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A Direct Current Self-Sustained Moisture-Electric Generator with 1D/2D Hierarchical Nanostructure for Continuous Operation of Off-Grid Electronics. 用于离网电子设备连续运行的具有一维/二维分层纳米结构的直流自持式湿电发生器
IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-22 Epub Date: 2024-10-07 DOI: 10.1021/acsnano.4c09494
Luyu Yang, Lei Zhang, Yang-Chun Yong, Dongping Sun

Ubiquitous moisture is a colossal reservoir of clean energy, and the emergence of moisture-electric generators (MEGs) is expected to provide direct power support for off-grid electronic devices anytime and anywhere. However, most MEGs rely on auxiliary energy storage devices and rectifier circuits to drive small electronic devices, which hinder scalability and widespread deployment, and the development of direct current (DC) MEGs with high power output that can directly drive off-grid electronic devices is highly promising but challenging. Herein, a self-sustained moisture-electric generator (SMEG) with a hierarchical nanostructure based on one-dimensional (1D) negatively charged nanofibers and two-dimensional (2D) conductive nanosheets was demonstrated to generate continuous DC electricity from atmospheric humidity. Sulfation of bacterial cellulose nanofibers lowers the surface potential and increases the surface charge energy, and reduced graphene oxide (rGO) provides a conduction pathway for electrons. The hierarchical nanostructures constructed by the combination of 1D nanofibers and 2D nanosheets endow the SMEG with self-sustained moisture gradients and structural anisotropy, which force the generation of a pseudocurrent. This combination also constructs microcapacitors that further enhance the moisture-electric power output. The SMEG can generate a continuous voltage in excess of 0.54 V for over 2160 h, with a power density of about 822 μW cm-3, demonstrating excellent operational durability. This research provides a feasible solution for the development of sustainable, versatile, and efficient power supplies for off-grid self-powered devices.

无处不在的水汽蕴藏着巨大的清洁能源,水汽发电机(MEG)的出现有望随时随地为离网电子设备提供直接的电力支持。然而,大多数 MEG 都依赖于辅助储能设备和整流电路来驱动小型电子设备,这阻碍了其可扩展性和广泛应用,而开发可直接驱动离网电子设备的高功率输出直流(DC)MEG 前景广阔,但也充满挑战。在此,我们展示了一种具有分层纳米结构的自持式湿电发生器(SMEG),该结构基于一维(1D)带负电纳米纤维和二维(2D)导电纳米片,可利用大气湿度产生连续的直流电。细菌纤维素纳米纤维的硫酸盐化降低了表面电位并增加了表面电荷能,还原氧化石墨烯(rGO)为电子提供了传导途径。由一维纳米纤维和二维纳米片组合而成的分层纳米结构赋予了 SMEG 自我维持的湿度梯度和结构各向异性,从而迫使其产生伪电流。这种组合还构建了微电容器,进一步增强了湿电功率输出。SMEG 可产生超过 0.54 V 的连续电压,持续时间超过 2160 小时,功率密度约为 822 μW cm-3,显示了出色的运行耐久性。这项研究为开发可持续、多功能、高效的离网自供电设备电源提供了可行的解决方案。
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引用次数: 0
Multifunctional Reconfigurable Operations in an Ultra-Scaled Ferroelectric Negative Transconductance Transistor. 超标量铁电负导晶体管中的多功能可重构操作
IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-22 Epub Date: 2024-10-11 DOI: 10.1021/acsnano.4c09598
Zhongyunshen Zhu, Anton E O Persson, Lars-Erik Wernersson

The integration of functional materials into electronic devices has become a key approach to extending Moore's law by increasing the functional density of electronic circuits. Here, we present a device technology based on ultrascaled ferroelectric, antiambipolar transistors (ferro-AAT) with robust negative transconductance, enabling a wide range of reconfigurable functionalities with applications in both the digital and analog domains. The device relies on the integration of a hafnia-based ferroelectric gate stack on a vertical nanowire tunnel field-effect transistor. Through intentional gate/source overlap and tunnel-junction engineering, we demonstrate enhanced antiambipolarity with a high negative transconductance that is reconfigurable using the nonvolatile remanent polarization of the ferroelectric. Experimental validation highlights the versatility of this ferro-AAT in two implementation scenarios: content addressable memory (CAM) for high-density data search and reconfigurable signal processing in analog circuits. As a single-transistor cell for CAMs, the ferro-AAT shows subpicojoule operation for one search with a compact footprint of ∼0.01 μm2. For single-transistor-based signal modulation, multistate reconfigurations and high power conversion (>95%) are achieved in the ferro-AAT, resulting in a significant reduction in the complexity of analog circuit design. Our results reveal that the distinctive device properties allow ferro-AATs to operate beyond conventional transistors with multiple reconfigurable functionalities, ultrascaled footprint, and low power consumption.

通过提高电子电路的功能密度,将功能材料集成到电子器件中已成为扩展摩尔定律的关键方法。在这里,我们介绍了一种基于超量级铁电反双极晶体管(ferro-AAT)的器件技术,它具有强大的负跨导功能,可实现广泛的可重构功能,在数字和模拟领域均有应用。该器件在垂直纳米线隧道场效应晶体管上集成了基于铪的铁电栅极堆栈。通过有意的栅极/源极重叠和隧道结工程,我们展示了增强的反双极性和高负跨导,并可利用铁电体的非易失性剩磁极化进行重新配置。实验验证凸显了这种铁-AAT 在两种应用场景中的多功能性:用于高密度数据搜索的内容可寻址存储器(CAM)和模拟电路中的可重构信号处理。作为用于 CAM 的单晶体管单元,铁氧体-AAT 在一次搜索中的运行功耗低于皮焦耳,占地面积仅为 ∼0.01 μm2。对于基于单晶体管的信号调制,铁氧体-AAT 实现了多态重配置和高功率转换(>95%),从而显著降低了模拟电路设计的复杂性。我们的研究结果表明,独特的器件特性使铁-AAT 能够超越传统晶体管,实现多种可重新配置功能、超大尺寸和低功耗。
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引用次数: 0
DNA-Based Chemical Unclonable Functions for Cryptographic Anticounterfeit Tagging of Pharmaceuticals
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-22 DOI: 10.1021/acsnano.4c10870
Anne M. Luescher, Wendelin J. Stark, Robert N. Grass
Counterfeit products are a problem known across many industries. Chemical products such as pharmaceuticals belong to the most targeted markets, with harmful consequences for consumer health and safety. However, many of the currently used anticounterfeit measures are associated with the packaging, with the readout method and level of security varying between different solutions. Identifiers that can be directly and safely mixed into the product to securely authenticate a batch would be desirable. For this purpose, we propose the use of chemical unclonable functions based on pools of short random DNA oligos, which allow the integration of a cryptographic authentication system into chemical products. We demonstrate and characterize a simplified workflow for readout, showing that results are robust and clearly differentiate between the correct tag and a counterfeit. As a proof of concept, we demonstrate the labeling of an acetaminophen formulation with a chemical unclonable function. The acetaminophen was successfully authenticated from a subsample of the product at a DNA admixing concentration of below 50 ng/g. Stability tests revealed that the readout is stable at room temperature for several years, exceeding the shelf life of most drug products. Our work thus shows that chemical unclonable functions are a valid alternative to state-of-the-art anticounterfeit methods, enabling a secure authentication scheme that is physically linked to the product and safe for consumption. The method is widely applicable beyond pharmaceuticals, allowing for more secure product tracing across industries.
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引用次数: 0
Coupling of Spectrin Repeat Modules for the Assembly of Nanorods and Presentation of Protein Domains. 将 Spectrin 重复模块耦合以组装纳米棒并呈现蛋白质域。
IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-22 Epub Date: 2024-10-11 DOI: 10.1021/acsnano.4c07701
Klemen Mezgec, Jaka Snoj, Liza Ulčakar, Ajasja Ljubetič, Magda Tušek Žnidarič, Miha Škarabot, Roman Jerala

Modular protein engineering is a powerful approach for fabricating high-molecular-weight assemblies and biomaterials with nanoscale precision. Herein, we address the challenge of designing an extended nanoscale filamentous architecture inspired by the central rod domain of human dystrophin, which protects sarcolemma during muscle contraction and consists of spectrin repeats composed of three-helical bundles. A module of three tandem spectrin repeats was used as a rigid building block self-assembling via coiled-coil (CC) dimer-forming peptides. CC peptides were precisely integrated to maintain the spectrin α-helix continuity in an appropriate frame to form extended nanorods. An orthogonal set of customizable CC heterodimers was harnessed for modular rigid domain association, which could be additionally regulated by metal ions and chelators. We achieved a robust assembly of rigid rods several micrometers in length, determined by atomic force microscopy and negative stain transmission electron microscopy. Furthermore, these rigid rods can serve as a scaffold for the decoration of diverse proteins or biologically active peptides along their length with adjustable spacing up to tens of nanometers, as confirmed by the DNA-PAINT super-resolution microscopy. This demonstrates the potential of modular bottom-up protein engineering and tunable CCs for the fabrication of functionalized protein biomaterials.

模块化蛋白质工程是以纳米级精度制造高分子量组装体和生物材料的有力方法。在此,我们以人类肌营养不良蛋白的中央杆状结构域为灵感,设计了一种扩展的纳米级丝状结构,该结构在肌肉收缩过程中保护肌浆膜,由三螺旋束组成的谱蛋白重复序列构成。由三个串联谱林重复序列组成的模块被用作刚性构件,通过形成盘绕线圈(CC)的二聚体肽进行自组装。CC 肽被精确地整合到一个适当的框架中,以保持谱蛋白 α-螺旋的连续性,从而形成延伸的纳米棒。我们利用一套可定制的正交 CC 异二聚体来实现模块化刚性结构域关联,金属离子和螯合剂可对其进行额外调节。通过原子力显微镜和负染色透射电子显微镜的测定,我们实现了几微米长的刚性棒的稳健组装。此外,DNA-PAINT 超分辨显微镜还证实,这些刚性棒可作为支架,沿其长度方向装饰各种蛋白质或生物活性肽,间距可调至数十纳米。这证明了模块化自下而上蛋白质工程和可调 CCs 在制造功能化蛋白质生物材料方面的潜力。
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引用次数: 0
Nanovibrational Stimulation of Escherichia coli Mitigates Surface Adhesion by Altering Cell Membrane Potential.
IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-22 DOI: 10.1021/acsnano.4c11000
Dario G Bazzoli, Nasim Mahmoodi, Terri-Anne Verrill, Tim W Overton, Paula M Mendes

Mechanical forces shape living matter from the macro- to the microscale as both eukaryotic and prokaryotic cells are force wielders and sensors. However, whereas such forces have been used to control mechanically dependent behaviors in mammalian cells, we lack the same level of understanding in bacteria. Surface adhesion, the initial stages of biofilm formation and surface biofouling, is a mechanically dependent process, which makes it an ideal target for mechano-control. In this study, we employed nanometer surface vibrations to mechanically stimulate bacteria and investigate their effect on adhesion. We discovered that vibrational stimulation at the nanoscale consistently reduces surface adhesion by altering cell membrane potential. Our findings identify a link between bacteria electrophysiology and surface adhesion and provide evidence that the nanometric mechanical "tickling" of bacteria can inhibit surface adhesion.

从宏观到微观层面,机械力都在塑造生命物质,因为真核细胞和原核细胞都是力的挥舞者和传感器。然而,虽然这种力已被用于控制哺乳动物细胞的机械依赖行为,但我们对细菌却缺乏同样程度的了解。表面粘附是生物膜形成和表面生物污损的初始阶段,是一个机械依赖过程,这使其成为机械控制的理想目标。在这项研究中,我们利用纳米表面振动对细菌进行机械刺激,并研究其对粘附的影响。我们发现,纳米级振动刺激可通过改变细胞膜电位持续降低表面粘附力。我们的研究结果确定了细菌电生理学与表面粘附力之间的联系,并提供了纳米级机械 "搔痒 "细菌可抑制表面粘附力的证据。
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引用次数: 0
Electrical Control of Valley Polarized Charged Exciton Species in Monolayer WS2
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-22 DOI: 10.1021/acsnano.4c11080
Sarthak Das, Ding Huang, Ivan A. Verzhbitskiy, Zi-En Ooi, Chit Siong Lau, Rainer Lee, Calvin Pei Yu Wong, Kuan Eng Johnson Goh
Excitons are key to the optoelectronic applications of van der Waals semiconductors, with the potential for versatile on-demand tuning of properties. Yet, their electrical manipulation remains challenging due to inherent charge neutrality and the additional loss channels induced by electrical doping. We demonstrate the dynamic electrical control of valley polarization in charged excitonic states of monolayer tungsten disulfide, achieving up to a 6-fold increase in the degree of circular polarization under off-resonant excitation. In contrast to the weak direct tuning of excitons typically observed using electrical gating, the charged exciton photoluminescence remains stable, even with increased scattering from electron doping. By exciting at the exciton resonances, we observed the reproducible nonmonotonic switching of the charged state population as the electron doping is varied under gate bias, indicating a resonant interplay between neutral and charged exciton states.
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引用次数: 0
Correction to"Specifically Formed Corona on Silica Nanoparticles Enhances Transforming Growth Factor beta 1 Activity in Triggering Lung Fibrosis". 更正 "二氧化硅纳米粒子上特殊形成的电晕增强了转化生长因子 beta 1 在诱发肺纤维化方面的活性"。
IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-22 Epub Date: 2024-10-11 DOI: 10.1021/acsnano.4c12340
Zhenzhen Wang, Chunming Wang, Shang Liu, Wei He, Lintao Wang, JingJing Gan, Zhen Huang, Zhenheng Wang, Haoyang Wei, Junfeng Zhang, Lei Dong
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引用次数: 0
Ultrafast Charge Transfer-Induced Unusual Nonlinear Optical Response in ReSe2/ReS2 Heterostructure
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-22 DOI: 10.1021/acsnano.4c11372
Yanqing Ge, Jiayu Tan, Guorong Xu, Xukun Feng, Erkang Li, Yijie Wang, Chunhui Lu, Xinlong Xu
Ultrafast charge transfer in van der Waals heterostructures can effectively engineer the optical and electrical properties of two-dimensional semiconductors for designing photonic and optoelectronic devices. However, the nonlinear absorption conversion dynamics with the pump intensity and the underlying physical mechanisms in a type-II heterostructure remain largely unexplored, yet hold considerable potential for all-optical logic gates. Herein, two-dimensional ReSe2/ReS2 heterostructure is designed to realize an unusual transition from reverse saturable absorption to saturable absorption (SA) with a conversion pump intensity threshold of approximately 170 GW/cm2. Such an intriguing phenomenon is attributed to the decrease of two-photon absorption (TPA) of ReS2 and the increase of SA of ReSe2 with the pump intensity. Based on the characterization results of X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, femtosecond transient absorption spectrum, Kelvin probe force microscopy, and density functional theory calculation, a type-II charge-transfer-energy level model is proposed combined with the TPA of ReS2 and SA of ReSe2 processes. The results reveal the critical role of ultrafast interfacial charge transfer in tuning the unusual nonlinear absorption and improving the SA of ReSe2/ReS2 under different excitation wavelengths. Our finding deepens the understanding of nonlinear absorption physical mechanisms in two-dimensional heterostructure materials, which may further diversify the nonlinear optical materials and photonic devices.
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引用次数: 0
2D Embedded Ultrawide Bandgap Devices for Extreme Environment Applications. 用于极端环境应用的二维嵌入式超宽带隙器件。
IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-22 DOI: 10.1021/acsnano.4c09173
Madani Labed, Ji-Yun Moon, Seung-Il Kim, Jang Hyeok Park, Justin S Kim, Chowdam Venkata Prasad, Sang-Hoon Bae, You Seung Rim

Ultrawide bandgap semiconductors such as AlGaN, AlN, diamond, and β-Ga2O3 have significantly enhanced the functionality of electronic and optoelectronic devices, particularly in harsh environment conditions. However, some of these materials face challenges such as low thermal conductivity, limited P-type conductivity, and scalability issues, which can hinder device performance under extreme conditions like high temperature and irradiation. In this review paper, we explore the integration of various two-dimensional materials (2DMs) to address these challenges. These materials offer excellent properties such as high thermal conductivity, mechanical strength, and electrical properties. Notably, graphene, hexagonal boron nitride, transition metal dichalcogenides, 2D and quasi-2D Ga2O3, TeO2, and others are investigated for their potential in improving ultrawide bandgap semiconductor-based devices. We highlight the significant improvement observed in the device performance after the incorporation of 2D materials. By leveraging the properties of these materials, ultrawide bandgap semiconductor devices demonstrate enhanced functionality and resilience in harsh environmental conditions. This review provides valuable insights into the role of 2D materials in advancing the field of ultrawide bandgap semiconductors and highlights opportunities for further research and development in this area.

AlGaN、AlN、金刚石和 β-Ga2O3 等超宽带隙半导体极大地增强了电子和光电设备的功能,尤其是在恶劣的环境条件下。然而,其中一些材料面临着挑战,如热导率低、P 型电导率有限以及可扩展性问题,这些都会阻碍器件在高温和辐照等极端条件下的性能。在这篇综述论文中,我们探讨了如何整合各种二维材料(2DM)来应对这些挑战。这些材料具有优异的性能,如高导热性、机械强度和电气性能。特别是石墨烯、六方氮化硼、过渡金属二掺杂物、二维和准二维 Ga2O3、TeO2 以及其他材料,我们研究了它们在改进基于超宽带隙半导体器件方面的潜力。我们强调了加入二维材料后器件性能的显著改善。利用这些材料的特性,超宽带隙半导体器件在恶劣的环境条件下显示出更强的功能性和适应性。本综述就二维材料在推动超宽带隙半导体领域发展中的作用提供了宝贵的见解,并强调了该领域进一步研究和开发的机会。
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引用次数: 0
Endogenous Magnetic Lipid Droplet-Mediated Cascade-Targeted Sonodynamic Therapy as an Approach to Reversing Breast Cancer Multidrug Resistance. 内源性磁脂滴介导的级联靶向声动力疗法作为逆转乳腺癌多药耐药性的一种方法
IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-22 Epub Date: 2024-10-10 DOI: 10.1021/acsnano.4c05938
Zhan Shi, Yiqing Zeng, Jiali Luo, Xue Wang, Guangrong Ma, Tao Zhang, Pintong Huang

Multidrug resistance (MDR) has emerged as a major barrier to effective breast cancer treatment, contributing to high rates of chemotherapy failure and disease recurrence. There is thus a pressing need to overcome MDR and to facilitate the efficient and precise treatment of breast cancer in a targeted manner. In this study, endogenous functional lipid droplets (IR780@LDs-Fe3O4/OA) were developed and used to effectively overcome the limited diffusion distance of reactive oxygen species owing to their amenability to cascade-targeted delivery, thereby facilitating precise and effective sonodynamic therapy (SDT) for MDR breast cancer. Initially, IR780@LDs-Fe3O4/OA was efficiently enriched within tumor sites in a static magnetic field, achieving the visualization of tumor treatment. Subsequently, the cascade-targeted SDT combined with the Fenton effect induced lysosome membrane permeabilization and relieved lysosomal sequestration, thus elevating drug concentration at the target site. This treatment approach also suppressed ATP production, thereby inhibiting P-glycoprotein-mediated chemotherapeutic drug efflux. This cascade-targeted SDT strategy significantly increased the sensitivity of MDR cells to doxorubicin, increasing the IC50 value of doxorubicin by approximately 10-fold. Moreover, the cascade-targeted SDT also altered the gene expression profiles of MDR cells and suppressed the expression of MDR-related genes. In light of these promising results, the combination of cascade-targeted SDT and conventional chemotherapy holds great clinical promise as an effective treatment modality with excellent biocompatibility that can improve MDR breast cancer patient outcomes.

多药耐药性(MDR)已成为乳腺癌有效治疗的主要障碍,导致化疗失败率和疾病复发率居高不下。因此,克服多药耐药性,促进乳腺癌高效、精准的靶向治疗迫在眉睫。本研究开发了内源性功能性脂滴(IR780@LDs-Fe3O4/OA),由于其适合级联靶向递送,可有效克服活性氧的有限扩散距离,从而促进对MDR乳腺癌进行精确有效的声动力治疗(SDT)。最初,IR780@LDs-Fe3O4/OA 在静态磁场中被有效地富集到肿瘤部位,实现了肿瘤治疗的可视化。随后,级联靶向 SDT 与芬顿效应相结合,诱导溶酶体膜通透,缓解溶酶体螯合,从而提高靶点的药物浓度。这种治疗方法还能抑制 ATP 的产生,从而抑制 P 糖蛋白介导的化疗药物外流。这种级联靶向 SDT 策略大大提高了 MDR 细胞对多柔比星的敏感性,使多柔比星的 IC50 值提高了约 10 倍。此外,级联靶向 SDT 还改变了 MDR 细胞的基因表达谱,抑制了 MDR 相关基因的表达。鉴于这些令人鼓舞的结果,级联靶向 SDT 与传统化疗的结合在临床上大有可为,它是一种有效的治疗模式,具有良好的生物相容性,可改善 MDR 乳腺癌患者的预后。
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引用次数: 0
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