拓扑绝缘体光电探测器研究进展

由于拓扑绝缘体具有优异的光学和电学特性以及特殊的能带结构,使其在发展高性能的宽光谱光电探测器方面具有巨大的前景。然而由于拓扑绝缘体的发现较晚,其在光电探测器领域的研究还处于初始阶段。因而存在许多亟待解决的问题,如制备更高质量的拓扑绝缘体材料。本综述概述了拓扑绝缘体材料的发展历程,并从材料制备和材料体系的角度阐述了基于拓扑绝缘体材料的光电探测器的研究进展,并展望了拓扑绝缘体材料在光电探测器领域的发展前景。     

Minimum Thermal Conductivity in Weak Topological Insulators with Bismuth‐Based Stack Structure

Contrary to the conventional belief that the consideration for topological insulators (TIs) as potential thermoelectrics is due to their excellent electrical properties benefiting from the topological surface states, this work shows that the 3D weak TIs, formed by alternating stacks of quantum spin Hall layers and normal insulator (NI) layers, can also be decent thermoelectrics because of their focus on minimum thermal conductivity. The minimum lattice thermal conductivity is experimentally confirmed in Bi₁₄Rh₃I₉ and theoretically predicted for Bi₂TeI at room temperature. It is revealed that the topologically “trivial” NI layers play a surprisingly critical role in hindering phonon propagation. The weak bonding in the NI layers gives rise to significantly low sound velocity, and the localized low‐frequency vibrations of the NI layers cause strong acoustic–optical interactions and lattice anharmonicity. All these features are favorable for the realization of exceptionally low lattice thermal conductivity, and therefore present remarkable opportunities for developing high‐performance thermoelectrics in weak TIs.     

Antisite Defect‐Enhanced Thermoelectric Performance of Topological Crystalline Insulators

As the first experimentally established topological crystalline insulator (TCI), SnTe also exhibits superior thermoelectricity upon proper doping; yet to date, whether such doping will preserve or destroy the salient topological properties in achieving outstanding thermoelectric (TE) performance remains elusive. Using first‐principles calculations combined with Boltzmann transport theory, here the elegant role of antisite defect in optimally enhancing the thermopower of SnTe while simultaneously preserving its topological nature is uncovered. It is first shown that Sn_Te antisite defect effectively induces pronounced variations in the low‐energy density of states rather than rigidly shifting the chemical potential, resulting in a higher Seebeck coefficient and power factor. Next, it is demonstrated that in a wide temperature range, the Seebeck coefficient of antisite‐doped SnTe distinctly outperforms previously identified systems invoking extrinsic dopants. It is further confirmed that such intrinsic antisite doping preserves the nontrivial topology, which in turn favors high electrical conductivity and thermoelectricity. These central findings not only identify an effective and powerful knob in future studies of TE materials, but also help to resolve standing controversies between theory and experiment surrounding the TE performances of both TCIs and topological insulators.     

拉盖尔-高斯光束在含拓扑绝缘体周期薄膜中的传输特性

基于平面角谱扩展法和4×4矩阵传输理论,研究了拉盖尔-高斯光束(LGB)在含拓扑绝缘体(TI)周期性层状薄膜中的反射和透射特性,对线偏振的LGB入射到周期性层状薄膜中的反射场和透射场的强度分布进行了分析和详细讨论。研究结果表明,TI的拓扑磁电极化率(TMEP)和薄膜的周期个数对强度分布有很大影响,通过改变TMEP或周期个数可以操纵涡旋光的光场。所提方法不仅可以推广到其他含TI的多层介质体系,而且对进一步研究TI光子晶体中的光子能带结构和带隙具有一定的意义。     

Modulation of Spin Dynamics via Voltage Control of Spin‐Lattice Coupling in Multiferroics

Motivated by the most recent progresses in both magnonics (spin dynamics) and multiferroics fields, this work aims at magnonics manipulation by the magnetoelectric coupling effect. Here, voltage control of magnonics, particularly the surface spin waves, is achieved in La_0.7Sr_0.3MnO₃/0.7Pb(Mg_1/3Nb_2/3)O₃‐0.3PbTiO₃ multiferroic heterostructures. With the electron spin resonance method, a large 135 Oe shift of surface spin wave resonance (≈7 times greater than conventional voltage‐induced ferromagnetic resonance shift of 20 Oe) is determined. A model of the spin‐lattice coupling effect, i.e., varying exchange stiffness due to voltage‐induced anisotropic lattice changes, has been established to explain experiment results with good agreement. Additionally, an “on” and “off” spin wave state switch near the critical angle upon applying a voltage is created. The modulation of spin dynamics by spin‐lattice coupling effect provides a platform for realizing energy‐efficient, tunable magnonics devices.     

All‐Layered 2D Optoelectronics: A High‐Performance UV–vis–NIR Broadband SnSe Photodetector with Bi2Te3 Topological Insulator Electrodes

Nanoelectronics is in urgent demand of exceptional device architecture with ultrathin thickness below 10 nm and dangling‐bond‐free surface to break through current physical bottleneck and achieve new record of integration level. The advance in 2D van der Waals materials endows scientists with new accessibility. This study reports an all‐layered 2D Bi₂Te₃‐SnSe‐Bi₂Te₃ photodetector, and the broadband photoresponse of the device from ultraviolet (370 nm) to near‐infrared (808 nm) is demonstrated. In addition, the optimized responsivity reaches 5.5 A W^?1, with the corresponding eternal quantum efficiency of 1833% and detectivity of 6 × 10¹⁰ cm Hz^1/2 W^?1. These figures‐of‐merits are among the best values of the reported all‐layered 2D photodetectors, which are several orders of magnitude higher than those of the previous SnSe photodetectors. The superior device performance is attributed to the synergy of highly conductive surface state of Bi₂Te₃ topological insulator, perfect band alignment between Bi₂Te₃ and SnSe as well as small interface potential fluctuation. Meanwhile, the all‐layered 2D device is further constructed onto flexible mica substrate and its photoresponse is maintained roughly unchanged upon 60 bending cycles. The findings represent a fundamental scenario for advancement of the next generation high performance and high integration level flexible optoelectronics.     

Ultrasensitive Room‐Temperature Terahertz Direct Detection Based on a Bismuth Selenide Topological Insulator

Despite their huge application capabilities, millimeter‐ and terahertz‐wave photodetectors still face challenges in the detection scheme. Topological insulators (TIs) are predicted to be promising candidates for long‐wavelength photodetection, due to the presence of Dirac fermions in their topologically protected surface states. However, photodetection based on TIs is usually hindered by the large dark current, originating from the mixing of bulk states with topological surface states (TSSs) in most realistic samples of TIs. Here millimeter and terahertz detectors based on a subwavelength metal–TI–metal (MTM) heterostructure are demonstrated. The achieved photoresponse stems from the asymmetric scattering of TSS, driven by the localized surface plasmon‐induced terahertz field, which ultimately produces direct photocarriers beyond the interband limit. The device enables high responsivity in both the self‐powered and bias modes even at room temperature. The achieved responsivity is over 75 A/W, with response time shorter than 60 ms in the self‐powered mode. Remarkably, the responsivity increases by several orders of magnitude in the biased configuration, with the noise‐equivalent power (NEP) of 3.6 × 10^?13 W Hz^?1/2 and a detectivity of 2.17 × 10¹¹ cm Hz^?1/2 W^?1 at room temperature. The detection performances open a way toward realistic exploitation of TIs for large‐area, real‐time imaging within long‐wavelength optoelectronics.     

Measuring Domain Sizes and Compositional Heterogeneities in P3HT‐PCBM Bulk Heterojunction Thin Films with 1H Spin Diffusion NMR Spectroscopy

The application of ¹H spin diffusion nuclear magnetic resonance (NMR) is expanded to polymer‐fullerene blends for bulk heterojunction (BHJ) organic photovoltaics (OPV) by developing a new experimental methodology for measuring the thin films used in poly‐3‐hexylthiophene–phenyl C61‐butyric acid methyl ester (P3HT‐PCBM) OPV devices and by creating an analysis framework for estimating domain size distributions. It is shown that variations in common P3HT‐PCBM BHJ processing parameters such as spin‐coating speed and thermal annealing can significantly affect domain size distributions, which in turn affect power conversion efficiency. ¹H spin diffusion NMR analysis reveals that films spin‐cast at fast speeds in dichlorobenzene are primarily composed of small (<10 nm) domains of each component; these devices exhibit low power conversion efficiencies (η = 0.4%). Fast‐cast films improve substantially by thermal annealing, which causes nanometer‐scale coarsening leading to higher efficiency (η = 2.2%). Films spin‐cast at slow speeds and then slowly dried exhibit larger domains and even higher efficiencies (η = 2.6%), but do not benefit from thermal annealing. The ¹H spin diffusion NMR results show that a significant population of domains tens of nanometers in size is a common characteristic of samples with higher efficiencies.     

Concepts of Spin Seebeck Effect in Ferromagnetic Metals

Spin Seebeck effect (SSE) and related spin caloritronics have attracted great interest recently. However, the definition of the SSE coefficient remains to be established, let alone a clean experiment to measure the SSE coefficient in ferromagnetic metals. The concept through a model based on the semi‐classical Botlzmann transport equation has been clarified. The model includes the vital spin‐flip process, which is frequent in metals, and points out that the length scale of SSE is much larger than the spin diffusion length. The model reveals how the spin‐flip process influences the transport equations and provides the simple relationship between the different spin‐flip relaxation times for spin‐up and ‐down electrons, which is very useful to understand the spin transport properties. This understanding allows to redefine the expression of the spin Seebeck coefficient.     

Transforming Common III–V and II–VI Semiconductor Compounds into Topological Heterostructures: The Case of CdTe/InSb Superlattices

Currently, known topological insulators (TIs) are limited to narrow gap compounds incorporating heavy elements, thus severely limiting the material pool available for such applications. It is shown via first‐principle calculations that a heterovalent superlattice made of common semiconductor building blocks can transform its non‐TI components into a topological nanostructure, illustrated by III–V/II–VI superlattice InSb/CdTe. The heterovalent nature of such interfaces sets up, in the absence of interfacial atomic exchange, a natural internal electric field that along with the quantum confinement leads to band inversion, transforming these semiconductors into a topological phase while also forming a giant Rashba spin splitting. The relationship between the interfacial stability and the topological transition is revealed, finding a “window of opportunity” where both conditions can be optimized. Once a critical InSb layer thickness above ≈1.5 nm is reached, both [111] and [100] superlattices have a relative energy of 1.7–9.5 meV Å^–2, higher than that of the atomically exchanged interface and an excitation gap up to ≈150 meV, affording room‐temperature quantum spin Hall effect in semiconductor superlattices. The understanding gained from this study could broaden the current, rather restricted repertoire of functionalities available from individual compounds by creating next‐generation superstructured functional materials.     

Structure Inversion Asymmetry and Rashba Effect in Quantum Confined Topological Crystalline Insulator Heterostructures

Structure inversion asymmetry is an inherent feature of quantum confined heterostructures with non-equivalent interfaces. It leads to a spin splitting of the electron states and strongly affects the electronic band structure. The effect is particularly large in topological insulators because the topological surface states are extremely sensitive to the interfaces. Here, the first experimental observation and theoretical explication of this effect are reported for topological crystalline insulator quantum wells made of Pb_1−xSn_xSe confined by Pb_1−yEu_ySe barriers on one side and by vacuum on the other. This provides a well defined structure asymmetry controlled by the surface condition. The electronic structure is mapped out by angle-resolved photoemission spectroscopy and tight binding calculations, evidencing that the spin splitting decisively depends on hybridization and, thus, quantum well width. Most importantly, the topological boundary states are not only split in energy but also separated in space—unlike conventional Rashba bands that are splitted only in momentum. The splitting can be strongly enhanced to very large values by control of the surface termination due to the charge imbalance at the polar quantum well surface. The findings thus, open up a wide parameter space for tuning of such systems for device applications.     

Large Area Artificial Spin Ice and Anti‐Spin Ice Ni80Fe20 Structures: Static and Dynamic Behavior

Artificial spin ice has been the subject of extensive investigation in the last few years due to advances in nanotechnology and characterization techniques. So far, most of the studies have been limited to local probe of small area magnetic elements due to limitations with lithographic techniques used. In this study, large area spin ice and anti‐spin ice Ni₈₀Fe₂₀ structures with three lattice configurations have been fabricated using deep ultraviolet lithography at 193 nm exposure wavelength. The static and dynamic properties are systematically characterized using vibrating sample magnetometer, magnetic force microscopy, and broadband ferromagnetic resonance spectroscopy. Intriguing static and dynamic behaviors are observed due to the geometrical arrangement of the nanomagnets in the lattice. When the nanomagnets are saturated at high field, multiple resonance peaks whose frequencies are strongly dependent on the orientation of the applied magnetic field are observed. The experimental results are in qualitative agreement with the micromagnetic simulations. These findings may find application in the design of magnetically controlled tunable microwave filters.     

Realization of a New Topological Crystalline Insulator and Lifshitz Transition in PbTe

Topological materials boast exotic metallic surface states with linear dispersion and spin‐momentum locking, which makes them potential candidates for dissipationless electronic and spintronic devices. Here, it is theoretically predicted that intrinsic Te antisite defects (Te_Pb) in the narrow‐gap semiconductor PbTe induce a band inversion, turning it into a topological crystalline insulator (TCI). To experimentally verify the exotic properties, Te_Pb antisites are introduced into PbTe crystals via nonstoichiometric growth by molecular beam epitaxy. Semimetallic resistivity and distinct quantum oscillations are observed on the Te_Pb doped PbTe. Most importantly, a π Berry phase is unambiguously revealed by a Landau index analysis, demonstrating the Dirac fermion nature of the topological surface states. The discovered TCI nature in Te_Pb doped PbTe is further explored using magneto‐transport measurements under external pressure, and the theoretical calculations of band structures with applying pressure indicate a pressure‐induced Lifshitz transition. Besides, it is proposed that the contribution of bulk states to transport can be reduced by enlarging the inverted gap with strain.     

Studies of Functional Defects for Fast Na‐Ion Conduction in Na3−yPS4−xClx with a Combined Experimental and Computational Approach

All‐solid‐state rechargeable sodium (Na)‐ion batteries are promising for inexpensive and high‐energy‐density large‐scale energy storage. In this contribution, new Na solid electrolytes, Na_3?yPS_4?xCl_x, are synthesized with a strategic approach, which allows maximum substitution of Cl for S (x = 0.2) without significant compromise of structural integrity or Na deficiency. A maximum conductivity of 1.96 mS cm^?1 at 25 °C is achieved for Na_3.0PS_3.8Cl_0.2, which is two orders of magnitude higher compared with that of tetragonal Na₃PS₄ (t‐Na₃PS₄). The activation energy (E_a) is determined to be 0.19 eV. Ab initio molecular dynamics simulations shed light on the merit of maximizing Cl‐doping while maintaining low Na deficiency in enhanced Na‐ion conduction. Solid‐state nuclear magnetic resonance (NMR) characterizations confirm the successful substitution of Cl for S and the resulting change of P oxidation state from 5+ to 4+, which is also verified by spin moment analysis. Ion transport pathways are determined with a tracer‐exchange NMR method. The functional detects that promote Na ‐ion transport are maximized for further improvement in ionic conductivity. Full‐cell performance is demonstrated using Na/Na_3.0PS_3.8Cl_0.2/Na₃V₂(PO₄)₃ with a reversible capacity of ≈100 mAh g^‐1 at room temperature.     

Electric‐Field‐Controlled Alignment of Rod‐Shaped Fluorescent Nanocrystals in Smectic Liquid Crystal Defect Arrays

Periodic micro‐arrays of straight linear defects containing nanoparticles can be created over large surface areas at the transition from the nematic to smectic‐A phase in a nanoparticle–liquid crystal (LC) composite material confined under the effect of conflicting anchoring conditions (unidirectional planar vs normal) and electric fields. Anisomeric dichroic dye molecules and rod‐shaped fluorescent semiconductor nanocrystals (dot‐in‐rods) with large permanent electric dipole and high linearly polarized photoluminescence quantum yield align parallel to the local LC molecular director and follow its reorientation under application of the electric field. In the nano‐sized core regions of linear defects, where the director is undefined, anisotropic particles align parallel to the defect whereas spherical quantum dots do not show any particular interaction with the defect. Under application of an electric field, ferroelectric semiconductor nanoparticles in the core region align along the field, perpendicular to the defect direction, whereas dichroic dyes remain parallel to the defect. This study provides useful insights into the complex interaction of anisotropic nanoparticles and anisotropic soft materials such as LCs in the presence of external fields, which may help the development of field‐responsive nanoparticle‐based functional materials.     

Plasmon‐Enhanced Photodetection in Ferromagnet/Nonmagnet Spin Thermoelectric Structures

The photothermoelectric (PTE) effect that originates from the temperature difference within thermoelectric materials induced by light absorption can be used as the mechanism for a light sensor in optoelectronic applications. In this work, a PTE‐based photodetector is reported using a spin thermoelectric structure consisting of CoFeB/Pt metallic bilayers and its signal enhancement achieved by incorporating a plasmonic structure consisting of Au nanorod arrays. The thermoelectric voltage of the bilayers markedly increases by 60 ± 10% when the plasmon resonance condition of the Au nanorods is matched to the wavelength of the incident laser. Full‐wave electromagnetic simulations reveal that the signal enhancement is due to the increase in light absorption and consequential local heating. Moreover, the alignment of the Au nanorods makes the thermoelectric voltages sensitive to the polarization state of the laser, thereby enabling the detection of light polarization. These results demonstrate the feasibility of a hybrid device utilizing plasmonic and spin‐thermoelectric effects as an efficient PTE‐based photodetector.     

Magnetically Enhanced Mechanical Stability and Super‐Size Effects in Self‐Assembled Superstructures of Nanocubes

Artificial materials from the self‐assembly of magnetic nanoparticles exhibit extraordinary collective properties; however, to date, the contribution of nanoscale magnetism to the mechanical properties of this class of materials is overlooked. Here, through a combination of Monte Carlo simulations and experimental magnetic measurements, this contribution is shown to be important in self‐assembled superstructures of magnetite nanocubes. By simulating the relaxation of interacting macrospins in the superstructure systems, the relationship between nanoscale magnetism, nanoparticle arrangement, superstructure size, and mechanical stability is established. For all considered systems, a significant enhancement in cohesive energy per nanocube (up to 45%), and thus in mechanical stability, is uncovered from the consideration of magnetism. Magnetic measurements fully support the simulations and confirm the strongly interacting character of the nanocube assembly. The studies also reveal a novel super‐size effect, whereby mechanically destabilization occurs through a decrease in cohesive energy per nanocube as the overall size (number of particles) of the system decreases. The discovery of this effect opens up new possibilities in size‐controlled tuning of superstructure properties, thus contributing to the design of next‐generation self‐assembled materials with simultaneous enhancement of magnetic and mechanical properties.