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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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Low-voltage complementary circuits comprising n-type and p-type van der Waals heterojunction vertical field-effect transistors (VFETs) are demonstrated. The resulting VFETs possess high on-state current densities (>3000 A cm-2) and on/off current ratios (>104) in a narrow voltage window (<3 V).
Origami is the art of folding two‐dimensional (2D) materials, such as a flat sheet of paper, into complex and elaborate three‐dimensional (3D) objects. This study reports origami‐based metamaterials whose electromagnetic responses are dynamically controllable via switching the folding state of Miura‐ori split‐ring resonators. The deformation of the Miura‐ori unit along the third dimension induces net electric and magnetic dipoles of split‐ring resonators parallel or anti‐parallel to each other, leading to the strong chiral responses. Circular dichroism as high as 0.6 is experimentally observed while the chirality switching is realized by controlling the deformation direction and kinematics. In addition, the relative density of the origami metamaterials can be dramatically reduced to only 2% of that of the unfolded structure. These results open a new avenue toward lightweight, reconfigurable, and deployable metadevices with simultaneously customized electromagnetic and mechanical properties.
To explore new constituents in two-dimensional (2D) materials and to combine their best in van der Waals heterostructures is in great demand as being a unique platform to discover new physical phenomena and to design novel functionalities in interface-based devices. Here in this paper, PbI 2 crystals as thin as a few layers are synthesized, particularly through a facile low-temperature solution approach with crystals of large size, regular shape, different thicknesses, and high yields. As a prototypical demonstration of band engineering of PbI 2 -based interfacial semiconductors, PbI 2 crystals are assembled with several transition metal dichalcogenide monolayers. The photoluminescence of MoS 2 is enhanced in MoS 2 /PbI 2 stacks, while a dramatic photoluminescence quenching of WS 2 and WSe 2 is revealed in WS2/PbI 2 and WSe 2 /PbI2 stacks. This is attributed to the effective heterojunction formation between PbI 2 and these monolayers; type I band alignment in MoS 2 /PbI2 stacks, where fast-transferred charge carriers accumulate in MoS 2 with high emission efficiency, results in photoluminescence enhancement, and type II in WS 2 /PbI 2 and WSe 2 /PbI 2 stacks, with separated electrons and holes suitable for light harvesting, results in photoluminescence quenching. The results demonstrate that MoS 2 , WS 2 , and WSe 2 monolayers with similar electronic structures show completely distinct light–matter interactions when interfacing with PbI 2 , providing unprecedented capabilities to engineer the device performance of 2D heterostructures.
Two-dimensional van der Waals ferromagnet Fe 5-x GeTe 2 (F5GT) is promising for spintronic applications due to its high Curie temperature, layered structure, and ability to host complex magnetic textures. However, the origin of its sample-dependent magnetic anisotropy remains unclear, hindering control of its magnetic behavior. Here, we use spatially resolved cryogenic scanning transmission electron microscopy (STEM) to correlatively map magnetism, lattice structure, and chemistry across atomic-to-micron scales. We reveal that only mesoscale, not nanoscale, inclusions of a Fe-deficient secondary phase significantly modify magnetic behavior, establishing a previously unrecognized critical length scale. This phase separation, induced by quenching, leads to in-plane magnetic anisotropy, while slow cooling confines separation to a few nanometers and preserves out-of-plane anisotropy. These findings reconcile prior inconsistencies and establish a predictive framework for tuning magnetism in F5GT through thermal processing, with broader implications for controlling anisotropy in other two-dimensional magnetic materials.
Abstract Two‐dimensional (2D) materials, such as graphene and boron nitride, have specific lattice structures independent of external conditions. In contrast, the structure of 2D boron sensitively depends on metal substrate, as we show herein using the cluster expansion method and a newly developed surface structure‐search method, both based on first‐principles calculations. The preferred 2D boron on weaker interacting Au is nonplanar with significant buckling and numerous polymorphs as in vacuum, whereas on more reactive Ag, Cu, and Ni, the polymorphic energy degeneracy is lifted and a particular planar structure is found to be most stable. We also show that a layer composed of icosahedral B 12 is unfavorable on Cu and Ni but unexpectedly becomes a possible minimum on Au and Ag. The substrate‐dependent 2D boron choices originate from a competition between the strain energy of buckling and chemical energy of electronic hybridization between boron and metal.
Abstract This contribution describes the synthesis of colloidal di‐patch particles functionalized with DNA on the patches and their assembly into colloidal superstructures via cooperative depletion and DNA‐mediated interactions. The assembly into flower‐like Kagome, brick‐wall like monolayer, orthogonal packed single or double layers, wrinkled monolayer, and colloidal honeycomb superstructures can be controlled by tuning the particles’ patch sizes and assembly conditions. Based on these experimental results, we generate an empirical phase diagram. The principles revealed by the phase diagram provide guidance in the design of two‐dimensional (2D) materials with desired superstructures. Our strategy might be translatable to the assembly of three‐dimensional (3D) colloidal structures.
Abstract Two‐dimensional (2D) materials, such as graphene and boron nitride, have specific lattice structures independent of external conditions. In contrast, the structure of 2D boron sensitively depends on metal substrate, as we show herein using the cluster expansion method and a newly developed surface structure‐search method, both based on first‐principles calculations. The preferred 2D boron on weaker interacting Au is nonplanar with significant buckling and numerous polymorphs as in vacuum, whereas on more reactive Ag, Cu, and Ni, the polymorphic energy degeneracy is lifted and a particular planar structure is found to be most stable. We also show that a layer composed of icosahedral B 12 is unfavorable on Cu and Ni but unexpectedly becomes a possible minimum on Au and Ag. The substrate‐dependent 2D boron choices originate from a competition between the strain energy of buckling and chemical energy of electronic hybridization between boron and metal.
Abstract This contribution describes the synthesis of colloidal di‐patch particles functionalized with DNA on the patches and their assembly into colloidal superstructures via cooperative depletion and DNA‐mediated interactions. The assembly into flower‐like Kagome, brick‐wall like monolayer, orthogonal packed single or double layers, wrinkled monolayer, and colloidal honeycomb superstructures can be controlled by tuning the particles’ patch sizes and assembly conditions. Based on these experimental results, we generate an empirical phase diagram. The principles revealed by the phase diagram provide guidance in the design of two‐dimensional (2D) materials with desired superstructures. Our strategy might be translatable to the assembly of three‐dimensional (3D) colloidal structures.
Thermal conductivity of two‐dimensional (2D) materials is important to characterize as this will govern thermal transport physics in the various thermal and energy applications benefitting from the unique properties of these materials. Here, analytical and numerical techniques are presented to determine the thermal conductivity and interfacial conductance of a 2D material coating using confocal micro‐Raman spectroscopy as a noncontact diagnostic. While several methods have been proposed for calculating the values of thermal conductivity, interfacial conductance, and spatial temperature profile, these models often do not consider effects of radiation, convection, and substrate resistance on the temperature and heat flux profiles. We present a model to calculate the thermal conductivity and interfacial conductance which accounts for convection, radiation, and substrate effects to characterize a variety of 2D material coatings, which is demonstrated using large area graphene transferred onto copper and nickel substrates. Convection and radiation effects are found to have a negligible effect on the temperature profile of supported coatings, while the substrate effects have a considerable effect and therefore impact the quantification of thermal conductivity and interfacial conductance in addition to limiting the spatial resolution of the technique. These findings will allow for more accurate and reproducible extraction of the thermal conductivity of graphene and other 2D material coatings when employing noncontact optothermal Raman spectroscopy methods.
Molybdenum disulfide (MoS 2 ) monolayers have the potential to revolutionize nanotechnology. To reach this potential, it will be necessary to understand the behavior of this two‐dimensional (2D) material on large length scales and under thermal conditions. Herein, we use molecular dynamics (MD) simulations to investigate the nature of the rippling induced by thermal fluctuations in monolayers of the 2H and 1T phases of MoS 2 . The 1T phase is found to be more rigid than the 2H phase. Both monolayer phases are predicted to follow long wavelength scaling behavior typical of systems with anharmonic coupling between vibrational modes as predicted by classic theories of membrane‐like systems.
Direct manufacturing of two-dimensional material-based double barrier (DB) tunnel junctions, based on a lithography-free approach was developed. Graphene/h-BN/Graphene/h-BN/Graphene devices were deposited on Si/SiO2 substrates by employing a plasma enhanced chemical vapor deposition technique in a sequential manner. DB tunneling junctions with varying barrier widths (by varying the thickness of the second graphene layer) were studied. Samples were characterized using Raman, Atomic Force Microscopy and X-ray photoemission spectroscopy. The I–V characteristics of tunneling current showed resonant tunneling behavior at room temperature with a negative differential conductance. The behavior could be explained with quantum mechanical double barrier tunneling model in which analytic solutions to Schrödinger’s equation were obtained in each region of the system. Resonances in transmission probability coefficient for varying barrier widths were evaluated and compared with the experimental results.
We report surface passivation in two-dimensional (2D) materials is one of the best approaches to modulate the structural, dynamical, and mechanical stabilities thereby enhancing chemical and physical properties for optoelectronic applications. Here, we report an ab-initio investigation on structurally, thermally, dynamically, and mechanically stable, and experimentally feasible fluorinated penta-BCN (F-BCN) monolayer. The structural reconstruction after fluorination, increases bond lengths and thickness to reduce the average stiffness and elasticity attaining the mechanical isotropy. Nevertheless, the value of 2D Young’s modulus of F-BCN is comparable to the pristine structure at 6% of compression without mechanical instability. A significant bandgap tailoring is achieved, similar to that of mechanical sensitivity, due to applied strain. Remarkably, following the fluorine passivation, the monolayer’s induced wide direct bandgap semiconducting behavior improves optical absorbance and reflectivity, decreases energy loss, changes optical anisotropy, and makes it a promising candidate material for optoelectronic and nanomechanical applications.
Electronic properties of two-dimensional (2D) materials are strongly influenced by their atomic arrangements, making the theoretically-aided characterization of experimentally-synthesized 2D structures crucial. Using first-principles density functional theory, we analyze nearly 200 configurations of intercalated Gd layers beneath buffer-layer graphene on SiC(0001) over a Gd coverage range of 0.01 < θ < 1.2. By fully relaxing selectively-constructed configurations at each coverage within a large, low-strain supercell, we determine the coverage dependence of the chemical potential for intercalated Gd structures. Thermodynamically-preferred configurations below θ ≈ 0.8 form single-atom-thick monolayers, while 3D-like or multilayer structures emerge beyond θ ≈ 0.9. Most structures are amorphous-like, including the configuration at the chemical potential minimum around θ ≈ 0.4. In contrast, a strongly stretched Gd(0001)-like monolayer at θ = 1/3 and a nearly perfect Gd(0001) monolayer at θ = 1 are significantly less favorable with 0.16 eV and 0.82 eV higher chemical potentials above the minimum, respectively. Furthermore, the graphene layer decoupled by intercalated Gd near the chemical potential minimum is significantly flatter compared to its morphology above intercalated 3D structures at higher coverages and nearly isolated Gd atoms in the lowest coverage region. In conclusion, these findings align with our experimental results and underscore the need for further research on this unique intercalated system, which holds significant potential for diverse applications.
Graphene is one of the most intriguing two-dimensional carbon materials. Its mechanical strength and failure are key concerns for materials engineering and applications. Despite the success of fracture mechanics, the mechanism of how pristine materials fail remains an elusive problem. While many theoretical studies based on molecular dynamics using empirical forcefields have tried to address this question, atomic-scale mechanics are not clearly understood. Especially, a widely employed bond-breaking approach based on the critical bond length has not been rigorously tested. Here, utilizing molecular dynamics simulations with density functional based tight binding, we investigate how the failure of the pristine material initiates. The Wiberg bond order (W BO ) to estimate the change of chemical bonds shows a transition from sp 2 (W BO ~ 1.33) to sp 3 (WBO < 1.0) during the deformation. However, it reveals that a single threshold value for either the WBO or bond length is insufficient to decide failure of pristine material without free edges or defects. Instead, collective behaviors of the local atomic group govern the fracture initiation of pristine graphene. Overall, our study provides dynamic mechanical responses based on quantum mechanics, which have not been captured by empirical forcefields, opening opportunities to design properties by precisely coupling the mechanics and quantum mechanics.
MXenes, a new family of functional two-dimensional (2D) materials, have shown great potential for an extensive variety of applications within the last decade. Atomic defects and functional groups in MXenes are known to have a tremendous influence on the functional properties. In this review, we focus on recent progress in the characterization of atomic defects and functional group chemistry in MXenes, and how to control them to directly influence various properties ( e.g ., electron transport, Li + adsorption, hydrogen evolution reaction (HER) activity, and magnetism) of 2D MXenes materials. Dynamic structural transformations such as oxidation and growth induced by atomic defects in MXenes are also discussed. The review thus provides perspectives on property optimization through atomic defect engineering, and bottom-up synthesis methods based on defect-assisted homoepitaxial growth of MXenes.
Two-dimensional graphene materials attracted much attention worldwide because of their superior performance in electronic devices, sensors, and energy storage. However, its application is limited by high cost and insufficient production. The work to find out a simple and environmentally friendly process is highly needed. Designed pyrolysis of biomass precursors can derive graphene-like materials. This review summarizes some typical preparation processes for graphene-like materials synthesis from biomass carbonization via pyrolysis, including salt-based activation, template-based confinement, chemical blowing, coupling with hydrothermal carbonization pretreatment, post exfoliation, and some other methods. The operation of these methods and the performance of obtained graphene-like materials were closely highlighted. The scalability of the techniques and the applications of the biomass graphene-like carbon were also discussed. Some advanced characterization methods, such as SEM, TEM, AFM, Raman, and XPS to determine the graphene-like structure and graphitization degree were also discussed. In the end, some current challenges and future perspectives of the synthesis of these graphene-like materials were concluded.
In the bourgeoning field of two dimensional layered materials and their atomically thin counterparts, it has been established that the electronic coupling between the layers of the material plays a key role in determining its properties. We are just beginning to understand how each material is unique in that respect while working our way up to building new materials with functionalities enabled by interlayer interactions. Here in this review, we will focus on a system that despite its apparent simplicity possesses a wealth of intriguing physics: layers of graphene with various degree of coupling. The situations discussed here are graphene layers vertically twisted with respect with each other, weakly decoupled electronically and laterally twisted forming grain boundaries. We emphasize experiments that atomically resolve the electronic properties.