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At least 253 records · Page 14

A native oxide high-κ gate dielectric for two-dimensional electronics

Silicon-based transistors are approaching their physical limits and thus new high-mobility semiconductors are sought to replace silicon in the microelectronics industry. Both bulk materials (such as silicon-germanium and III–V semiconductors) and low-dimensional nanomaterials (such as one-dimensional carbon nanotubes and two-dimensional transition metal dichalcogenides) have been explored, but, unlike silicon, which uses silicon dioxide (SiO 2 ) as its gate dielectric, these materials suffer from the absence of a high-quality native oxide as a dielectric counterpart. This can lead to compatibility problems in practical devices. Here, we show that an atomically thin gate dielectric of bismuth selenite (Bi 2 SeO 5 ) can be conformally formed via layer-by-layer oxidization of an underlying high-mobility two-dimensional semiconductor, Bi 2 O 2 Se. Using this native oxide dielectric, high-performance Bi 2 O 2 Se field-effect transistors can be created, as well as inverter circuits that exhibit a large voltage gain (as high as 150). The high dielectric constant (~21) of Bi 2 SeO 5 allows its equivalent oxide thickness to be reduced to 0.9 nm while maintaining a gate leakage lower than thermal SiO 2 . The Bi 2 SeO 5 can also be selectively etched away by a wet chemical method that leaves the mobility of the underlying Bi 2 O 2 Se semiconductor almost unchanged.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Crystal phases of charged interlayer excitons in van der Waals heterostructures

Throughout the years, strongly correlated coherent states of excitons have been the subject of intense theoretical and experimental studies. This topic has recently boomed due to new emerging quantum materials such as van der Waals (vdW) bound atomically thin layers of transition metal dichalcogenides (TMDs). We analyze the collective properties of charged interlayer excitons observed recently in bilayer TMD heterostructures. We predict strongly correlated phases—crystal and Wigner crystal—that can be selectively realized with TMD bilayers of properly chosen electron-hole effective masses by just varying their interlayer separation distance. Our results can be used for nonlinear coherent control, charge transport and spinoptronics application development with quantum vdW heterostuctures.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Understanding and tuning magnetism in van der Waals-type metal thiophosphates

Over the past two decades, significant progress in two-dimensional (2D) materials has invigorated research in condensed matter and material physics in low dimensions. While traditionally studied in three-dimensional systems, magnetism has now been extended to the 2D realm. Recent breakthroughs in 2D magnetism have attracted substantial interest from the scientific community, owing to the stable magnetic order achievable in atomically thin layers of the van der Waals (vdW)-type layered magnetic materials. These advances offer an exciting platform for investigating related phenomena in low dimensions and hold promise for spintronic applications. Consequently, vdW magnetic materials with tunable magnetism have attracted significant attention. Specifically, antiferromagnetic metal thiophosphates MPX 3 (M = transition metal, P = phosphorus, X = chalcogen) have been investigated extensively. These materials exhibit long-range magnetic order spanning from bulk to the 2D limit. The magnetism in MPX 3 arises from localized moments associated with transition metal ions, making it tunable via substitutions and intercalations. In this review, we focus on such tuning by providing a comprehensive summary of various metal- and chalcogen-substitution and intercalation studies, along with the mechanism of magnetism modulation, and a perspective on the development of this emergent material family.

42 ENGINEERING↗

Thermal Conductivity of Graphene Coated Copper Under Uniaxial Tensile Mechanical Strain

Graphene continues to demonstrate promise as a highly effective barrier coating, even at only one atom thick. The thermal properties of this coating are also promising to allow diffusion of heat across the surface, as the isolated graphene is an intrinsically good thermal conductor, yet this and its behavior under mechanical deformation has been less extensively studied. This report demonstrates that the in-plane thermal conductivity and interfacial thermal conductance of graphene coatings on copper are affected by mechanical strain. By inducing a strain in the copper substrate, the Raman-active 2D peak exhibits a change in position as well as a change in laser power dependence as the copper substrate is uniaxially elongated to a maximum of 0.5%. Non-linear trends in thermal conductivity are observed with tensile strain in samples with differing strain transfer rates from the substrate, indicating the close correlation between intrinsic thermal conduction and interfacial properties in atomically thin coatings transferred onto metals.

36 MATERIALS SCIENCE↗

Multiscale analysis of large twist ferroelectricity and swirling dislocations in bilayer hexagonal boron nitride

With its atomically thin structure and intrinsic ferroelectric properties, heterodeformed bilayer hexagonal boron nitride (hBN) has gained prominence in next-generation non-volatile memory applications. However, studies to date have focused almost exclusively on small-twist bilayer hBN, leaving the question of whether ferroelectricity can persist under small heterostrain and large heterodeformation entirely unexplored. In this work, we establish the crystallographic origin of ferroelectricity in bilayer hBN configurations heterodeformed relative to high-symmetry configurations such as AA-stacking and 21.786789° twisted configurations (Σ7), using Smith normal form bicrystallography. We then demonstrate out-of-plane ferroelectricity in bilayer hBN across configurations vicinal to both the AA and Σ7 stackings. Atomistic simulations reveal that AA-vicinal systems support ferroelectricity under both small twist and small strain, with polarization switching in the latter governed by the deformation of swirling dislocations rather than the straight interface dislocations seen in the former. For Σ7-vicinal systems, where existing interatomic potentials underperform particularly under extreme out-of-plane compression, we develop a density-functional-theory-informed continuum framework—the bicrystallography-informed frame-invariant multiscale (BFIM) model, which captures out-of-plane ferroelectricity in heterodeformed configurations vicinal to Σ7 stacking. Interface dislocations in these large heterodeformed bilayer configurations exhibit markedly smaller Burgers vectors compared to interface dislocations in small-twist and small-strain bilayer hBN. The BFIM model reproduces experimental results and provides a powerful, computationally efficient framework for predicting ferroelectricity in large-unit-cell heterostructures where atomistic simulations are prohibitively expensive.

Ahmed, Md Tusher [Univ. of Illinois at Urbana-Cham↗

Andreev reflection between aluminum and graphene across van der Waals barriers

We present planar aluminum superconductor–graphene junctions whose hybrid interface is engineered for couplings ranging from tunneling to the strongly coupled regime by employing an atomically thin van der Waals tunneling barrier. Without the vdW barrier, we find Al makes strongly coupled contacts with the fully proximities graphene channel underneath. Using a large band gap hexagonal boron nitride (hBN) barrier, we find the junctions always remain in the weak coupling regime, exhibiting tunneling characteristics. Using monolayer semi-conducting transition metal dichalcogenides (TMDs) such as MoS2, we realize intermediate coupling with enhanced junction conductance due to the Andreev process. In this intermediate regime, we find that junction resistance changes in discrete steps when sweeping a perpendicular magnetic field. The period of the resistance steps in the magnetic field is inversely proportional to the junction area, suggesting the physical origin of our observations is due to magnetic-field-induced vortex formation in the planar junction.

Physics↗

Nanoscale imaging of Gilbert damping using signal amplitude mapping

Ferromagnetic resonance force microscopy (FMRFM) is a powerful scanned probe technique that uses sub-micrometer-scale, spatially localized standing spin wave modes (LMs) to perform local ferromagnetic resonance (FMR) measurements. In this work, we show the spatially resolved imaging of Gilbert damping in a ferromagnetic material (FM) using FMRFM. Typically damping is measured from the FMR linewidth. We demonstrate an approach to image the spatial variation of Gilbert damping utilizing the LM resonance peak height to measure the LM resonance cone angle. This approach enables determination of damping through field-swept FMRFM at a single excitation frequency. The extreme force sensitivity of similar to 2 fN at room temperature can resolve changes of Gilbert damping as small as ~2 x 10 -4 at 2GHz, corresponding to ~0.16Oe in FMR linewidth resolution. This high sensitivity, high spatial resolution, and single frequency imaging of Gilbert damping creates the opportunity to study spin interactions at the interface between an insulating FM and a small volume of nonmagnetic material such as atomically thin two-dimensional materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Non-conventional bell-shaped diffuse scattering in low-energy electron diffraction from high-quality epitaxial 2D-materials

A broad, bell-shaped intensity component is observed in low-energy electron diffraction from high-quality epitaxial 2D-systems. Three 2D-systems, graphene on Ir(111), graphene on SiC(0001), and hexagonal boron nitride on Ir(111), have been prepared in situ under ultra-high vacuum conditions. In all three systems—independent of substrate material—similar strong diffuse intensity is observed, exhibiting a width as large as 50% of the Brillouin zone and an integrated intensity more than 10 times the intensity of the Bragg spots. The presented experimental results provide evidence for a common origin of such diffuse diffraction intensity in different atomically thin 2D-materials.

Omambac, K. (ORCID:0000000250139567)↗

Opportunities in electrically tunable 2D materials beyond graphene: Recent progress and future outlook

The interest in two-dimensional and layered materials continues to expand, driven by the compelling properties of individual atomic layers that can be stacked and/or twisted into synthetic heterostructures. The plethora of electronic properties as well as the emergence of many different quasiparticles, including plasmons, polaritons, trions, and excitons with large, tunable binding energies that all can be controlled and modulated through electrical means, has given rise to many device applications. In addition, these materials exhibit both room-temperature spin and valley polarization, magnetism, superconductivity, piezoelectricity that are intricately dependent on the composition, crystal structure, stacking, twist angle, layer number, and phases of these materials. Initial results on graphene exfoliated from single bulk crystals motivated the development of wide-area, high purity synthesis and heterojunctions with atomically clean interfaces. Now by opening this design space to new synthetic two-dimensional materials “beyond graphene,” it is possible to explore uncharted opportunities in designing novel heterostructures for electrically tunable devices. To fully reveal the emerging functionalities and opportunities of these atomically thin materials in practical applications, this review highlights several representative and noteworthy research directions in the use of electrical means to tune these aforementioned physical and structural properties, with an emphasis on discussing major applications of beyond graphene 2D materials in tunable devices in recent years and an outlook of what is to come in the next decade.

Vincent, Tom (ORCID:0000000159749137)↗

Spectral and polarization based imaging in deep-ultraviolet excited photoelectron microscopy

Using photoelectron emission microscopy, nanoscale spectral imaging of atomically thin MoS2 buried between Al2O3 and SiO2 is achieved by monitoring the wavelength and polarization dependence of the photoelectron signal excited by deep-ultraviolet light. Although photons induce the photoemission, images can exhibit resolutions below the photon wavelength as electrons sense the response. To validate this concept, the dependence of photoemission yield on the wavelength and polarization of the exciting light was first measured and then compared to simulations of the optical response quantified with classical optical theory. A close correlation between experiment and theory indicates that photoemission probes the optical interaction of UV-light with the material stack directly. The utility of this probe is then demonstrated when both the spectral and polarization dependence of photoemission observe spatial variation consistent with grains and defects in buried MoS2. Taken together, these new modalities of photoelectron microscopy allow mapping of optical property variation at length scales unobtainable with conventional light-based microscopy.

Beechem, Thomas E. (ORCID:0000000275360719)↗

Area-selective deposition of germanium on patterned graphene/monolayer molybdenum disulfide stacks via dipole engineering

Heterogeneous integration of two-dimensional materials and the conventional semiconductor has opened opportunities for next-generation semiconductor devices and their processing. Heterogeneous integration has been studied for economical manufacturing by substrate recycling and novel functionalities by a combination of incommensurate materials. However, utilizing the integration requires controlling locations of the integrated architectures. Here, we show area-selective deposition (ASD) of germanium on the graphene/MoS 2 stack. Ge nucleation precisely occurred on the surfaces of the patterned graphene/MoS 2 stack via dipole engineering. In this study, the growth temperature of ASD of Ge was significantly lower than that based on precursor desorption on SiO 2 . The first-principles calculations revealed that Ge deposited by ASD on the graphene/MoS 2 stack was not affected by charge transfer. This work provides a viable way to utilize atomically thin materials for next-generation semiconductor devices, which can be applicable for “Beyond Moore” and “More Moore” approaches.

2D materials↗

Nonlinear optics in 2D materials: From classical to quantum

Nonlinear optics has long been a cornerstone of modern photonics, enabling a wide array of technologies, from frequency conversion to the generation of ultrafast light pulses. Recent breakthroughs in two-dimensional (2D) materials have opened a frontier in this field, offering new opportunities for both classical and quantum nonlinear optics. These atomically thin materials exhibit strong light–matter interactions and large nonlinear responses, thanks to their tunable lattice symmetries, strong resonance effects, and highly engineerable band structures. In this paper, we explore the potential that 2D materials bring to nonlinear optics, covering topics from classical nonlinear optics to nonlinearities at the few-photon level. We delve into how these materials enable possibilities, such as symmetry control, phase matching, and integration into photonic circuits. The fusion of 2D materials with nonlinear optics provides insights into the fundamental behaviors of elementary excitations—such as electrons, excitons, and photons—in low-dimensional systems and has the potential to transform the landscape of next-generation photonic and quantum technologies.

2D materials↗

Superconductivity enhancement in phase-engineered molybdenum carbide/disulfide vertical heterostructures

Stacking layers of atomically thin transition-metal carbides and two-dimensional (2D) semiconducting transition-metal dichalcogenides, could lead to nontrivial superconductivity and other unprecedented phenomena yet to be studied. In this work, superconducting α-phase thin molybdenum carbide flakes were first synthesized, and a subsequent sulfurization treatment induced the formation of vertical heterolayer systems consisting of different phases of molybdenum carbide—ranging from α to γ' and γ phases—in conjunction with molybdenum sulfide layers. These transition-metal carbide/disulfide heterostructures exhibited critical superconducting temperatures as high as 6 K, higher than that of the starting single-phased α-Mo 2 C (4 K). We analyzed possible interface configurations to explain the observed moiré patterns resulting from the vertical heterostacks. Our density-functional theory (DFT) calculations indicate that epitaxial strain and moiré patterns lead to a higher interfacial density of states, which favors superconductivity. Such engineered heterostructures might allow the coupling of superconductivity to the topologically nontrivial surface states featured by transition-metal carbide phases composing these heterostructures potentially leading to unconventional superconductivity. Moreover, we envisage that our approach could also be generalized to other metal carbide and nitride systems that could exhibit high-temperature superconductivity.

heterostructure↗

Unveiling defect-mediated carrier dynamics in monolayer semiconductors by spatiotemporal microwave imaging

The optoelectronic properties of atomically thin transition-metal dichalcogenides are strongly correlated with the presence of defects in the materials, which are not necessarily detrimental for certain applications. For instance, defects can lead to an enhanced photoconduction, a complicated process involving charge generation and recombination in the time domain and carrier transport in the spatial domain. Here, we report the simultaneous spatial and temporal photoconductivity imaging in two types of WS 2 monolayers by laser-illuminated microwave impedance microscopy. The diffusion length and carrier lifetime were directly extracted from the spatial profile and temporal relaxation of microwave signals, respectively. Time-resolved experiments indicate that the critical process for photoexcited carriers is the escape of holes from trap states, which prolongs the apparent lifetime of mobile electrons in the conduction band. As a result, counterintuitively, the long-lived photoconductivity signal is higher in chemical-vapor deposited (CVD) samples than exfoliated monolayers due to the presence of traps that inhibits recombination. Overall, our work reveals the intrinsic time and length scales of electrical response to photoexcitation in van der Waals materials, which is essential for their applications in optoelectronic devices.

42 ENGINEERING↗

Moiréless correlations in ABCA graphene

Atomically thin van der Waals materials stacked with an interlayer twist have proven to be an excellent platform toward achieving gate-tunable correlated phenomena linked to the formation of flat electronic bands. In this work we demonstrate the formation of emergent correlated phases in multilayer rhombohedral graphene––a simple material that also exhibits a flat electronic band edge but without the need of having a moiré superlattice induced by twisted van der Waals layers. We show that two layers of bilayer graphene that are twisted by an arbitrary tiny angle host large (micrometer-scale) regions of uniform rhombohedral four-layer (ABCA) graphene that can be independently studied. Scanning tunneling spectroscopy reveals that ABCA graphene hosts an unprecedentedly sharp van Hove singularity of 3–5-meV half-width. We demonstrate that when this van Hove singularity straddles the Fermi level, a correlated many-body gap emerges with peak-to-peak value of 9.5 meV at charge neutrality. Mean-field theoretical calculations for model with short-ranged interactions indicate that two primary candidates for the appearance of this broken symmetry state are a charge-transfer excitonic insulator and a ferrimagnet. Finally, we show that ABCA graphene hosts surface topological helical edge states at natural interfaces with ABAB graphene which can be turned on and off with gate voltage, implying that small-angle twisted double-bilayer graphene is an ideal programmable topological quantum material.

42 ENGINEERING↗

In vitro investigation of protein assembly by combined microscopy and infrared spectroscopy at the nanometer scale

The nanoscale structure and dynamics of proteins on surfaces has been extensively studied using various imaging techniques, such as transmission electron microscopy and atomic force microscopy (AFM) in liquid environments. These powerful imaging techniques, however, can potentially damage or perturb delicate biological material and do not provide chemical information, which prevents a fundamental understanding of the dynamic processes underlying their evolution under physiological conditions. Here, we use a platform developed in our laboratory that enables acquisition of infrared (IR) spectroscopy and AFM images of biological material in physiological liquids with nanometer resolution in a cell closed by atomically thin graphene membranes transparent to IR photons. In this work, we studied the self-assembly process of S-layer proteins at the graphene-aqueous solution interface. The graphene acts also as the membrane separating the solution containing the proteins and Ca 2+ ions from the AFM tip, thus eliminating sample damage and contamination effects. The formation of S-layer protein lattices and their structural evolution was monitored by AFM and by recording the amide I and II IR absorption bands, which reveal the noncovalent interaction between proteins and their response to the environment, including ionic strength and solvation. Our measurement platform opens unique opportunities to study biological material and soft materials in general.

59 BASIC BIOLOGICAL SCIENCES↗

Interlayer engineering of Fe 3 GeTe 2 : From 3D superlattice to 2D monolayer

The discoveries of ferromagnetism down to the atomically thin limit in van der Waals (vdW) crystals by mechanical exfoliation have enriched the family of magnetic thin films [C. Gong et al., Nature 546 , 265–269 (2017) and B. Huang et al., Nature 546 , 270–273 (2017)]. However, compared to the study of traditional magnetic thin films by physical deposition methods, the toolbox of the vdW crystals based on mechanical exfoliation and transfer suffers from low yield and ambient corrosion problem and now is facing new challenges to study magnetism. For example, the formation of magnetic superlattice is difficult in vdW crystals, which limits the study of the interlayer interaction in vdW crystals [M. Gibertini, M. Koperski, A. F. Morpurgo, K. S. Novoselov, Nat. Nanotechnol. 14 , 408–419 (2019)]. Here, we report a strategy of interlayer engineering of the magnetic vdW crystal Fe 3 GeTe 2 (FGT) by intercalating quaternary ammonium cations into the vdW spacing. Both three-dimensional (3D) vdW superlattice and two-dimensional (2D) vdW monolayer can be formed by using this method based on the amount of intercalant. On the one hand, the FGT superlattice shows a strong 3D critical behavior with a decreased coercivity and increased domain wall size, attributed to the co-engineering of the anisotropy, exchange interaction, and electron doping by intercalation. On the other hand, the 2D vdW few layers obtained by over-intercalation are capped with organic molecules from the bulk crystal, which not only enhances the ferromagnetic transition temperature ( T C ), but also substantially protects the thin samples from degradation, thus allowing the preparation of large-scale FGT ink in ambient environment.

36 MATERIALS SCIENCE↗