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Enhanced interlayer electron transfer by surface treatments in mixed-dimensional van der Waals semiconductor heterostructures 在混合维范德华半导体异质结构中通过表面处理增强层间电子转移
IF 6.1 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-26 DOI: 10.1063/5.0214718
Takeshi Odagawa, Sota Yamamoto, Chaoliang Zhang, Kazuki Koyama, Jun Ishihara, Giacomo Mariani, Yoji Kunihashi, Haruki Sanada, Junsaku Nitta, Makoto Kohda
We investigate the excitonic species in WS2 monolayers transferred onto III–V semiconductor substrates with different surface treatments. When the III–V substrates were covered with amorphous native oxides, negatively charged excitons dominated the spectral weight in low-temperature near-resonance photoluminescence (PL) measurements. However, when the native oxides of the III–V substrates were reduced, neutral excitons began to dominate the spectral weight, indicating a reduction in the electron density in the WS2 monolayers. The removal of the native oxides enhanced the electron transfer from the WS2 monolayer to the III–V substrate. In addition, an additional shoulder-like PL feature appeared ∼50 meV below the emission of neutral excitons, which can be attributed to the emission of localized excitons. When the III–V substrate surface was passivated by sulfur after the reduction of the native oxides, neutral excitons still dominated the spectral weight. However, the low-energy PL shoulder disappeared again, suggesting the effective delocalization of excitons through substrate surface passivation. Surface engineering of the semiconductor substrates for two-dimensional (2D) materials can provide a novel approach to control the carrier density of the 2D materials, implement deterministic carrier localization or delocalization for the 2D materials, and facilitate the interlayer transfer of charge, spin, and valley currents. These findings open the avenue for novel device concepts and phenomena in mixed-dimensional semiconductor heterostructures.
我们研究了转移到经过不同表面处理的 III-V 族半导体衬底上的 WS2 单层中的激子种类。当 III-V 族基底被无定形原生氧化物覆盖时,带负电荷的激子在低温近共振光致发光(PL)测量的光谱权重中占主导地位。然而,当 III-V 族基底的原生氧化物被还原时,中性激子开始主导光谱权重,这表明 WS2 单层中的电子密度降低了。去除原生氧化物增强了从 WS2 单层到 III-V 基底的电子转移。此外,在中性激子发射的下方 50 meV 处出现了一个额外的肩状聚光特征,这可以归因于局部激子的发射。在还原原生氧化物后,用硫对 III-V 基底表面进行钝化处理,中性激子仍然主导光谱权重。然而,低能 PL 肩再次消失,这表明激子通过衬底表面钝化实现了有效的去局域化。二维(2D)材料半导体衬底的表面工程可以提供一种新方法来控制二维材料的载流子密度,实现二维材料的确定性载流子定位或去定位,并促进电荷、自旋和谷电流的层间转移。这些发现为混合二维半导体异质结构中的新型器件概念和现象开辟了道路。
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引用次数: 0
High-temperature insulating ferromagnetic state in charge-disproportionated and spin-state-disproportionated strained SrCoO2.5 thin film 电荷不成比例和自旋态不成比例应变 SrCoO2.5 薄膜中的高温绝缘铁磁态
IF 6.1 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-05-30 DOI: 10.1063/5.0188767
Sourav Chowdhury, Anupam Jana, Ritu Rawat, Priyanka Yadav, Rajibul Islam, Fei Xue, A. K. Mandal, Sumit Sarkar, Rajan Mishra, R. Venkatesh, D. M. Phase, R. J. Choudhary
Ferromagnetic insulators (FMIs) have widespread applications in microwave devices, magnetic tunneling junctions, and dissipationless electronic and quantum-spintronic devices. However, the sparsity of the available high-temperature FMIs has led to the quest for a robust and controllable insulating ferromagnetic state. Here, we present compelling evidence of modulation of the magnetic ground state in a SrCoO2.5 (SCO) thin film via strain engineering. The SCO system is an antiferromagnetic insulator with a Neel temperature, TN, of ∼550 K. Applying in-plane compressive strain, the SCO thin film reveals an insulating ferromagnetic state with an extraordinarily high Curie temperature, TC, of ∼750 K. The emerged ferromagnetic state is associated with charge-disproportionation (CD) and spin-state-disproportionation (SSD), involving high-spin Co2+ and low-spin Co4+ ions. The density functional theory calculation also produces an insulating ferromagnetic state in the strained SCO system, consistent with the CD and SSD, which is associated with the structural ordering in the system. Transpiring the insulating ferromagnetic state through modulating the electronic correlation parameters via strain engineering in the SCO thin film will have a significant impact in large areas of modern electronic and spintronic applications.
铁磁绝缘体(FMIs)在微波设备、磁隧道结、无耗散电子设备和量子自旋电子设备中有着广泛的应用。然而,由于现有高温铁磁绝缘体的稀缺性,人们开始寻求一种稳健、可控的绝缘铁磁态。在这里,我们提出了通过应变工程调制 SrCoO2.5 (SCO) 薄膜磁基态的有力证据。SCO 系统是一种反铁磁绝缘体,其 Neel 温度(TN)为 ∼550 K。施加面内压应变后,SCO 薄膜显示出一种绝缘铁磁态,其居里温度(TC)超高,达到 ∼750 K。密度泛函理论计算还得出了应变 SCO 系统中的绝缘铁磁态,与 CD 和 SSD 相一致,这与系统中的结构有序性有关。通过应变工程调控 SCO 薄膜中的电子相关参数来激发绝缘铁磁态,将对现代电子和自旋电子应用领域产生重大影响。
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引用次数: 0
Reciprocal space x-ray computed tomography 对等空间 X 射线计算机断层扫描
IF 6.1 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-05-30 DOI: 10.1063/5.0203995
Arturas Vailionis, Liyan Wu, Jonathan E. Spanier
Three-dimensional reciprocal space mapping (3D-RSM) offers crucial insights into the intricate microstructural properties of materials, including spatial domain distribution, directional long-range ordering, multilayer-substrate mismatch, layer tilting, and defect structure. Traditionally, 3D-RSMs are conducted at synchrotron facilities where instrumental resolution is constrained in all three directions. Lab-based sources have often been considered suboptimal for 3D-RSM measurements due to poor instrumental resolution along the axial direction. However, we demonstrate that, by employing three-dimensional reciprocal space x-ray computed tomography (RS-XCT), the same perceived limitation in resolution can be effectively leveraged to acquire high quality 3D-RSMs. Through a combination of ultrafast reciprocal space mapping and computed tomography reconstruction routines, lab-based 3D-RSMs achieve resolutions comparable to those obtained with synchrotron-based techniques. RS-XCT introduces a practical modality for lab-based x-ray diffractometers, enabling high-resolution 3D-RSM measurements on a variety of materials exhibiting complex three-dimensional scattering landscapes in reciprocal space.
三维倒易空间制图(3D-RSM)可帮助人们深入了解材料错综复杂的微观结构特性,包括空间畴分布、定向长程有序、多层衬底错配、层倾斜和缺陷结构。传统上,3D-RSM 是在同步辐射设施中进行的,在同步辐射设施中,仪器在所有三个方向上的分辨率都受到限制。由于沿轴向的仪器分辨率较低,基于实验室的光源通常被认为是 3D-RSM 测量的次优选择。然而,我们证明,通过采用三维往复空间 X 射线计算机断层扫描 (RS-XCT),可以有效地利用同样的分辨率限制来获取高质量的三维 RSM。通过结合超快倒易空间映射和计算机断层扫描重建程序,基于实验室的三维 RSM 可达到与同步加速器技术相媲美的分辨率。RS-XCT 为基于实验室的 X 射线衍射仪引入了一种实用模式,可对在倒易空间呈现复杂三维散射景观的各种材料进行高分辨率 3D-RSM 测量。
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引用次数: 0
Impact of sulfur addition on the structure and dynamics of Ni–Nb alloy melts 加硫对 Ni-Nb 合金熔体结构和动力学的影响
IF 6.1 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-05-29 DOI: 10.1063/5.0205058
Nicolai Grund, Dirk Holland-Moritz, Saba Khademorezaian, Lucas P. Kreuzer, Nico Neuber, Lucas M. Ruschel, Hendrik Voigt, Johanna Wilden, Fan Yang, Soham Banerjee, Malte Blankenburg, Ann-Christin Dippel, Jan Peter Embs, Sergiy Divinski, Ralf Busch, Andreas Meyer, Gerhard Wilde
We investigated the change in the structure and dynamics of a Ni–Nb bulk metallic glass upon sulfur addition on both microscopic and macroscopic scales. With the sulfur concentration of 3 at. %, where the composition Ni58Nb39S3 exhibits the best glass forming ability in the investigated sulfur concentration range, both the equilibrium and undercooled melt dynamics remain almost unchanged. Only in the glassy state does sulfur seem to result in mass transport less decoupled to the viscosity of the undercooled liquid, where the measured Ag tracer diffusion coefficient is slower in the ternary alloy. With the structural disorder introduced by the alloying sulfur, the improved glass forming ability is attributed to geometrical frustration, where crystal nucleation requires a depletion of sulfur and hence long range diffusion, as long as no primary sulfur-containing crystalline phase is involved.
我们从微观和宏观两个尺度研究了 Ni-Nb 块状金属玻璃在添加硫后的结构和动力学变化。硫浓度为 3 at.%时,平衡和欠冷熔体动力学几乎保持不变。只有在玻璃态时,硫似乎才会导致质量传输与过冷液体粘度的脱钩程度降低,在三元合金中测量到的银示踪剂扩散系数较慢。由于合金中的硫造成了结构紊乱,玻璃形成能力的提高归因于几何挫折,在这种情况下,只要不涉及原生含硫结晶相,晶体成核就需要硫的耗竭,从而导致长程扩散。
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引用次数: 0
Development of one-step roll-to-roll system with incorporated vacuum sputtering for large-scale production of plasmonic sensing chips 开发用于大规模生产等离子传感芯片的一步式卷对卷系统,其中包含真空溅射技术
IF 6.1 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-05-29 DOI: 10.1063/5.0211084
Tae Eon Kim, Sunghoon Jung, Soo Hyun Lee, ChaeWon Mun, Eun-Yeon Byeon, Jun-Yeong Yang, Jucheol Park, Seunghun Lee, Heemin Kang, Sung-Gyu Park
The trade-off relationship between cost and performance is a major challenge in the development of surface-enhanced Raman spectroscopy (SERS) sensors for practical applications. We propose a roll-to-roll system with incorporated vacuum sputtering to manufacture Ag-coated nanodimples (Ag/NDs) on A4-scale films in a single step. The Ag/ND SERS platforms were prepared via O2 ion beam sputtering and Ag sputtering deposition. The concave three-dimensional spaces in the Ag/NDs functioned as hotspots, and their optimal fabrication conditions were investigated with two variables: moving speed and Ag thickness. The entire process was automated, which resulted in highly consistent optical responses (i.e., relative standard deviation of ∼10%). The activation of plasmonic hotspots was demonstrated by electric-field profiles calculated via the finite-difference time-domain method. The wavelength dependency of the Ag/ND platforms was also examined by dark-field microscopy. The results indicate that the developed engineering technique for the large-scale production of Ag/ND plasmonic chips would likely be competitive in the commercial market.
在开发实际应用的表面增强拉曼光谱(SERS)传感器时,成本与性能之间的权衡关系是一大挑战。我们提出了一种结合真空溅射的辊对辊系统,可在 A4 级薄膜上一步制备 Ag 涂层纳米微粒(Ag/ND)。Ag/ND SERS 平台是通过 O2 离子束溅射和 Ag 溅射沉积制备的。Ag/ND 中的凹面三维空间起到了热点的作用,通过两个变量:移动速度和 Ag 厚度,研究了其最佳制备条件。整个过程都是自动化的,因此产生了高度一致的光学响应(即相对标准偏差∼10%)。通过有限差分时域法计算的电场曲线证明了等离子热点的激活。此外,还通过暗场显微镜检查了 Ag/ND 平台的波长依赖性。结果表明,所开发的大规模生产 Ag/ND 等离子芯片的工程技术很可能在商业市场上具有竞争力。
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引用次数: 0
Speed limits of the laser-induced phase transition in FeRh 激光诱导 FeRh 相变的速度极限
IF 6.1 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-05-28 DOI: 10.1063/5.0206095
M. Mattern, J. Jarecki, J. A. Arregi, V. Uhlíř, M. Rössle, M. Bargheer
We use ultrafast x-ray diffraction and the polar time-resolved magneto-optical Kerr effect to study the laser-induced metamagnetic phase transition in two FeRh films with thicknesses below and above the optical penetration depth. In the thin film, we identify an intrinsic timescale for the light-induced nucleation of ferromagnetic (FM) domains in the antiferromagnetic material of 8ps, which is substantially longer than the time it takes for strain waves to traverse the film. For the inhomogeneously excited thicker film, only the optically excited near-surface part transforms within 8ps. For strong excitations, we observe an additional slow rise of the FM phase, which we experimentally relate to a growth of the FM phase into the depth of the layer by comparing the transient magnetization in frontside and backside excitation geometry. In the lower lying parts of the film, which are only excited via near-equilibrium heat transport, the FM phase emerges significantly slower than 8ps after heating above the transition temperature.
我们利用超快 X 射线衍射和极地时间分辨磁光克尔效应,研究了厚度低于和高于光学穿透深度的两层 FeRh 薄膜中激光诱导的元磁相变。在薄膜中,我们确定了反铁磁材料中铁磁(FM)畴的光诱导成核的固有时间尺度为 8ps,大大长于应变波穿过薄膜所需的时间。对于不均匀激发的较厚薄膜,只有光学激发的近表面部分会在 8ps 内发生转变。对于强激励,我们观察到调频相的额外缓慢上升,通过比较正面和背面激励几何形状下的瞬态磁化,我们在实验中将其与调频相向膜层深处的增长联系起来。在薄膜的低层部分,仅通过近平衡热传导激发,调频相在加热到转变温度以上后出现的速度明显慢于 8ps。
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引用次数: 0
Effective polysulfide control in lithium–sulfur batteries utilizing BiFeO3 nanoparticles 利用 BiFeO3 纳米粒子有效控制锂硫电池中的多硫化物
IF 6.1 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-05-28 DOI: 10.1063/5.0209845
Mohan K. Bhattarai, Balram Tripathi, Shweta Shweta, Satyam Kumar, Claudia C. Zuluaga-Gómez, Rajesh K. Katiyar, Brad R. Weiner, Ram S. Katiyar, Gerardo Morell
Lithium–sulfur batteries (LiSBs) offer high energy density, cost-effectiveness, and eco-friendliness, making them promising for future energy storage. This study explores using BiFeO3 (BFO) nanoparticles (NPs) to tackle challenges such as lithium polysulfides (LiPs) and shuttle issues in LiSBs. It employs a solid-state melt diffusion technique, encapsulates sulfur in single-walled carbon nanotubes (SCNTs), and utilizes BFO for effective polysulfide control. Herein, composite cathodes of sulfur (S)/SCNTs (abbr. SCNT) were fabricated, and cells were designed using a BFO-coated separator (SCNT-BFS). In addition, a cathode modification was performed with composite S/SCNTs/BFO (SCNT-BF), and a comparative analysis was conducted to assess the effectiveness of the BFO in the separator and the cathode. Cyclic voltammetry measurements revealed that the increased current peak intensity at lower reduction potential in SCNT-BF and SCNT-BFS indicated control of higher-order LiPs (Li2Sx, where 4 ≤ x ≤ 8), resulting in the generation of more stable lower-order products (Li2S2/Li2S). The charge/discharge analysis revealed controlled LiPs, resulting in high-capacity retention in SCNT-BF (∼75%) and SCNT-BFS (∼88%) over 200 cycles, which yielded capacities of 526 and 700 mAh/g at C/8 (1C = 1675 mA/g). These promising results suggest that incorporating BFO into the cathode and separator can advance the commercialization of durable LiSBs.
锂硫电池(LiSBs)具有能量密度高、成本效益高和生态友好的特点,因此在未来的能源存储中大有可为。本研究探讨了如何利用 BiFeO3(BFO)纳米粒子(NPs)来应对锂多硫化物(LiPs)和锂硫电池中的穿梭问题等挑战。该研究采用固态熔融扩散技术,将硫封装在单壁碳纳米管(SCNT)中,并利用 BFO 有效控制多硫化物。本文制备了硫(S)/单壁碳纳米管(SCNT)复合阴极,并设计了使用 BFO 涂层隔膜(SCNT-BFS)的电池。此外,还使用 S/SCNTs/BFO 复合材料(SCNT-BF)对阴极进行了改性,并进行了对比分析,以评估 BFO 在隔膜和阴极中的有效性。循环伏安法测量结果表明,SCNT-BF 和 SCNT-BFS 在较低还原电位下的电流峰值强度增加,表明高阶锂聚合物(Li2Sx,其中 4 ≤ x ≤ 8)受到控制,从而生成了更稳定的低阶产物(Li2S2/Li2S)。充电/放电分析表明,受控的 LiPs 使 SCNT-BF(∼75%)和 SCNT-BFS(∼88%)在 200 次循环中保持高容量,在 C/8 条件下(1C = 1675 mA/g),容量分别为 526 和 700 mAh/g。这些充满希望的结果表明,在阴极和分离器中加入 BFO 可以推动耐用锂电池的商业化。
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引用次数: 0
Patterning and epitaxy of large-area arrays of nanoscale complex oxide epitaxial heterostructures 纳米级复杂氧化物外延异质结构大面积阵列的制图和外延
IF 6.1 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-05-28 DOI: 10.1063/5.0203258
Miguel A. Betancourt-Ponce, Rui Liu, Jian Sun, Paul G. Evans, Padma Gopalan
A combination of block copolymer (BCP) lithography and solid-phase epitaxy can be employed to form large areas, on the order of square centimeters, of a high density of epitaxial crystalline complex oxide nanostructures. We have used BCP lithography with a poly(styrene-block-methyl methacrylate) (PS-b-PMMA) copolymer to template a nanohole array either directly on an (001)-oriented SrTiO3 (STO) single crystal substrate or on a 20 nm-thick Si3N4 layer deposited on the STO substrate. BCPs with the selected compositions assembled in a cylindrical phase with 16 nm diameter PMMA cylinders and a cylinder-to-cylinder spacing of 32 nm. The substrate was modified with an energetically non-preferential polymer layer to allow for the vertical alignment of the cylinders. The PMMA cylinders were removed using a subtractive process, leaving an array of cylindrical holes. For BCPs assembled on Si3N4/STO, the pattern was transferred to the Si3N4 layer using reactive ion etching, exposing the underlying STO substrate in the nanoholes. An amorphous LaAlO3 (LAO) layer was deposited on the patterned Si3N4/STO at room temperature. The amorphous LAO epitaxially crystallized within the nanoscale-patterned holes with fully relaxed lattice parameters through solid phase epitaxy, resulting in the formation of nanoscale LAO/STO epitaxial heterostructures.
将嵌段共聚物 (BCP) 光刻技术和固相外延技术相结合,可以形成大面积、约平方厘米的高密度外延结晶复合氧化物纳米结构。我们使用聚(苯乙烯-嵌段-甲基丙烯酸甲酯)(PS-b-PMMA)共聚物进行 BCP 光刻,在取向为 (001) 的 SrTiO3(STO)单晶基底上或沉积在 STO 基底上的 20 纳米厚 Si3N4 层上直接模板化纳米孔阵列。所选成分的 BCP 以直径为 16 nm 的 PMMA 圆柱和 32 nm 的圆柱间距组装成圆柱相。基底被改性为无能量偏好的聚合物层,以实现圆柱的垂直排列。使用减法工艺去除 PMMA 圆柱,留下圆柱孔阵列。对于组装在 Si3N4/STO 上的 BCP,使用反应离子蚀刻将图案转移到 Si3N4 层,从而在纳米孔中暴露出下层的 STO 基底。室温下,在图案化的 Si3N4/STO 上沉积了非晶 LaAlO3(LAO)层。通过固相外延,非晶态 LAO 以完全松弛的晶格参数在纳米级图案孔内外延结晶,从而形成了纳米级 LAO/STO 外延异质结构。
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引用次数: 0
Double pulse all-optical coherent control of ultrafast spin-reorientation in an antiferromagnetic rare-earth orthoferrite 反铁磁稀土正铁氧体超快自旋定向的双脉冲全光相干控制
IF 6.1 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-05-17 DOI: 10.1063/5.0197976
N. E. Khokhlov, A. E. Dolgikh, B. A. Ivanov, A. V. Kimel
A pair of circularly polarized laser pulses of opposite helicities are shown to control the route of spin reorientation phase transition in the rare-earth antiferromagnetic orthoferrite (Sm0.55Tb0.45)FeO3. The route can be efficiently controlled by the delay between the pulses and the sample temperature. Simulations employing previously published models of laser-induced spin dynamics in orthoferrites failed to reproduce the experimental results. We suggest that the failure is due to neglected temperature dependence of the antiferromagnetic resonance damping in the material. Taking into account the experimentally deduced temperature dependence of the damping, we obtained good agreement between the simulations and the experiment.
研究表明,一对螺旋方向相反的圆偏振激光脉冲可以控制稀土反铁磁性正铁(Sm0.55Tb0.45)FeO3的自旋重新定向相变路线。脉冲之间的延迟和样品温度可以有效地控制自旋重新定向相变的路线。利用以前发表的正铁中激光诱导自旋动力学模型进行的模拟未能再现实验结果。我们认为,失败的原因是忽略了材料中反铁磁共振阻尼的温度依赖性。考虑到实验推导出的阻尼温度依赖性,我们在模拟和实验之间获得了良好的一致性。
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引用次数: 0
Mechanical intelligence via fully reconfigurable elastic neuromorphic metasurfaces 通过完全可重构的弹性神经形态元表面实现机械智能
IF 6.1 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-05-15 DOI: 10.1063/5.0201761
M. Moghaddaszadeh, M. Mousa, A. Aref, M. Nouh
The ability of mechanical systems to perform basic computations has gained traction over recent years, providing an unconventional alternative to digital computing in off grid, low power, and severe environments, which render the majority of electronic components inoperable. However, much of the work in mechanical computing has focused on logic operations via quasi-static prescribed displacements in origami, bistable, and soft deformable matter. Here, we present a first attempt to describe the fundamental framework of an elastic neuromorphic metasurface that performs distinct classification tasks, providing a new set of challenges, given the complex nature of elastic waves with respect to scattering and manipulation. Multiple layers of reconfigurable waveguides are phase-trained via constant weights and trainable activation functions in a manner that enables the resultant wave scattering at the readout location to focus on the correct class within the detection plane. We further demonstrate the neuromorphic system’s reconfigurability in performing two distinct tasks, eliminating the need for costly remanufacturing.
近年来,机械系统执行基本计算的能力受到越来越多的关注,它为离网、低功耗和恶劣环境下的数字计算提供了一种非常规的替代方案,而这些环境会导致大多数电子元件无法工作。然而,机械计算的大部分工作都集中在通过折纸、双稳态和软可变形物质中的准静态规定位移进行逻辑运算。在此,我们首次尝试描述弹性神经形态元表面的基本框架,它可以执行不同的分类任务,鉴于弹性波在散射和操纵方面的复杂性质,它提供了一系列新的挑战。多层可重构波导通过恒定权重和可训练激活函数进行相位训练,从而使读出位置的波散射结果聚焦于检测平面内的正确类别。我们进一步展示了神经形态系统在执行两项不同任务时的可重构性,从而消除了昂贵的再制造需求。
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引用次数: 0
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