Single-photon detection using large-scale high-temperature MgB2 sensors at 20 K.

Ultra-fast single-photon detectors with high current density and operating temperature can benefit space and ground applications, including quantum optical communication systems, lightweight cryogenics for space crafts, and medical use. Here we demonstrate magnesium diboride (MgB2) thin-film superconducting microwires capable of single-photon detection at 1.55 µm optical wavelength. We used helium ions to alter the properties of MgB2, resulting in microwire-based detectors exhibiting single-photon sensitivity across a broad temperature range of up to 20 K, and detection efficiency saturation for 1 µm wide microwires at 3.7 K. Linearity of detection rate vs incident power was preserved up to at least 100 Mcps. Despite the large active area of up to 400 × 400 µm2, the reset time was found to be as low as ~ 1 ns. Our research provides possibilities for breaking the operating temperature limit and maximum single-pixel count rate, expanding the detector area, and raises inquiries about the fundamental mechanisms of single-photon detection in high-critical-temperature superconductors.

High energy density in artificial heterostructures through relaxation time modulation.

Electrostatic capacitors are foundational components of advanced electronics and high-power electrical systems owing to their ultrafast charging-discharging capability. Ferroelectric materials offer high maximum polarization, but high remnant polarization has hindered their effective deployment in energy storage applications. Previous methodologies have encountered problems because of the deteriorated crystallinity of the ferroelectric materials. We introduce an approach to control the relaxation time using two-dimensional (2D) materials while minimizing energy loss by using 2D/3D/2D heterostructures and preserving the crystallinity of ferroelectric 3D materials. Using this approach, we were able to achieve an energy density of 191.7 joules per cubic centimeter with an efficiency greater than 90%. This precise control over relaxation time holds promise for a wide array of applications and has the potential to accelerate the development of highly efficient energy storage systems.

Salt-Assisted Vapor-Liquid-Solid Growth of 1D van der Waals Materials.

The method of salt-assisted vapor-liquid-solid (VLS) growth is introduced to synthesize 1D nanostructures of trichalcogenide van der Waals (vdW) materials, exemplified by niobium trisulfide (NbS3 ). The method uses a unique catalyst consisting of an alloy of Au and an alkali metal halide (NaCl) to enable rapid and directional growth. High yields of two types of NbS3 1D nanostructures, nanowires and nanoribbons, each with sub-ten nanometer diameter, tens of micrometers length, and distinct 1D morphology and growth orientation are demonstrated. Strategies to control the location, size, and morphology of growth, and extend the growth method to synthesize other transition metal trichalcogenides, NbSe3 and TiS3 , as nanowires are demonstrated. Finally, the role of the Au-NaCl alloy catalyst in guiding VLS synthesis is described and the growth mechanism based on the relationships measured between structure (growth orientation, morphology, and dimensions) and growth conditions (catalyst volume and growth time) is discussed. These results introduce opportunities to expand the library of emerging 1D vdW materials to make use of their unique properties through controlled growth at nanoscale dimensions.

Monolithic 3D integration of 2D materials-based electronics towards ultimate edge computing solutions.

Three-dimensional (3D) hetero-integration technology is poised to revolutionize the field of electronics by stacking functional layers vertically, thereby creating novel 3D circuity architectures with high integration density and unparalleled multifunctionality. However, the conventional 3D integration technique involves complex wafer processing and intricate interlayer wiring. Here we demonstrate monolithic 3D integration of two-dimensional, material-based artificial intelligence (AI)-processing hardware with ultimate integrability and multifunctionality. A total of six layers of transistor and memristor arrays were vertically integrated into a 3D nanosystem to perform AI tasks, by peeling and stacking of AI processing layers made from bottom-up synthesized two-dimensional materials. This fully monolithic-3D-integrated AI system substantially reduces processing time, voltage drops, latency and footprint due to its densely packed AI processing layers with dense interlayer connectivity. The successful demonstration of this monolithic-3D-integrated AI system will not only provide a material-level solution for hetero-integration of electronics, but also pave the way for unprecedented multifunctional computing hardware with ultimate parallelism.

Atomic-Scale Mechanisms of MoS2 Oxidation for Kinetic Control of MoS2/MoO3 Interfaces.

Oxidation of transition metal dichalcogenides (TMDs) occurs readily under a variety of conditions. Therefore, understanding the oxidation processes is necessary for successful TMD handling and device fabrication. Here, we investigate atomic-scale oxidation mechanisms of the most widely studied TMD, MoS2. We find that thermal oxidation results in α-phase crystalline MoO3 with sharp interfaces, voids, and crystallographic alignment with the underlying MoS2. Experiments with remote substrates prove that thermal oxidation proceeds via vapor-phase mass transport and redeposition, a challenge to forming thin, conformal films. Oxygen plasma accelerates the kinetics of oxidation relative to the kinetics of mass transport, forming smooth and conformal oxides. The resulting amorphous MoO3 can be grown with subnanometer to several-nanometer thickness, and we calibrate the oxidation rate for different instruments and process parameters. Our results provide quantitative guidance for managing both the atomic scale structure and thin-film morphology of oxides in the design and processing of TMD devices.

Direct Visualization of Subnanometer Variations in the Excitonic Spectra of 2D/3D Semiconductor/Metal Heterostructures.

The integration of metallic contacts with two-dimensional (2D) semiconductors is routinely required for the fabrication of nanoscale devices. However, nanometer-scale variations in the 2D/metal interface can drastically alter the local optoelectronic properties. Here, we map local excitonic changes of the 2D semiconductor MoS2 in contact with Au. We utilize a suspended and epitaxially grown 2D/metal platform that allows correlated electron energy-loss spectroscopy (EELS) and angle resolved photoelectron spectroscopy (nanoARPES) mapping. Spatial localization of MoS2 excitons uncovers an additional EELS peak related to the MoS2/Au interface. NanoARPES measurements indicate that Au-S hybridization decreases substantially with distance from the 2D/metal interface, suggesting that the observed EELS peak arises due to dielectric screening of the excitonic Coulomb interaction. Our results suggest that increasing the van der Waals distance could optimize excitonic spectra of mixed-dimensional 2D/3D interfaces and highlight opportunities for Coulomb engineering of exciton energies by the local dielectric environment or moiré engineering.

Strong and Localized Luminescence from Interface Bubbles Between Stacked hBN Multilayers.

Extraordinary optoelectronic properties of van der Waals (vdW) heterostructures can be tuned via strain caused by mechanical deformation. Here, we demonstrate strong and localized luminescence in the ultraviolet region from interface bubbles between stacked multilayers of hexagonal boron nitride (hBN). Compared to bubbles in stacked monolayers, bubbles formed by stacking vdW multilayers show distinct mechanical behavior. We use this behavior to elucidate radius- and thickness-dependent bubble geometry and the resulting strain across the bubble, from which we establish the thickness-dependent bending rigidity of hBN multilayers. We then utilize the polymeric material confined within the bubbles to modify the bubble geometry under electron beam irradiation, resulting in strong luminescence and formation of optical standing waves. Our results open a route to design and modulate microscopic-scale optical cavities via strain engineering in vdW materials, which we suggest will be relevant to both fundamental mechanical studies and optoelectronic applications.

Mechanisms of Quasi van der Waals Epitaxy of Three-Dimensional Metallic Nanoislands on Suspended Two-Dimensional Materials.

Understanding structure at the interface between two-dimensional (2D) materials and 3D metals is crucial for designing novel 2D/3D heterostructures and improving the performance of many 2D material devices. Here, we quantify and discuss the 2D/3D interface structure and the 3D morphology in several materials systems. We first deposit faceted Au nanoislands on graphene and transition metal dichalcogenides, using measurements of the equilibrium island shape to determine values for the 2D/Au interface energy and examining the role of surface reconstructions, chemical identity, and defects on the grown structures. We then deposit the technologically relevant metals Ti and Nb under conditions where kinetic rather than thermodynamic factors govern growth. We describe a transition from dendritic to faceted islands as a function of growth temperature and discuss the factors determining island shape in these materials systems. Finally, we show that suspended 2D materials enable the fabrication of a novel type of 3D/2D/3D heterostructure and discuss the growth mechanism. We suggest that emerging nanodevices will utilize versatile fabrication of 2D/3D heterostructures with well-characterized interfaces and morphologies.

Suspended Graphene Membranes to Control Au Nucleation and Growth.

Control of nucleation sites is an important goal in materials growth: nuclei in regular arrays may show emergent photonic or electronic behavior, and once the nuclei coalesce into thin films, the nucleation density influences parameters such as surface roughness, stress, and grain boundary structure. Tailoring substrate properties to control nucleation is therefore a powerful tool for designing functional thin films and nanomaterials. Here, we examine nucleation control for metals deposited on two-dimensional materials in a situation where substrate effects are absent and heterogeneous nucleation sites are minimized. Through quantification of faceted, epitaxial Au island nucleation on graphene, we show that ultralow nucleation densities with nuclei several micrometers apart can be achieved on suspended graphene under conditions where we measure 2-3 orders of magnitude higher nucleation density on the adjacent supported substrate. We estimate diffusion distances using nucleation theory and find a strong sensitivity of nucleation and diffusion to suspended graphene thickness. Finally, we discuss the role of surface roughness as the main factor determining nucleation density on clean free-standing graphene.

Real-time imaging of nanoscale electrochemical Ni etching under thermal conditions.

The ability to vary the temperature of an electrochemical cell provides opportunities to control reaction rates and pathways and to drive processes that are inaccessible at ambient temperature. Here, we explore the effect of temperature on electrochemical etching of Ni-Pt bimetallic nanoparticles. To observe the process at nanoscale resolution we use liquid cell transmission electron microscopy with a modified liquid cell that enables simultaneous heating and biasing. By controlling the cell temperature, we demonstrate that the reaction rate and dissolution potential of the electrochemical Ni etching process can be changed. The in situ measurements suggest that the destabilization of the native nickel oxide layer is the slow step prior to subsequent fast Ni removal in the electrochemical Ni dissolution process. These experiments highlight the importance of in situ structural characterization under electrochemical and thermal conditions as a strategy to provide deeper insights into nanomaterial transformations as a function of temperature and potential.

Direct imaging and electronic structure modulation of moiré superlattices at the 2D/3D interface.

The atomic structure at the interface between two-dimensional (2D) and three-dimensional (3D) materials influences properties such as contact resistance, photo-response, and high-frequency electrical performance. Moiré engineering is yet to be utilized for tailoring this 2D/3D interface, despite its success in enabling correlated physics at 2D/2D interfaces. Using epitaxially aligned MoS2/Au{111} as a model system, we demonstrate the use of advanced scanning transmission electron microscopy (STEM) combined with a geometric convolution technique in imaging the crystallographic 32 Å moiré pattern at the 2D/3D interface. This moiré period is often hidden in conventional electron microscopy, where the Au structure is seen in projection. We show, via ab initio electronic structure calculations, that charge density is modulated according to the moiré period, illustrating the potential for (opto-)electronic moiré engineering at the 2D/3D interface. Our work presents a general pathway to directly image periodic modulation at interfaces using this combination of emerging microscopy techniques.