ACS Nano最新文献_第6页

3D Bioprinting of Artificial Skin Substitute with Improved Mechanical Property and Regulated Cell Behavior through Integrating Patterned Nanofibrous Films 通过整合图案化纳米纤维膜，三维生物打印出具有更佳机械性能和可调细胞行为的人造皮肤替代物

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2024-06-28 DOI: 10.1021/acsnano.4c04088

Shaoquan Bian, Xiaohua Hu, Hao Zhu, Weili Du, Chenmin Wang, Liangliang Wang, Liuzhi Hao, Yuming Xiang, Fengzhen Meng, Chengwei Hu, Zhiyun Wu, Jing Wang, Xiaohua Pan, Min Guan, William Weijia Lu, Xiaoli Zhao

Three-dimensional (3D) bioprinting has advantages for constructing artificial skin tissues in replicating the structures and functions of native skin. Although many studies have presented improved effect of printing skin substitutes in wound healing, using hydrogel inks to fabricate 3D bioprinting architectures with complicated structures, mimicking mechanical properties, and appropriate cellular environments is still challenging. Inspired by collagen nanofibers withstanding stress and regulating cell behavior, a patterned nanofibrous film was introduced to the printed hydrogel scaffold to fabricate a composite artificial skin substitute (CASS). The artificial dermis was printed using gelatin–hyaluronan hybrid hydrogels containing human dermal fibroblasts with gradient porosity and integrated with patterned nanofibrous films simultaneously, while the artificial epidermis was formed by seeding human keratinocytes upon the dermis. The collagen-mimicking nanofibrous film effectively improved the tensile strength and fracture resistance of the CASS, making it sewable for firm implantation into skin defects. Meanwhile, the patterned nanofibrous film also provided the biological cues to guide cell behavior. Consequently, CASS could effectively accelerate the regeneration of large-area skin defects in mouse and pig models by promoting re-epithelialization and collagen deposition. This research developed an effective strategy to prepare composite bioprinting architectures for enhancing mechanical property and regulating cell behavior, and CASS could be a promising skin substitute for treating large-area skin defects.

三维（3D）生物打印在构建人造皮肤组织方面具有复制原生皮肤结构和功能的优势。尽管许多研究表明打印皮肤替代物在伤口愈合方面有更好的效果，但使用水凝胶油墨制造具有复杂结构、模拟机械特性和适当细胞环境的三维生物打印架构仍具有挑战性。受胶原蛋白纳米纤维可承受应力和调节细胞行为的启发，我们在打印的水凝胶支架上引入了图案化纳米纤维膜，以制造复合人造皮肤替代物（CASS）。人造真皮是用明胶-透明质酸混合水凝胶印制的，其中含有具有梯度孔隙率的人类真皮成纤维细胞，并同时与图案化纳米纤维膜集成；人造表皮则是通过在真皮上播种人类角质形成的。仿胶原纳米纤维膜有效提高了 CASS 的拉伸强度和抗断裂强度，使其可缝合牢固地植入皮肤缺损部位。同时，图案化纳米纤维膜还提供了引导细胞行为的生物线索。因此，CASS 可通过促进再上皮化和胶原沉积，有效加速小鼠和猪模型大面积皮肤缺损的再生。这项研究为制备复合生物打印结构提供了一种有效的策略，可用于提高机械性能和调节细胞行为，CASS可作为一种有前途的皮肤替代物用于治疗大面积皮肤缺损。

{"title":"3D Bioprinting of Artificial Skin Substitute with Improved Mechanical Property and Regulated Cell Behavior through Integrating Patterned Nanofibrous Films","authors":"Shaoquan Bian, Xiaohua Hu, Hao Zhu, Weili Du, Chenmin Wang, Liangliang Wang, Liuzhi Hao, Yuming Xiang, Fengzhen Meng, Chengwei Hu, Zhiyun Wu, Jing Wang, Xiaohua Pan, Min Guan, William Weijia Lu, Xiaoli Zhao","doi":"10.1021/acsnano.4c04088","DOIUrl":"https://doi.org/10.1021/acsnano.4c04088","url":null,"abstract":"Three-dimensional (3D) bioprinting has advantages for constructing artificial skin tissues in replicating the structures and functions of native skin. Although many studies have presented improved effect of printing skin substitutes in wound healing, using hydrogel inks to fabricate 3D bioprinting architectures with complicated structures, mimicking mechanical properties, and appropriate cellular environments is still challenging. Inspired by collagen nanofibers withstanding stress and regulating cell behavior, a patterned nanofibrous film was introduced to the printed hydrogel scaffold to fabricate a composite artificial skin substitute (CASS). The artificial dermis was printed using gelatin–hyaluronan hybrid hydrogels containing human dermal fibroblasts with gradient porosity and integrated with patterned nanofibrous films simultaneously, while the artificial epidermis was formed by seeding human keratinocytes upon the dermis. The collagen-mimicking nanofibrous film effectively improved the tensile strength and fracture resistance of the CASS, making it sewable for firm implantation into skin defects. Meanwhile, the patterned nanofibrous film also provided the biological cues to guide cell behavior. Consequently, CASS could effectively accelerate the regeneration of large-area skin defects in mouse and pig models by promoting re-epithelialization and collagen deposition. This research developed an effective strategy to prepare composite bioprinting architectures for enhancing mechanical property and regulating cell behavior, and CASS could be a promising skin substitute for treating large-area skin defects.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":17.1,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141463987","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}

引用次数: 0

Photo-uncaging Triggers on Self-Blinking to Control Single-Molecule Fluorescence Kinetics for Super-resolution Imaging 通过自连接上的光诱发控制单分子荧光动力学，实现超分辨率成像

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2024-06-28 DOI: 10.1021/acsnano.4c03809

Ying Zheng, Zhiwei Ye, Xue Zhang, Yi Xiao

Super-resolution imaging, especially a single-molecule localization approach, has raised a fluorophore engineering revolution chasing sparse single-molecule dark-bright blinking transforms. Yet, it is a challenge to structurally devise fluorophores manipulating the single-molecule blinking kinetics. In this pursuit, we have developed a triggering strategy by innovatively integrating the photoactivatable nitroso-caging strategy into self-blinking sulfonamide to form a nitroso-caged sulfonamide rhodamine (NOSR). Our fluorophore demonstrated controllable self-blinking events upon phototriggered caging unit release. This exceptional blink kinetics improved the super-resolution imaging integrity on microtubules compared to self-blinking analogues. With the aid of paramount single-molecule fluorescence kinetics, we successfully reconstructed the ring structure of nuclear pores and the axial morphology of mitochondrial outer membranes. We foresee that our synthetic approach of photoactivation and self-blinking would facilitate rhodamine devising for super-resolution imaging.

超分辨率成像，尤其是单分子定位方法，引发了一场荧光团工程革命，追逐稀疏单分子暗-亮闪烁变换。然而，如何从结构上设计操纵单分子闪烁动力学的荧光团是一项挑战。为了实现这一目标，我们开发了一种触发策略，创新性地将可光激活的亚硝基笼化策略整合到自闪烁磺酰胺中，形成了亚硝基笼化磺酰胺罗丹明（NOSR）。我们的荧光团在光电触发的笼式单元释放时显示出可控的自闪烁事件。与自闪烁类似物相比，这种特殊的闪烁动力学提高了微管超分辨率成像的完整性。借助最重要的单分子荧光动力学，我们成功地重建了核孔的环状结构和线粒体外膜的轴向形态。我们预计，我们的光激活和自闪烁合成方法将促进罗丹明在超分辨率成像中的应用。

引用次数: 0

Scalable Compliant Graphene Fiber-Based Thermal Interface Material with Metal-Level Thermal Conductivity via Dual-Field Synergistic Alignment Engineering 通过双场协同配准工程实现具有金属级导热性的可扩展兼容石墨烯纤维热界面材料

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2024-06-28 DOI: 10.1021/acsnano.4c04349

Jiahao Lu, Xin Ming, Min Cao, Yingjun Liu, Bo Wang, Hang Shi, Yuanyuan Hao, Peijuan Zhang, Kaiwen Li, Lidan Wang, Peng Li, Weiwei Gao, Shengying Cai, Bin Sun, Zhong-Zhen Yu, Zhen Xu, Chao Gao

High-performance thermal interface materials (TIMs) are highly desired for high-power electronic devices to accelerate heat dissipation. However, the inherent trade-off conflict between achieving high thermal conductivity and excellent compliance of filler-enhanced TIMs results in the unsatisfactory interfacial heat transfer efficiency of existing TIM solutions. Here, we report the graphene fiber (GF)-based elastic TIM with metal-level thermal conductivity via mechanical–electric dual-field synergistic alignment engineering. Compared with state-of-the-art carbon fiber (CF), GF features both superb high thermal conductivity of ∼1200 W m^–1 K^–1 and outstanding flexibility. Under dual-field synergistic alignment regulation, GFs are vertically aligned with excellent orientation (0.88) and high array density (33.5 mg cm^–2), forming continuous thermally conductive pathways. Even at a low filler content of ∼17 wt %, GF-based TIM demonstrates extraordinarily high through-plane thermal conductivity of up to 82.4 W m^–1 K^–1, exceeding most CF-based TIMs and even comparable to commonly used soft indium foil. Benefiting from the low stiffness of GF, GF-based TIM shows a lower compressive modulus down to 0.57 MPa, an excellent resilience rate of 95% after compressive cycles, and diminished contact thermal resistance as low as 7.4 K mm² W^–1. Our results provide a superb paradigm for the directed assembly of thermally conductive and flexible GFs to achieve scalable and high-performance TIMs, overcoming the long-standing bottleneck of mechanical–thermal mismatch in TIM design.

高性能导热界面材料（TIM）是大功率电子设备加速散热的理想材料。然而，填料增强型热界面材料在实现高热导率和优异顺应性之间存在固有的权衡冲突，导致现有热界面材料解决方案的界面传热效率不尽人意。在此，我们报告了基于石墨烯纤维（GF）的弹性 TIM，该 TIM 通过机械-电气双场协同配向工程实现了金属级别的热导率。与最先进的碳纤维（CF）相比，石墨烯纤维具有高达 ∼1200 W m-1 K-1 的超高导热率和出色的柔韧性。在双场协同配向调节下，GF 垂直配向良好（0.88），阵列密度高（33.5 mg cm-2），形成了连续的导热通道。即使填料含量较低，仅为 17 wt %，基于 GF 的 TIM 也能表现出极高的通面热导率，高达 82.4 W m-1 K-1，超过了大多数基于 CF 的 TIM，甚至可与常用的软铟箔相媲美。得益于 GF 的低刚度，GF 基 TIM 的压缩模量低至 0.57 MPa，压缩循环后的回弹率高达 95%，接触热阻低至 7.4 K mm2 W-1。我们的研究结果为导热柔性 GF 的定向组装提供了一个极好的范例，从而实现了可扩展的高性能 TIM，克服了 TIM 设计中长期存在的机械热不匹配瓶颈。

{"title":"Scalable Compliant Graphene Fiber-Based Thermal Interface Material with Metal-Level Thermal Conductivity via Dual-Field Synergistic Alignment Engineering","authors":"Jiahao Lu, Xin Ming, Min Cao, Yingjun Liu, Bo Wang, Hang Shi, Yuanyuan Hao, Peijuan Zhang, Kaiwen Li, Lidan Wang, Peng Li, Weiwei Gao, Shengying Cai, Bin Sun, Zhong-Zhen Yu, Zhen Xu, Chao Gao","doi":"10.1021/acsnano.4c04349","DOIUrl":"https://doi.org/10.1021/acsnano.4c04349","url":null,"abstract":"High-performance thermal interface materials (TIMs) are highly desired for high-power electronic devices to accelerate heat dissipation. However, the inherent trade-off conflict between achieving high thermal conductivity and excellent compliance of filler-enhanced TIMs results in the unsatisfactory interfacial heat transfer efficiency of existing TIM solutions. Here, we report the graphene fiber (GF)-based elastic TIM with metal-level thermal conductivity via mechanical–electric dual-field synergistic alignment engineering. Compared with state-of-the-art carbon fiber (CF), GF features both superb high thermal conductivity of ∼1200 W m–1 K–1 and outstanding flexibility. Under dual-field synergistic alignment regulation, GFs are vertically aligned with excellent orientation (0.88) and high array density (33.5 mg cm–2), forming continuous thermally conductive pathways. Even at a low filler content of ∼17 wt %, GF-based TIM demonstrates extraordinarily high through-plane thermal conductivity of up to 82.4 W m–1 K–1, exceeding most CF-based TIMs and even comparable to commonly used soft indium foil. Benefiting from the low stiffness of GF, GF-based TIM shows a lower compressive modulus down to 0.57 MPa, an excellent resilience rate of 95% after compressive cycles, and diminished contact thermal resistance as low as 7.4 K mm2 W–1. Our results provide a superb paradigm for the directed assembly of thermally conductive and flexible GFs to achieve scalable and high-performance TIMs, overcoming the long-standing bottleneck of mechanical–thermal mismatch in TIM design.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":17.1,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141464021","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}

引用次数: 0

Locally Varying Surface Binding Affinity on Pd–Au Nanocrystals Enhances Electrochemical Ethanol Oxidation Activity 钯金纳米晶体上局部变化的表面结合亲和力增强了电化学乙醇氧化活性

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2024-06-28 DOI: 10.1021/acsnano.4c06063

Xiaoxiao Wang, Hao Yang, Moxuan Liu, Zhaojun Liu, Kai Liu, Zerui Mu, Yan Zhang, Tao Cheng, Chuanbo Gao

Noble metal nanocrystals face challenges in effectively catalyzing electrochemical ethanol oxidation reaction (EOR)-represented multistep, multielectron transfer processes due to the linear scaling relationship among binding energies of intermediates, impeding independent optimization of individual elemental steps. Herein, we develop noble metal nanocrystals with a range of local surface binding affinities in close proximity to overcome this challenge. Experimentally, this is demonstrated by applying tensile strain to a Pd surface and decorating it with discrete Au atoms, forming a diversity of binding sites with varying affinities in close proximity for guest molecules, as evidenced by CO probing and density functional theory calculations. Such a surface enables reaction intermediates to migrate between different binding sites as needed for each elemental step, thereby reducing the energy barrier for the overall EOR when compared to reactions at a single site. On these tailored surfaces, we attain specific and mass activities of 32.7 mA cm^–2 and 47.8 A mg_Pd^–1 in EOR, surpassing commercial Pd/C by 10.9 and 43.8 times, respectively, and outperforming state-of-the-art Pd-based catalysts. These results highlight the promise of this approach in improving a variety of multistep, multielectron transfer reactions, which are crucial for energy conversion applications.

贵金属纳米晶体在有效催化以电化学乙醇氧化反应（EOR）为代表的多步骤、多电子转移过程方面面临挑战，原因是中间产物的结合能之间存在线性比例关系，阻碍了单个元素步骤的独立优化。在此，我们开发了具有一系列接近的局部表面结合亲和力的贵金属纳米晶体，以克服这一挑战。实验证明，通过对钯表面施加拉伸应变并用离散的金原子进行装饰，就能在客体分子附近形成具有不同亲和力的多种结合位点，这一点已通过二氧化碳探测和密度泛函理论计算得到证实。这种表面可使反应中间产物根据每个元素步骤的需要在不同结合位点之间迁移，从而与在单一位点上的反应相比，降低了整个 EOR 的能量障碍。在这些定制表面上，我们在 EOR 中获得了 32.7 mA cm-2 和 47.8 A mgPd-1 的比活度和质量活度，分别是商用 Pd/C 的 10.9 倍和 43.8 倍，超过了最先进的钯基催化剂。这些结果凸显了这种方法在改善各种多步骤、多电子转移反应方面的前景，而这些反应对于能源转换应用至关重要。

{"title":"Locally Varying Surface Binding Affinity on Pd–Au Nanocrystals Enhances Electrochemical Ethanol Oxidation Activity","authors":"Xiaoxiao Wang, Hao Yang, Moxuan Liu, Zhaojun Liu, Kai Liu, Zerui Mu, Yan Zhang, Tao Cheng, Chuanbo Gao","doi":"10.1021/acsnano.4c06063","DOIUrl":"https://doi.org/10.1021/acsnano.4c06063","url":null,"abstract":"Noble metal nanocrystals face challenges in effectively catalyzing electrochemical ethanol oxidation reaction (EOR)-represented multistep, multielectron transfer processes due to the linear scaling relationship among binding energies of intermediates, impeding independent optimization of individual elemental steps. Herein, we develop noble metal nanocrystals with a range of local surface binding affinities in close proximity to overcome this challenge. Experimentally, this is demonstrated by applying tensile strain to a Pd surface and decorating it with discrete Au atoms, forming a diversity of binding sites with varying affinities in close proximity for guest molecules, as evidenced by CO probing and density functional theory calculations. Such a surface enables reaction intermediates to migrate between different binding sites as needed for each elemental step, thereby reducing the energy barrier for the overall EOR when compared to reactions at a single site. On these tailored surfaces, we attain specific and mass activities of 32.7 mA cm–2 and 47.8 A mgPd–1 in EOR, surpassing commercial Pd/C by 10.9 and 43.8 times, respectively, and outperforming state-of-the-art Pd-based catalysts. These results highlight the promise of this approach in improving a variety of multistep, multielectron transfer reactions, which are crucial for energy conversion applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":17.1,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141464065","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}

引用次数: 0

Direct Measurement of the Thermal Expansion Coefficient of Epitaxial WSe2 by Four-Dimensional Scanning Transmission Electron Microscopy 通过四维扫描透射电子显微镜直接测量外延 WSe2 的热膨胀系数

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2024-06-27 DOI: 10.1021/acsnano.4c02996

Theresa M. Kucinski, Rohan Dhall, Benjamin H. Savitzky, Colin Ophus, Rijan Karkee, Avanish Mishra, Enkeleda Dervishi, Jung Hoon Kang, Chul-Ho Lee, Jinkyoung Yoo, Michael T. Pettes

Current reports of thermal expansion coefficients (TEC) of two-dimensional (2D) materials show large discrepancies that span orders of magnitude. Determining the TEC of any 2D material remains difficult due to approaches involving indirect measurement of samples that are atomically thin and optically transparent. We demonstrate a methodology to address this discrepancy and directly measure TEC of nominally monolayer epitaxial WSe₂ using four-dimensional scanning transmission electron microscopy (4D-STEM). Experimentally, WSe₂ from metal–organic chemical vapor deposition (MOCVD) was heated through a temperature range of 18–564 °C using a barrel-style heating sample holder to observe temperature-induced structural changes without additional alterations or destruction of the sample. By combining 4D-STEM measurements with quantitative structural analysis, the thermal expansion coefficient of nominally monolayer polycrystalline epitaxial 2D WSe₂ was determined to be (3.5 ± 0.9) × 10^–6 K^–1 and (5.7 ± 2) × 10^–5 K^–1 for the in- and out-of-plane TEC, respectively, and (3.6 ± 0.2) × 10^–5 K^–1 for the unit cell volume TEC, in good agreement with historically determined values for bulk crystals.

目前有关二维（2D）材料热膨胀系数（TEC）的报告显示，二维材料的热膨胀系数之间存在着巨大的差异，其数量级相差悬殊。确定任何二维材料的热膨胀系数仍然十分困难，这是因为采用的方法涉及对原子薄且光学透明的样品进行间接测量。我们展示了一种解决这一差异的方法，即利用四维扫描透射电子显微镜（4D-STEM）直接测量名义上单层外延 WSe2 的 TEC。实验中，使用桶式加热样品架将金属有机化学气相沉积（MOCVD）产生的 WSe2 加热到 18-564 ℃ 的温度范围，以观察温度引起的结构变化，而不会对样品造成额外的改变或破坏。通过将 4D-STEM 测量与定量结构分析相结合，确定了名义上单层多晶外延二维 WSe2 的热膨胀系数：面内和面外 TEC 分别为 (3.5 ± 0.9) × 10-6 K-1 和 (5.7 ± 2) × 10-5 K-1，单位晶胞体积 TEC 为 (3.6 ± 0.2) × 10-5 K-1，与块状晶体的历史测定值非常一致。

{"title":"Direct Measurement of the Thermal Expansion Coefficient of Epitaxial WSe2 by Four-Dimensional Scanning Transmission Electron Microscopy","authors":"Theresa M. Kucinski, Rohan Dhall, Benjamin H. Savitzky, Colin Ophus, Rijan Karkee, Avanish Mishra, Enkeleda Dervishi, Jung Hoon Kang, Chul-Ho Lee, Jinkyoung Yoo, Michael T. Pettes","doi":"10.1021/acsnano.4c02996","DOIUrl":"https://doi.org/10.1021/acsnano.4c02996","url":null,"abstract":"Current reports of thermal expansion coefficients (TEC) of two-dimensional (2D) materials show large discrepancies that span orders of magnitude. Determining the TEC of any 2D material remains difficult due to approaches involving indirect measurement of samples that are atomically thin and optically transparent. We demonstrate a methodology to address this discrepancy and directly measure TEC of nominally monolayer epitaxial WSe2 using four-dimensional scanning transmission electron microscopy (4D-STEM). Experimentally, WSe2 from metal–organic chemical vapor deposition (MOCVD) was heated through a temperature range of 18–564 °C using a barrel-style heating sample holder to observe temperature-induced structural changes without additional alterations or destruction of the sample. By combining 4D-STEM measurements with quantitative structural analysis, the thermal expansion coefficient of nominally monolayer polycrystalline epitaxial 2D WSe2 was determined to be (3.5 ± 0.9) × 10–6 K–1 and (5.7 ± 2) × 10–5 K–1 for the in- and out-of-plane TEC, respectively, and (3.6 ± 0.2) × 10–5 K–1 for the unit cell volume TEC, in good agreement with historically determined values for bulk crystals.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":17.1,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141464093","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}

引用次数: 0

Unidirectional Charge Orders Induced by Oxygen Vacancies on SrTiO₃(001). SrTiO3(001)上的氧空位诱发的单向电荷秩序。

IF 15.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2024-06-27 DOI: 10.1021/acsnano.4c03317

Cui Ding, Wenfeng Dong, Xiaotong Jiao, Zhiyu Zhang, Guanming Gong, Zhongxu Wei, Lili Wang, Jin-Feng Jia, Qi-Kun Xue

The discovery of high-mobility two-dimensional electron gas and low carrier density superconductivity in multiple SrTiO₃-based heterostructures has stimulated intense interest in the surface properties of SrTiO₃. The recent discovery of high-T_c superconductivity in the monolayer FeSe/SrTiO₃ led to the upsurge and underscored the atomic precision probe of the surface structure. By performing atomically resolved cryogenic scanning tunneling microscopy/spectroscopy characterization on dual-TiO_2-δ-terminated SrTiO₃(001) surfaces with (√13 × √13), c(4 × 2), mixed (2 × 1), and (2 × 2) reconstructions, we disclosed universally broken rotational symmetry and contrasting bias- and temperature-dependent electronic states for apical and equatorial oxygen sites. With the sequentially evolved surface reconstructions and simultaneously increasing equatorial oxygen vacancies, the surface anisotropy reduces and the work function lowers. Intriguingly, unidirectional stripe orders appear on the c(4 × 2) surface, whereas local (4 × 4) order emerges and eventually forms long-range unidirectional c(4 × 4) charge order on the (2 × 2) surface. This work reveals robust unidirectional charge orders induced by oxygen vacancies due to strong and delicate electronic-lattice interaction under broken rotational symmetry, providing insights into understanding the complex behaviors in perovskite oxide-based heterostructures.

在多个基于 SrTiO3 的异质结构中发现的高迁移率二维电子气和低载流子密度超导现象激发了人们对 SrTiO3 表面特性的浓厚兴趣。最近在单层 FeSe/SrTiO3 中发现的高锝超导电性引发了这一热潮，并强调了对表面结构进行原子精度探测的重要性。通过对具有 (√13 × √13)、c(4 × 2)、混合 (2 × 1) 和 (2 × 2) 重构的双 TiO2-δ 端 SrTiO3(001)表面进行原子分辨低温扫描隧道显微镜/光谱表征，我们揭示了顶端和赤道氧位点的普遍断裂旋转对称性以及与偏置和温度相关的对比电子态。随着表面重构的连续演化和赤道氧空位的同时增加，表面各向异性减小，功函数降低。有趣的是，c（4 × 2）表面出现了单向条纹阶，而局部（4 × 4）阶出现了，并最终在（2 × 2）表面形成了长程单向 c（4 × 4）电荷阶。这项研究揭示了氧空位在旋转对称性被打破的情况下，由于强烈而微妙的电子-晶格相互作用而诱导出的稳健的单向电荷秩，为理解基于过氧化物的异质结构的复杂行为提供了启示。

{"title":"Unidirectional Charge Orders Induced by Oxygen Vacancies on SrTiO3(001).","authors":"Cui Ding, Wenfeng Dong, Xiaotong Jiao, Zhiyu Zhang, Guanming Gong, Zhongxu Wei, Lili Wang, Jin-Feng Jia, Qi-Kun Xue","doi":"10.1021/acsnano.4c03317","DOIUrl":"https://doi.org/10.1021/acsnano.4c03317","url":null,"abstract":"The discovery of high-mobility two-dimensional electron gas and low carrier density superconductivity in multiple SrTiO3-based heterostructures has stimulated intense interest in the surface properties of SrTiO3. The recent discovery of high-Tc superconductivity in the monolayer FeSe/SrTiO3 led to the upsurge and underscored the atomic precision probe of the surface structure. By performing atomically resolved cryogenic scanning tunneling microscopy/spectroscopy characterization on dual-TiO2-δ-terminated SrTiO3(001) surfaces with (√13 × √13), c(4 × 2), mixed (2 × 1), and (2 × 2) reconstructions, we disclosed universally broken rotational symmetry and contrasting bias- and temperature-dependent electronic states for apical and equatorial oxygen sites. With the sequentially evolved surface reconstructions and simultaneously increasing equatorial oxygen vacancies, the surface anisotropy reduces and the work function lowers. Intriguingly, unidirectional stripe orders appear on the c(4 × 2) surface, whereas local (4 × 4) order emerges and eventually forms long-range unidirectional c(4 × 4) charge order on the (2 × 2) surface. This work reveals robust unidirectional charge orders induced by oxygen vacancies due to strong and delicate electronic-lattice interaction under broken rotational symmetry, providing insights into understanding the complex behaviors in perovskite oxide-based heterostructures.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":15.8,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453676","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}

引用次数: 0

Strain-Sensor-In-Pixel Technology for Resolution-Sustainable Stretchable Displays. 用于可持续分辨率可拉伸显示器的像素内应变传感器技术。

IF 15.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2024-06-27 DOI: 10.1021/acsnano.4c03015

Won Kyung Min, Jong Bin An, Byung Ha Kang, Hyunji Son, Gwan In Kim, Seok Gyu Hong, Dong Hyun Choi, Jusung Chung, Moon Ho Lee, Beom Soo Kim, Hyun Jae Kim

One of the limitations of stretchable displays is the severe degradation of resolution or the decrease in the number of pixels per unit area when stretched. Hence, we suggest a strain-sensor-in-pixel (S-SIP) system through the adoption of hidden pixels that are activated only during the stretch mode for maintaining the density of on-state pixels. For the S-SIP system, the gate and source electrodes of InGaZnO thin-film transistors (TFTs) in an existing pixel are connected to a resistive strain sensor through the facile and selective deposition of silver nanowires (AgNWs) via electrohydrodynamic-jet-printing. With this approach, the strain sensor integrated TFT functions as a strain-triggered switch, which responds only to stretching along the designated axes by finely tuning the orientation and cycles of AgNW printing. The strain sensor-integrated TFT remains in an off-state when unstretched and switches to an on-state when stretched, exhibiting a large negative gauge factor of -1.1 × 10¹⁰ and a superior mechanical stability enduring 6000 cycles, which enables the efficient structure to operate hidden pixels without requiring additional signal processing. Furthermore, the stable operation of the S-SIP in a 5 × 5-pixel array is demonstrated via circuit simulation, implying the outstanding applicability and process compatibility to the conventional active-matrix display backplanes.

可拉伸显示器的局限之一是拉伸时分辨率严重下降或单位面积像素数减少。因此，我们建议采用应变传感器嵌入像素（S-SIP）系统，通过采用仅在拉伸模式下激活的隐藏像素来保持导通像素的密度。在 S-SIP 系统中，现有像素中 InGaZnO 薄膜晶体管（TFT）的栅极和源电极通过电流体动力喷射打印技术选择性地沉积银纳米线（AgNW），从而与电阻应变传感器相连。采用这种方法，应变传感器集成 TFT 可作为应变触发开关使用，通过微调 AgNW 印刷的方向和周期，只对沿指定轴的拉伸做出响应。应变传感器集成 TFT 在未拉伸时保持关闭状态，而在拉伸时则切换到开启状态，显示出-1.1 × 1010 的大负测量系数和经受 6000 次循环的卓越机械稳定性，这使得这种高效结构无需额外的信号处理即可运行隐藏像素。此外，还通过电路仿真演示了 S-SIP 在 5 × 5 像素阵列中的稳定运行，这意味着它对传统有源矩阵显示器背板具有出色的适用性和工艺兼容性。

{"title":"Strain-Sensor-In-Pixel Technology for Resolution-Sustainable Stretchable Displays.","authors":"Won Kyung Min, Jong Bin An, Byung Ha Kang, Hyunji Son, Gwan In Kim, Seok Gyu Hong, Dong Hyun Choi, Jusung Chung, Moon Ho Lee, Beom Soo Kim, Hyun Jae Kim","doi":"10.1021/acsnano.4c03015","DOIUrl":"https://doi.org/10.1021/acsnano.4c03015","url":null,"abstract":"One of the limitations of stretchable displays is the severe degradation of resolution or the decrease in the number of pixels per unit area when stretched. Hence, we suggest a strain-sensor-in-pixel (S-SIP) system through the adoption of hidden pixels that are activated only during the stretch mode for maintaining the density of on-state pixels. For the S-SIP system, the gate and source electrodes of InGaZnO thin-film transistors (TFTs) in an existing pixel are connected to a resistive strain sensor through the facile and selective deposition of silver nanowires (AgNWs) via electrohydrodynamic-jet-printing. With this approach, the strain sensor integrated TFT functions as a strain-triggered switch, which responds only to stretching along the designated axes by finely tuning the orientation and cycles of AgNW printing. The strain sensor-integrated TFT remains in an off-state when unstretched and switches to an on-state when stretched, exhibiting a large negative gauge factor of -1.1 × 1010 and a superior mechanical stability enduring 6000 cycles, which enables the efficient structure to operate hidden pixels without requiring additional signal processing. Furthermore, the stable operation of the S-SIP in a 5 × 5-pixel array is demonstrated via circuit simulation, implying the outstanding applicability and process compatibility to the conventional active-matrix display backplanes.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":15.8,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453703","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}

引用次数: 0

Bottlebrush Polyethylene Glycol Nanocarriers Translocate across Human Airway Epithelium via Molecular Architecture-Enhanced Endocytosis. Bottlebrush 聚乙二醇纳米载体通过分子结构增强的内吞作用在人的气道上皮细胞中转运

IF 15.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2024-06-27 DOI: 10.1021/acsnano.4c01983

Zhi-Jian He, Baiqiang Huang, Li-Heng Cai

Pulmonary drug delivery is critical for the treatment of respiratory diseases. However, the human airway surface presents multiple barriers to efficient drug delivery. Here, we report a bottlebrush poly(ethylene glycol) (PEG-BB) nanocarrier that can translocate across all barriers within the human airway surface. Guided by a molecular theory, we design a PEG-BB molecule consisting of a linear backbone densely grafted by many (∼1000) low molecular weight (∼1000 g/mol) polyethylene glycol (PEG) chains; this results in a highly anisotropic, wormlike nanocarrier featuring a contour length of ∼250 nm, a cross-section of ∼20 nm, and a hydrodynamic diameter of ∼40 nm. Using the classic air-liquid-interface culture system to recapitulate essential biological features of the human airway surface, we show that PEG-BB rapidly penetrates through endogenous airway mucus and periciliary brush layer (mesh size of 20-40 nm) to be internalized by cells across the whole epithelium. By quantifying the cellular uptake of polymeric carriers of various molecular architectures and manipulating cell proliferation and endocytosis pathways, we show that the translocation of PEG-BB across the epithelium is driven by bottlebrush architecture-enhanced endocytosis. Our results demonstrate that large, wormlike bottlebrush PEG polymers, if properly designed, can be used as a carrier for pulmonary and mucosal drug delivery.

肺部给药对于治疗呼吸系统疾病至关重要。然而，人体气道表面存在多重障碍，阻碍了药物的有效输送。在此，我们报告了一种能穿过人体气道表面所有障碍的底层聚乙二醇（PEG-BB）纳米载体。在分子理论指导下，我们设计了一种 PEG-BB 分子，它由许多（∼1000）低分子量（∼1000 g/mol）聚乙二醇（PEG）链密集接枝的线性骨架组成；这就形成了一种高度各向异性的蠕虫状纳米载体，其轮廓长度为 ∼250 nm，横截面为 ∼20 nm，流体力学直径为 ∼40 nm。我们利用经典的气液界面培养系统再现了人体气道表面的基本生物学特征，结果表明 PEG-BB 可迅速穿透内源性气道粘液和纤毛刷层（网眼尺寸为 20-40 nm），被整个上皮细胞内化。通过量化细胞对不同分子结构的聚合物载体的摄取，并操纵细胞增殖和内吞途径，我们发现 PEG-BB 在上皮细胞内的转运是由瓶刷结构增强的内吞作用驱动的。我们的研究结果表明，如果设计得当，大型蠕虫状瓶丛 PEG 聚合物可用作肺部和粘膜给药的载体。

{"title":"Bottlebrush Polyethylene Glycol Nanocarriers Translocate across Human Airway Epithelium via Molecular Architecture-Enhanced Endocytosis.","authors":"Zhi-Jian He, Baiqiang Huang, Li-Heng Cai","doi":"10.1021/acsnano.4c01983","DOIUrl":"https://doi.org/10.1021/acsnano.4c01983","url":null,"abstract":"Pulmonary drug delivery is critical for the treatment of respiratory diseases. However, the human airway surface presents multiple barriers to efficient drug delivery. Here, we report a bottlebrush poly(ethylene glycol) (PEG-BB) nanocarrier that can translocate across all barriers within the human airway surface. Guided by a molecular theory, we design a PEG-BB molecule consisting of a linear backbone densely grafted by many (∼1000) low molecular weight (∼1000 g/mol) polyethylene glycol (PEG) chains; this results in a highly anisotropic, wormlike nanocarrier featuring a contour length of ∼250 nm, a cross-section of ∼20 nm, and a hydrodynamic diameter of ∼40 nm. Using the classic air-liquid-interface culture system to recapitulate essential biological features of the human airway surface, we show that PEG-BB rapidly penetrates through endogenous airway mucus and periciliary brush layer (mesh size of 20-40 nm) to be internalized by cells across the whole epithelium. By quantifying the cellular uptake of polymeric carriers of various molecular architectures and manipulating cell proliferation and endocytosis pathways, we show that the translocation of PEG-BB across the epithelium is driven by bottlebrush architecture-enhanced endocytosis. Our results demonstrate that large, wormlike bottlebrush PEG polymers, if properly designed, can be used as a carrier for pulmonary and mucosal drug delivery.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":15.8,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453616","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}

引用次数: 0

Controlled Crystal Growth of All-Inorganic CsPbI2Br via Sequential Vacuum Deposition for Efficient Perovskite Solar Cells 通过序贯真空沉积实现全无机 CsPbI2Br 的可控晶体生长，从而实现高效的 Perovskite 太阳能电池

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2024-06-27 DOI: 10.1021/acsnano.4c03079

Min Hyeong Lee, Dae Woo Kim, Young Wook Noh, Hye Seung Kim, Jongmin Han, Heunjeong Lee, Kyoung Jin Choi, Shinuk Cho, Myoung Hoon Song

Vacuum deposition of perovskites is a promising method for scale-up fabrication and uniform film growth. However, improvements in the photovoltaic performance of perovskites are limited by the fabrication of perovskite films, which are not optimized for high device efficiency in the vacuum evaporation process. Herein, we fabricate CsPbI₂Br perovskite with high crystallinity and larger grain size by controlling the deposition sequence between PbI₂ and CsBr. The nucleation barrier for perovskite formation is significantly lowered by first evaporating CsBr and then PbI₂ (CsBr–PbI₂), followed by the sequential evaporation of multiple layers. The results show that the reduced Gibbs free energy of CsBr–PbI₂, compared with that of PbI₂–CsBr, accelerates perovskite formation, resulting in larger grain size and reduced defect density. Furthermore, surface-modified homojunction perovskites are fabricated to efficiently extract charge carriers and enhance the efficiency of perovskite solar cells (PeSCs) by modulating the final PbI₂ thickness before thermal annealing. Using these strategies, the best PeSC exhibits a power conversion efficiency of 13.41% for a small area (0.135 cm²), the highest value among sequential thermal deposition inorganic PeSCs, and 11.10% for a large area PeSC (1 cm²). This study presents an effective way to understand the crystal growth of thermally deposited perovskites and improve their performance in optoelectronic devices.

包晶石的真空沉积是一种很有前景的放大制造和薄膜均匀生长的方法。然而，由于在真空蒸发过程中未对包晶薄膜的制造进行优化以实现高器件效率，因此限制了包晶光伏性能的提高。在本文中，我们通过控制 PbI2 和 CsBr 之间的沉积顺序，制备出了具有高结晶度和较大晶粒尺寸的 CsPbI2Br 包晶体。通过先蒸发 CsBr 后蒸发 PbI2（CsBr-PbI2），再依次蒸发多层，显著降低了包晶体形成的成核势垒。结果表明，与 PbI2-CsBr 相比，CsBr-PbI2 的吉布斯自由能降低，从而加速了包晶的形成，使晶粒尺寸增大，缺陷密度降低。此外，通过在热退火前调节最终的 PbI2 厚度，制备出表面修饰的同质结包晶石，从而有效地提取电荷载流子并提高包晶石太阳能电池（PeSC）的效率。利用这些策略，小面积（0.135 平方厘米）的最佳 PeSC 功率转换效率为 13.41%，是顺序热沉积无机 PeSC 中的最高值；大面积 PeSC（1 平方厘米）的功率转换效率为 11.10%。这项研究为了解热沉积过氧化物晶体的晶体生长和提高其在光电器件中的性能提供了有效途径。

{"title":"Controlled Crystal Growth of All-Inorganic CsPbI2Br via Sequential Vacuum Deposition for Efficient Perovskite Solar Cells","authors":"Min Hyeong Lee, Dae Woo Kim, Young Wook Noh, Hye Seung Kim, Jongmin Han, Heunjeong Lee, Kyoung Jin Choi, Shinuk Cho, Myoung Hoon Song","doi":"10.1021/acsnano.4c03079","DOIUrl":"https://doi.org/10.1021/acsnano.4c03079","url":null,"abstract":"Vacuum deposition of perovskites is a promising method for scale-up fabrication and uniform film growth. However, improvements in the photovoltaic performance of perovskites are limited by the fabrication of perovskite films, which are not optimized for high device efficiency in the vacuum evaporation process. Herein, we fabricate CsPbI2Br perovskite with high crystallinity and larger grain size by controlling the deposition sequence between PbI2 and CsBr. The nucleation barrier for perovskite formation is significantly lowered by first evaporating CsBr and then PbI2 (CsBr–PbI2), followed by the sequential evaporation of multiple layers. The results show that the reduced Gibbs free energy of CsBr–PbI2, compared with that of PbI2–CsBr, accelerates perovskite formation, resulting in larger grain size and reduced defect density. Furthermore, surface-modified homojunction perovskites are fabricated to efficiently extract charge carriers and enhance the efficiency of perovskite solar cells (PeSCs) by modulating the final PbI2 thickness before thermal annealing. Using these strategies, the best PeSC exhibits a power conversion efficiency of 13.41% for a small area (0.135 cm2), the highest value among sequential thermal deposition inorganic PeSCs, and 11.10% for a large area PeSC (1 cm2). This study presents an effective way to understand the crystal growth of thermally deposited perovskites and improve their performance in optoelectronic devices.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":17.1,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141463986","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}

引用次数: 0

Unveiling Local Current Behavior and Manipulating Grain Homogenization of Perovskite Films for Efficient Solar Cells 揭示过氧化物薄膜的局部电流行为并操纵晶粒均匀化以实现高效太阳能电池

IF 17.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Nano

Pub Date : 2024-06-27 DOI: 10.1021/acsnano.4c00911

Liu Yang, Fei Zheng, Jun Wu, Yanna Hou, Xiaorong Qi, Yuchen Miao, Xu Wang, Like Huang, Xiaohui Liu, Jing Zhang, Yuejin Zhu, Ziyang Hu

Achieving high power conversion efficiency in perovskite solar cells (PSCs) heavily relies on fabricating homogeneous perovskite films. However, understanding microscopic-scale properties such as current generation and open-circuit voltage within perovskite crystals has been challenging due to difficulties in quantifying intragrain behavior. In this study, the local current intensity within state-of-the-art perovskite films mapped by conductive atomic force microscopy reveals a distinct heterogeneity, which exhibits a strong anticorrelation to the external biases. Particularly under different external bias polarities, specific regions in the current mapping show contrasting conductivity. Moreover, grains oriented differently exhibit varied surface potentials and currents, leading us to associate this local current heterogeneity with the grain orientation. It was found that the films treated with isopropanol exhibit ordered grain orientation, demonstrating minimized lattice heterogeneity, fewer microstructure defects, and reduced electronic disorder. Importantly, devices exhibiting an ordered orientation showcase elevated macroscopic optoelectronic properties and boosted device performance. These observations underscore the critical importance of fine-tuning the grain homogenization of perovskite films, offering a promising avenue for further enhancing the efficiency of PSCs.

要在透辉石太阳能电池（PSCs）中实现高功率转换效率，在很大程度上有赖于制造均匀的透辉石薄膜。然而，由于难以量化晶粒内部的行为，要了解透辉石晶体内部的电流产生和开路电压等微观尺度特性一直具有挑战性。在这项研究中，通过导电原子力显微镜绘制的最先进的包晶体薄膜内的局部电流强度显示出明显的异质性，与外部偏压呈现出强烈的反相关性。特别是在不同的外部偏压极性下，电流图谱中的特定区域显示出截然不同的导电性。此外，不同取向的晶粒表现出不同的表面电位和电流，这使我们将这种局部电流异质性与晶粒取向联系起来。研究发现，用异丙醇处理的薄膜呈现出有序的晶粒取向，显示出最小的晶格异质性、较少的微结构缺陷和较低的电子无序性。重要的是，表现出有序取向的器件具有更高的宏观光电特性，并能提高器件性能。这些观察结果强调了微调包晶体薄膜晶粒均匀化的重要性，为进一步提高 PSCs 的效率提供了一条大有可为的途径。

{"title":"Unveiling Local Current Behavior and Manipulating Grain Homogenization of Perovskite Films for Efficient Solar Cells","authors":"Liu Yang, Fei Zheng, Jun Wu, Yanna Hou, Xiaorong Qi, Yuchen Miao, Xu Wang, Like Huang, Xiaohui Liu, Jing Zhang, Yuejin Zhu, Ziyang Hu","doi":"10.1021/acsnano.4c00911","DOIUrl":"https://doi.org/10.1021/acsnano.4c00911","url":null,"abstract":"Achieving high power conversion efficiency in perovskite solar cells (PSCs) heavily relies on fabricating homogeneous perovskite films. However, understanding microscopic-scale properties such as current generation and open-circuit voltage within perovskite crystals has been challenging due to difficulties in quantifying intragrain behavior. In this study, the local current intensity within state-of-the-art perovskite films mapped by conductive atomic force microscopy reveals a distinct heterogeneity, which exhibits a strong anticorrelation to the external biases. Particularly under different external bias polarities, specific regions in the current mapping show contrasting conductivity. Moreover, grains oriented differently exhibit varied surface potentials and currents, leading us to associate this local current heterogeneity with the grain orientation. It was found that the films treated with isopropanol exhibit ordered grain orientation, demonstrating minimized lattice heterogeneity, fewer microstructure defects, and reduced electronic disorder. Importantly, devices exhibiting an ordered orientation showcase elevated macroscopic optoelectronic properties and boosted device performance. These observations underscore the critical importance of fine-tuning the grain homogenization of perovskite films, offering a promising avenue for further enhancing the efficiency of PSCs.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":17.1,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141464028","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}

引用次数: 0