Graphene-based Heterostructures Research Articles

Effect of grain boundaries on thermal transport in bi-layer graphene nano-ribbons

Defects and grain boundaries (GBs) in graphene often form during its growth and have been extensively characterized experimentally. Moreover, in graphene with two or more layers, distinct defect profiles have been identified in different layers. Although these defects and GBs are known to reduce the thermal transport in monolayer graphene, their impact on the overall thermal transport in graphene with two or more layers remains obscure, especially when unique defect profiles exist in different layers. In this study, we employ molecular dynamics simulations to investigate the role of GBs in one of the bi-layer graphene nanoribbons (GNRs), which results in a moiré-like pattern on one side of the GB. We discovered that while the GBs in one of the bi-layer GNR sheets reduce the overall in-plane thermal conductivity, κ, the reduction is mitigated by the pristine layer due to the interlayer van der Waals interaction. By closely examining different phonon modes in individual layers, we elucidate the κ reduction mechanisms in each layer. Our findings offer valuable insights into thermal engineering in graphene-based heterostructures as well as into exotic graphene bi-layer structures, such as those with moiré patterns.

Modeling and Simulation of 2D Transducers Based on Suspended Graphene-Based Heterostructures in Nanoelectromechanical Pressure Sensors.

Graphene-based two-dimensional (2D) heterostructures exhibit excellent mechanical and electrical properties, which are expected to exhibit better performances than graphene for nanoelectromechanical pressure sensors. Here, we built pressure sensor models based on suspended heterostructures of graphene/h-BN, graphene/MoS2, and graphene/MoSe2 by using COMSOL Multiphysics finite element software. We found that suspended circular 2D membranes show the best sensitivity to pressures compared to rectangular and square ones. We simulated the deflections, strains, resonant frequencies, and Young's moduli of suspended graphene-based heterostructures under the conditions of different applied pressures and geometrical sizes, built-in tensions, and the number of atomic layers of 2D membranes. The Young's moduli of 2D heterostructures of graphene, graphene/h-BN, graphene/MoS2, and graphene/MoSe2 were estimated to be 1.001 TPa, 921.08, 551.11, and 475.68 GPa, respectively. We also discuss the effect of highly asymmetric cavities on device performance. These results would contribute to the understanding of the mechanical properties of graphene-based heterostructures and would be helpful for the design and manufacture of high-performance NEMS pressure sensors.

Non-volatile Fermi level tuning for the control of spin-charge conversion at room temperature

Current silicon-based CMOS devices face physical limitations in downscaling size and power loss, restricting their capability to meet the demands for data storage and information processing of emerging technologies. One possible alternative is to encode the information in a non-volatile magnetic state and manipulate this spin state electronically, as in spintronics. However, current spintronic devices rely on the current-driven control of magnetization, which involves Joule heating and power dissipation. This limitation has motivated intense research into the voltage-driven manipulation of spin signals to achieve energy-efficient device operation. Here, we show non-volatile control of spin-charge conversion at room temperature in graphene-based heterostructures through Fermi level tuning. We use a polymeric ferroelectric film to induce non-volatile charging in graphene. To demonstrate the switching of spin-to-charge conversion we perform ferromagnetic resonance and inverse Edelstein effect experiments. The sign change of output voltage is derived by the change of carrier type, which can be achieved solely by a voltage pulse. Our results provide an alternative approach for the electric-field control of spin-charge conversion, which constitutes a building block for the next generation of spin-orbitronic memory and logic devices.

Twist-angle-tunable spin texture in WSe2/graphene van der Waals heterostructures.

Twist engineering has emerged as a powerful approach for modulating electronic properties in van der Waals heterostructures. While theoretical works have predicted the modulation of spin texture in graphene-based heterostructures by twist angle, experimental studies are lacking. Here, by performing spin precession experiments, we demonstrate tunability of the spin texture and associated spin-charge interconversion with twist angle in WSe2/graphene heterostructures. For specific twist angles, we detect a spin component radial with the electron's momentum, in addition to the standard orthogonal component. Our results show that the helicity of the spin texture can be reversed by twist angle, highlighting the critical role of the twist angle in the spin-orbit properties of WSe2/graphene heterostructures and paving the way for the development of spin-twistronic devices.

Raman spectroscopy and photoluminescence study of PN junction p-graphene/n-GaAs.

Single layer graphene (SLG) was synthesized via high-quality chemical vapor deposition (CVD) on high-quality copper and subsequently transferred onto SiO2 and on n-GaAs substrates with varying doping electron concentrations (n = 1016, 1017, 5 × 1017, 1018, and 5 × 1018cm-3). The n-GaAs substrates were grown by molecular beam epitaxy. The optical properties of the SLG were investigated through photoluminescence (PL) and Raman spectroscopy measurements. Carrier concentration n or p and Fermi energy (EF) values in SLG were determined both before and after the transfer onto n-GaAs, and these findings were validated through PL studies. The Raman spectroscopy results indicated an increase in the transfer of electrons from n-GaAs to SLG as the doping electron density in n-GaAs increased. PL analysis revealed a significant change in the bandgap energy (Eg) of n-GaAs due to bandgap narrowing and the Burstein-Moss shift. Our data enable us to determine the energy band diagrams. Upon aligning the energy bands, an increase in transferred carrier density is accompanied by changes in Fermi energies and an increase in the potential barrier (∆U). The increase in ∆U is of significant interest to ensure that charges are directed more efficiently toward the cell's electrical contacts in the case of photovoltaic application. There, they can contribute significantly to the generated electric current, thereby enhancing the performance of a cell. Our results can provide insights into the interaction in graphene-based heterostructures and aid in selecting the best parameters for developing new advanced devices.

Charge Transfer in Graphene-MoS2 Vertical Heterostructures Tuned by Stacking Order and Substrate-Introduced Electric Field.

Vertical van der Waals heterostructures composed of graphene (Gr) and transition metal dichalcogenides (TMDs) have created a fascinating platform for exploring optical and electronic properties in the two-dimensional limit. Numerous studies have focused on Gr/TMDs heterostructures to elucidate the underlying mechanisms of charge-energy transfer, quasiparticle formation, and relaxation following optical excitation. Nevertheless, a comprehensive understanding of interfacial charge separation and subsequent dynamics in graphene-based heterostructures remains elusive. Here, we have investigated the carrier dynamics of Gr-MoS2 heterostructures (including Gr/MoS2 and MoS2/Gr stacking sequences) grown on a fused silica substrate under varying photoexcitation energies by comprehensive ultrafast means, including time-resolved terahertz (THz) spectroscopy, THz emission spectroscopy, and transient absorption spectroscopy. Our findings highlight the impact of the substrate electric field on the efficiency of modulating the interfacial charge transfer (CT). Specifically, the optical excitation in Gr/MoS2 generates thermal electron injection from the graphene layer into the MoS2 layer with photon energy well below A-exciton of MoS2, whereas the interfacial CT in the MoS2/Gr is blocked by the electric field of the substrate. In turn, photoexcitation of the A exciton above leads to hole transfer from MoS2 to graphene, which occurs for both Gr-MoS2 heterostructures with opposite stacking orders, resulting in the opposite orientations of the interfacial photocurrent, as directly demonstrated by the out-of-phase THz emission. Moreover, we demonstrate that the recombination time of interfacial exciton is approximately ∼18 ps, whereas the defect-assisted interfacial recombination occurs on a time scale of ∼ns. This study provides valuable insights into the interplay between interfacial CT, substrate effects, and defect engineering in Gr-TMDs heterostructures, thereby facilitating the development of next-generation optoelectronic devices.

Integrated graphene-based semimetal/metallic-like MSe2 (M = Pt, Re) heterostructures for mid-infrared ultrafast photonics

Mid-infrared (MIR) ultrafast photonics has received significant interest due to the development of compact and robust MIR laser sources capable of emitting wavelengths beyond 2 μm. Transition metal selenides (TMSes), with the properties of feasibly tunable bandgaps, desirable photocarrier transmission property, and broadband nonlinear optical response, have become a research focus on ultrafast photonic applications. However, the relatively large bandgap (around 1 eV) of the TMSes greatly restricts their applications in the MIR region. Here, the synergetic interaction between multilayer graphene (Gr) and semimetal or metallic-like (PtSe2 and ReSe2) is employed to tune the optical properties and to further optimize the optical performance of TMSes in the MIR region. Benefiting from the ultrafast photocarrier relaxation time, appropriate modulation depth, and almost zero non-saturated loss of Gr-PtSe2 and Gr-ReSe2 heterostructures, stable Q-switched laser operation at 1.9 μm has been achieved in an integrated design based on waveguide laser platform. The results demonstrate that combining the semimetal or metallic-like TMSes with van der Waals (vdW) heterostructures is a promising strategy to extend the photonic applications of TMSes into the MIR region, indicating the potential applications of graphene-based TMSes vdW heterostructures for MIR integrated photonics.

CVD graphene contacts for lateral heterostructure MoS2 field effect transistors

Intensive research has been carried out on two-dimensional materials, in particular molybdenum disulfide, towards high-performance field effect transistors for integrated circuits1. Fabricating transistors with ohmic contacts is a challenging task due to the formation of a high Schottky barrier that severely limits the performance of the transistors for real-world applications. Graphene-based heterostructures can be used in addition to, or as a substitute for unsuitable metals. In this paper, we present lateral heterostructure transistors made of scalable chemical vapor-deposited molybdenum disulfide and chemical vapor-deposited graphene achieving a low contact resistances of about 9 kΩ·µm and high on/off current ratios of 108. Furthermore, we also present a theoretical model calibrated on our experiments showing further potential for scaling transistors and contact areas into the few nanometers range and the possibility of a substantial performance enhancement by means of layer optimizations that would make transistors promising for use in future logic integrated circuits.

Gate-Tunable Asymmetric Quantum Dots in Graphene-Based Heterostructures: Pure Valley Polarization and Confinement

We explore the possibility of attaining valley-dependent tunnelling and confinement using proximity-induced spin-orbit couplings (SOCs) in graphene-based heterostructures. We consider gate-tunable asymmetric quantum dots (AQDs) on graphene heterostructures and exhibiting a C3v and/or C6v symmetry. By employing a tight-binding model, we explicitly reveal a pure valley confinement and valley signal in AQDs by streaming the valley local density, leading to valley-charge separation in real space. The confinement of the valley quasi-bound states is sensitive to the locally induced SOCs and to the spatial distribution of the induced AQDs; it is also robust against on-site disorder. The adopted process of attaining a pure valley-Hall conductivity and confinement with zero charge currents is expected to provide more options towards valley-dependent electron optics.

Infrared photodetection in graphene-based heterostructures: bolometric and thermoelectric effects at the tunneling barrier

Graphene/hBN/graphene tunnel devices offer promise as sensitive mid-infrared photodetectors but the microscopic origin underlying the photoresponse in them remains elusive. In this work, we investigated the photocurrent generation in graphene/hBN/graphene tunnel structures with localized defect states under mid-IR illumination. We demonstrate that the photocurrent in these devices is proportional to the second derivative of the tunnel current with respect to the bias voltage, peaking during tunneling through the hBN impurity level. We revealed that the origin of the photocurrent generation lies in the change of the tunneling probability upon radiation-induced electron heating in graphene layers, in agreement with the theoretical model that we developed. Finally, we show that at a finite bias voltage, the photocurrent is proportional to either of the graphene layers heating under the illumination, while at zero bias, it is proportional to the heating difference. Thus, the photocurrent in such devices can be used for accurate measurements of the electronic temperature, providing a convenient alternative to Johnson noise thermometry.

Unveiling the electronic properties of BiP[formula omitted] triphosphide from bulk to graphene-based heterostructures by first-principles calculations

In our study, we investigated the structural and electronic properties of bismuth triphosphide (BiP3) in its bulk, few-layer, and monolayer forms. We found that BiP3 in bulk exhibits a metallic stable layered structure. The exfoliation energy of 1.07 J/m2 indicates ease exfoliation, comparable to other triphosphides. The band gap varies with thickness, transitioning from semiconductor–metal between four to five layers, influenced by interlayer coupling and quantum confinement. We also investigated the heterostructure created by depositing graphene (G) on few-layer BiP3. In monolayer (G/m-BiP3) and bilayer (G/2L-BiP3) forms, a metal–semiconductor junction is formed, characterized by weak vdW interactions at the interface and exhibiting p-type Schottky contacts. We observed that the Schottky Barrier Height (SBH) can be modulated by altering the interlayer distance between G and BiP3. This adjustment allows transitions between n-type and p-type Schottky contacts in G/m-BiP3 and the formation of an ohmic contact in G/2L-BiP3. Furthermore, applying an electric field affects the SBH, leading to similar transitions and the development of an ohmic contact. Additionally, our study shows that n-doping in graphene increases with the number of BiP3 layers and external electric field application. These properties position BiP3 few-layer as a promising material for nanoelectronic, optoelectronic, and graphene-based devices.

Broadband nonlinear optical response and sub-picosecond carrier dynamics in graphene-SnSe2 van der Waals heterostructures.

The van der Waals (vdWs) heterostructures, with vertical layer stacking structure of various two-dimensional (2D) materials, maintain the reliable photonic characteristics while compensating the shortcomings of the participating individual components. In this work, we combine the less-studied multilayer tin selenide (SnSe2) thin film with one of the traditional 2D materials, graphene, to fabricate the graphene-based vdWs optical switching element (Gr-SnSe2) with superior broadband nonlinear optical response. The transient absorption spectroscopy (TAS) measurement results verify that graphene acts as the recombination channel for the photogenerated carrier in the Gr-SnSe2 sample, and the fast recovery time can be reduced to hundreds of femtoseconds which is beneficial for the optical modulation process. The optical switching properties are characterized by the I-scan measurements, exhibiting a saturable energy intensity of 2.82 mJ·cm-2 (0.425 µJ·cm-2) and a modulation depth of 15.6% (22.5%) at the wavelength of 1030 nm (1980nm). Through integrating Gr-SnSe2 with a cladding waveguide, high-performance picosecond Q-switched operation in the near-infrared (NIR) and mid-infrared (MIR) spectral regions are both achieved. This work experimentally demonstrates the great potential of graphene-based vdWs heterostructures for applications in broadband ultrafast photonics.

Spin and charge fluctuation induced pairing in ABCB tetralayer graphene

Motivated by the recent experimental realization of ABCB stacked tetralayer graphene [Wirth , ], we study correlated phenomena in moiré-less graphene tetralayers for realistic interaction profiles using an orbital resolved random phase approximation approach. We demonstrate that magnetic fluctuations originating from local interactions are crucial close to the van Hove singularities on the electron- and hole-doped side promoting layer selective ferrimagnetic states. Spin fluctuations around these magnetic states enhance unconventional spin-triplet, valley-singlet superconductivity with f-wave symmetry due to intervalley scattering. Charge fluctuations arising from long range Coulomb interactions promote doubly degenerate p-wave superconductivity close to the van Hove singularities. At the conduction band edge of ABCB graphene, we find that both spin and charge fluctuations drive f-wave superconductivity. Our analysis suggests a strong competition between superconducting states emerging from long- and short-ranged Coulomb interactions and thus stresses the importance of microscopically derived interaction profiles to make reliable predictions for the origin of superconductivity in graphene-based heterostructures. Published by the American Physical Society 2024

Recent advances in nitrogen-doped graphene-based heterostructures and composites: mechanism and active sites for electrochemical ORR and HER

Role of different strategies in improving active sites of N-doped graphene based electrocatalysts for sustainable energy.

Modulating the Electrochemical Intercalation of Graphene Interfaces with α-RuCl3 as a Solid-State Electron Acceptor.

Intercalation reactions modify the charge density in van der Waals (vdW) materials through coupled electronic-ionic charge accumulation and are susceptible to modulation by interlayer hybridization in vdW heterostructures. Here, we demonstrate that charge transfer between graphene and α-RuCl3, which hole-dopes the graphene, greatly favors the intercalation of lithium ions into graphene-based vdW heterostructures. We systematically tune this effect on Li+ ion intercalation, modulating the intercalation potential, by using varying thicknesses of hexagonal boron nitride (hBN) as spacer layers between graphene and α-RuCl3. Confocal Raman spectroscopy and electronic transport measurements are used to monitor electrochemical intercalation, and density functional theory computations help quantify charge transfer to both α-RuCl3 and graphene upon Li intercalation. This work demonstrates a versatile approach for systematically modulating the electrochemical intercalation behavior of two-dimensional layers akin to electron donating/withdrawing substituent effects used to tune molecular redox potentials.

Completely switchable multi-mode narrowband terahertz absorber: Monolayer graphene, coupled topological interface states, and Rabi splitting

In the present study, we have explored the absorption properties of a monolayer graphene-based photonic heterostructure, which consists of topological photonic configurations, graphene, and a Bragg mirror. The optical attributes were computed by using the 4×4 transfer matrix method. The results indicate that the creation of topological interface states and strong coupling between these resonant modes result in mode splitting, leading to the formation of hybrid modes known as coupled topological interface states with unity transmittance. The number of absorption modes can be modulated with an appropriate selection of cascaded photonic structures. Our proposed design with 1, 3, 5, and 7 cascaded topological photonic structures provides 1, 5, 9, and 13 absorption modes with greater than 90% absorption. The findings also reveal that absorption peak strength is greatly influenced by Fermi-level and magnetic fields; switching of the modes from absorption to reflection and vice versa is achieved by suitable electrical and magnetic biasing. Our proposed design offers various applications, such as switchable filters, absorbers, and modulators.

Recent Advances in Graphene-Based Mesoporous Nanosheets for Supercapacitors

Among typical energy storage devices, supercapacitors play a predominant role in industry and our life owing to their rapid charge/discharge rate, superior lifespan, high power density, low cost, and outstanding safety. However, their low energy density has severely hindered their further development. For active electrode materials, graphene-based mesoporous nanosheets (GMNs) can combine the advantages from graphene and mesoporous materials, which can be applied to significantly enhance the energy density of supercapacitors. Here, we review the recent advances in GMNs for supercapacitors, focusing on in-plane mesoporous graphene and sandwich-like graphene-based heterostructures. Firstly, the synthesis of in-plane mesoporous graphene with ordered and disordered mesopores for supercapacitors is introduced. Secondly, sandwich-like graphene-based heterostructures are classified into mesoporous carbon/graphene, mesoporous heteroatom-doped carbon/graphene, mesoporous conducting polymer/graphene, and mesoporous metal oxide/graphene, and their applications in supercapacitors are discussed in detail. Finally, the challenges and opportunities of GMNs for high-performance supercapacitors are proposed.

The fundamental 1/f noise in monolayer graphene

A lower bound on the voltage noise power spectrum set by quantum indeterminacy exists in any conducting material. This bound is calculated explicitly for monolayer graphene taking into account graphene pseudospin/valley band structure. It is found to be of the form characteristic of the observed [Formula: see text] noise. It is shown that the deviation of [Formula: see text] from unity is a result of the piezoelectric interaction of charge carriers with acoustic phonons. A comparison with the measured [Formula: see text] noise in graphene and graphene-based heterostructures shows that the observed noise intensity is near the quantum bound. It is demonstrated that the recently observed sharp peak in [Formula: see text] at small gate voltages in the field-effect transistors based on graphene/boron nitride heterostructure is well reproduced by the theory, and is to be attributed to the out-of-plane piezoelectric activity in this heterostructure. A simple kinetic model is proposed to describe the effect of the charge carrier trapping on [Formula: see text].

Identification of Borophosphene/graphene heterostructure as anode for Li-ion Batteries and its origin

The development of two-dimensional (2D) material or heterostructure as an anode material is necessary to enhance the electrochemical performance of Li-ion batteries (LIBs) but finding the correct combination is a challenge. In the present work, using First principles study, we have proposed borophosphene (BP-ML) and graphene-based multilayer heterostructure as a possible anode material. We have found that BP-ML and graphene-based heterostructure are conductive in nature. Here, we have also investigated the role of Pz (π) and Py (σ) atomic orbital bands of BP-ML and graphene. On Li intercalation, charge transfer is mainly site and interface definitely which helps to improve the specific capacity. The specific capacity of the proposed heterostructure varies from 546 to 427 mA h/g. For maximum Li confirmation, the volume expansion of these heterostructures is about 14–16%. The presence of graphene helps to maintain the open-circuit voltage (OCV) of heterostructure on an average 0.7 V. Also, helps to support the diffusion barrier energy in the range of 0.27–0.71 eV. This proposed 2D heterostructure could be the future material for the LIB's anode material.

Analytical study of highly adjustable plasmonic modes in graphene-based heterostructure for THz applications

Analytical study of highly adjustable plasmonic modes in graphene-based heterostructure for THz applications