortens lifetimes due to energy and charge transfer at the graphene/Eu-organic interface. Moreover, the Eu-organic layer lowers the graphene work function and shifts the Dirac point, indicating a controllable n-type doping. The same laser modification strategy is also demonstrated on other 2D materials, as shown for MoS2 and WS2. This resist-free approach enables area-selective growth on 2D surfaces with tunable optical and electronic properties, providing compact integration of patterned emitters and photodetectors on a single chip.
由于其表面惰性，在二维材料上开发一种可控的、无缺陷的、空间选择性的分子和杂化薄膜沉积仍然是将其集成到多功能光电系统中的关键挑战。在这里，我们展示了利用直接飞秒激光双光子氧化在石墨烯上区域选择性沉积铕有机（Eu-BDC）薄膜的原子/分子层。激光剂量决定了成核位点的密度，并精确控制了Eu-BDC膜的厚度和均匀性。通过优化沉积参数和精心选择转移聚合物，我们在亚微米分辨率的活化区实现了90%以上的选择性和高膜均匀性。在532 nm激发下，石墨烯/Eu-BDC在612 nm处表现出强烈的发射，在579、592和652nm处有额外的发光线。它还在~ 566 nm处显示出绿带，这在Si/SiO2上没有观察到。由于石墨烯/ eu -有机界面上的能量和电荷转移，石墨烯上的光致发光猝灭缩短了寿命。此外，eu -有机层降低了石墨烯的功函数并移动了狄拉克点，表明这是一种可控的n型掺杂。同样的激光修饰策略也在其他二维材料上得到了证明，如MoS2和WS2。这种无电阻的方法可以在具有可调光学和电子特性的二维表面上实现区域选择性生长，在单个芯片上提供了图案发射器和光电探测器的紧凑集成。
{"title":"Area-Selective Atomic/Molecular Layer Deposition of Europium-Organic Thin Films on Graphene and Other 2D Materials for Photoluminescent Heterostructures","authors":"Aleksei V. Emelianov, Kamila K. Mentel, Amr Ghazy, Joona Pekkanen, Yu-Han Wang, Andreas Johansson, Maarit Karppinen, Mika Pettersson","doi":"10.1021/acsnano.5c22728","DOIUrl":"https://doi.org/10.1021/acsnano.5c22728","url":null,"abstract":"Developing a controlled, defect-free, and spatially selective deposition of molecular and hybrid thin films on 2D materials remains a key challenge for their integration into multifunctional optoelectronic systems due to their surface inertness. Here, we demonstrate area-selective atomic/molecular layer deposition of europium-organic (Eu-BDC) thin films on graphene utilizing direct femtosecond laser two-photon oxidation. The laser dose defines the density of nucleation sites and precisely controls Eu-BDC film thickness and uniformity. By optimizing the deposition parameters and carefully choosing a transfer polymer, we achieve over 90% selectivity and high film homogeneity in the activated areas with submicron resolution. Upon 532 nm excitation, graphene/Eu-BDC exhibits strong emission at 612 nm with additional lines at 579, 592, and 652 nm. It also shows a green band at ∼566 nm, which is not observed on Si/SiO<sub>2</sub>. Photoluminescence quenching on graphene shortens lifetimes due to energy and charge transfer at the graphene/Eu-organic interface. Moreover, the Eu-organic layer lowers the graphene work function and shifts the Dirac point, indicating a controllable n-type doping. The same laser modification strategy is also demonstrated on other 2D materials, as shown for MoS<sub>2</sub> and WS<sub>2</sub>. This resist-free approach enables area-selective growth on 2D surfaces with tunable optical and electronic properties, providing compact integration of patterned emitters and photodetectors on a single chip.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"87 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147466016","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}
The ongoing downscaling of semiconductor devices necessitates gate dielectric materials that simultaneously possess a wide bandgap and ultrahigh dielectric constant to ensure efficient gate control. However, such materials remain scarce due to the inherent trade-off between bandgap widening and dielectric response enhancement in conventional insulators. Here, we demonstrate bismuth oxyfluoride (BiOF) as a promising dielectric candidate with a wide bandgap (Eg ≈ 4.5 eV) and a high out-of-plane dielectric constant (κ = 22.5). Moreover, we develop a scalable solid-state route for synthesizing phase-pure BiOF powder and achieve the chemical vapor deposition (CVD) growth of ultrathin BiOF nanosheets. The free-standing characteristic, temperature-stable dielectric properties, and inert van der Waals (vdW) surface of BiOF facilitate its seamless integration with two-dimensional (2D) materials to enhance device performance. Few-layer graphene double-encapsulated by BiOF demonstrates superior electron Hall mobility (μe,2K ≈ 134,000 cm2 V-1 s-1) and pronounced Shubnikov-de Haas (SdH) oscillations at 2 K. Our work not only expands the library of high-κ vdW materials but also overcomes the intrinsic trade-off between dielectric constant and bandgap.
{"title":"A Layered Wide-Bandgap BiOF Gate Dielectric with a High Dielectric Constant.","authors":"Jiabiao Chen,Xinyue Dong,Yameng Hou,Xiang Chen,Lan Lan,Zhaochao Liu,Fengbo Yan,Zunxian Lv,Yuyu He,Mingjian Yang,Huixia Fu,Xuewen Fu,Wenbin Li,Feng Luo,Jinxiong Wu","doi":"10.1021/acsnano.5c18038","DOIUrl":"https://doi.org/10.1021/acsnano.5c18038","url":null,"abstract":"The ongoing downscaling of semiconductor devices necessitates gate dielectric materials that simultaneously possess a wide bandgap and ultrahigh dielectric constant to ensure efficient gate control. However, such materials remain scarce due to the inherent trade-off between bandgap widening and dielectric response enhancement in conventional insulators. Here, we demonstrate bismuth oxyfluoride (BiOF) as a promising dielectric candidate with a wide bandgap (Eg ≈ 4.5 eV) and a high out-of-plane dielectric constant (κ = 22.5). Moreover, we develop a scalable solid-state route for synthesizing phase-pure BiOF powder and achieve the chemical vapor deposition (CVD) growth of ultrathin BiOF nanosheets. The free-standing characteristic, temperature-stable dielectric properties, and inert van der Waals (vdW) surface of BiOF facilitate its seamless integration with two-dimensional (2D) materials to enhance device performance. Few-layer graphene double-encapsulated by BiOF demonstrates superior electron Hall mobility (μe,2K ≈ 134,000 cm2 V-1 s-1) and pronounced Shubnikov-de Haas (SdH) oscillations at 2 K. Our work not only expands the library of high-κ vdW materials but also overcomes the intrinsic trade-off between dielectric constant and bandgap.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"86 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147461660","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}
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