Bilayer Graphene Devices Research Articles

Revealing flat bands and hybridization gaps in a twisted bilayer graphene device with microARPES

Controlling the electronic structure of two-dimensional materials using the combination of twist angle and electrostatic doping is an effective means to induce emergent phenomena. In bilayer graphene with an interlayer twist angle near the magic angle, the electronic dispersion is strongly modified by a manifold of hybridizing moiré Dirac cones leading to flat band segments with strong electronic correlations. Numerous technical challenges arising from spatial inhomogeneity of interlayer interactions, twist angle and device functionality have so far limited momentum-resolved electronic structure measurements of these systems to static conditions. Here, we present a detailed characterization of the electronic structure exhibiting miniband dispersions for twisted bilayer graphene, near the magic angle, integrated in a functional device architecture using micro-focused angle-resolved photoemission spectroscopy. The optimum conditions for visualizing the miniband dispersion are determined by exploiting the spatial resolution and photon energy tunability of the light source and applied to extract a hybridization gap size of eV and flat band segments extending across a moiré mini Brillouin zone. In situ electrostatic gating of the sample enables significant electron-doping, causing the conduction band states to shift below the Fermi energy. Our work emphasizes key challenges in probing the electronic structure of magic angle bilayer graphene devices and outlines conditions for exploring the doping-dependent evolution of the dispersion that underpins the ability to control many-body interactions in the material.

Valley-dependent transport in a mescoscopic twisted bilayer graphene device

We study the valley-dependent electron transport in a four-terminal mesoscopic device of the two monolayer graphene nanoribbons vertically stacked together, where the intersection forms a bilayer graphene lattice with a controllable twist angle. Using a tight-binding lattice model, we show that the longitudinal and transverse conductances exhibit significant valley polarization in the low energy regime for small twist angles. As the twist angle increases, the valley polarization shifts to the high energy regime. This arises from the regrouping effect of the electron band in the twisted bilayer graphene region. But for relatively large twist angles, no significant valley polarization is observed. These results are consistent with the spectral densities of the twisted bilayer graphene.

Electron-hole asymmetric magnetotransport of graphene-colloidal quantum dot device

Interfacing graphene with other low-dimensional material has gained attentions recently due to its potential to stimulate new physics and device innovations for optoelectronic and electronic applications. Here, we exploit a solution-processed approach to introduce colloidal quantum dot (CQD) to the bilayer graphene device. The magnetotransport properties of the graphene device is drastically altered due to the presence of the CQD potential, leading to the observation of AB-like oscillation in the quantum Hall regime and screening of the intervalley scattering. The anomalous magnetotransport behavior is attributed to the coulombic scattering introduced by the CQDs and is shown to be highly asymmetric depending on the polarity of the transport carriers. These results prove the potential of such flexible method for engineering microscopic scattering process and performance of the graphene device that may lead to intriguing device application in such hybrid system.

Intrinsic Nonlinear Hall Effect and Gate-Switchable Berry Curvature Sliding in Twisted Bilayer Graphene.

Though the observation of the quantum anomalous Hall effect and nonlocal transport response reveals nontrivial band topology governed by the Berry curvature in twisted bilayer graphene, some recent works reported nonlinear Hall signals in graphene superlattices that are caused by the extrinsic disorder scattering rather than the intrinsic Berry curvature dipole moment. In this Letter, we report a Berry curvature dipole induced intrinsic nonlinear Hall effect in high-quality twisted bilayer graphene devices. We also find that the application of the displacement field substantially changes the direction and amplitude of the nonlinear Hall voltages, as a result of a field-induced sliding of the Berry curvature hotspots. Our Letter not only proves that the Berry curvature dipole could play a dominant role in generating the intrinsic nonlinear Hall signal in graphene superlattices with low disorder densities, but also demonstrates twisted bilayer graphene to be a sensitive and fine-tunable platform for second harmonic generation and rectification.

Layer-Dependent Interaction Effects in the Electronic Structure of Twisted Bilayer Graphene Devices.

Near the magic angle, strong correlations drive many intriguing phases in twisted bilayer graphene (tBG) including unconventional superconductivity and chern insulation. Whether correlations can tune symmetry breaking phases in tBG at intermediate (≳ 2°) twist angles remains an open fundamental question. Here, using ARPES, we study the effects of many-body interactions and displacement field on the band structure of tBG devices at an intermediate (3°) twist angle. We observe a layer- and doping-dependent renormalization of bands at the K points that is qualitatively consistent with moiré models of the Hartree-Fock interaction. We provide evidence of correlation-enhanced inversion symmetry-breaking, manifested by gaps at the Dirac points that are tunable with doping. These results suggest that electronic interactions play a significant role in the physics of tBG even at intermediate twist angles and present a new pathway toward engineering band structure and symmetry-breaking phases in moiré heterostructures.

Efficient Chebyshev polynomial approach to quantum conductance calculations: Application to twisted bilayer graphene

In recent years, Chebyshev polynomial expansions of tight-binding Green's functions have been successfully applied to the study of a wide range of spectral and transport properties of materials. However, the application of the Chebyshev approach to the study of quantum transport properties of noninteracting mesoscopic systems with leads has been hampered by the lack of a suitable Chebyshev expansion of Landaeur's formula or one of its equivalent formulations in terms of Green's functions in Keldysh's perturbation theory. Here, we tackle this issue by means of a hybrid approach that combines the efficiency of Chebyshev expansions with the convenience of complex absorbing potentials to calculate the conductance of two-terminal devices in a computationally expedient and accurate fashion. The versatility of the approach is demonstrated for mesoscopic twisted bilayer graphene (TBG) devices with up to $2.3\times10^6$ atomic sites. Our results highlight the importance of moir\'e effects, interlayer scattering events and twist-angle disorder in determining the conductance curves in devices with a small twist angle near the TBG magic angle $\theta_m \approx 1.1^\circ$.

Impact of Electric Field Disorder on Broken-Symmetry States in Ultraclean Bilayer Graphene.

Bilayer graphene (BLG) has multiple internal degrees of freedom and a constant density of states down to the charge neutrality point when trigonal warping is ignored. Consequently, it is susceptible to various competing ground states. However, a coherent experimental determination of the ground state has been challenging due to the interaction-disorder interplay. Here we present an extensive transport study in a series of dually gated freestanding BLG devices and identify the layer-antiferromagnet as the ground state with a continuous strength across all devices. This strength correlates with the width of the state in the electric field. We systematically identify electric-field disorder─spatial variations in the interlayer potential difference─as the main source responsible for the observations. Our results pinpoint for the first time the importance of electric-field disorder on spontaneous symmetry breaking in BLG and solve a long-standing debate on its ground state. The electric-field disorder should be universal to all 2D materials.

Fluctuation-driven thermal transport in graphene double-layers at charge neutrality

We develop a theory of fluctuation-driven phenomena in thermal transport in graphene double-layers. We work in the regime of electron hydrodynamics and focus on the double charge neutrality point. Although at the neutrality point charge transport is decoupled from the hydrodynamic flow, thermal fluctuations of electron density cause both drag and heat transfer between the layers. The thermal transport in the bilayer system is governed by these two phenomena. We express the drag friction coefficient and the interlayer thermal conductivity in terms of the interlayer distance and the intrinsic conductivity of the electron liquid. We then obtain the thermal conductance matrix and determine the spatial dependence of the hydrodynamic velocity and temperature in the system. For shorter system the thermal drag resistance is determined by drag. In longer systems the situation of perfect thermal drag is realized, in which the hydrodynamic velocities in both layers become equal in the interior of the systems. Estimates are given for the monolayer and bilayer graphene devices. The predictions of our theory can be tested by the high-resolution thermal imaging and Johnson-Nyquist nonlocal noise thermometry.

Energy Relaxation and Cooling in Impure Bilayer Graphene at Low Temperatures

Understanding the physical mechanism of heat dissipation is a matter of increasing concern from the perspective of waste heat management in nanostructure-based devices. The impurity-driven electron–phonon scattering is a significant channel for energy relaxation in graphene and its bilayer. The recently developed Keldysh formalism for single-layer graphene (SLG) is extended to investigate the transport phenomena due to phonon interaction via the deformation potential in disordered bilayer graphene (BLG) at low temperatures within the impure limit, q l ≪ 1 . It is observed that in the BLG system also, the temperature dependence of the relaxation rate and the cooling power are affected by the occurrence of disorder and screening, with the temperature exponent of pure BLG T 4 modified to T 3 in impure BLG. A comparison with the temperature and mean free path exponents of SLG reveals that the exponents in BLG turn out to be the same, but they both differ from the conventional 2DEG. However, the magnitude of the scattering rate and cooling power is more pronounced in BLG in a low-temperature regime. As the magnitude of the relaxation rate and the cooling rate varies with impurity, the impurity-assisted electron–phonon scattering has rich implications on hot carrier transport in BLG devices.

Observation of ballistic upstream modes at fractional quantum Hall edges of graphene

The presence of “upstream” modes, moving against the direction of charge current flow in the fractional quantum Hall (FQH) phases, is critical for the emergence of renormalized modes with exotic quantum statistics. Detection of excess noise at the edge is a smoking gun for the presence of upstream modes. Here, we report noise measurements at the edges of FQH states realized in dual graphite-gated bilayer graphene devices. A noiseless dc current is injected at one of the edge contacts, and the noise generated at contacts at length, L = 4 μm and 10 μm away along the upstream direction is studied. For integer and particle-like FQH states, no detectable noise is measured. By contrast, for “hole-conjugate” FQH states, we detect a strong noise proportional to the injected current, unambiguously proving the existence of upstream modes. The noise magnitude remains independent of length, which matches our theoretical analysis demonstrating the ballistic nature of upstream energy transport, quite distinct from the diffusive propagation reported earlier in GaAs-based systems.

Heterostrain-enabled dynamically tunable moir\xe9 superlattice in twisted bilayer graphene

The ability to precisely control moiré patterns in two-dimensional materials has enabled the realization of unprecedented physical phenomena including Mott insulators, unconventional superconductivity, and quantum emission. Along with the twist angle, the application of independent strain in each layer of stacked two-dimensional materials—termed heterostrain—has become a powerful means to manipulate the moiré potential landscapes. Recent experimental studies have demonstrated the possibility of continuously tuning the twist angle and the resulting physical properties. However, the dynamic control of heterostrain that allows the on-demand manipulation of moiré superlattices has yet to be experimentally realized. Here, by harnessing the weak interlayer van der Waals bonding in twisted bilayer graphene devices, we demonstrate the realization of dynamically tunable heterostrain of up to 1.3%. Polarization-resolved Raman spectroscopy confirmed the existence of substantial heterostrain by presenting triple G peaks arising from the independently strained graphene layers. Theoretical calculations revealed that the distorted moiré patterns via heterostrain can significantly alter the electronic structure of twisted bilayer graphene, allowing the emergence of multiple absorption peaks ranging from near-infrared to visible spectral ranges. Our experimental demonstration presents a new degree of freedom towards the dynamic modulation of moiré superlattices, holding the promise to unveil unprecedented physics and applications of stacked two-dimensional materials.

Proximity Effect of Epitaxial Iron Phthalocyanine Molecules on High-Quality Graphene DevicesSupported by the National Natural Science Foundation of China (Grant No. 11674150), the Key-Area Research and DevelopmentProgram of Guangdong Province (Grant No. 2019B010931001), the Guangdong Innovative and Entrepreneurial Research Team Program (Grant No. 2016ZT06D348), the SUSTech CRF, and the Hong Kong RGC (Grant Nos. 16300617 and C6012-17E).

Depositing magnetic insulators on graphene has been a promising route to introduce magnetism via exchange proximity interaction in graphene for future spintronics applications. Molecule-based magnets may offer unique opportunities because of their synthesis versatility. Here, we investigate the magnetic proximity effect of epitaxial iron phthalocyanine (FePc) molecules on high-quality monolayer and bilayer graphene devices on hexagonal boron nitride substrates by probing the local and nonlocal transport. Although the FePc molecules introduce large hole doping effects combined with mobility degradation, the magnetic proximity gives rise to a canted antiferromagnetic state under a magnetic field in the monolayer graphene. On bilayer graphene and FePc heterostructure devices, the nonlocal transport reveals a pronounced Zeeman spin-Hall effect. Further analysis of the scattering mechanism in the bilayer shows a dominated long-range scattering. Our findings in graphene/organic magnetic insulator heterostructure provide a new insight for use of molecule-based magnets in two-dimensional spintronic devices.

(Invited) Experimental Quantum Transport in Strained Graphene and SWCNTs - Towards Noems

We measure ballistic charge conductivity in strained suspended graphene and observe the theoretically predicted [1] strain-induced scalar and vector potentials. To do so, we built an experimental platform for in-situ quantum transport strain engineering in 2D materials. This instrumentation also permits low temperature (0.3 K) transport in 0 to 9 Tesla magnetic fields. The tunable uniaxial strain (up to 3%) is completely decoupled from the gate-tunable charge density, permitting quantitative understanding of strain effects. We show slippage-free mechanical clamping of high aspect-ratio graphene crystals, where atomically ordered edges are unnecessary for quantitative straintronics. We study in detail transport in a ballistic graphene channel whose length is 90 nm and width is 600 nm. By applying strain up to 0.6 % in this device, we observe that the strain-induced scalar potential shifts its low energy band structure downward by up to 30 meV. We show precise control of the gauge vector potential which reversibly suppresses the conductance. We discuss our progress towards strain engineering in SWCNTs, and calculations showing its potential in valley filtering and tuning electron-hole asymmetric quantum transistors.We conclude with an overview of another project to integrate suspended bilayer graphene devices in planar optical cavities towards achieving fully tunable nano-opto-electro-mechanical (NOEMS) carbon systems. To do so, we discuss a nitrocellulose-based dry-stamping method to manipulate and suspend individual 2D materials [2]. Using this method we assembled optical cavities able to a widely tune Raman scattering and absorption in graphene. [1] A. C. McRae, G. Wei, and A. R. Champagne, Phys. Rev. Applied 11, 054019 (2019). [2] I. G. Rebollo, F. C. Rodrigues-Machado, W. Wright, G. J. Melin, A. R. Champagne, ArXiv:2011.14166 Figure 1

Vanishing Thermal Equilibration for Hole-Conjugate Fractional Quantum Hall States in Graphene

Transport through edge channels is responsible for conduction in quantum Hall (QH) phases. Robust quantized values of charge and thermal conductances dictated by bulk topology appear when equilibration processes become dominant. We report on measurements of electrical and thermal conductances of integer and fractional QH phases, realized in hexagonal boron nitride encapsulated graphite-gated bilayer graphene devices for both electron and hole doped sides with different valley and orbital symmetries. Remarkably, for complex edges at filling factors ν=5/3 and 8/3, closely related to the paradigmatic hole-conjugate ν=2/3 phase, we find quantized thermal conductance whose values (3κ_{0}T and 4κ_{0}T, respectively where κ_{0}T is the thermal conductance quantum) are markedly inconsistent with the values dictated by topology (1κ_{0}T and 2κ_{0}T, respectively). The measured thermal conductance values remain insensitive to different symmetries, suggesting its universal nature. Our findings are supported by a theoretical analysis, which indicates that, whereas electrical equilibration at the edge is established over a finite length scale, the thermal equilibration length diverges for strong electrostatic interaction. Our results elucidate the subtle nature of crossover from coherent, mesoscopic to topology-dominated transport.

Visualizing delocalized correlated electronic states in twisted double bilayer graphene

The discovery of interaction-driven insulating and superconducting phases in moiré van der Waals heterostructures has sparked considerable interest in understanding the novel correlated physics of these systems. While a significant number of studies have focused on twisted bilayer graphene, correlated insulating states and a superconductivity-like transition up to 12 K have been reported in recent transport measurements of twisted double bilayer graphene. Here we present a scanning tunneling microscopy and spectroscopy study of gate-tunable twisted double bilayer graphene devices. We observe splitting of the van Hove singularity peak by ~20 meV at half-filling of the conduction flat band, with a corresponding reduction of the local density of states at the Fermi level. By mapping the tunneling differential conductance we show that this correlated system exhibits energetically split states that are spatially delocalized throughout the different regions in the moiré unit cell, inconsistent with order originating solely from onsite Coulomb repulsion within strongly-localized orbitals. We have performed self-consistent Hartree-Fock calculations that suggest exchange-driven spontaneous symmetry breaking in the degenerate conduction flat band is the origin of the observed correlated state. Our results provide new insight into the nature of electron-electron interactions in twisted double bilayer graphene and related moiré systems.

In Operando Angle‐Resolved Photoemission Spectroscopy with Nanoscale Spatial Resolution: Spatial Mapping of the Electronic Structure of Twisted Bilayer Graphene

To pinpoint the electronic and structural mechanisms that affect intrinsic and extrinsic performance limits of 2D material devices, it is of critical importance to resolve the electronic properties on the mesoscopic length scale of such devices under operating conditions. Herein, angle‐resolved photoemission spectroscopy with nanoscale spatial resolution (nanoARPES) is used to map the quasiparticle electronic structure of a twisted bilayer graphene device. The dispersion and linewidth of the Dirac cones associated with top and bottom graphene layers are determined as a function of spatial position on the device under both static and operating conditions. The analysis reveals that microscopic rotational domains in the two graphene layers establish a range of twist angles from 9.8° to 12.7°. Application of current and electrostatic gating lead to strong electric fields with peak strengths of 0.75 V/μm at the rotational domain boundaries in the device. These proof‐of‐principle results demonstrate the potential of nanoARPES to link mesoscale structural variations with electronic states in operating device conditions and to disentangle such extrinsic factors from the intrinsic quasiparticle dispersion.

Valley polarized transport in graphene cross-junctions

Abstract Valley polarized transport was studied in graphene cross junctions consisting of a bilayer graphene device region connected to 4 monolayer graphene leads. Electrons injected from the armchair leads to the zigzag leads can be valley polarized in a range of Fermi energies. The valley polarization is produced by quantum interference and the Fano resonance effect in the device region. We also studied the dependence of the valley polarization on the dimensions of the junction and a vertical electric field applied to the device region. The valley polarization depends sensitively on the electric field, which enables us to control the valley polarization electrically.

Phonon scattering induced carrier resistivity in twisted double-bilayer graphene

In this work we carry out a theoretical study of the phonon-induced resistivity in twisted double bilayer graphene (TDBG), in which two Bernal-stacked bilayer graphene devices are rotated relative to each other by a small angle $\theta$. We show that at small twist angles ($\theta\sim 1^\circ$) the effective mass of the TDBG system is greatly enhanced, leading to a drastically increased phonon-induced resistivity in the high-temperature limit where phonon scattering leads to a linearly increasing resistivity with increasing temperature. We also discuss possible implications of our theory on superconductivity in such a system, and provide an order of magnitude estimation of the superconducting transition temperature.

Electronic correlations in twisted bilayer graphene near the magic angle

Twisted bilayer graphene with a twist angle of around 1.1{\deg} features a pair of isolated flat electronic bands and forms a strongly correlated electronic platform. Here, we use scanning tunneling microscopy to probe local properties of highly tunable twisted bilayer graphene devices and show that the flat bands strongly deform when aligned with the Fermi level. At half filling of the bands, we observe the development of gaps originating from correlated insulating states. Near charge neutrality, we find a previously unidentified correlated regime featuring a substantially enhanced flat band splitting that we describe within a microscopic model predicting a strong tendency towards nematic ordering. Our results provide insights into symmetry breaking correlation effects and highlight the importance of electronic interactions for all filling factors in twisted bilayer graphene.

Energetics of the complex phase diagram of a tunable bilayer graphene probed by quantum capacitance

Bilayer graphene provides a unique platform to explore the rich physics in quantum Hall effect. The unusual combination of spin, valley and orbital degeneracy leads to interesting symmetry broken states with electric and magnetic field. Conventional transport measurements like resistance measurements have been performed to probe the different ordered states in bilayer graphene. However, not much work has been done to directly map the energetics of those states in bilayer graphene. Here, we have carried out the magneto capacitance measurements with electric and magnetic field in a hexagonal boron nitride encapsulated dual gated bilayer graphene device. At zero magnetic field, using the quantum capacitance technique we measure the gap around the charge neutrality point as a function of perpendicular electric field and the obtained value of the gap matches well with the theory. In presence of perpendicular magnetic field, we observe Landau level crossing in our magneto-capacitance measurements with electric field. The gap closing and reopening of the lowest Landau level with electric and magnetic field shows the transition from one ordered state to another one. Further more we observe the collapsing of the Landau levels near the band edge at higher electric field ($\bar D > 0.5$ V/nm), which was predicted theoretically. The complete energetics of the Landau levels of bilayer graphene with electric and magnetic field in our experiment paves the way to unravel the nature of ground states of the system.