Yichao Zou

Arrayed van der Waals Vertical Heterostructures Based on 2D GaSe Grown by Molecular Beam Epitaxy

Vertically stacking two-dimensional (2D) materials can enable the design of novel electronic and optoelectronic devices and realize complex functionality. However, the fabrication of such artificial heterostructures on a wafer scale with an atomically sharp interface poses an unprecedented challenge. Here, we demonstrate a convenient and controllable approach for the production of wafer-scale 2D GaSe thin films by molecular beam epitaxy. In situ reflection high-energy electron diffraction oscillations and Raman spectroscopy reveal a layer-by-layer van der Waals epitaxial growth mode. Highly efficient photodetector arrays were fabricated, based on few-layer GaSe on Si. These photodiodes show steady rectifying characteristics and a high external quantum efficiency of 23.6%. The resultant photoresponse is super-fast and robust, with a response time of 60 μs. Importantly, the device shows no sign of degradation after 1 million cycles of operation. We also carried out numerical simulations to understand the underlying device working principles. Our study establishes a new approach to produce controllable, robust, and large-area 2D heterostructures and presents a crucial step for further practical applications.

Wafer-scale arrayed p-n junctions based on few-layer epitaxial GaTe

Two-dimensional (2D) materials have attracted substantial attention in electronic and optoelectronic applications with the superior advantages of being flexible, transparent, and highly tunable. Gapless graphene exhibits ultra-broadband and fast photoresponse while the 2D semiconducting MoS2 and GaTe exhibit high sensitivity and tunable responsivity to visible light. However, the device yield and repeatability call for further improvement to achieve large-scale uniformity. Here, we report a layer-by-layer growth of wafer-scale GaTe with a high hole mobility of 28.4 cm2/(V·s) by molecular beam epitaxy. The arrayed p-n junctions were developed by growing few-layer GaTe directly on three-inch Si wafers. The resultant diodes reveal good rectifying characteristics and a high photovoltaic external quantum efficiency up to 62% at 4.8 µW under zero bias. The photocurrent reaches saturation fast enough to capture a time constant of 22 µs and shows no sign of device degradation after 1.37 million cycles of operation. Most strikingly, such high performance has been achieved across the entire wafer, making the volume production of devices accessible. Finally, several photoimages were acquired by the GaTe/Si photodiodes with reasonable contrast and spatial resolution, demonstrating the potential of integrating the 2D materials with silicon technology for novel optoelectronic devices.

Realizing zT of 2.3 in Ge1−x−ySbxInyTe via Reducing the Phase‐Transition Temperature and Introducing Resonant Energy Doping

GeTe with rhombohedral-to-cubic phase transition is a promising lead-free thermoelectric candidate. Herein, theoretical studies reveal that cubic GeTe has superior thermoelectric behavior, which is linked to (1) the two valence bands to enhance the electronic transport coefficients and (2) stronger enharmonic phonon-phonon interactions to ensure a lower intrinsic thermal conductivity. Experimentally, based on Ge1-x Sbx Te with optimized carrier concentration, a record-high figure-of-merit of 2.3 is achieved via further doping with In, which induces the distortion of the density of states near the Fermi level. Moreover, Sb and In codoping reduces the phase-transition temperature to extend the better thermoelectric behavior of cubic GeTe to low temperature. Additionally, electronic microscopy characterization demonstrates grain boundaries, a high-density of stacking faults, and nanoscale precipitates, which together with the inevitable point defects result in a dramatically decreased thermal conductivity. The fundamental investigation and experimental demonstration provide an important direction for the development of high-performance Pb-free thermoelectric materials.

Scalable Growth of High Mobility Dirac Semimetal Cd3As2 Microbelts.

Three-dimensional (3D) Dirac semimetals are 3D analogues of graphene, which display Dirac points with linear dispersion in k-space, stabilized by crystal symmetry. Cd3As2 has been predicted to be 3D Dirac semimetals and was subsequently demonstrated by angle-resolved photoemission spectroscopy. As unveiled by transport measurements, several exotic phases, such as Weyl semimetals, topological insulators, and topological superconductors, can be deduced by breaking time reversal or inversion symmetry. Here, we reported a facile and scalable chemical vapor deposition method to fabricate high-quality Dirac semimetal Cd3As2 microbelts; they have shown ultrahigh mobility up to 1.15 × 10(5) cm(2) V(-1) s(-1) and pronounced Shubnikov-de Haas oscillations. Such extraordinary features are attributed to the suppression of electron backscattering. This research opens a new avenue for the scalable fabrication of Cd3As2 materials toward exciting electronic applications of 3D Dirac semimetals.

In3Se4 and S-doped In3Se4 nano/micro-structures as new anode materials for Li-ion batteries

In3Se4 and S-doped In3Se4 nano/micro-structures consisting of thin nanosheets have been developed as new anode materials for Li-ion batteries. Electrochemical performance measurement shows that In3Se4 nano/micro-structures deliver high discharge capacity (e.g. 651.0 mA h g−1 obtained in the 30th cycle at a current density of 50 mA g−1). Through detailed transmission electron microscopy analysis, it has been found that the electrochemical reaction mechanism is the conversion between In3Se4 and Li13In3 + LixSe. Moreover, S doping is demonstrated to be an effective approach to further improve the electrochemical performance of In3Se4 nano/micro-structures. S-doped In3Se4 nano/micro-structures achieve enhanced discharge capacity and cycling stability, with a discharge capacity of 850.6 mA h g−1 in the 30th cycle. This study demonstrates the potential of In3Se4-based nano/micro-structures as anode materials for rechargeable Li-ion batteries.

Planar Vacancies in Sn1–xBixTe Nanoribbons

Vacancy engineering is a crucial approach to manipulate physical properties of semiconductors. Here, we demonstrate that planar vacancies are formed in Sn1-xBixTe nanoribbons by using Bi dopants via a facile chemical vapor deposition. Through combination of sub-angstrom-resolution imaging and density functional theory calculations, these planar vacancies are found to be associated with Bi segregations, which significantly lower their formation energies. The planar vacancies exhibit polymorphic structures with local variations in the lattice relaxation level, determined by their proximity to the nanoribbon surface. Such polymorphic planar vacancies, in conjunction with Bi dopants, trigger distinct localized electronic states, offering platforms for device applications of ternary chalcogenide materials.

Wafer-scale two-dimensional ferromagnetic Fe 3 GeTe 2 thin films grown by molecular beam epitaxy

Recently, layered two-dimensional ferromagnetic materials (2D FMs) have attracted a great deal of interest for developing low-dimensional magnetic and spintronic devices. Mechanically exfoliated 2D FMs were discovered to possess ferromagnetism down to monolayer. It is therefore of great importance to investigate the distinct magnetic properties at low dimensionality. Here, we report the wafer-scale growth of 2D ferromagnetic thin films of Fe3GeTe2 via molecular beam epitaxy, and their exotic magnetic properties can be manipulated via the Fe composition and the interface coupling with antiferromagnetic MnTe. A 2D layer-by-layer growth mode has been achieved by in situ reflection high-energy electron diffraction oscillations, yielding a well-defined interlayer distance of 0.82 nm along {002} surface. The magnetic easy axis is oriented along c-axis with a Curie temperature of 216.4 K. Remarkably, the Curie temperature can be enhanced when raising the Fe composition. Upon coupling with MnTe, the coercive field dramatically increases 50% from 0.65 to 0.94 Tesla. The large-scale layer-by-layer growth and controllable magnetic properties make Fe3GeTe2 a promising candidate for spintronic applications. It also opens up unprecedented opportunities to explore rich physics when coupled with other 2D superconductors and topological matters.2D synthesis: molecular beam epitaxy enables growth of ferromagnetic Fe 3 GeTe 2Molecular beam epitaxy enables wafer-scale growth of Fe3GeTe2, an atomically thin ferromagnetic compound. A team led by Faxian Xiu at Fudan University demonstrated layer-by-layer growth of large-area, 8 nm-thick films of Fe3GeTe2 on sapphire and GaAs substrates in a high-vacuum molecular beam epitaxy system. The measured Curie temperature of 216.4 K was found to vary systematically with the Fe composition, indicating that Fe doping is a viable route to achieving tailored ferromagnetic ternary compounds with tunable Curie temperature. Furthermore, upon coupling Fe3GeTe2 with antiferromagnetic MnTe, the magnetic properties of the former could be enhanced owing to the exchange interaction from the ferromagnetic/antiferromagnetic superlattice interface. As a result, the coercive field increased by 50% with respect to bare Fe3GeTe2. These results highlight that Fe3GeTe2 and its heterostructures are promising candidates for spintronic devices.

Long wavelength emissions of Se4+-doped In2O 3 hierarchical nanostructures

Se4+-doped cubic-structured In2O3 hierarchical nanostructures have been synthesized by controllable thermal oxidation of In3Se4 nanostructures. The synthesized nanostructures preserve the original hierarchical morphology of In3Se4 nanosheet-assembled nanostructures. Moreover, the In3Se4 single crystalline nanosheets can be transformed into Se4+-doped In2O3 polycrystalline structures consisting of interconnected nanoparticles. The photoluminescence property measurements show that the Se4+-doped In2O3 hierarchical nanostructures have red light emissions centered at 630, 670, and 770 nm and near infrared emissions centered at 910 nm, which is ascribed to the Se4+ doping.

Atomic disorders in layer structured topological insulator SnBi2Te4 nanoplates

Identification of atomic disorders and their subsequent control has proven to be a key issue in predicting, understanding, and enhancing the properties of newly emerging topological insulator materials. Here, we demonstrate direct evidence of the cation antisites in single-crystal SnBi2Te4 nanoplates grown by chemical vapor deposition, through a combination of sub-ångström-resolution imaging, quantitative image simulations, and density functional theory calculations. The results of these combined techniques revealed a recognizable amount of cation antisites between Bi and Sn, and energetic calculations revealed that such cation antisites have a low formation energy. The impact of the cation antisites was also investigated by electronic structure calculations together with transport measurement. The topological surface properties of the nanoplates were further probed by angle-dependent magnetotransport, and from the results, we observed a two-dimensional weak antilocalization effect associated with surface carriers. Our approach provides a pathway to identify the antisite defects in ternary chalcogenides and the application potential of SnBi2Te4 nanostructures in next-generation electronic and spintronic devices.

Author correction: Wafer-scale two-dimensional ferromagnetic Fe 3 GeTe 2 thin films grown by molecular beam epitaxy

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