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Logic Gates Based on 3D Vertical Junctionless Gate-All-Around Transistors with Reliable Multilevel Contact Engineering 基于三维垂直无结环栅晶体管的逻辑门与可靠的多级触点工程。
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-17 DOI: 10.1021/acs.nanolett.3c04180
Abhishek Kumar, Jonas Müller, Sylvain Pelloquin, Aurélie Lecestre and Guilhem Larrieu*, 

Vertical gate-all-around (V-GAA) represents the ultimate configuration in the forthcoming transistor industry, but it still encounters challenges in the semiconductor community. This paper introduces, for the first time, a dual-input logic gate circuit achieved using 3D vertical transistors with nanoscale sub-20-nm GAA, employing a novel technique for creating contacts and patterning metallic lines at the bottom level without the conventional lift-off process. This involves a two-step oxidation process: patterning the first field oxide to form bottom metal lines and then creating the gate oxide layer on nanowires (NWs), followed by selective removal from the top and bottom of the nanostructures. VGAA-NW transistors, fabricated using the lift-off-free approach, exhibit improved yield and reduced access resistance, leading to an enhanced drive current while maintaining good immunity against short-channel effects. Finally, elementary two-input logic gates within a single cell, using VNW transistors, demonstrate novel possibilities in advanced logic circuitry design and routing options in 3D.

垂直全方位栅极(V-GAA)代表了未来晶体管行业的终极配置,但它在半导体界仍面临挑战。本文首次介绍了利用三维垂直晶体管和纳米级 20 纳米以下 GAA 实现的双输入逻辑栅极电路,采用了一种新技术在底层创建触点和图案化金属线,而无需传统的掀离工艺。这涉及一个两步氧化工艺:将第一层场氧化物图案化以形成底部金属线,然后在纳米线 (NW) 上创建栅极氧化层,接着选择性地从纳米结构的顶部和底部去除。采用无掀离方法制造的 VGAA-NW 晶体管提高了成品率,降低了接入电阻,从而提高了驱动电流,同时保持了对短沟道效应的良好抗扰性。最后,利用 VNW 晶体管在单个单元内制造出基本的双输入逻辑门,展示了三维高级逻辑电路设计和路由选择的新可能性。
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引用次数: 0
A “Ferroptosis-Amplifier” Hydrogel for Eliminating Refractory Cancer Stem Cells Post-lumpectomy 一种用于消除肿瘤切除术后难治性癌症干细胞的 "铁突变-增殖 "水凝胶
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-17 DOI: 10.1021/acs.nanolett.4c02192
Yutong Zhu, Xi Deng, Zideng Dai, Qing Liu, Yichen Kuang, Tianzhi Liu* and Hangrong Chen*, 

The unique “Iron Addiction” feature of cancer stem cells (CSCs) with tumorigenicity and plasticity generally contributes to the tumor recurrence and metastasis after a lumpectomy. Herein, a novel “Ferroptosis Amplification” strategy is developed based on integrating gallic acid-modified FeOOH (GFP) and gallocyanine into Pluronic F-127 (F127) and carboxylated chitosan (CC)-based hydrogel for CSCs eradication. This “Ferroptosis Amplifier” hydrogel is thermally sensitive and achieves rapid gelation at the postsurgical wound in a breast tumor model. Specifically, gallocyanine, as the Dickkopf-1 (DKK1) inhibitor, can decrease the expression of SLC7A11 and GPX4 and synergistically induce ferroptosis of CSCs with GFP. Encouragingly, it is found that this combination suppresses the migratory and invasive capability of cancer cells via the downregulation of matrix metalloproteinase 7 (MMP7). The in vivo results further confirm that this “Ferroptosis Amplification” strategy is efficient in preventing tumor relapse and lung metastasis, manifesting an effective and promising postsurgical treatment for breast cancer.

癌症干细胞(CSCs)具有独特的 "铁瘾 "特征,具有致瘤性和可塑性,通常会导致肿瘤切除术后的复发和转移。本文基于将没食子酸修饰的FeOOH(GFP)和没食子色素整合到基于Pluronic F-127(F127)和羧基壳聚糖(CC)的水凝胶中,开发出一种新型的 "铁嗜性放大 "策略,用于消灭癌干细胞。这种 "铁突变放大器 "水凝胶对热敏感,可在乳腺肿瘤模型的手术后伤口处快速凝胶化。具体来说,五倍子菁作为Dickkopf-1(DKK1)抑制剂,可以降低SLC7A11和GPX4的表达,并协同诱导带有GFP的CSCs铁突变。令人鼓舞的是,研究还发现这种组合能通过下调基质金属蛋白酶 7(MMP7)抑制癌细胞的迁移和侵袭能力。体内研究结果进一步证实,这种 "铁突变放大 "策略能有效防止肿瘤复发和肺转移,是一种有效且有前景的乳腺癌术后治疗方法。
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引用次数: 0
Epitaxial Growth of Two-Dimensional MoO2-MoSe2 Metal-Semiconductor Heterostructures for Schottky Diodes. 用于肖特基二极管的二维 MoO2-MoSe2 金属半导体异质结构的外延生长。
IF 10.8 1区 材料科学 Q1 Engineering Pub Date : 2024-06-17 DOI: 10.1021/acs.nanolett.4c01865
Ting Kang, Jiawen You, Jun Wang, Yuyin Li, Yunxia Hu, Tsz Wing Tang, Xiaohui Lin, Yunxin Li, Liting Liu, Zhaoli Gao, Yuan Liu, Zhengtang Luo

The metal-semiconductor interface fabricated by conventional methods often suffers from contamination, degrading transport performance. Herein, we propose a one-pot chemical vapor deposition (CVD) process to create a two-dimensional (2D) MoO2-MoSe2 heterostructure by growing MoO2 seeds under a hydrogen environment, followed by depositing MoSe2 on the surface and periphery. The ultraclean interface is verified by cross-sectional scanning transmission electron microscopy and photoluminescence. Along with the high work function of semimetallic MoO2 (Ef = -5.6 eV), a high-rectification Schottky diode is fabricated based on this heterostructure. Furthermore, the Schottky diode exhibits an excellent photovoltaic effect with a high open-circuit voltage of 0.26 eV and ultrafast photoresponse, owing to the naturally formed metal-semiconductor contact with suppressed pinning effect. Our method paves the way for the fabrication of an ultraclean 2D metal-semiconductor interface, without defects or contamination, offering promising prospects for future nanoelectronics.

传统方法制造的金属-半导体界面经常受到污染,从而降低传输性能。在此,我们提出了一种一锅化学气相沉积(CVD)工艺,通过在氢气环境下生长 MoO2 种子,然后在其表面和外围沉积 MoSe2,从而制造出二维(2D)MoO2-MoSe2 异质结构。横截面扫描透射电子显微镜和光致发光验证了超净界面。结合半金属 MoO2 的高功函数(Ef = -5.6 eV),基于这种异质结构制造出了高整流肖特基二极管。此外,由于自然形成的金属-半导体接触抑制了针销效应,该肖特基二极管表现出卓越的光伏效应,开路电压高达 0.26 eV,并且光响应速度极快。我们的方法为制造无缺陷、无污染的超洁净二维金属-半导体界面铺平了道路,为未来的纳米电子学提供了广阔的前景。
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引用次数: 0
Tuning Dynamic Structural Evolution of Bi24O31Cl10 for Enhancing Piezo-Photocatalytic Nitrogen Oxidation to Nitrate 调整 Bi24O31Cl10 的动态结构演化以增强压电光催化氮氧化为硝酸盐的能力
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-17 DOI: 10.1021/acs.nanolett.4c01697
Yi Wang, Haiyan Peng, Meiyang Song, Henghui Song, Yuhui Liu, Peng Chen* and Shuang-Feng Yin*, 

Direct nitrogen oxidation into nitrate under ambient conditions presents a promising strategy for harsh and multistep industrial processes. However, the dynamic structural evolution of active sites in surface reactions constitutes a highly intricate endeavor and remains in its nascent stage. Here, we constructed a Bi24O31Cl10 material with moiré superlattice structure (BCMS) for direct piezo-photocatalytic oxidation of nitrogen into nitrate. Excitingly, BCMS achieved excellent nitric acid production (15.44 mg g–1 h–1) under light and pressure conditions. Detailed experimental results show that the unique structure extracts the local strain tensor from the constricting Bi–Bi bond and Bi–O bond for internal structural reconstruction, which promotes the formation of electron and reactive molecule vortexes to facilitate charge transfer as well as N2 and O2 adsorption. Ultimately, these initiatives strengthen electron exchange between the superoxide radical and nitrogen as well as the binding strength of multiple intermediates, which swayingly adjusts the reaction path and energy barriers.

在环境条件下直接将氮氧化成硝酸盐是一种很有前途的策略,适用于苛刻的多步骤工业流程。然而,表面反应中活性位点的动态结构演化是一项非常复杂的工作,目前仍处于起步阶段。在此,我们构建了一种具有摩尔超晶格结构的 Bi24O31Cl10 材料(BCMS),用于直接压电光催化将氮氧化成硝酸盐。令人兴奋的是,在光和压力条件下,BCMS 实现了优异的硝酸生产(15.44 mg g-1 h-1)。详细的实验结果表明,这种独特的结构可从收缩的 Bi-Bi 键和 Bi-O 键中提取局部应变张量,用于内部结构重建,从而促进电子和活性分子涡旋的形成,促进电荷转移以及 N2 和 O2 的吸附。最终,这些举措加强了超氧自由基与氮之间的电子交换以及多个中间产物的结合强度,从而对反应路径和能垒进行了摇摆式调整。
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引用次数: 0
Two-Dimensional Transition Metal Phosphides As Cathode Additive in Robust Lithium–Sulfur Batteries 二维过渡金属磷化物作为强效锂硫电池的阴极添加剂。
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-17 DOI: 10.1021/acs.nanolett.4c01618
Jie Zhang, Dawei Yang*, Canhuang Li, Qianhong Gong, Wei Bi, Xuejiao Zheng, Jordi Arbiol, Shengjun Li and Andreu Cabot*, 

The development of advanced cathode materials able to promote the sluggish redox kinetics of polysulfides is crucial to bringing lithium–sulfur batteries to the market. Herein, two electrode materials: namely, Zr2PS2 and Zr2PTe2, are identified through screening several hundred thousand compositions in the Inorganic Crystal Structure Database. First-principles calculations are performed on these two materials. These structures are similar to that of the classical MXenes. Concurrently, calculations show that Zr2PS2 and Zr2PTe2 possess high electrical conductivity, promote Li ion diffusion, and have excellent electrocatalytic activity for the Li–S reaction and particularly for the Li2S decomposition. Besides, the mechanisms behind the excellent predicted performance of Zr2PS2 and Zr2PTe2 are elucidated through electron localization function, charge density difference, and localized orbital locator. This work not only identifies two candidate sulfur cathode additives but may also serve as a reference for the identification of additional electrode materials in new generations of batteries, particularly in sulfur cathodes.

开发能够促进多硫化物缓慢氧化还原动力学的先进阴极材料对于将锂硫电池推向市场至关重要。在此,通过筛选无机晶体结构数据库中的几十万种成分,确定了两种电极材料:即 Zr2PS2 和 Zr2PTe2。对这两种材料进行了第一性原理计算。这些材料的结构与经典的 MXenes 相似。同时,计算表明 Zr2PS2 和 Zr2PTe2 具有高导电性,能促进锂离子扩散,对锂-S 反应特别是锂-2S 的分解具有优异的电催化活性。此外,还通过电子定位功能、电荷密度差和定位轨道定位器阐明了 Zr2PS2 和 Zr2PTe2 卓越预测性能背后的机理。这项研究不仅确定了两种候选硫阴极添加剂,还可为新一代电池,尤其是硫阴极中其他电极材料的确定提供参考。
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引用次数: 0
Perfect Zeeman Anisotropy in Rotationally Symmetric Quantum Dots with Strong Spin–Orbit Interaction 具有强自旋轨道相互作用的旋转对称量子点中的完美泽曼各向异性。
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-17 DOI: 10.1021/acs.nanolett.4c01247
Markus Aspegren, Lila Chergui, Mikelis Marnauza, Rousan Debbarma, Jakob Bengtsson, Sebastian Lehmann, Kimberly A. Dick, Stephanie M. Reimann and Claes Thelander*, 

In nanoscale structures with rotational symmetry, such as quantum rings, the orbital motion of electrons combined with a spin–orbit interaction can produce a very strong and anisotropic Zeeman effect. Since symmetry is sensitive to electric fields, ring-like geometries provide an opportunity to manipulate magnetic properties over an exceptionally wide range. In this work, we show that it is possible to form rotationally symmetric confinement potentials inside a semiconductor quantum dot, resulting in electron orbitals with large orbital angular momentum and strong spin−orbit interactions. We find complete suppression of Zeeman spin splitting for magnetic fields applied in the quantum dot plane, similar to the expected behavior of an ideal quantum ring. Spin splitting reappears as orbital interactions are activated with symmetry-breaking electric fields. For two valence electrons, representing a common basis for spin-qubits, we find that modulating the rotational symmetry may offer new prospects for realizing tunable protection and interaction of spin–orbital states.

在具有旋转对称性的纳米级结构(如量子环)中,电子的轨道运动与自旋轨道相互作用相结合,可产生极强的各向异性泽曼效应。由于对称性对电场非常敏感,因此环状几何结构为在极宽的范围内操纵磁性提供了机会。在这项研究中,我们发现有可能在半导体量子点内部形成旋转对称的约束势,从而产生具有大轨道角动量和强自旋轨道相互作用的电子轨道。我们发现,在量子点平面上施加磁场时,泽曼自旋分裂被完全抑制,这与理想量子环的预期行为相似。当轨道相互作用被打破对称的电场激活时,自旋分裂再次出现。对于代表自旋比特共同基础的两个价电子,我们发现调节旋转对称性可为实现自旋轨道态的可调保护和相互作用提供新的前景。
{"title":"Perfect Zeeman Anisotropy in Rotationally Symmetric Quantum Dots with Strong Spin–Orbit Interaction","authors":"Markus Aspegren,&nbsp;Lila Chergui,&nbsp;Mikelis Marnauza,&nbsp;Rousan Debbarma,&nbsp;Jakob Bengtsson,&nbsp;Sebastian Lehmann,&nbsp;Kimberly A. Dick,&nbsp;Stephanie M. Reimann and Claes Thelander*,&nbsp;","doi":"10.1021/acs.nanolett.4c01247","DOIUrl":"10.1021/acs.nanolett.4c01247","url":null,"abstract":"<p >In nanoscale structures with rotational symmetry, such as quantum rings, the orbital motion of electrons combined with a spin–orbit interaction can produce a very strong and anisotropic Zeeman effect. Since symmetry is sensitive to electric fields, ring-like geometries provide an opportunity to manipulate magnetic properties over an exceptionally wide range. In this work, we show that it is possible to form rotationally symmetric confinement potentials inside a semiconductor quantum dot, resulting in electron orbitals with large orbital angular momentum and strong spin−orbit interactions. We find complete suppression of Zeeman spin splitting for magnetic fields applied in the quantum dot plane, similar to the expected behavior of an ideal quantum ring. Spin splitting reappears as orbital interactions are activated with symmetry-breaking electric fields. For two valence electrons, representing a common basis for spin-qubits, we find that modulating the rotational symmetry may offer new prospects for realizing tunable protection and interaction of spin–orbital states.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.nanolett.4c01247","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141416627","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Coexistence of Superconductivity and Antiferromagnetism in Topological Magnet MnBi2Te4 Films 拓扑磁体 MnBi2Te4 薄膜中的超导性与反铁磁性共存。
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-17 DOI: 10.1021/acs.nanolett.4c01407
Wei Yuan, Zi-Jie Yan, Hemian Yi, Zihao Wang, Stephen Paolini, Yi-Fan Zhao, Lingjie Zhou, Annie G. Wang, Ke Wang, Thomas Prokscha, Zaher Salman, Andreas Suter, Purnima P. Balakrishnan, Alexander J. Grutter, Laurel E. Winter, John Singleton, Moses H. W. Chan and Cui-Zu Chang*, 

The interface of two materials can harbor unexpected emergent phenomena. One example is interface-induced superconductivity. In this work, we employ molecular beam epitaxy to grow a series of heterostructures formed by stacking together two nonsuperconducting antiferromagnetic materials, an intrinsic antiferromagnetic topological insulator MnBi2Te4 and an antiferromagnetic iron chalcogenide FeTe. Our electrical transport measurements reveal interface-induced superconductivity in these heterostructures. By performing scanning tunneling microscopy and spectroscopy measurements, we observe a proximity-induced superconducting gap on the top surface of the MnBi2Te4 layer, confirming the coexistence of superconductivity and antiferromagnetism in the MnBi2Te4 layer. Our findings will advance the fundamental inquiries into the topological superconducting phase in hybrid devices and provide a promising platform for the exploration of chiral Majorana physics in MnBi2Te4-based heterostructures.

两种材料的界面可能蕴藏着意想不到的新现象。界面诱导超导就是一个例子。在这项研究中,我们采用分子束外延技术,将两种非超导反铁磁性材料--本征反铁磁性拓扑绝缘体 MnBi2Te4 和反铁磁性铁掺杂物 FeTe 堆叠在一起,生长出一系列异质结构。我们的电输运测量揭示了这些异质结构中的界面诱导超导性。通过扫描隧道显微镜和光谱测量,我们在 MnBi2Te4 层的顶面观察到了近距离诱导的超导间隙,证实了 MnBi2Te4 层中超导和反铁磁性的共存。我们的发现将推动对混合器件中拓扑超导阶段的基础研究,并为探索基于 MnBi2Te4 的异质结构中的手性马约拉纳物理学提供了一个前景广阔的平台。
{"title":"Coexistence of Superconductivity and Antiferromagnetism in Topological Magnet MnBi2Te4 Films","authors":"Wei Yuan,&nbsp;Zi-Jie Yan,&nbsp;Hemian Yi,&nbsp;Zihao Wang,&nbsp;Stephen Paolini,&nbsp;Yi-Fan Zhao,&nbsp;Lingjie Zhou,&nbsp;Annie G. Wang,&nbsp;Ke Wang,&nbsp;Thomas Prokscha,&nbsp;Zaher Salman,&nbsp;Andreas Suter,&nbsp;Purnima P. Balakrishnan,&nbsp;Alexander J. Grutter,&nbsp;Laurel E. Winter,&nbsp;John Singleton,&nbsp;Moses H. W. Chan and Cui-Zu Chang*,&nbsp;","doi":"10.1021/acs.nanolett.4c01407","DOIUrl":"10.1021/acs.nanolett.4c01407","url":null,"abstract":"<p >The interface of two materials can harbor unexpected emergent phenomena. One example is interface-induced superconductivity. In this work, we employ molecular beam epitaxy to grow a series of heterostructures formed by stacking together two nonsuperconducting antiferromagnetic materials, an intrinsic antiferromagnetic topological insulator MnBi<sub>2</sub>Te<sub>4</sub> and an antiferromagnetic iron chalcogenide FeTe. Our electrical transport measurements reveal interface-induced superconductivity in these heterostructures. By performing scanning tunneling microscopy and spectroscopy measurements, we observe a proximity-induced superconducting gap on the top surface of the MnBi<sub>2</sub>Te<sub>4</sub> layer, confirming the coexistence of superconductivity and antiferromagnetism in the MnBi<sub>2</sub>Te<sub>4</sub> layer. Our findings will advance the fundamental inquiries into the topological superconducting phase in hybrid devices and provide a promising platform for the exploration of chiral Majorana physics in MnBi<sub>2</sub>Te<sub>4</sub>-based heterostructures.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141416672","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
Inversion Symmetry-Broken Tetralayer Graphene Probed by Second-Harmonic Generation. 通过二次谐波发生探究反转对称破损的四层石墨烯
IF 9.6 1区 材料科学 Q1 Engineering Pub Date : 2024-06-17 DOI: 10.1021/acs.nanolett.4c01880
Wenqiang Zhou, Jiannan Hua, Naitian Liu, Jing Ding, Hanxiao Xiang, Wei Zhu, Shuigang Xu

Stacking orders provide a unique way to tune the properties of two-dimensional materials. Recently, ABCB-stacked tetralayer graphene has been predicted to possess atypical elemental ferroelectricity arising from its symmetry breaking but has been experimentally explored very little. Here, we observe pronounced nonlinear optical second-harmonic generation (SHG) in ABCB-stacked tetralayer graphene while absent in both ABAB- and ABCA-stacked allotropes. Our results provide direct evidence of symmetry breaking in ABCB-stacked tetralayer graphene. The remarkable contrast in the SHG spectra of tetralayer graphene allows straightforward identification of ABCB domains from the other two kinds of stacking order and facilitates the characterization of their crystalline orientation. The employed SHG technique serves as a convenient tool for exploring the intriguing physics and novel nonlinear optics in ABCB-stacked graphene, where spontaneous polarization and intrinsically gapped flat bands coexist. Our results establish ABCB-stacked graphene as a unique platform for studying the rare ferroelectricity in noncentrosymmetric elemental structures.

堆叠阶提供了一种调整二维材料特性的独特方法。最近,人们预测 ABCB 堆垛四层石墨烯因其对称性破缺而具有非典型元素铁电性,但对其进行的实验探索却很少。在这里,我们在 ABCB 层四层石墨烯中观察到了明显的非线性光学二次谐波发生(SHG),而在 ABAB 层和 ABCA 层的同素异形体中却没有观察到。我们的研究结果提供了 ABCB 层四层石墨烯对称性破缺的直接证据。四层石墨烯 SHG 光谱的显著对比可以直接从其他两种堆叠顺序中识别出 ABCB 结构域,并有助于确定它们的结晶取向。所采用的 SHG 技术是探索 ABCB 叠层石墨烯中有趣的物理学和新型非线性光学的便捷工具,在 ABCB 叠层石墨烯中,自发极化和固有间隙平带共存。我们的研究结果使 ABCB 层石墨烯成为研究非中心对称元素结构中罕见铁电性的独特平台。
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引用次数: 0
Hole Relaxation Bottlenecks in CdSe/CdTe/CdSe Lateral Heterostructures Lead to Bicolor Emission CdSe/CdTe/CdSe 侧向异质结构中的孔弛豫瓶颈导致双色发射。
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-17 DOI: 10.1021/acs.nanolett.4c01250
Benjamin T. Diroll*, Corentin Dabard, Muchuan Hua, Juan I. Climente, Emmanuel Lhuillier and Sandrine Ithurria, 

Concentric lateral CdSe/CdTe/CdSe heterostructures show bicolor photoluminescence from both a red charge transfer band of the CdSe/CdTe interface and a green fluorescence from CdSe. This work uses visible and near-infrared transient spectroscopy measurements to demonstrate that the deviation from Kasha’s rule arises from a hole relaxation bottleneck from CdSe to CdTe. Hole transfer can take up to 1 ns, which permits radiative relaxation of excitons remaining in CdSe. Simulations indicate that the hole relaxation bottleneck arises due to the sparse density of states and poor spatial overlap of hole states at energies near the CdSe band edge. The divergent kinetics of transfer for band edge and hot holes is exploited to vary the ratio of green and red photoluminescence with excitation wavelength, providing another knob to control emission color. These findings support the use of lateral heterojunctions as a method for slowing carrier relaxation in two-dimensional materials.

同心横向镉硒/镉碲/镉硒异质结构显示出来自镉硒/镉碲界面红色电荷转移带和镉硒绿色荧光的双色光致发光。这项研究利用可见光和近红外瞬态光谱测量法证明,卡沙规则的偏差源于从碲化镉到碲化镉之间的空穴弛豫瓶颈。空穴传输可长达 1 ns,这使得残留在硒化镉中的激子得以辐射弛豫。模拟结果表明,空穴弛豫瓶颈的产生是由于硒化镉带边缘附近能量处的空穴态密度稀疏、空间重叠性差。利用带边空穴和热空穴的不同转移动力学,可以随激发波长改变绿色和红色的光致发光比例,为控制发射颜色提供了另一种方法。这些发现支持使用横向异质结作为减缓二维材料中载流子弛豫的方法。
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引用次数: 0
DNA Anchoring Strength Directly Correlates with Spherical Nucleic Acid–Based HPV E7 Cancer Vaccine Potency DNA 锚定强度与球形核酸型 HPV E7 癌症疫苗的效力直接相关。
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-14 DOI: 10.1021/acs.nanolett.4c01392
Jeongmin Hwang, Jasper Wilson Dittmar, Janice Kang, Tonatiuh Ocampo, Michael Evangelopoulos, Zhenyu Han, Sergej Kudruk, Jochen Lorch* and Chad A. Mirkin*, 

Vaccination for cancers arising from human papillomavirus (HPV) infection holds immense potential, yet clinical success has been elusive. Herein, we describe vaccination studies involving spherical nucleic acids (SNAs) incorporating a CpG adjuvant and a peptide antigen (E711–19) from the HPV-E7 oncoprotein. Administering the vaccine to humanized mice induced immunity-dependent on the oligonucleotide anchor chemistry (cholesterol vs (C12)9). SNAs containing a (C12)9-anchor enhanced IFN-γ production >200-fold, doubled memory CD8+ T-cell formation, and delivered more than twice the amount of oligonucleotide to lymph nodes in vivo compared to a simple admixture. Importantly, the analogous construct with a weaker cholesterol anchor performed similar to admix. Moreover, (C12)9-SNAs activated 50% more dendritic cells and generated T-cells cytotoxic toward an HPV+ cancer cell line, UM-SCC-104, with near 2-fold greater efficiency. These observations highlight the pivotal role of structural design, and specifically oligonucleotide anchoring strength (which correlates with overall construct stability), in developing efficacious therapeutic vaccines.

针对人类乳头瘤病毒(HPV)感染引起的癌症的疫苗接种具有巨大的潜力,但临床上一直未能取得成功。在此,我们介绍了结合了 CpG 佐剂和 HPV-E7 肿瘤蛋白多肽抗原(E711-19)的球形核酸(SNA)疫苗接种研究。给人源化小鼠注射疫苗后,其免疫力取决于寡核苷酸锚化学成分(胆固醇与 (C12)9)。与简单混合相比,含有 (C12)9 锚的 SNA 可使 IFN-γ 生成量提高 200 倍以上,使记忆 CD8+ T 细胞的形成增加一倍,并将两倍多的寡核苷酸输送到体内淋巴结。重要的是,胆固醇锚较弱的类似构建物与掺杂物的表现相似。此外,(C12)9-SNA 激活的树突状细胞增加了 50%,产生的 T 细胞对 HPV+ 癌细胞系 UM-SCC-104 具有细胞毒性,效率提高了近 2 倍。这些观察结果凸显了结构设计,特别是寡核苷酸锚定强度(与整体结构稳定性相关)在开发有效治疗疫苗中的关键作用。
{"title":"DNA Anchoring Strength Directly Correlates with Spherical Nucleic Acid–Based HPV E7 Cancer Vaccine Potency","authors":"Jeongmin Hwang,&nbsp;Jasper Wilson Dittmar,&nbsp;Janice Kang,&nbsp;Tonatiuh Ocampo,&nbsp;Michael Evangelopoulos,&nbsp;Zhenyu Han,&nbsp;Sergej Kudruk,&nbsp;Jochen Lorch* and Chad A. Mirkin*,&nbsp;","doi":"10.1021/acs.nanolett.4c01392","DOIUrl":"10.1021/acs.nanolett.4c01392","url":null,"abstract":"<p >Vaccination for cancers arising from human papillomavirus (HPV) infection holds immense potential, yet clinical success has been elusive. Herein, we describe vaccination studies involving spherical nucleic acids (SNAs) incorporating a CpG adjuvant and a peptide antigen (E7<sub>11–19</sub>) from the HPV-E7 oncoprotein. Administering the vaccine to humanized mice induced immunity-dependent on the oligonucleotide anchor chemistry (cholesterol vs (C12)<sub>9</sub>). SNAs containing a (C12)<sub>9</sub>-anchor enhanced IFN-γ production &gt;200-fold, doubled memory CD8<sup>+</sup> T-cell formation, and delivered more than twice the amount of oligonucleotide to lymph nodes <i>in vivo</i> compared to a simple admixture. Importantly, the analogous construct with a weaker cholesterol anchor performed similar to admix. Moreover, (C12)<sub>9</sub>-SNAs activated 50% more dendritic cells and generated T-cells cytotoxic toward an HPV<sup>+</sup> cancer cell line, UM-SCC-104, with near 2-fold greater efficiency. These observations highlight the pivotal role of structural design, and specifically oligonucleotide anchoring strength (which correlates with overall construct stability), in developing efficacious therapeutic vaccines.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141316011","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
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