Selective binding and periodic arrangement of magic boron clusters on monolayer borophene.

The synthesis and characterization of small boron clusters with unique size and regular arrangement are crucial for boron chemistry and two-dimensional borophene materials. In this study, together with theoretical calculations, the joint molecular beam epitaxy and scanning tunneling microscopy experiments achieve the formation of unique B5 clusters on monolayer borophene (MLB) on a Cu(111) surface. The B5 clusters tend to selectively bind to specific sites of MLB with covalent boron-boron bonds in the periodic arrangement, which can be ascribed to the charge distribution and electron delocalization character of MLB and also prohibits nearby co-adsorption of B5 clusters. Furthermore, the close-packed adsorption of B5 clusters would facilitate the synthesis of bilayer borophene, exhibiting domino effect-like growth mode. The successful growth and characterization of uniform boron clusters on a surface enrich the boron-based nanomaterials and reveal the essential role of small clusters during the growth of borophene.

Unveiling the Anomalous Hall Response of the Magnetic Structure Changes in the Epitaxial MnBi2Te4 Films.

Recently discovered as an intrinsic antiferromagnetic topological insulator, MnBi2Te4 has attracted tremendous research interest, as it provides an ideal platform to explore the interplay between topological and magnetic orders. MnBi2Te4 displays distinct exotic topological phases that are inextricably linked to the different magnetic structures of the material. In this study, we conducted electrical transport measurements and systematically investigated the anomalous Hall response of epitaxial MnBi2Te4 films when subjected to an external magnetic field sweep, revealing the different magnetic structures stemming from the interplay of applied fields and the material's intrinsic antiferromagnetic (AFM) ordering. Our results demonstrate that the nonsquare anomalous Hall loop is a consequence of the distinct reversal processes within individual septuple layers. These findings shed light on the intricate magnetic structures in MnBi2Te4 and related materials, offering insights into understanding their transport properties and facilitating the implementation of AFM topological electronics.

Engineering Plateau Phase Transition in Quantum Anomalous Hall Multilayers.

The plateau phase transition in quantum anomalous Hall (QAH) insulators corresponds to a quantum state wherein a single magnetic domain gives way to multiple domains and then reconverges back to a single magnetic domain. The layer structure of the sample provides an external knob for adjusting the Chern number C of the QAH insulators. Here, we employ molecular beam epitaxy to grow magnetic topological insulator multilayers and realize the magnetic field-driven plateau phase transition between two QAH states with odd Chern number change ΔC. We find that critical exponents extracted for the plateau phase transitions with ΔC = 1 and ΔC = 3 in QAH insulators are nearly identical. We construct a four-layer Chalker-Coddington network model to understand the consistent critical exponents for the plateau phase transitions with ΔC = 1 and ΔC = 3. This work will motivate further investigations into the critical behaviors of plateau phase transitions with different ΔC in QAH insulators.

High-Mobility Carriers in Epitaxial IrO2 Films Grown using Hybrid Molecular Beam Epitaxy.

Binary rutile oxides of 5d metals such as IrO2 stand out in comparison to their 3d and 4d counterparts due to limited experimental studies, despite rich predicted quantum phenomena. Here, we investigate the electrical transport properties of IrO2 by engineering epitaxial thin films grown using hybrid molecular beam epitaxy. Our findings reveal phonon-limited carrier transport and thickness-dependent anisotropic in-plane resistance in IrO2 (110) films, the latter suggesting a complex relationship between strain relaxation and orbital hybridization. Magnetotransport measurements reveal a previously unobserved nonlinear Hall effect. A two-carrier analysis of this effect shows the presence of minority carriers with mobility exceeding 3000 cm2/(V s) at 1.8 K. These results point toward emergent properties in 5d metal oxides that can be controlled using dimensionality and epitaxial strain.

Excited State Band Mapping and Ultrafast Nonequilibrium Dynamics in Topological Dirac Semimetal 1T-ZrTe2.

We performed time- and polarization-resolved extreme ultraviolet momentum microscopy on the topological Dirac semimetal candidate 1T-ZrTe2. Excited state band mapping uncovers the previously inaccessible linear dispersion of the Dirac cone above the Fermi level. We study the orbital texture of bands using linear dichroism in photoelectron angular distributions. These observations provide hints about the topological character of 1T-ZrTe2. Time-, energy-, and momentum-resolved nonequilibrium carrier dynamics reveal that intra- and interband scattering processes play a major role in the relaxation mechanism, leading to multivalley electron-hole accumulation near the Fermi level. We also show that electrons' inverse lifetime has a linear dependence as a function of their excess energy. Our time- and polarization-resolved XUV photoemission results shed light on the excited state electronic structure of 1T-ZrTe2 and provide valuable insights into the relatively unexplored field of quantum-state-resolved ultrafast dynamics in 3D topological Dirac semimetals.

Spin-Orbit Torques and Magnetization Switching in (Bi,Sb)2Te3/Fe3GeTe2 Heterostructures Grown by Molecular Beam Epitaxy.

Topological insulators (TIs) hold promise for manipulating the magnetization of a ferromagnet (FM) through the spin-orbit torque (SOT) mechanism. However, integrating TIs with conventional FMs often leads to significant device-to-device variations and a broad distribution of SOT magnitudes. In this work, we present a scalable approach to grow a full van der Waals FM/TI heterostructure by molecular beam epitaxy, combining the charge-compensated TI (Bi,Sb)2Te3 with 2D FM Fe3GeTe2 (FGT). Harmonic magnetotransport measurements reveal that the SOT efficiency exhibits a non-monotonic temperature dependence and experiences a substantial enhancement with a reduction of the FGT thickness to 2 monolayers. Our study further demonstrates that the magnetization of ultrathin FGT films can be switched with a current density of Jc ∼ 1010 A/m2, with minimal device-to-device variations compared to previous investigations involving traditional FMs.

Strain Solitons in an Epitaxially Strained van der Waals-like Material.

Strain solitons are quasi-dislocations that form in van der Waals materials to relieve the energy associated with lattice or rotational mismatch. Novel electronic properties of strain solitons were predicted and observed. To date, strain solitons have been observed only in exfoliated crystals or mechanically strained crystals. The lack of a scalable approach toward the generation of strain solitons poses a significant challenge in the study of and use of their properties. Here, we report the formation of strain solitons with epitaxial growth of bismuth on InSb(111)B by molecular beam epitaxy. The morphology of the strain solitons for films of varying thickness is characterized with scanning tunneling microscopy, and the local strain state is determined from atomic resolution images. Bending in the solitons is attributed to interactions with the interface, and large angle bending is associated with edge dislocations. Our results enable the scalable generation of strain solitons.

Controlling the Charge Density Wave Transition in Single-Layer TiTe2xSe2(1-x) Alloys by Band Gap Engineering.

Closing the band gap of a semiconductor into a semimetallic state gives a powerful potential route to tune the electronic energy gains that drive collective phases like charge density waves (CDWs) and excitonic insulator states. We explore this approach for the controversial CDW material monolayer (ML) TiSe2 by engineering its narrow band gap to the semimetallic limit of ML-TiTe2. Using molecular beam epitaxy, we demonstrate the growth of ML-TiTe2xSe2(1-x) alloys across the entire compositional range and unveil how the (2 × 2) CDW instability evolves through the normal state semiconductor-semimetal transition via in situ angle-resolved photoemission spectroscopy. Through model electronic structure calculations, we identify how this tunes the relative strength of excitonic and Peierls-like coupling, demonstrating band gap engineering as a powerful method for controlling the microscopic mechanisms underpinning the formation of collective states in two-dimensional materials.

Spectrally Pure, High Operational Dynamic Range, Deep Red Micro-LEDs.

III-nitride-based micro-light-emitting diodes (micro-LEDs) are currently under rapid development for next-generation high-resolution and high-brightness displays and augmented/virtual reality (AR/VR) technologies. However, it remains elusive to achieve red-emitting III-nitride micro-LEDs with a microscale size, high efficiency, and high spectral stability, posing significant impediments to the development of full-color micro-LEDs. In this work, through detailed strain engineering and control of charge carrier transport, we achieved pure red emission (≥620 nm) micro-LEDs over 2 orders of magnitude of injection current variation. We show both theoretically and experimentally that the combination of a short-period InGaN/GaN superlattice and a thick n-type GaN interlayer can not only relieve the quantum-confined Stark effect in the active region but also suppress parasitic emission from the superlattice. The optimized deep red micro-LEDs with a device lateral dimension of ∼1 µm feature a maximal external quantum efficiency of over 3% emitting at ∼660 nm.

Coexistence of Superconductivity and Antiferromagnetism in Topological Magnet MnBi2Te4 Films.

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.

Offcut Substrate-Induced Defect Trapping at Step Edges.

We report step edge-induced localized defects suppressing subsequent antiphase boundary formation in the bulk structure of a trilayer oxide heterostructure. The heterostructure encompasses a layer of La0.66Sr0.34MnO3 sandwiched between a superconducting La1.84Sr0.16CuO4 bottom layer and an insulating La2CuO4 top layer. The combination of a minor a-axis mismatch (0.11 Å) and a pronounced c-axis mismatch (2.73 Å) at the step edges leads to the emergence of localized defects exclusively forming at the step edge. Employing atomically resolved electron energy-loss spectroscopy maps, we discern the electronic state of those structures in the second La0.66Sr0.34MnO3 unit cell near the step edge. In particular, a reduction in the pre-edge region of the O-K edge indicates the formation of oxygen vacancies induced by the strained step edge. This study underscores our capability to control defects at the nanoscale.

Wafer-Scale Two-Dimensional Semiconductors for Deep UV Sensing.

2D semiconductors (2SEM) can transform many sectors, from information and communication technology to healthcare. To date, top-down approaches to their fabrication, such as exfoliation of bulk crystals by "scotch-tape," are widely used, but have limited prospects for precise engineering of functionalities and scalability. Here, a bottom-up technique based on epitaxy is used to demonstrate high-quality, wafer-scale 2SEM based on the wide band gap gallium selenide (GaSe) compound. GaSe layers of well-defined thickness are developed using a bespoke facility for the epitaxial growth and in situ studies of 2SEM. The dominant centrosymmetry and stacking of the individual van der Waals layers are verified by theory and experiment; their optical anisotropy and resonant absorption in the UV spectrum are exploited for photon sensing in the technological UV-C spectral range, offering a scalable route to deep-UV optoelectronics.

Growth of Single Crystalline 2D Materials beyond Graphene on Non-metallic Substrates.

The advent of 2D materials has ushered in the exploration of their synthesis, characterization and application. While plenty of 2D materials have been synthesized on various metallic substrates, interfacial interaction significantly affects their intrinsic electronic properties. Additionally, the complex transfer process presents further challenges. In this context, experimental efforts are devoted to the direct growth on technologically important semiconductor/insulator substrates. This review aims to uncover the effects of substrate on the growth of 2D materials. The focus is on non-metallic substrate used for epitaxial growth and how this highlights the necessity for phase engineering and advanced characterization at atomic scale. Special attention is paid to monoelemental 2D structures with topological properties. The conclusion is drawn through a discussion of the requirements for integrating 2D materials with current semiconductor-based technology and the unique properties of heterostructures based on 2D materials. Overall, this review describes how 2D materials can be fabricated directly on non-metallic substrates and the exploration of growth mechanism at atomic scale.

Novel Polytype of III-VI Metal Chalcogenides Nano Crystals Realized in Epitaxially Grown InTe.

III-VI metal chalcogenides have garnered considerable research attention as a novel group of layered van der Waals materials because of their exceptional physical properties and potential technological applications. Here, the epitaxial growth and stacking sequences of InTe is reported, an essential and intriguing material from III-VI metal chalcogenides. Aberration-corrected scanning transmission electron microscopy (STEM) is utilized to directly reveal the interlayer stacking modes and atomic structure, leading to a discussion of a new polytype. Furthermore, correlations between the stacking sequences and interlayer distances are substantiated by atomic-resolution STEM analysis, which offers evidence for strong interlayer coupling of the new polytype. It is proposed that layer-by-layer deposition is responsible for the formation of the unconventional stacking order, which is supported by ab initio density functional theory calculations. The results thus establish molecular beam epitaxy as a viable approach for synthesizing novel polytypes. The experimental validation of the InTe polytype here expands the family of materials in the III-VI metal chalcogenides while suggesting the possibility of new stacking sequences for known materials in this system.

Selective area epitaxy of in-plane HgTe nanostructures on CdTe(001) substrate.

Semiconductor nanowires (NWs) are believed to play a crucial role for future applications in electronics, spintronics and quantum technologies. A potential candidate is HgTe but its sensitivity to nanofabrication processes restrain its development. A way to circumvent this obstacle is the selective area growth technique. Here, in-plane HgTe nanostructures are grown thanks to selective area molecular beam epitaxy on a semi-insulating CdTe substrate covered with a patterned SiO2mask. The shape of these nanostructures is defined by the in-plane orientation of the mask aperture along the <110>, <11¯0>, or <100> direction, the deposited thickness, and the growth temperature (GT). Several micron long in-plane NWs can be achieved as well as more complex nanostructures such as networks, diamond structures or rings. A good selectivity is achieved with very little parasitic growth on the mask even for a GT as low as 140 °C and growth rate up to 0.5 monolayer per second. For <110> oriented NWs, the center of the nanostructure exhibits a trapezoidal shape with {111}B facets and two grains on the sides, while <11¯0> oriented NWs show {111}A facets with adatoms accumulation on the sides of the top surface. Transmission electron microscopy observations reveal a continuous epitaxial relation between the CdTe substrate and the HgTe NW. Measurements of the resistance with four-point scanning tunneling microscopy indicates a good electrical homogeneity along the main NW axis and a thermally activated transport. This growth method paves the way toward the fabrication of complex HgTe-based nanostructures for electronic transport measurements.

Optical properties of two-dimensional tin nanosheets epitaxially grown on graphene.

Heterostacks formed by combining two-dimensional materials show novel properties which are of great interest for new applications in electronics, photonics and even twistronics, the new emerging field born after the outstanding discoveries on twisted graphene. Here, we report the direct growth of tin nanosheets at the two-dimensional limit via molecular beam epitaxy on chemical vapor deposited graphene on Al2O3(0001). The mutual interaction between the tin nanosheets and graphene is evidenced by structural and chemical investigations. On the one hand, Raman spectroscopy indicates that graphene undergoes compressive strain after the tin growth, while no charge transfer is observed. On the other hand, chemical analysis shows that tin nanosheets interaction with sapphire is mediated by graphene avoiding the tin oxidation occurring in the direct growth on this substrate. Remarkably, optical measurements show that the absorption of tin nanosheets exhibits a graphene-like behavior with a strong absorption in the ultraviolet photon energy range, therein resulting in a different optical response compared to tin nanosheets on bare sapphire. The optical properties of ultra-thin tin films therefore represent an open and flexible playground for the absorption of light in a broad range of the electromagnetic spectrum and technologically relevant applications for photon harvesting and sensors.

Transition from fractal-dendritic to compact islands for the 2D-ferroelectric SnSe on graphene/Ir(111).

Epitaxial growth is a versatile method to prepare two-dimensional van der Waals ferroelectrics like group IV monochalcogenides which have potential for novel electronic devices and sensors. We systematically study SnSe monolayer islands grown by molecular beam epitaxy, especially the effect of annealing temperature on shape and morphology of the edges. Characterization of the samples by scanning tunneling microscopy reveals that the shape of the islands changes from fractal-dendritic after deposition at room temperature to a compact rhombic shape through annealing, but ripening processes are absent up to the desorption temperature. A two-step growth process leads to large, epitaxially aligned rhombic islands bounded by well-defined110-edges (armchair-like), which we claim to be the equilibrium shape of the stoichiometric SnSe monolayer islands. The relaxation of the energetically favorable edges is detected in atomically resolved STM images. The experimental findings are supported by the results of our first-principles calculations, which provide insights into the energetics of the edges, their reconstructions, and yields the equilibrium shapes of the islands which are in good agreement with the experiment.

Non-radiative recombination centres in InGaN/GaN nanowires revealed by statistical analysis of cathodoluminescence intensity maps and electron microscopy.

The methodology of statistical analysis of cathodoluminescence (CL) intensity mappings on ensembles of several hundreds of InGaN/GaN nanowires (NWs) used to quantify non-radiative recombination centres (NRCs) was validated on InGaN/GaN NWs exhibiting spatially homogeneous cathodoluminescence at the scale of single NWs. Cathodoluminescence intensity variations obeying Poisson's statistics were assigned to the presence of randomly incorporated point defects acting as NRCs. Additionally, another type of NRCs, namely extended defects leading to spatially inhomogeneous cathodoluminescence intensity at the scale of single InGaN/GaN NWs are revealed by high resolution scanning transmission electron microscopy, geometrical phase analysis and two-beam diffraction conditions techniques. Such defects are responsible for deviations from Poisson's statistics, allowing one to achieve a rapid evaluation of the crystallographic and optical properties of several hundreds of NWs in a single cathodoluminescence intensity mapping experiment.

Room-temperature infrared photoluminescence and broadband photodetection characteristics of Ge/GeSi islands on silicon-on-insulator.

In this study, molecular beam epitaxial growth of strain-driven three-dimensional self-assembled Ge/GeSi islands on silicon-on-insulator (SOI) substrates, along with their optical and photodetection characteristics, have been demonstrated. The as-grown islands exhibit a bimodal size distribution, consisting of both Ge and GeSi alloy islands, and show significant photoluminescence (PL) emission at room temperature, specifically near optical communication wavelengths. Additionally, these samples were used to fabricate a Ge/GeSi islands/Si nanowire (NW) based phototransistor using a typical e-beam lithography process. The fabricated device exhibited broadband photoresponse characteristics, spanning a wide wavelength range (300-1600 nm) coupled with superior photodetection characteristics and relatively low dark current (~ tens of pA). The remarkable photoresponsivity of the fabricated device, with a peak value of ~11.4 A/W (λ ~ 900 nm) in the near-infrared (NIR) region and ~ 1.36 A/W (λ ~ 1500 nm) in the short-wave infrared (SWIR) region, is a direct result of the photoconductive gain exceeding unity. The room-temperature optical emission and outstanding photodetection performance, covering a wide spectral range from the visible to the SWIR region, showcased by the single layer of Ge/GeSi islands on SOI substrate, highlight their potential towards advanced applications in broadband infrared Si-photonics and imaging. These capabilities make them highly promising for cutting-edge applications compatible with complementary metal-oxide-semiconductor (CMOS) technology.

Catalyst-free MBE growth of PbSnTe nanowires with tunable aspect ratio.

Topological crystalline insulators (TCIs) are interesting for their topological surface states, which hold great promise for scattering-free transport channels and fault-tolerant quantum computing. A promising TCI is SnTe. However, Sn-vacancies form in SnTe, causing a high hole density, hindering topological transport from the surface being measured. This issue could be relieved by using nanowires with a high surface-to-volume ratio. Furthermore, SnTe can be alloyed with Pb reducing the Sn-vacancies while maintaining its topological phase. Here we present the catalyst-free growth of monocrystalline PbSnTe in molecular beam epitaxy. By the addition of a pre-deposition stage before the growth, we have control over the nucleation phase and thereby increase the nanowire yield. This facilitates tuning the nanowire aspect ratio by a factor of four by varying the growth parameters. These results allow us to grow specific morphologies for future transport experiments to probe the topological surface states in a Pb1-xSnxTe-based platform.