Highly Thermoconductive, Strong Graphene-Based Composite Films by Eliminating Nanosheets Wrinkles.

Graphene-based thermally conductive composites have been proposed as effective thermal management materials for cooling high-power electronic devices. However, when flexible graphene nanosheets are assembled into macroscopic thermally conductive composites, capillary forces induce shrinkage of graphene nanosheets to form wrinkles during solution-based spontaneous drying, which greatly reduces the thermal conductivity of the composites. Herein, graphene nanosheets/aramid nanofiber (GNS/ANF) composite films with high thermal conductivity were prepared by in-plane stretching of GNS/ANF composite hydrogel networks with hydrogen bonds and π-π interactions. The in-plane mechanical stretching eliminates graphene nanosheets wrinkles by suppressing inward shrinkage due to capillary forces during drying and achieves a high in-plane orientation of graphene nanosheets, thereby creating a fast in-plane heat transfer channel. The composite films (GNS/ANF-60 wt%) with eliminated graphene nanosheets wrinkles showed a significant increase in thermal conductivity (146 W m-1 K-1) and tensile strength (207 MPa). The combination of these excellent properties enables the GNS/ANF composite films to be effectively used for cooling flexible LED chips and smartphones, showing promising applications in the thermal management of high-power electronic devices.

First-Principles Investigation of Nucleobase Detection by Tetranitrogen Coordinated Transition Metal Doped Graphene Nanoribbons.

Detection of nucleobases is of great significance in DNA sequencing, which is one of the main goals of the Human Genome Project. By employing the nonequilibrium Green function method combined with density functional theory, we proposed a biosensor based on the TMN4 (TM = Ni, Cu) embedded graphene nanoribbons for nucleobase detection. The adsorption energy calculations show that all five nucleobases are physisorbed on the TMN4-doped graphene nanoribbons. Utilizing the distinction of current, the bases T, C, and U can be gradually detected at the biases of 0.4, 0.6, and 0.8 V by NiN4-doped graphene nanoribbons, respectively. The bases A and G can be finally distinguished by CuN4-doped graphene nanoribbons under an external bias of not less than 0.8 V. The identification of individual nucleobases at specific biases could provide a novel mechanism for the further development of biosensors in rapid genome sequencing applications.

Tunable valley splitting in two-dimensional CrBr3/VSe2van der Waals heterostructure under strains and electric fields.

Valleytronics opens up fascinating opportunities for using the valley degree of freedom in information storage and quantum computation. Here, based on the first-principles calculations, we investigate the effects of biaxial strains and electric fields on the magnetic, electronic, and valleytronic properties of two-dimensional CrBr3/VSe2van der Waals (vdW) heterostructure consisting of two ferromagnetic monolayers. An interlayer magnetic phase transition from parallel to antiparallel is found when a compressive strain exceeds-2%or a tensile strain exceeds 4% is applied, while the interlayer magnetic configuration remains parallel under perpendicular electric fields. The valley splitting in the conduction bands is significantly enhanced by a compressive strain or an electric field pointing from the VSe2to the CrBr3layer. Specifically, a large valley splitting about 30.8 meV is obtained in the system with antiparallel interlayer magnetic configurations under a compressive strain of-4%, which is more than three times that of pristine CrBr3/VSe2heterostructure. Our findings provide new insights into the future valleytronic applications for two-dimensional magnetic vdW heterostructures.

Ballistic thermal rectification in asymmetric homojunctions.

Ballistic thermal rectification is of significance for the management of thermal transport at the nanoscale since the size of thermal devices shrinks down to the phonon mean free path. By using the single-particle Lorentz gas model, the ballistic thermal transport in asymmetric homojunctions is investigated. The ballistic thermal rectification of the asymmetric rectangular homojunction is enhanced by the increasing structural asymmetry. A hyperbolic tangent profile is introduced to the interface to study the effect of interface steepness on thermal transport. We find that the thermal rectification ratio increases with the decreasing interface steepness, indicating that a gradual interface is of benefit to increase the thermal rectification. Moreover, the thermal rectification of the asymmetric homojunction can be improved by either increasing the temperature gradient or decreasing the average temperature of two heat sources.

Enhanced robustness of half-metallicity in VBr3 nanowires by strains and transition metal doping.

The study of half-metallic behavior for transition metal tribromide nanowires is of great significance to the basic research and application in spintronics. We have theoretically investigated the spin transport properties of half-metallic VBr3 nanowires sandwiched between Au(100) electrodes. For the VBr3 nanowire with a length of 24.75 Å, the spin-filter efficiency (SFE) achieves 100% when the applied bias is less than 0.4 V. The robustness of half-metallic behavior in VBr3 nanowires is investigated by strains and transition metal doping. The bias range of VBr3 nanowires exhibiting perfect SFE is extended by tensile strains, while it becomes narrower under compressive strains. For VBr3 nanowires doped with Co and Cr, the bias range with ideal SFE is significantly broadened at a low doping concentration. In particular, the VBr3 nanowire doped with 1 Cr atom exhibits perfect SFE in an extremely wide bias range of 0-1.0 V. Our results show that the robustness of half-metallicity of VBr3 nanowires can be improved by tensile strains or certain doping, which provides promising ways for further design of high-performance spintronic devices.

Thermal Hall effect from a modified Lorentz gas model.

We systematically investigate the thermal Hall effect in a Lorentz gas model with rotating circular scatterers; the rotating scatterers play a role similar to the magnetic field. The modified Lorentz gas model is a normal thermal transport system that satisfies Fourier law: the thermal conductivity is independent of the model length. We find that the intensity of the Hall effect changes its sign when the rotating direction of disks changes and it is independent of the magnitude of longitudinal temperature difference and only dependent of the average longitudinal temperature: it decreases with increasing the average temperature, especially at low angular velocity. The thermal Hall effect found in the modified Lorentz gas will help us understand the mechanism of the thermal Hall system and provide guidance for the application of the thermal Hall effect.

First principles modeling of pure black phosphorus devices under pressure.

Black phosphorus (BP) has a pressure-dependent bandgap width and shows the potential for applications as a low-dimensional pressure sensor. We built two kinds of pure BP devices with zigzag or armchair conformation, and explored their pressure-dependent conductance in detail by using first principles calculations. The zigzag BP devices and the armchair BP devices exhibit different conductance-pressure relationships. For the zigzag BP devices conductance is robust against stress when the out-of-plane pressure ratio is less than 15%, and then increases rapidly until the conductive channels are fully opened. For the armchair pure BP devices conductance decreases at first by six orders of magnitude under increasing pressure and then increases quickly with further increase of pressure until the devices enter the on-state. This shows that the pure zigzag BP devices are more suitable for the application as flexible electronic devices with almost constant conductance under small pressure, while armchair BP devices can serve as bidirectional pressure sensors. Real-space distributions of band alignments were explored to understand the different pressure-related properties. We fitted a set of parameters based on the results from the empirical Wentzel-Kramers-Brillouin method, which provides an effortless approximation to quantitatively predict the pressure-related behaviors of large pure BP devices.

Magnetization dynamics induced by the Rashba effect in ferromagnetic films.

Manipulating the magnetization of ferromagnets by the current-induced spin-orbit torque has great potential application in the design of low energy consumption spintronic devices. Normally, an external magnetic field is needed for the reversal of current assisted magnetization by the spin-orbit torque. Recently, the switching of magnetization driven by the spin-orbit torque in the absence of an external magnetic field was reported in a Ta/Co20Fe60B20/TaOx system with lateral structural asymmetry. To understand the physics behind this experiment, we performed first principles calculations on the potential profile at the interface between the ferromagnetic film and the wedge-shaped deposited metal oxide in the Ta/Co/TaO system. This revealed that the lateral structural asymmetry generates two additional Rashba interactions which can reduce the minimum external field required to reverse the magnetization. In addition, we derived the Landau-Lifshitz-Gilbert equation from a quantum transport perspective and numerically investigated the magnetization dynamics in ferromagnetic films induced by Rashba interactions including those generated by lateral asymmetry. Our theoretical simulation provides microscopic explanations of experimental observations of magnetization switching in the absence of an external field of devices with lateral structural asymmetry.

Ultraviolet Photoluminescence of Carbon Nanospheres and its Surface Plasmon-Induced Enhancement.

Ultraviolet (UV) light can be used in versatile applications ranging from photoelectronic devices to biomedical imaging. In the development of new UV light sources, in this study, stable UV emission at ≈350 nm is unprecedentedly obtained from carbon nanospheres (CNSs). The origin of the UV fluorescence is comprehensively investigated via various characterization methods, including Raman and Fourier transform infrared analyses, with comparison to the visible emission of carbon nanodots. Based on the density functional calculations, the UV fluorescence is assigned to the carbon nanostructures bonded to bridging O atoms and dangling -OH groups. Moreover, a twofold enhancement in the UV emission is acquired for Au-carbon core-shell nanospheres (Au-CNSs). This remarkable modification of the UV emission is primarily ascribed to charge transfer between the CNSs and the Au surface.

Nonequilibrium spin injection in monolayer black phosphorus.

Monolayer black phosphorus (MBP) is an interesting emerging electronic material with a direct band gap and relatively high carrier mobility. In this work we report a theoretical investigation of nonequilibrium spin injection and spin-polarized quantum transport in MBP from ferromagnetic Ni contacts, in two-dimensional magnetic tunneling structures. We investigate physical properties such as the spin injection efficiency, the tunnel magnetoresistance ratio, spin-polarized currents, charge currents and transmission coefficients as a function of external bias voltage, for two different device contact structures where MBP is contacted by Ni(111) and by Ni(100). While both structures are predicted to give respectable spin-polarized quantum transport, the Ni(100)/MBP/Ni(100) trilayer has the superior properties where the spin injection and magnetoresistance ratio maintains almost a constant value against the bias voltage. The nonequilibrium quantum transport phenomenon is understood by analyzing the transmission spectrum at nonequilibrium.

First-principles investigation of quantum transport through an endohedral N@C60 in the Coulomb blockade regime.

We report an investigation of Coulomb blockade transport through an endohedral N@C60 weakly coupled with aluminum leads, employing the first-principles method combined with the Keldysh non-equilibrium Green's function derived from the equation of motion beyond the Hartree-Fock approximation. The differential conductance characteristics of the molecular device are calculated within the Coulomb blockade regime, which shows the Coulomb diamond as observed experimentally. When the gate voltage is less than that of the degeneracy point, there are two peaks in the differential conductance with an excited state induced by the change of the exchange interaction between the spin of C60 and the encapsulated nitrogen atom due to the transition from N@C(1-)(60) to N@C(2-)(60), while for a gate voltage larger than that of the degeneracy point, no excited state is available due to the quenching of exchange energy. As a result, there is only one Coulomb blockade peak in the differential conductance from the electron tunneling through the highest energy level below the Fermi level. Our first-principles results are in good agreement with experimental data obtained by an endohedral N@C60 molecular device.

Boro-norleucine as a P1 residue for the design of selective and potent DPP7 inhibitors.

Dipeptide-based inhibitors with C-substituted (alkyl or aminoalkyl) alpha-amino acids in the P2 position and boro-norleucine (boro-Nle) in the P1 position were synthesized. Relative to boro-proline, boro-Nle as a P1 residue was shown able to significantly dial out DPP4, FAP, DPP8, and DPP9 activity. Dab-boro-Nle (4g) proved to be the most selective and potent DPP7 inhibitor with a DPP7 IC50 value of 480 pM.

Synthesis and structure-activity relationship of N-alkyl Gly-boro-Pro inhibitors of DPP4, FAP, and DPP7.

The structure-activity relationship of various N-alkyl Gly-boro-Pro derivatives against three dipeptidyl peptidases (DPPs) was studied. In a series of N-cycloalkyl analogs, DPP4 and fibroblast activation protein-alpha (FAP) optimally preferred N-cycloheptyl whereas DPP7 tolerated even larger cycloalkyl rings. Gly alpha-carbon derivatization of N-cyclohexyl or N-(2-adamantyl) Gly-boro-Pro resulted in a significant decrease in potency against all the three DPPs.