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Hybrid semiconductor‐polymer nanostructured solar cells hold the promise of photovoltaic energy conversion based on abundant and nontoxic materials and scalable manufacturing processes. After a decade of intense research activity, hybrid solar cells still exhibit low short‐circuit currents and moderate open‐circuit voltages. These bottlenecks call for a detailed understanding of the physics underlying the device operation at the nanoscale. Using first‐principles calculations the ideal energy‐level alignment of hybrid solar cell interfaces based on the wide bandgap semiconductor ZnO and the polymer poly(3‐hexylthiophene) (P3HT) is investigated. The interfacial charge transfer is quantified and it is shown that this effect increases the ideal open‐circuit voltage with respect to the electron‐affinity rule by as much as 0.5 V. The results of this work suggests that there is significant room for optimizing this class of excitonic solar cells by tailoring the semiconductor/polymer interface at the nanoscale.  相似文献   

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By modifying the entangled multi-degrees of freedom of transition-metal oxides, interlayer coupling usually produces interfacial phases with unusual functionalities. Herein, a symmetry-mismatch-driven interfacial phase transition from paramagnetic to ferromagnetic state is reported. By constructing superlattices using CaRuO3 and SrTiO3, two oxides with different oxygen octahedron networks, the tilting/rotation of oxygen octahedra near interface is tuned dramatically, causing an angle increase from ≈150° to ≈165° for the Ru O Ru bond. This in turn drives the interfacial layer of CaRuO3, ≈3 unit cells in thickness, from paramagnetic into ferromagnetic state. The ferromagnetic order is robust, showing the highest Curie temperature of ≈120 K and the largest saturation magnetization of ≈0.7 µB per formula unit. Density functional theory calculations show that the reduced tilting/rotation of RuO6 octahedra favors an itinerant ferromagnetic ground state. This work demonstrates an effective phase tuning by coupled octahedral rotations, offering a new approach to explore emergent materials with desired functionalities.  相似文献   

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The judicious design of 3D giant organic dye molecules to enable the formation of a porous photoactive layer on the surface of titania is one of the viable tactics to abate the adverse interfacial charge recombination in dye‐sensitized solar cells (DSCs) employing outer‐sphere redox couples. Here 2′,6′‐bis(octyloxy)‐biphenyl substituted dithieno[3,2‐b:2′,3′‐d]pyrrole segment is constructed and employed as the π‐linker of a high molar absorption coefficient organic push‐pull dye. With respect to its congener possessing the hexyl substituted dithieno[3,2‐b:2′,3′‐d]pyrrole linker, the new dye can self‐assemble on the surface of titania to afford a porous organic coating, which effectively slow down the kinetics of charge recombination of titania electrons with both outer‐sphere tris(1,10‐phenanthroline)cobalt(III) ions and photooxidized dye molecules, improving the cell photovoltage. In addition, the diminishments of charge recombination via modulating the microstructure of interfacial functional zone can also overcompensate the disadvantageous impact of reduced light‐harvesting and evoke an enhanced photocurrent output, bringing forth an efficiency improvement from 7.5% to 9.3% at the 100 mW cm?2, simulated AM1.5 conditions.  相似文献   

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MXene nanosheets with attractive electrical conductivity and tunable work function have been adopted as multifunctional interfacial modifier between InGaN nanorods and Si for photoelectrochemical water oxidation for the first time. Compared to bare InGaN/Si systems, MXene interfacial layers give rise to an ultralow onset potential of 75 mV versus reversible hydrogen electrode (RHE), which is the highest ever reported for InGaN‐ or Si‐based photoanodes by interfacial modification. Furthermore, the modified photoanode exhibits a significantly enhanced photocurrent density (7.27 mA cm?2) at 1.23 V versus RHE, which is about 10 times higher than that achieved with the InGaN/Si photoanode. The detailed mechanism demonstrates that the formed type‐II band alignment in InGaN/MXene heterojunction and an Ohmic junction at the MXene/Si interface make MXene an ideal electron‐migration channel to enhance charge separation and transfer process. This synergetic effect of MXene can significantly decrease the charge resistance at semiconductor/Si and semiconductor/electrolyte hetero‐interfaces, eventually resulting in the fast hole injection efficiency of 82% and superior stability against photocorrosion. This work not only provides valuable guidance for designing high‐efficiency photoelectrodes through the integration of multiscale and multifunctional materials, but also presents a novel strategy for achieving high‐performance artificial photosynthesis by introducing interfacial modifier.  相似文献   

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The understanding and manipulating of photoluminescence blinking is essential in nano-photonics and related device applications. The formation of mixed-dimensional semiconductor heterostructures provides an important platform for the generation of blinking phenomena, which can be utilized to realize quantum emission properties of the heterostructures that are beyond the pure single material. Here, one-dimensional (1D)/two-dimensional (2D) heterostructures consisting of MoSe2 monolayer and a single CsPbBr3 perovskite nanowire are constructed. By studying the photoluminescence (PL) intensity time trajectory and lifetime, MoSe2 in heterostructure exhibits fluorescent blinking behavior, which has a negative correlation relation with the PL blinking in CsPbBr3 nanowire due to its super-trap states. The excitation power dependent blinking and PL lifetime measurements of the heterostructure, as well as the low-temperature PL spectroscopy, are performed to conclude that the bright state of MoSe2 in heterostructure is due to the suppressed interfacial charge transfer. In addition, MoSe2/hBN/PVK heterostructure is prepared and investigated, showing no blinking phenomena due to the dominated energy transfer process. This study not only provides a deeper understanding of interfacial charge transfer process in 1D/2D heterostructure, but also offers guidance for the design of photonic device with extended functionality.  相似文献   

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The fullerene (C60)/copper phthalocyanine (CuPc) interface is one of the widely used donor/acceptor (DA) interfaces for organic photovoltaics (OPVs), and information on the electronic structure at the interface is essential for fully understanding the energetics of excitons and carriers in OPVs. Here, an investigation into the energy levels at the C60/CuPc interface is made using UV photoelectron, X‐ray photoelectron, and inverse photoemission spectroscopies. The vacuum level and core levels rise with C60 deposition on the CuPc film, which indicates that the interfacial dipole is formed with the negative charge on the C60 side. The interfacial dipole can be formed by the electron transfer from CuPc to C60 in the ground state at the interface, which is indicated by the analysis of the UV–vis–NIR absorption spectrum of the CuPc/C60 blended film. On the other hand, the highest occupied and lowest unoccupied molecular orbitals of CuPc and C60 shift in opposite directions at the interface. This is attributed to the changes of the polarization energies of CuPc and C60 at the interface. The formation of the interfacial dipole and the change of the polarization energy result in the anomalous energy band offsets at the C60/CuPc interface, which are entirely different from those in inorganic p–n junctions.  相似文献   

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Resistance drift is one of the key challenges in phase‐change memory, especially in multilevel storage applications. Although many efforts have been proposed to reduce the probability error caused by resistance drift, the most effective method to suppress resistance drift is by material design. Since resistance drift in amorphous materials comes from changes in the distributions of defects and tail states that are caused by spontaneous structural relaxation, it is possible to suppress resistance drift by confine defect relaxation. A superlattice‐like structure is used to construct relatively controllable interfaces different from those inherent in amorphous chalcogenide for the regulation of resistance drift. By adjusting structural parameters, amorphous GeTe/Sb2Te3 achieves a very low resistance drift. A low‐field electrical transport test based on a trapping band model shows that a change in the structural parameters directly affects the transport process in GeTe/Sb2Te3 such that the resistance drift is suppressed. X‐ray photoelectron spectroscopy characterization reveals that defects at interfaces in superlattice‐like GeTe/Sb2Te3 vary with the structural parameters. Compared with traditional doping and other methods, the interfacial structure introduces controllable defects and provides another strategy for the design of multilevel data storage.  相似文献   

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Heterojunctions between high‐work‐function metals and metal oxides typically lead to Schottky‐type transport barriers resulting from charge transfer between the neighboring materials. These yield versatile electronic functionality exploited for current rectification, memristive behavior, or photocatalysis. Height, width, and shape of the interfacial transport barrier are strongly affected by charge screening via ionic defects, which are often extremely difficult to probe. The ionic nature of a variable contact resistance in heterojunctions between Nb‐doped SrTiO3 (Nb:SrTiO3) and platinum is explored. A control of cationic vacancy defects at the interface is achieved by different annealing procedures in oxidizing and reducing conditions before establishing Pt/Nb:SrTiO3 heterojunctions. Detailed analysis of electronic transport across the heterojunctions reveal significantly varied transport barriers resulting from the cationic defect structure at the interface. These findings are supported by conductive‐tip atomic force microscopy and in situ photoemission spectroscopy showing diminished conductivity of the Nb:SrTiO3 surface and the formation of an insulating surface skin layer after oxygenation. At high doping level, oxygen stoichiometry cannot explain the observed behavior. The increased transport barrier height is therefore linked to strontium vacancy defects. The tailored cation disorder yields access to the ionic control of electronic transport in functional oxide heterojunctions.  相似文献   

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Interfacial charge transfer has a vital role in tailoring the thermoelectric performance of superlattices (SLs), which, however, is rarely clarified by experiments. Herein, based on epitaxially grown p-type (MnTe)x(Sb2Te3)y superlattice-like films, synergistically optimized thermoelectric parameters of carrier density, carrier mobility, and Seebeck coefficient are achieved by introducing interfacial charge transfer, in which effects of hole injection, modulation doping, and energy filtering are involved. Carrier transport measurements and angle-resolved photoemission spectroscopy (ARPES) characterizations reveal a strong hole injection from the MnTe layer to the Sb2Te3 layer in the SLs, originating from the work function difference between MnTe and Sb2Te3. By reducing the thickness of MnTe less than one monolayer, all electronic transport parameters are synergistically optimized in the quantum-dots (MnTe)x(Sb2Te3)12 superlattice-like films, leading to much improved thermoelectric power factors (PFs). The (MnTe)0.1(Sb2Te3)12 obtains the highest room-temperature PF of 2.50 mWm−1K−2, while the (MnTe)0.25(Sb2Te3)12 possesses the highest PF of 2.79 mWm−1K−2 at 381 K, remarkably superior to the values acquired in binary MnTe and Sb2Te3 films. This research provides valuable guidance on understanding and rationally tailoring the interfacial charge transfer of thermoelectric SLs to further enhance thermoelectric performances.  相似文献   

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Transition-metal oxide (TMO) heterostructures provide fertile grounds for creating and manipulating intriguing properties and functionalities. At the interface of TMO heterostructures, electronic reconstructions generally occur via charge transfer and lead to an extraordinary spectrum of emergent phenomena but unattainable in their bulk constituents. However, the basic mechanism of charge transfer at the interface is not fully determined or even understood in heterostructures, which may hide the underlying mechanisms and intriguing physics. Herein, an intrinsic charge transfer and resultant exotic ferromagnetism are unambiguously observed in the heterostructures between the nonmagnetic LaCoO3 (LCO) and SrTiO3 (STO). Combining element-specific X-ray absorption spectroscopy and atomic multiplet fitting, direct evidence of charge transfer-induced multivalence of cobalt ions, interactions of which would contribute to the novel magnetism beyond the intuition, in concert with first-principles density-functional-theory calculations, is demonstrated. Beyond LCO/STO system, a more broadly applicable principle for the heterostructures between 3d TMO and STO where charge transfer and resultant multivalence or conducting interfaces are coexistent is establish. This study represents an advance that the electronic reconstruction and the multiple electron configurations of 3d transition metal ions will constitute a powerful tool for the designs of functional materials and creations of unconventional physical properties.  相似文献   

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Functional oxides are an untapped resource for futuristic devices and functionalities. These functionalities can range from high temperature superconductivity to multiferroicity and novel catalytic schemes. The most prominent route for transforming these ideas from a single device in the lab to practical technologies is by integration with semiconductors. Moreover, coupling oxides with semiconductors can herald new and unexpected functionalities that exist in neither of the individual materials. Therefore, oxide epitaxy on semiconductors provides a materials platform for novel device technologies. As oxides and semiconductors exhibit properties that are complementary to one another, epitaxial heterostructures comprised of the two are uniquely poised to deliver rich functionalities. This review discusses recent advancements in the growth of epitaxial oxides on semiconductors, and the electronic and physical structure of their interfaces. Leaning on these fundamentals and practicalities, the material behavior and functionality of semiconductor–oxide heterostructures is discussed, and their potential as device building blocks is highlighted. The culmination of this discussion is a review of recent advances in the development of prototype devices based on semiconductor–oxide heterostructures, in areas ranging from silicon photonics to photocatalysis. This overview is intended to stimulate ideas for new concepts of functional devices and lay the groundwork for their realization.  相似文献   

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由低维InAs材料和其他二维层状材料堆叠而成的垂直范德华异质结构在纳米电子、光电子和量子信息等新兴领域中应用广泛.探索跨结界面的电荷转移机制对于全面理解该类器件的非凡特性至关重要.第一性原理计算在揭示界面电荷转移特性与各种能量稳定型InAs基范德华异质结的电、光、磁等原理物理特性和器件性能变化之间的内在关系方面发挥着不可比拟的作用.文中梳理、总结和探讨了近年来InAs基范德华异质结间界面电荷转移特性的理论研究工作与潜在的功能应用,提出在理论方法和计算精度方面大力发展第一性原理计算的几个途径,为更好地开展InAs基范德华异质结的基础科学研究和应用器件设计提供可借鉴的量化研究基础.  相似文献   

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This article reports the respective photovoltaic processes of singlet and triplet photoexcited states in dissociation and charge reactions based on the studies of magnetic‐field effects of photocurrents. The magnetic‐field effects of photocurrents reveal that weak donor‐acceptor interactions lead to a two‐step photovoltaic process: dissociation in polaron‐pair states evolved from singlet excitonic states and exciton‐charge reactions occurred in triplet excitonic states in the generation of the photocurrent. However, strong donor‐acceptor interactions yield a one‐step photovoltaic process: direct dissociation of both singlet and triplet excitons in bulk‐heterojunction organic solar cells. In addition, the magnetic‐field effects of photocurrents indicate that the dissociated electrons and holes form charge‐transfer complexes with singlet and triplet spin configurations at donor‐acceptor intermolecular interfaces. As a result, the magnetic‐field effects of photocurrents can deliver a critical understanding of singlet and triplet photovoltaic processes to design advanced solar‐energy materials and devices.  相似文献   

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Exploring cheap and efficient cocatalysts for enhancing the performance of photocatalysts is a challenge in the energy conversion field. Herein, 2D ultrathin Ti3C2 nanosheets, a kind of MXenes, are prepared by etching Ti3AlC2 with subsequent ultrasonic exfoliation. A novel 2D/2D heterojunction of ultrathin Ti3C2/Bi2WO6 nanosheets is then successfully prepared by in situ growth of Bi2WO6 ultrathin nanosheets on the surface of these Ti3C2 ultrathin nanosheets. The resultant Ti3C2/Bi2WO6 hybrids exhibit a short charge transport distance and a large interface contact area, assuring excellent bulk‐to‐surface and interfacial charge transfer abilities. Meanwhile, the improved specific surface area and pore structure endow Ti3C2/Bi2WO6 hybrids with an enhanced CO2 adsorption capability. As a result, the 2D/2D heterojunction of ultrathin Ti3C2/Bi2WO6 nanosheets shows significant improvement on the performance of photocatalytic CO2 reduction under simulated solar irradiation. The total yield of CH4 and CH3OH obtained on the optimized Ti3C2/Bi2WO6 hybrid is 4.6 times that obtained on pristine Bi2WO6 ultrathin nanosheets. This work provides a new protocol for constructing 2D/2D photocatalytic systems and demonstrates Ti3C2 as a promising and cheap cocatalyst.  相似文献   

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Vertical organic transistors are an attractive alternative to realize short channel transistors, which are required for powerful electronic devices and flexible electronic circuits operating at high frequencies. Unfortunately, the vertical device architecture comes along with an increased device fabrication complexity, limiting the potential of this technology for application. A new design of vertical organic field‐effect transistors (VOFETs) with superior electrical performance and simplified processing is reported. By using electrochemical oxidized aluminum oxide (AlOx) as a pseudo self‐aligned charge‐blocking structure in vertical organic transistors, direct leakage current between the source and drain can be effectively suppressed, enabling VOFETs with very low off‐current levels despite the short channel length. The anodization technique is easy to apply and can be surprisingly used on both n‐type and p‐type organic semiconductor thin films with significant signs of degradation. Hence, the anodization technique enables a simplified process of high‐performance p‐type and n‐type VOFETs, paving the road toward complementary circuits made of vertical transistors.  相似文献   

17.
采用传输矩阵法和图解法对InAs/GaSb二型超晶格的能带结构参数进行了理论计算,确定量子阱宽、垒宽、垒高、响应波长等参数。针对不同的结构,采用传输矩阵法和图解法得到不同的响应波长,与实际波长相比较,分析了两种算法的优劣之处。结果表明:采用传输矩阵法计算得到的子能带位置进而推算得到的响应波长与实际波长更吻合,而图解法由于本身的局限性,对超晶格结构中能带的计算会带来一定的偏差。  相似文献   

18.
石墨烯是一种新型的碳元素二维材料。本文利用传输矩阵方法研究了由电压调制形成的三元周期序列石墨烯超晶格的透射率禁带。作为入射电子能量函数的透射率会形成多个透射禁带。电子隧穿经过石墨烯超晶格形成的透射率禁带,可以由石墨烯超晶格的周期数、电子的入射角、势垒的高度和宽度来调节。石墨烯超晶格的这些性质在设计石墨烯多通道电子滤波器等电子器件中有潜在的应用价值。  相似文献   

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Exceptionally high specific surface area, mechanical strength, electrical conductivity, and a special two‐dimensional structure make graphene a highly promising material for electromechanical actuators. Electromechanical actuators are fabricated using flexible graphene‐based paper prepared via a filtration process, and the stroke of these graphene‐based actuators is directly measured during electrochemical double‐layer charge injection. Actuation strain up to 0.064% was obtained for pristine graphene paper in response to an applied potential of –1 V in 1 M NaCl solution. Double‐layer charge injection in graphene sheets is believed to induce actuation strain through a combination of coulombic and quantum‐chemical‐based expansion. To increase electrochemical‐double‐layer capacitance and actuator performance, Fe3O4 nanoparticles were used to partially prevent graphene sheets from restacking and allow the electrolyte ions to infiltrate the resulting magnetic graphene paper more easily. The magnetic graphene paper exhibits actuation strain as large as 0.1% at –1 V applied potential, which is about 56% higher than that of the pristine graphene paper.  相似文献   

20.
采用掠入射X射线反射谱技术与原子力显微技术对属有机化合物化学气相淀积生长的AlxGa1-xN/GaN超晶格结构的表面和界面进行了精确表征。结合高分辨率X射线衍射谱与反射谱数据分析获得外延层各层厚度与AlGaN层的Al摩尔组分。掠入射x射线反射谱的显著强度振荡与原子力显微镜所观察到的台阶流动形貌表明了平整的界面和表面的存在。研究发现,低Al组分(x=0.25)且阱宽小的样品界面与表面粗糙度最小,通过原子力显微技术得到的表面粗糙度均方根偏差为0.45nm。  相似文献   

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