Exceptional electronic transport and quantum oscillations in thin bismuth crystals grown inside van der Waals materials.

Confining materials to two-dimensional forms changes the behaviour of the electrons and enables the creation of new devices. However, most materials are challenging to produce as uniform, thin crystals. Here we present a synthesis approach where thin crystals are grown in a nanoscale mould defined by atomically flat van der Waals (vdW) materials. By heating and compressing bismuth in a vdW mould made of hexagonal boron nitride, we grow ultraflat bismuth crystals less than 10 nm thick. Due to quantum confinement, the bismuth bulk states are gapped, isolating intrinsic Rashba surface states for transport studies. The vdW-moulded bismuth shows exceptional electronic transport, enabling the observation of Shubnikov-de Haas quantum oscillations originating from the (111) surface state Landau levels. By measuring the gate-dependent magnetoresistance, we observe multi-carrier quantum oscillations and Landau level splitting, with features originating from both the top and bottom surfaces. Our vdW mould growth technique establishes a platform for electronic studies and control of bismuth's Rashba surface states and topological boundary modes1-3. Beyond bismuth, the vdW-moulding approach provides a low-cost way to synthesize ultrathin crystals and directly integrate them into a vdW heterostructure.

Structural alignment of ZnO columns across multiple monolayer MoS2 layers as compliant substrates.

Understanding the behavior of materials in multi-dimensional architectures composed of atomically thin two-dimensional (2D) materials and three-dimensional (3D) materials has become mandatory for progress in materials preparation via various epitaxy techniques, such as van der Waals and remote epitaxy methods. We investigated the growth behavior of ZnO on monolayer MoS2 as a model system to study the growth of a 3D material on a 2D material, which is beyond the scope of remote and van der Waals epitaxy. The study revealed column-to-column alignment and inversion of crystallinity, which can be explained by combinatorial epitaxy, grain alignment across an atomically sharp interface, and a compliant substrate. The growth study enabled the formation of a ZnO/MoS2 heterostructure with type-I band alignment. Our findings will have a scientific impact on realizing 2D/3D heterostructures for practical device applications.

Controllable strain-driven topological phase transition and dominant surface-state transport in HfTe5.

The fine-tuning of topologically protected states in quantum materials holds great promise for novel electronic devices. However, there are limited methods that allow for the controlled and efficient modulation of the crystal lattice while simultaneously monitoring the changes in the electronic structure within a single sample. Here, we apply significant and controllable strain to high-quality HfTe5 samples and perform electrical transport measurements to reveal the topological phase transition from a weak topological insulator phase to a strong topological insulator phase. After applying high strain to HfTe5 and converting it into a strong topological insulator, we found that the resistivity of the sample increased by 190,500% and that the electronic transport was dominated by the topological surface states at cryogenic temperatures. Our results demonstrate the suitability of HfTe5 as a material for engineering topological properties, with the potential to generalize this approach to study topological phase transitions in van der Waals materials and heterostructures.

Manipulating Interlayer Excitons for Near-Infrared Quantum Light Generation.

Interlayer excitons (IXs) formed at the interface of van der Waals materials possess various novel properties. In parallel development, strain engineering has emerged as an effective means for creating 2D quantum emitters. Exploring the intersection of these two exciting areas, we use MoS2/WSe2 heterostructure as a model system and demonstrate how strain, defects, and layering can be utilized to create defect-bound IXs capable of bright, robust, and tunable quantum light emission in the technologically important near-infrared spectral range. Our work presents defect-bound IXs as a promising platform for pushing the performance of 2D quantum emitters beyond their current limitations.

Proximity-induced chiral quantum light generation in strain-engineered WSe2/NiPS3 heterostructures.

Quantum light emitters capable of generating single photons with circular polarization and non-classical statistics could enable non-reciprocal single-photon devices and deterministic spin-photon interfaces for quantum networks. To date, the emission of such chiral quantum light relies on the application of intense external magnetic fields, electrical/optical injection of spin-polarized carriers/excitons or coupling with complex photonic metastructures. Here we report the creation of free-space chiral quantum light emitters via the nanoindentation of monolayer WSe2/NiPS3 heterostructures at zero external magnetic field. These quantum light emitters emit with a high degree of circular polarization (0.89) and single-photon purity (95%), independent of pump laser polarization. Scanning diamond nitrogen-vacancy microscopy and temperature-dependent magneto-photoluminescence studies reveal that the chiral quantum light emission arises from magnetic proximity interactions between localized excitons in the WSe2 monolayer and the out-of-plane magnetization of defects in the antiferromagnetic order of NiPS3, both of which are co-localized by strain fields associated with the nanoscale indentations.

Induced Ferromagnetism in Epitaxial Uranium Dioxide Thin Films.

Actinide materials have various applications that range from nuclear energy to quantum computing. Most current efforts have focused on bulk actinide materials. Tuning functional properties by using strain engineering in epitaxial thin films is largely lacking. Using uranium dioxide (UO2 ) as a model system, in this work, the authors explore strain engineering in actinide epitaxial thin films and investigate the origin of induced ferromagnetism in an antiferromagnet UO2 . It is found that UO2+ x thin films are hypostoichiometric (x<0) with in-plane tensile strain, while they are hyperstoichiometric (x>0) with in-plane compressive strain. Different from strain engineering in non-actinide oxide thin films, the epitaxial strain in UO2 is accommodated by point defects such as vacancies and interstitials due to the low formation energy. Both epitaxial strain and strain relaxation induced point defects such as oxygen/uranium vacancies and oxygen/uranium interstitials can distort magnetic structure and result in magnetic moments. This work reveals the correlation among strain, point defects and ferromagnetism in strain engineered UO2+ x thin films and the results offer new opportunities to understand the influence of coupled order parameters on the emergent properties of many other actinide thin films.

Visualizing Grain Statistics in MOCVD WSe2 through Four-Dimensional Scanning Transmission Electron Microscopy.

Using four-dimensional scanning transmission electron microscopy, we demonstrate a method to visualize grains and grain boundaries in WSe2 grown by metal organic chemical vapor deposition (MOCVD) directly onto silicon dioxide. Despite the chemical purity and uniform thickness and texture of the MOCVD-grown WSe2, we observe a high density of small grains that corresponds with the overall selenium deficiency we measure through ion beam analysis. Moreover, reconstruction of grain information permits the creation of orientation maps that demonstrate the nucleation mechanism for new layers-triangular domains with the same orientation as the layer underneath induces a tensile strain increasing the lattice parameter at these sites.

Site-controlled telecom-wavelength single-photon emitters in atomically-thin MoTe2.

Quantum emitters (QEs) in two-dimensional transition metal dichalcogenides (2D TMDCs) have advanced to the forefront of quantum communication and transduction research. To date, QEs capable of operating in O-C telecommunication bands have not been demonstrated in TMDCs. Here we report site-controlled creation of telecom QEs emitting over the 1080 to 1550 nm telecommunication wavelength range via coupling of 2D molybdenum ditelluride (MoTe2) to strain inducing nano-pillar arrays. Hanbury Brown and Twiss experiments conducted at 10 K reveal clear photon antibunching with 90% single-photon purity. The photon antibunching can be observed up to liquid nitrogen temperature (77 K). Polarization analysis further reveals that while some QEs display cross-linearly polarized doublets with ~1 meV splitting resulting from the strain induced anisotropic exchange interaction, valley degeneracy is preserved in other QEs. Valley Zeeman splitting as well as restoring of valley symmetry in cross-polarized doublets are observed under 8 T magnetic field.

Intrinsic helical twist and chirality in ultrathin tellurium nanowires.

Robust atomic-to-meso-scale chirality is now observed in the one-dimensional form of tellurium. This enables a large and counter-intuitive circular-polarization dependent second harmonic generation response above 0.2 which is not present in two-dimensional tellurium. Orientation variations in 1D tellurium nanowires obtained by four-dimensional scanning transmission electron microscopy (4D-STEM) and their correlation with unconventional non-linear optical properties by second harmonic generation circular dichroism (SHG-CD) uncovers an unexpected circular-polarization dependent SHG response from 1D nanowire bundles - an order-of-magnitude higher than in single-crystal two-dimensional tellurium structures - suggesting the atomic- and meso-scale crystalline structure of the 1D material possesses an inherent chirality not present in its 2D form; and which is strong enough to manifest even in the aggregate non-linear optical (NLO) properties of aggregates.

Thermoelectric properties of antimony selenide hexagonal nanotubes.

Antimony selenide (Sb2Se3) is a material widely used in photodetectors and relatively new as a possible material for thermoelectric applications. Taking advantage of the new properties after nanoscale fabrication, this material shows great potential for the development of efficient low temperature thermoelectric devices. Here we study the synthesis, the crystal properties and the thermal and thermoelectric transport response of Sb2Se3 hexagonal nanotubes (HNT) in the temperature range between 120 and 370 K. HNT have a moderate electrical conductivity ∼102 S m-1 while maintaining a reasonable Seebeck coefficient ∼430 µV K-1 at 370 K. The electrical conductivity in Sb2Se3 HNT is about 5 orders of magnitude larger and its thermal conductivity one half of what is found in bulk. Moreover, the calculated figure of merit (ZT) at room temperature is the largest value reported in antimony selenide 1D structures.

1D to 2D Transition in Tellurium Observed by 4D Electron Microscopy.

A new microwave-enhanced synthesis method for the production of tellurium nanostructures is reported-with control over products from the 1D regime (sub-5 nm diameter nanowires), to nanoribbons, to the 2D tellurene regime-along with a new methodology for local statistical quantification of the crystallographic parameters of these materials at the nanometer scale. Using a direct electron detector and image-corrected microscope, large and robust 4D scanning transmission electron microscopy datasets for accurate structural analysis are obtained. These datasets allow the adaptation of quantitative techniques originally developed for X-ray diffraction (XRD) refinement analyses to transmission electron microscopy, enabling the first demonstration of sub-picometer accuracy lattice parameter extraction while also obtaining both the size of the coherent crystallite domains and the nanostrain, which is observed to decrease as nanowires transition to tellurene. This new local analysis is commensurate with global powder XRD results, indicating the robustness of both the new synthesis approach and new structural analysis methodology for future scalable production of 2D tellurene and characterization of nanomaterials.

Thermoelectric properties of SnSe nanowires with different diameters.

Tin selenide (SnSe) has been the subject of great attention in the last years due to its highly efficient thermoelectricity and its possibilities as a green material, free of Pb and Te. Here, we report for the first time a thermoelectricity and transport study of individual SnSe micro- and nano-wires with diameters in the range between 130 nm and 1.15 µm. X-ray diffraction and transmission electron microscopy analyses confirm an orthorhombic SnSe structure with Pnma (62) symmetry group and 1:1 Sn:Se atomic ratio. Electrical and thermal conductivity and the Seebeck coefficient were measured in each individual nanowire using a specialized suspended microdevice in the 150-370 K temperature range, yielding a thermal conductivity of 0.55 Wm-1 K-1 at room temperature and ZT ~ 0.156 at 370 K for the 130 nm diameter nanowire. The measured properties were correlated with electronic information obtained by model simulations and with phonon scattering analysis. The results confirm these structures as promising building blocks to develop efficient temperature sensors, refrigerators and thermoelectric energy converters. The thermoelectric response of the nanowires is compared with recent reports on crystalline, polycrystalline and layered bulk structures.

Giant Mechano-Optoelectronic Effect in an Atomically Thin Semiconductor.

Transition metal dichalcogenides (TMDs) are particularly sensitive to mechanical strain because they are capable of experiencing high atomic displacements without nucleating defects to release excess energy. Being promising for photonic applications, it has been shown that as certain phases of layered TMDs MX2 (M = Mo or W; X = S, Se, or Te) are scaled to a thickness of one monolayer, the photoluminescence response is dramatically enhanced due to the emergence of a direct electronic band gap compared with their multilayer or bulk counterparts, which typically exhibit indirect band gaps. Recently, mechanical strain has also been predicted to enable direct excitonic recombination in these materials, in which large changes in the photoluminescence response will occur during an indirect-to-direct band gap transition brought on by elastic tensile strain. Here, we demonstrate an enhancement of 2 orders of magnitude in the photoluminescence emission intensity in uniaxially strained single crystalline WSe2 bilayers. Through a theoretical model that includes experimentally relevant system conditions, we determine this amplification to arise from a significant increase in direct excitonic recombination. Adding confidence to the high levels of elastic strain achieved in this report, we observe strain-independent, mode-dependent Grüneisen parameters over the entire range of tensile strain (1-3.59%), which were obtained as 1.149 ± 0.027, 0.307 ± 0.061, and 0.357 ± 0.103 for the E2g, A1g, and A21g optical phonon modes, respectively. These results can inform the predictive strain-engineered design of other atomically thin indirect semiconductors, in which a decrease in out-of-plane bonding strength may lead to an increase in the strength of strain-coupled optoelectronic effects.

Magnetic field-induced helical mode and topological transitions in a topological insulator nanoribbon.

The spin-helical Dirac fermion topological surface states in a topological insulator nanowire or nanoribbon promise novel topological devices and exotic physics such as Majorana fermions. Here, we report local and non-local transport measurements in Bi2Te3 topological insulator nanoribbons that exhibit quasi-ballistic transport over ∼2 µm. The conductance versus axial magnetic flux Φ exhibits Aharonov-Bohm oscillations with maxima occurring alternately at half-integer or integer flux quanta (Φ0 = h/e, where h is Planck's constant and e is the electron charge) depending periodically on the gate-tuned Fermi wavevector (kF) with period 2π/C (where C is the nanoribbon circumference). The conductance versus gate voltage also exhibits kF-periodic oscillations, anti-correlated between Φ = 0 and Φ0/2. These oscillations enable us to probe the Bi2Te3 band structure, and are consistent with the circumferentially quantized topological surface states forming a series of one-dimensional subbands, which undergo periodic magnetic field-induced topological transitions with the disappearance/appearance of the gapless Dirac point with a one-dimensional spin helical mode.

Significant electronic thermal transport in the conducting polymer poly(3,4-ethylenedioxythiophene).

Suspended microdevices are employed to measure the in-plane electrical conductivity, thermal conductivity, and Seebeck coefficient of suspended poly(3,4-ethylenedioxythiophene) (PEDOT) thin films. The measured thermal conductivity is higher than previously reported for PEDOT and generally increases with the electrical conductivity. The increase exceeds that predicted by the Wiedemann-Franz law for metals and can be explained by significant electronic thermal transport in PEDOT.

Gate tunable relativistic mass and Berry's phase in topological insulator nanoribbon field effect devices.

Transport due to spin-helical massless Dirac fermion surface state is of paramount importance to realize various new physical phenomena in topological insulators, ranging from quantum anomalous Hall effect to Majorana fermions. However, one of the most important hallmarks of topological surface states, the Dirac linear band dispersion, has been difficult to reveal directly in transport measurements. Here we report experiments on Bi2Te3 nanoribbon ambipolar field effect devices on high-κ SrTiO3 substrates, where we achieve a gate-tuned bulk metal-insulator transition and the topological transport regime with substantial surface state conduction. In this regime, we report two unambiguous transport evidences for gate-tunable Dirac fermions through π Berry's phase in Shubnikov-de Haas oscillations and effective mass proportional to the Fermi momentum, indicating linear energy-momentum dispersion. We also measure a gate-tunable weak anti-localization (WAL) with 2 coherent conduction channels (indicating 2 decoupled surfaces) near the charge neutrality point, and a transition to weak localization (indicating a collapse of the Berry's phase) when the Fermi energy approaches the bulk conduction band. The gate-tunable Dirac fermion topological surface states pave the way towards a variety of topological electronic devices.

High thermal conductivity of chain-oriented amorphous polythiophene.

Polymers are usually considered thermal insulators, because the amorphous arrangement of the molecular chains reduces the mean free path of heat-conducting phonons. The most common method to increase thermal conductivity is to draw polymeric fibres, which increases chain alignment and crystallinity, but creates a material that currently has limited thermal applications. Here we show that pure polythiophene nanofibres can have a thermal conductivity up to ∼ 4.4 W m(-1) K(-1) (more than 20 times higher than the bulk polymer value) while remaining amorphous. This enhancement results from significant molecular chain orientation along the fibre axis that is obtained during electropolymerization using nanoscale templates. Thermal conductivity data suggest that, unlike in drawn crystalline fibres, in our fibres the dominant phonon-scattering process at room temperature is still related to structural disorder. Using vertically aligned arrays of nanofibres, we demonstrate effective heat transfer at critical contacts in electronic devices operating under high-power conditions at 200 °C over numerous cycles.

Reexamination of thermal transport measurements of a low-thermal conductance nanowire with a suspended micro-device.

An increasingly used technique for measuring the thermal conductance of a nanowire is based on a suspended micro-device with built-in resistance thermometers. In the past, the technique has been limited to samples with thermal conductance larger than 1 × 10(-9) W/K because of temperature fluctuations in the sample environment and the presence of background heat transfer through residual gas molecules and radiation between the two thermometers. In addition, parasitic heat loss from the long supporting beams and asymmetry in the fabricated device results in two additional errors, which have been ignored in previous use of this method. To address these issues, we present a comprehensive measurement approach, where the device asymmetry is determined by conducting thermal measurements with two opposite heat flow directions along the nanowire, the background heat transfer is eliminated by measuring the differential heat transfer signal between the nanowire device and a reference device without a nanowire sample, and the parasitic heat loss from the supporting beams is obtained by measuring the average temperature rise of one of the beams. This technique is demonstrated on a nanofiber sample with a thermal conductance of 3.7 × 10(-10) W/K, against a background conductance of 8.2 × 10(-10) W/K at 320 K temperature. The results reveal the need to reduce the background thermal conductance in order to employ the micro-device to measure a nanowire sample with the thermal conductance less than 1 × 10(-10) W/K.

Ultrathin graphite foam: a three-dimensional conductive network for battery electrodes.

We report the use of free-standing, lightweight, and highly conductive ultrathin graphite foam (UGF), loaded with lithium iron phosphate (LFP), as a cathode in a lithium ion battery. At a high charge/discharge current density of 1280 mA g(-1), the specific capacity of the LFP loaded on UGF was 70 mAh g(-1), while LFP loaded on Al foil failed. Accounting for the total mass of the electrode, the maximum specific capacity of the UGF/LFP cathode was 23% higher than that of the Al/LFP cathode and 170% higher than that of the Ni-foam/LFP cathode. Using UGF, both a higher rate capability and specific capacity can be achieved simultaneously, owing to its conductive (∼1.3 × 10(5) S m(-1) at room temperature) and three-dimensional lightweight (∼9.5 mg cm(-3)) graphitic structure. Meanwhile, UGF presents excellent electrochemical stability comparing to that of Al and Ni foils, which are generally used as conductive substrates in lithium ion batteries. Moreover, preparation of the UGF electrode was facile, cost-effective, and compatible with various electrochemically active materials.