Pub Date : 2024-10-22Epub Date: 2024-10-07DOI: 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。
{"title":"A Direct Current Self-Sustained Moisture-Electric Generator with 1<i>D</i>/2D Hierarchical Nanostructure for Continuous Operation of Off-Grid Electronics.","authors":"Luyu Yang, Lei Zhang, Yang-Chun Yong, Dongping Sun","doi":"10.1021/acsnano.4c09494","DOIUrl":"10.1021/acsnano.4c09494","url":null,"abstract":"<p><p>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<sup>-3</sup>, 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.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":15.8,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142379394","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-22Epub Date: 2024-10-11DOI: 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.
{"title":"Multifunctional Reconfigurable Operations in an Ultra-Scaled Ferroelectric Negative Transconductance Transistor.","authors":"Zhongyunshen Zhu, Anton E O Persson, Lars-Erik Wernersson","doi":"10.1021/acsnano.4c09598","DOIUrl":"10.1021/acsnano.4c09598","url":null,"abstract":"<p><p>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 μm<sup>2</sup>. 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.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":15.8,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142398655","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}
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.
{"title":"DNA-Based Chemical Unclonable Functions for Cryptographic Anticounterfeit Tagging of Pharmaceuticals","authors":"Anne M. Luescher, Wendelin J. Stark, Robert N. Grass","doi":"10.1021/acsnano.4c10870","DOIUrl":"https://doi.org/10.1021/acsnano.4c10870","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":17.1,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142487130","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}
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。
{"title":"Coupling of Spectrin Repeat Modules for the Assembly of Nanorods and Presentation of Protein Domains.","authors":"Klemen Mezgec, Jaka Snoj, Liza Ulčakar, Ajasja Ljubetič, Magda Tušek Žnidarič, Miha Škarabot, Roman Jerala","doi":"10.1021/acsnano.4c07701","DOIUrl":"10.1021/acsnano.4c07701","url":null,"abstract":"<p><p>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.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":15.8,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142398653","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}
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.
{"title":"Nanovibrational Stimulation of <i>Escherichia coli</i> Mitigates Surface Adhesion by Altering Cell Membrane Potential.","authors":"Dario G Bazzoli, Nasim Mahmoodi, Terri-Anne Verrill, Tim W Overton, Paula M Mendes","doi":"10.1021/acsnano.4c11000","DOIUrl":"https://doi.org/10.1021/acsnano.4c11000","url":null,"abstract":"<p><p>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.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":15.8,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453139","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}
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.
{"title":"Electrical Control of Valley Polarized Charged Exciton Species in Monolayer WS2","authors":"Sarthak Das, Ding Huang, Ivan A. Verzhbitskiy, Zi-En Ooi, Chit Siong Lau, Rainer Lee, Calvin Pei Yu Wong, Kuan Eng Johnson Goh","doi":"10.1021/acsnano.4c11080","DOIUrl":"https://doi.org/10.1021/acsnano.4c11080","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":17.1,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142487132","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}
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.
{"title":"Ultrafast Charge Transfer-Induced Unusual Nonlinear Optical Response in ReSe2/ReS2 Heterostructure","authors":"Yanqing Ge, Jiayu Tan, Guorong Xu, Xukun Feng, Erkang Li, Yijie Wang, Chunhui Lu, Xinlong Xu","doi":"10.1021/acsnano.4c11372","DOIUrl":"https://doi.org/10.1021/acsnano.4c11372","url":null,"abstract":"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 ReSe<sub>2</sub>/ReS<sub>2</sub> 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/cm<sup>2</sup>. Such an intriguing phenomenon is attributed to the decrease of two-photon absorption (TPA) of ReS<sub>2</sub> and the increase of SA of ReSe<sub>2</sub> 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 ReS<sub>2</sub> and SA of ReSe<sub>2</sub> processes. The results reveal the critical role of ultrafast interfacial charge transfer in tuning the unusual nonlinear absorption and improving the SA of ReSe<sub>2</sub>/ReS<sub>2</sub> 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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":17.1,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142487131","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}
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.
{"title":"2D Embedded Ultrawide Bandgap Devices for Extreme Environment Applications.","authors":"Madani Labed, Ji-Yun Moon, Seung-Il Kim, Jang Hyeok Park, Justin S Kim, Chowdam Venkata Prasad, Sang-Hoon Bae, You Seung Rim","doi":"10.1021/acsnano.4c09173","DOIUrl":"https://doi.org/10.1021/acsnano.4c09173","url":null,"abstract":"<p><p>Ultrawide bandgap semiconductors such as AlGaN, AlN, diamond, and β-Ga<sub>2</sub>O<sub>3</sub> 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 Ga<sub>2</sub>O<sub>3</sub>, TeO<sub>2</sub>, 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.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":15.8,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453231","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}
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.
{"title":"Endogenous Magnetic Lipid Droplet-Mediated Cascade-Targeted Sonodynamic Therapy as an Approach to Reversing Breast Cancer Multidrug Resistance.","authors":"Zhan Shi, Yiqing Zeng, Jiali Luo, Xue Wang, Guangrong Ma, Tao Zhang, Pintong Huang","doi":"10.1021/acsnano.4c05938","DOIUrl":"10.1021/acsnano.4c05938","url":null,"abstract":"<p><p>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-Fe<sub>3</sub>O<sub>4</sub>/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-Fe<sub>3</sub>O<sub>4</sub>/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 IC<sub>50</sub> 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.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":15.8,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142386358","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}