Future Nanodevices Research Articles

Ferroelectric Size Effects on Statics and Dynamics of Domain Wall.

Domain walls separating differently oriented polarization regions of ferroelectric materials are known to greatly impact nanoscale materials and device functionalities. Though the understanding of size effects in ferroelectric nanostructures has progressed, the effect of thickness downsizing on domain wall scaling behavior has remained unexplored. Using piezoresponse force microscopy, epitaxial BaTiO3 film thickness size (2-90nm) effects on the critical scaling universality of the domain wall dynamical creep and static roughness exponents including dimensionality is demonstrated. Independently estimated static roughness exponents ranging between 0.34 and 0.28 and dynamical creep exponents transition from 0.54 to 0.22 elucidate the domain wall dimensionality transition from two- to quasi-one-dimension in the thickness range of 10-25nm, which is later validated by evaluating effective dimensionality within the paradigm of random-bond universality. The observed interdimensional transition is further credenced to the compressive strain and long-range strain-dipolar interactions, as revealed by the structural analyses and additional measurements with modified substrate-induced strain. These results provide new insights into the understanding of size effects in nanoscale ferroelectricity, paving the way toward future nanodevices.

Nanometer-Sized Te Pistons in Carbon Cylinders as Nano-Motor Prototypes: Implications for Nano-Electromechanical Device Fabrication

Manipulation of nano-objects is fascinating as it not only facilitates the understanding of the essential properties of nanomaterials but also enlightens the design of future nano-devices beyond current micro-electromechanical systems. In this paper, a piston-cylinder-configured nano-motor prototype is designed and fabricated, in which nanometer-sized Te segments are electrically controlled to reciprocate inside the carbon cylinder serving as nano-pistons. The nano-motor prototype has a length of ∼550 nm, an outer diameter of ∼150 nm, and a piston diameter of ∼30 nm. Electron-wind and thermal expansion are two reciprocal forces that create a dynamic equilibrium on the Te pistons and enable the circulating motions. With bias control, a circulating rate of 0–4.3 counts per second has been achieved. This prototype is the smallest piston-cylinder-type nano-motor that has ever been reported and can provide new insights into investment casting-assisted nano-electromechanical device fabrication.

Evolutionary Plasmonic Properties of Single Truncated Ag Nanowire-on-Au Film Nanocavity

Noble metal nanocavities have been widely demonstrated to possess great potential applications in nano-optics and nanophotonics due to their extraordinary localized surface plasmon resonance. However, most metal nanocrystals synthesized by chemical methods often suffer from truncation with different degrees due to oxidation and dissolution of metal atoms at corner and edges. We investigate the influence of shape truncation on the plasmonic properties of single Ag nanowire on Au film nanocavity using the finite difference time domain method. When the Ag nanowire (the circumradius R 2 = 50 nm) is gradually truncated from pentagonal to circular geometry, the scattering peak position of the nanocavity shows prominent blue shift from 962 nm to 608 nm, suggesting a nonnegligible role of truncation on plasmonic properties. The electric field strength and charge distribution of the structure reveal the evolution from dipole mode to quadrupole mode. It is also found that the plasmon resonance wavelength is linearly dependent on the truncation ratio R 1/R 2 (R 1 is the inradius) and the modulation slope is also reliable to the size of Ag nanowire. Our observations could shed light on developing high-performance tunable optical nano-devices in future.

Nonvolatile electrical control of spin polarization in the 2D bipolar magnetic semiconductor VSeF

Nonvolatile electrical control of spin polarization in two-dimensional (2D) magnetic semiconductors is greatly appealing toward future low-dissipation spintronic nanodevices. Here, we report a 2D material VSeF, which is an intrinsic bipolar magnetic semiconductor (BMS) featured with opposite spin-polarized valence and conduction band edges. We then propose a general nonvolatile strategy to manipulate both spin-polarized orientations in BMS materials by introducing a ferroelectric gate with proper band alignment. The spin-up/spin-down polarization of VSeF is successfully controlled by the electric dipole of ferroelectric bilayer Al2Se3, verifying the feasibility of the design strategy. The interfacial doping effect from ferroelectric gate also plays a role in enhancing the Curie temperature of the VSeF layer. Two types of spin field effect transistors, namely multiferroic memory and spin filter, are further achieved in VSeF/Al2Se3 and VSeF/Al2Se3/Al2Se3 multiferroic heterostructures, respectively. This work will stimulate the application of 2D BMS materials in future spintronic nanodevices.

Nonvolatile Electrical Control and Reversible Gas Capture by Ferroelectric Polarization Switching in 2D FeI2/In2S3 van der Waals Heterostructures

Nonvolatile electrical control is the core of future magnetoelectric nanodevices. In this work, we systematically explore both the electronic structures and transport properties of multiferroic van der Waals (vdW) heterostructures consisting of a ferromagnetic FeI2 monolayer and a ferroelectric In2S3 monolayer using density functional theory and the nonequilibrium Green's function method. The results reveal that the FeI2 monolayer can be reversibly switched between semiconducting and half-metallic properties by nonvolatile control of the In2S3 ferroelectric polarization states. Correspondingly, the proof-of-concept two-probe nanodevice based on the FeI2/In2S3 vdW heterostructure exhibits a significant valving effect by modulating the ferroelectric switching. Moreover, it is also found that the preference of nitrogen-containing gases such as NH3, NO, and NO2 for adsorption on the surface of FeI2/In2S3 vdW heterostructures strongly depends on the polarization direction of the ferroelectric layer. In particular, the FeI2/In2S3 heterostructure shows reversible capture behavior for NH3. As a result, the FeI2/In2S3 vdW heterostructure-based gas sensor demonstrates high selectivity and sensitivity. These findings may open up a new route for the application of multiferroic heterostructures to spintronics, nonvolatile memories, and gas sensors.

Identifying, Resolving, and Quantifying Anisotropy in ReS2 Nanomechanical Resonators.

As an emerging two-dimensional semiconductor, rhenium disulfide (ReS2 ) is renowned for its strong in-plane anisotropy in electrical, optical, and thermal properties. In contrast to the electrical, optical, optoelectrical, and thermal anisotropies that are extensively studied in ReS2 , experimental characterization of mechanical properties has largely remained elusive. Here, it is demonstrated that the dynamic response in ReS2 nanomechanical resonators can be leveraged to unambiguously resolve such disputes. Using anisotropic modal analysis, the parameter space for ReS2 resonators in which mechanical anisotropy is best manifested in resonant responses is determined. By measuring their dynamic response in both spectral and spatial domains using resonant nanomechanical spectromicroscopy, it is clearly shown that ReS2 crystal is mechanically anisotropic. Through fitting numerical models to experimental results, it is quantitatively determined that the in-plane Young's moduli are 127 and 201GPa along the two orthogonal mechanical axes. In combination with polarized reflectance measurements, it is shown that the mechanical soft axis aligns with the Re-Re chain in the ReS2 crystal. These results demonstrate that dynamic responses in nanomechanical devices can offer important insights into intrinsic properties in 2D crystals and provide design guidelines for future nanodevices with anisotropic resonant responses.

Layer-dependent dielectric modulation in WS2/GaN heterostructures

Controlling over the electronic structure of two-dimensional (2D) semiconductors is crucial to unlock their full potential in the applications in future nanodevices. Here, we demonstrate a layer-dependent dielectric modulation of electronic structures in multilayer ${\mathrm{WS}}_{2}/\mathrm{GaN}$ heterostructures. The results investigated by means of in situ scanning tunneling microscopy/spectroscopy and photoluminescence spectroscopy show that the fluctuations of the dielectric environment induced by local corrugation of the GaN surface dramatically tune the band structure of monolayer ${\mathrm{WS}}_{2}$ with a large downshift of the valence band maximum by about 1.12 eV. Under the shielding effect of the first-layer ${\mathrm{WS}}_{2}$, the dielectric environment shows a weak modulation effect on the second-layer, and even has negligible influence on the third- and fourth-layer ${\mathrm{WS}}_{2}$. The relationship between dielectric environment and interfacial distance is further simulated through first-principles calculations. The electrostatic potential energy, differential charge densities, and charge transfer of the ${\mathrm{WS}}_{2}/\mathrm{GaN}$ heterostructure under different interfacial distances reveal that the differences of charge redistributions between the ${\mathrm{WS}}_{2}/\mathrm{GaN}$ interface and ${\mathrm{WS}}_{2}$ interlayer are responsible for the layer-dependent dielectric modulation. This work offers some references for the design and fabrication of novel 2D optoelectronic devices.

Phonon Dominated Thermal Transport in Metallic Niobium Diselenide from First Principles Calculations.

Niobium diselenide (NbSe2) is a layered transition metal dichalcogenide material which possesses unique electrical and superconducting properties for future nanodevices. While the superconducting, electrical, and bulk thermal transport properties of NbSe2 have been widely studied, the in-plane thermal transport property of NbSe2, which is important for potential thermoelectric applications, has not been thoroughly investigated. In this report, we study the lattice in-plane thermal transport of 2D NbSe2 by solving the phonon Boltzmann transport equation with the help of the first principles calculation. The thermal conductivity obtained at room temperature is 12.3 W/mK. A detailed analysis shows that the transverse acoustic phonon dominates the lattice thermal transport, and an anomalously small portion of electron contribution to the total thermal conductivity is observed for this metallic phase. The results agree well with experimental measurements and provide detailed mode-by-mode thermal conductivity contribution from different phonon modes. This study can provide useful information for integrating NbSe2 in nanodevices where both electrical and thermal properties are critical, showing great potential for integrating monolayer NbSe2 to thermoelectric devices.

Electric-field induced half-metallic properties in an experimentally synthesized CrSBr monolayer.

Two-dimensional (2D) half-metallic materials are highly desirable for nanoscale spintronic applications. Here, we propose a new mechanism that can achieve half-metallicity in 2D ferromagnetic (FM) materials with two-layer magnetic atoms by electric field tuning. We use a concrete example of an experimentally synthesized CrSBr monolayer to illustrate our proposal through first-principles calculations. It is found that half-metallic properties can be achieved in CrSBr within an appropriate electric field range, and the corresponding amplitude of electric field intensity can be realized experimentally. Janus monolayer Cr2S2BrI is constructed, which possesses a built-in electric field due to broken horizontal mirror symmetry. However, Cr2S2BrI without and with an applied external electric field is always a FM semiconductor. A possible memory device is also proposed based on the CrSBr monolayer. Our work will stimulate the application of 2D FM CrSBr in future spintronic nanodevices.

Hybrid normal-superconducting Aharonov-Bohm quantum thermal device

We propose and theoretically investigate the behavior of a ballistic Aharonov-Bohm (AB) ring when embedded in a N-S two-terminal setup, consisting of a normal metal (N) and superconducting (S) leads. This device is based on available current technologies and we show in this work that it constitutes a promising hybrid quantum thermal device, as a quantum heat engine and quantum thermal rectifier. Remarkably, we evidence the interplay of single-particle quantum interferences in the AB ring and of the superconducting properties of the structure to achieve the hybrid operating mode for this quantum device. Its efficiency as a quantum heat engine reaches of the Carnot efficiency, and we predict a thermal rectification factor attaining 350%. These results make this device highly promising for future phase-coherent caloritronic nanodevices.

Electric Field and Strain Tuning of 2D Semiconductor van der Waals Heterostructures for Tunnel Field-Effect Transistors.

Heterostacks consisting of low-dimensional materials are attractive candidates for future electronic nanodevices in the post-silicon era. In this paper, using first-principles calculations based on density functional theory (DFT), we explore the structural and electronic properties of MoTe2/ZrS2 heterostructures with various stacking patterns and thicknesses. Our simulations show that the valence band (VB) edge of MoTe2 is almost aligned with the conduction band (CB) edge of ZrS2, and (MoTe2)m/(ZrS2)m (m = 1, 2) heterostructures exhibit the long-sought broken gap band alignment, which is pivotal for realizing tunneling transistors. Electrons are found to spontaneously flow from MoTe2 to ZrS2, and the system resembles an ultrascaled parallel plate capacitor with an intrinsic electric field pointed from MoTe2 to ZrS2. The effects of strain and external electric fields on the electronic properties are also investigated. For vertical compressive strains, the charge transfer increases due to the decreased coupling between the layers, whereas tensile strains lead to the opposite behavior. For negative electric fields a transition from the type-III to the type-II band alignment is induced. In contrast, by increasing the positive electric fields, a larger overlap between the valence and conduction bands is observed, leading to a larger band-to-band tunneling (BTBT) current. Low-strained heterostructures with various rotation angles between the constituent layers are also considered. We find only small variations in the energies of the VB and CB edges with respect to the Fermi level, for different rotation angles up to 30°. Overall, our simulations offer insights into the fundamental properties of low-dimensional heterostructures and pave the way for their future application in energy-efficient electronic nanodevices.

Orthogonal Grade-Separated Nanowiring of Molecular Single Chains

Quasi-one-dimensional (1D) compounds are suitable models to develop future nanodevices. The critical issue is that most of the several hundred reported 1D compounds adopt parallel arrangements. Here, we report the first example of an orthogonal grade-separated arrangement of the halogen-bridged metal complex (MX-Chain) [PtII(en)2][PtIVCl2(en)2][FeIIICl5]2, abbreviated as [Pt(en)2Cl][FeIIICl5] (en = ethylenediamine), which is the first example of that arrangement of molecular single chains. The space group and topology are coincidentally same as alchemists’ gold, Hg3−δAsF6, which aligns as atomic single chains. This molecular nanostructure is very rare and valuable as a three-dimensional (3D) nanowiring model. The hydrogen bond network found in [Pt(en)2Cl][FeIIICl5] represents a new strategy for making such nanostructures. The structural and optical relationships are similar to those of typical Pt(II)/Pt(IV) mixed valent MX-Chains in charge-density-wave (CDW) states. Polarized Raman spectra strongly supported the presence of orthogonal grade-separated chains in CDW states. Thus, this work proved the concept of molecular single-chain grade-separated nanowiring.

Observation of charge density wave in layered hexagonal Cu1.89Te single crystal

Abstract We report comprehensive transport, electron microscopy and Raman spectroscopy studies on the transition-metal chalcogenides Cu1.89Te single crystals. The metallic Cu1.89Te displays successive metal-semiconductor transitions at low temperatures and almost ideal linear MR when magnetic field up to 33T. Through the electron diffraction patterns, the stable room temperature phase is identified as a 3×3×2 modulated superstructure based on Nowotny hexagonal structure. The superlattice spots of Transmission electron microscopy and Scanning tunneling microscopy clearly show the structural transitions from the room temperature Commensurate Ⅰ (C-Ⅰ) phase to the low temperature Commensurate Ⅱ (C-Ⅱ) phase. All the results can be understood in term of charge density wave (CDW) instability, yielding intuitive evidences for the CDW formations in Cu1.89Te. The additional Raman modes below room temperature further reveal that the zone-folded phonon modes may play an important role on the CDW transitions. Our research sheds light on the novel electron features of Cu1.89Te at low temperature, and may provide potential applications for future nano-devices.

Observation of Charge Density Wave in Layered Hexagonal Cu1.89Te Single Crystal

We report comprehensive transport, electron microscopy and Raman spectroscopy studies on transition-metal chalcogenides Cu1.89Te single crystals. The metallic Cu1.89Te displays successive metal-semiconductor transitions at low temperatures and almost ideal linear MR when magnetic field up to 33 T. Through the electron diffraction patterns, the stable room-temperature phase is identified as a 3 × 3 × 2 modulated superstructure based on the Nowotny hexagonal structure. The superlattice spots of transmission electron microscopy and scanning tunneling microscopy clearly show the structural transitions from the room-temperature commensurate I phase, named as C-I phase, to the low temperature commensurate II (C-II) phase. All the results can be understood in terms of charge density wave (CDW) instability, yielding intuitive evidences for the CDW formations in Cu1.89Te. The additional Raman modes below room temperature further reveal that the zone-folded phonon modes may play an important role on the CDW transitions. Our research sheds light on the novel electron features of Cu1.89Te at low temperature, and may provide potential applications for future nano-devices.

Vacancy-Regulated Charge Carrier Dynamics and Suppressed Nonradiative Recombination in Two-Dimensional ReX2 (X = S, Se).

Point defects in semiconductors usually act as nonradiative charge carrier recombination centers, which severely limit the performance of optoelectronic devices. In this work, by combining time-domain density functional theory with nonadiabatic molecular dynamics simulations, we demonstrate suppressed nonradiative charge carrier recombination and prolonged carrier lifetime in two-dimensional (2D) ReX2 (X = S, Se) with S/Se vacancies. In particular, a S vacancy introduces a shallow hole trap state in ReS2, while a Se vacancy introduces both hole and electron trap states in ReSe2. Photoexcited electrons and holes can be rapidly captured by these defect states, while the release process is slow, which contributes to an elongated photocarrier lifetime. The suppressed charge carrier recombination lies in the vacancy-induced low-frequency phonon modes that weaken electron-phonon coupling, as well as the reduced overlap between electron and hole wave functions that decreases nonadiabatic coupling. This work provides physical insights into the charge carrier dynamics of 2D ReX2, which may stimulate considerable interest in using defect engineering for future optoelectronic nanodevices.

Preparation, Supramolecular Organization, and On-Surface Reactivity of Enantiopure Subphthalocyanines: From Bulk to 2D-Polymerization.

The development of chiral materials is severely limited by the challenge to achieve enantiopure derivatives with both configurational stability and good optoelectronic properties. Herein we demonstrate that enantiopure subphthalocyanines (SubPcs) fulfill such demanding requirements and bear the prospect of becoming components of chiral technologies. Particularly, we describe the synthesis of enantiopure SubPcs and assess the impact of chirality on aspects as fundamental as the supramolecular organization, the behavior in contact with metallic surfaces, and the on-surface reactivity and polymerization. We find that enantiopure SubPcs remarkably tend to organize in columnar polar assemblies at the solid state and highly ordered chiral superstructures on Au(111) surfaces. At the metal interface, such SubPcs are singled out by scanning tunneling microscopy. DFT calculations suggest that SubPcs undergo a bowl-to-bowl inversion that was shown to be dependent on the axial substituent. Finally, we polymerize by means of on-surface synthesis a highly regular 2D, porous and chiral, π-extended polymer that paves the way to future nanodevice fabrication.

Synergy effect of temperature, electric and magnetic field on the depth structure of the FeRh/BaTiO3 composite multiferroic

FeRh based composite multiferroic materials have attracted great scientific interest due to their wide variety of possible applications in future nano device technology. In the recent work, a comprehensive study on the depth dependence of the metamagnetic phase transition in FeRh/BaTiO3 heterostructure is reported by means of single or combined external stimulus such as heat, magnetic or electric field. Grazing-incidence nuclear scattering experiments revealed significant discrepancies in the mechanism of the antiferromagnetic/ferromagnetic reordering induced by the different effects, with distinguished role of both upper and lower interfaces.

Mechanical and electronic properties of α−M2X3 ( M =Ga, In; X =S, Se) monolayers

Due to the atomic level thickness and novel properties, two-dimensional (2D) materials have received extensive attention on the research and application of future nanodevices. In this paper, the mechanical and electronic properties of $\ensuremath{\alpha}\text{\ensuremath{-}}{M}_{2}{X}_{3}$ ($M$ = Ga, In; $X$ = S, Se) monolayers are studied to explore their applications in 2D electronic devices. First-principles calculations based on density functional theory indicate that these four $\ensuremath{\alpha}\text{\ensuremath{-}}{M}_{2}{X}_{3}$ monolayers are all semiconductors and possess Young's modulus of less than 100 ${\mathrm{N}\phantom{\rule{0.16em}{0ex}}\mathrm{m}}^{\ensuremath{-}1}$ with a deformation range up to about 30%. In addition, the carrier mobility of the $\ensuremath{\alpha}\text{\ensuremath{-}}{M}_{2}{X}_{3}$ monolayer exceeds 600 ${\mathrm{cm}}^{2}\phantom{\rule{0.16em}{0ex}}{\mathrm{V}}^{\ensuremath{-}1}\phantom{\rule{0.16em}{0ex}}{\mathrm{s}}^{\ensuremath{-}1}$ and remains high under strain. In particular, because the band edge shifts under compressive strain, the electron mobility of the $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{Ga}}_{2}{\mathrm{S}}_{3}$ monolayer increases to about 1800 ${\mathrm{cm}}^{2}\phantom{\rule{0.16em}{0ex}}{\mathrm{V}}^{\ensuremath{-}1}\phantom{\rule{0.16em}{0ex}}{\mathrm{s}}^{\ensuremath{-}1}$ at $\ensuremath{-}3%$ strain, which is approximately three times the value without strain. The excellent ductility and strain-promoted electronic properties make the 2D $\ensuremath{\alpha}\text{\ensuremath{-}}{M}_{2}{X}_{3}$ promising candidates for the application of flexible electronic devices.

Evaluation of TEM methods for their signature of the number of layers in mono- and few-layer TMDs as exemplified by MoS2 and MoTe2

In mono- and few-layer 2D materials, the exact number of layers is a critical parameter, determining the materials’ properties and thus their performance in future nano-devices. Here, we evaluate in a systematic manner the signature of exfoliated free-standing mono- and few-layer MoS2 and MoTe2 in TEM experiments such as high-resolution transmission electron microscopy, electron energy-loss spectroscopy, and 3D electron diffraction. A reference for the number of layers has been determined by optical contrast and AFM measurements on a substrate. Comparing the results, we discuss strengths and limitations, benchmarking the three TEM methods with respect to their ability to identify the exact number of layers.

Size-Specific Magnetic Configurations in Electrodeposited Epitaxial Iron Nanocuboids: From Landau Pattern to Vortex and Single Domain States.

As the size of magnetic devices continuously decreases, the creation of three-dimensional nanomagnets and the understanding of their magnetic configurations become increasingly important for modern applications. Here, by progressive nucleation during epitaxial nanoelectrodeposition, we synthesize single-crystal iron nanocuboids with sizes ranging 10 to 200 nm on one sample. The size-dependent magnetic configurations of these nanocuboids are studied by quantitative magnetic force microscopy and electron holography. In conjunction, a "magnetic configuration versus size" phase diagram is established via micromagnetic simulations. Both experiment and theory reveal a sequential transition from Landau pattern to vortex and finally single domain when decreasing the sizes of the nanocuboids. The combinatorial-like approach leads to a quantitative understanding of the magnetic configurations of the nanomagnets in a broad size range. It can be transferred to other materials and shapes and thereby presents an advanced route to enrich the material library for future nanodevice design.