Twisted Double Bilayer Graphene Research Articles

Strongly coupled magneto-exciton condensates in large-angle twisted double bilayer graphene

Excitons, pairs of electrons and holes, undergo a Bose-Einstein condensation at low temperatures. An important platform to study excitons is double-layer two-dimensional electron gases, with two parallel planes of electrons and holes separated by a thin insulating layer. Lowering this separation (d) strengthens the exciton binding energy, however, leads to the undesired interlayer tunneling, resulting in annihilation of excitons. Here, we report the observation of a sequences of robust exciton condensates (ECs) in double bilayer graphene twisted to ~ 10° with no insulating mid-layer. The large momentum mismatch between two graphene layers suppresses interlayer tunneling, reaching a d ~ 0.334 nm. Measuring the bulk and edge transport, we find incompressible states corresponding to ECs when both layers are in half-filled N = 0, 1 Landau levels (LLs). Theoretical calculations suggest that the low-energy charged excitation of ECs can be meron-antimeron or particle-hole pair, which relies on both LL index and carrier type. Our results establish a novel platform with extreme coupling strength for studying quantum bosonic phase.

Interplay of Landau Quantization and Interminivalley Scatterings in a Weakly Coupled Moiré Superlattice.

Double-layer quantum systems are promising platforms for realizing novel quantum phases. Here, we report a study of quantum oscillations (QOs) in a weakly coupled double-layer system composed of a large-angle twisted-double-bilayer graphene (TDBG). We quantify the interlayer coupling strength by measuring the interlayer capacitance from the QOs pattern at low temperatures, revealing electron-hole asymmetry. At high temperatures when SdHOs are thermally smeared, we observe resistance peaks when Landau levels (LLs) from two moiré minivalleys are aligned, regardless of carrier density; eventually, it results in a 2-fold increase of oscillating frequency in D, serving as compelling evidence of the magneto-intersub-band oscillations (MISOs) in double-layer systems. The temperature dependence of MISOs suggests that electron-electron interactions play a crucial role and the scattering times obtained from MISO thermal damping are correlated with the interlayer coupling strength. Our study reveals intriguing interplays among Landau quantization, moiré band structure, and scatterings.

Observation of dichotomic field-tunable electronic structure in twisted monolayer-bilayer graphene

Twisted bilayer graphene (tBLG) provides a fascinating platform for engineering flat bands and inducing correlated phenomena. By designing the stacking architecture of graphene layers, twisted multilayer graphene can exhibit different symmetries with rich tunability. For example, in twisted monolayer-bilayer graphene (tMBG) which breaks the C2z symmetry, transport measurements reveal an asymmetric phase diagram under an out-of-plane electric field, exhibiting correlated insulating state and ferromagnetic state respectively when reversing the field direction. Revealing how the electronic structure evolves with electric field is critical for providing a better understanding of such asymmetric field-tunable properties. Here we report the experimental observation of field-tunable dichotomic electronic structure of tMBG by nanospot angle-resolved photoemission spectroscopy (NanoARPES) with operando gating. Interestingly, selective enhancement of the relative spectral weight contributions from monolayer and bilayer graphene is observed when switching the polarity of the bias voltage. Combining experimental results with theoretical calculations, the origin of such field-tunable electronic structure, resembling either tBLG or twisted double-bilayer graphene (tDBG), is attributed to the selectively enhanced contribution from different stacking graphene layers with a strong electron-hole asymmetry. Our work provides electronic structure insights for understanding the rich field-tunable physics of tMBG.

Ferroelectricity in twisted double bilayer graphene

Two-dimensional (2D) ferroelectrics can maintain electrical polarization up to room temperature and are, therefore, promising for next-generation nonvolatile memories. Although natural 2D ferroelectrics are few, moiré superlattices provide us with a generalized method to construct ferroelectrics from non-ferroelectric parent materials. We report a realization of ferroelectric hysteresis in an AB-BA stacked twisted double bilayer graphene (TDBG) system. The ferroelectric polarization is prominent at zero external displacement field and reduces upon increasing displacement fields. TDBG in the AB-BA configuration is an intriguing system, which facilitates ferroelectricity even without the assistance of any boron nitride layers; however, in the AB-AB stacking case, the development of polarization necessitates the presence of a second superlattice induced by the adjacent boron nitride layer. Therefore, twisted multilayer graphene offers us a fascinating field to explore 2D ferroelectricity.

Visualizing localized nematic states in twisted double bilayer graphene.

Direct visualization of the states originating from electron-electron interactions is of great importance for engineering the surface and interfacial properties of graphene-based quantum materials. For instance, the rotational symmetry breaking or nematic phase inferred from spectroscopic imaging has confirmed the existence of correlated states in a wide range of moiré materials. Here, we study the atomic-scale spatial distributions and symmetry of wave functions in gate-tunable twisted double bilayer graphene by employing scanning tunneling microscopy/spectroscopy and continuum model calculations. A series of spectroscopic imaging analyses are used to identify dominant symmetry breaking of the emergent states. Interestingly, in non-integer hole fillings, a completely new localized electronic state with rotational symmetry breaking is observed on the left side of the valence flat band. The degree of anisotropy is found to increase from the conduction flat band through the valence flat band to the new state. Our results provide an essential microscopic insight into the flat band and its adjacent state for a full understanding of their electric field response in twisted graphene systems.

Evidence of compensated semimetal with electronic correlations at charge neutrality of twisted double bilayer graphene

Recently, magic-angle twisted bilayer graphene (MATBLG) has emerged with various interaction-driven novel quantum phases at the commensurate fillings of the moiré superlattice, while the charge neutrality point (CNP) remains mostly a trivial insulator. Here, we show an emerging phase of compensated semimetallicity at the CNP of twisted double bilayer graphene (TDBLG), a close cousin of MATBLG, with signatures of electronic correlation. Using electrical and thermal transport, we find two orders of magnitude enhancement of the thermopower at magnetic fields much smaller than the extreme quantum limit, accompanied by large magnetoresistance ( ~ 2500%) at CNP, providing strong experimental evidence of compensated semimetallicity at CNP of TDBLG. Moreover, at low temperatures, we observe unusual sublinear temperature dependence of resistance. A recent theory1 predicts the formation of an excitonic metal near CNP, where small electron and hole pockets co-exist. We understand this sublinear temperature dependence in terms of critical fluctuations in this theory.

Symmetry-Broken Chern Insulators in Twisted Double Bilayer Graphene.

Twisted double bilayer graphene (tDBG) has emerged as a rich platform for studying strongly correlated and topological states, as its flat bands can be continuously tuned by both a perpendicular displacement field and a twist angle. Here, we construct a phase diagram representing the correlated and topological states as a function of these parameters, based on measurements of over a dozen tDBG devices encompassing two distinct stacking configurations. We find a hierarchy of symmetry-broken states that emerge sequentially as the twist angle approaches an apparent optimal value of θ ≈ 1.34°. Nearby this angle, we discover a symmetry-broken Chern insulator (SBCI) state associated with a band filling of 7/2 as well as an incipient SBCI state associated with 11/3 filling. We further observe an anomalous Hall effect at zero field in all samples supporting SBCI states, indicating spontaneous time-reversal symmetry breaking and possible moiré unit cell enlargement at zero magnetic field.

Superconductivity in twisted double bilayer graphene stabilized by WSe2.

Identifying the essential components of superconductivity in graphene-based systems remains a critical problem in two-dimensional materials research. This field is connected to the mysteries that underpin investigations of unconventional superconductivity in condensed-matter physics. Superconductivity has been observed in magic-angle twisted stacks of monolayer graphene but conspicuously not in twisted stacks of bilayer graphene, although both systems host topological flat bands and symmetry-broken states. Here we report the discovery of superconductivity in twisted double bilayer graphene (TDBG) in proximity to WSe2. Samples with twist angles 1.24° and 1.37° superconduct in small pockets of the gate-tuned phase diagram within the valence and conduction band, respectively. Superconductivity emerges from unpolarized phases near van Hove singularities and next to regions with broken isospin symmetry. Our results show the correlation between a high density of states and the emergence of superconductivity in TDBG while revealing a possible role for isospin fluctuations in the pairing.

Machine learning the microscopic form of nematic order in twisted double-bilayer graphene

Modern scanning probe techniques, such as scanning tunneling microscopy, provide access to a large amount of data encoding the underlying physics of quantum matter. In this work, we show how convolutional neural networks can be used to learn effective theoretical models from scanning tunneling microscopy data on correlated moiré superlattices. Moiré systems are particularly well suited for this task as their increased lattice constant provides access to intra-unit-cell physics, while their tunability allows for the collection of high-dimensional data sets from a single sample. Using electronic nematic order in twisted double-bilayer graphene as an example, we show that incorporating correlations between the local density of states at different energies allows convolutional neural networks not only to learn the microscopic nematic order parameter, but also to distinguish it from heterostrain. These results demonstrate that neural networks are a powerful method for investigating the microscopic details of correlated phenomena in moiré systems and beyond.

Observation of First-Order Quantum Phase Transitions and Ferromagnetism in Twisted Double Bilayer Graphene

Observation of First-Order Quantum Phase Transitions and Ferromagnetism in Twisted Double Bilayer Graphene

Quantum oscillations in field-induced correlated insulators of a moiré superlattice

We report an observation of quantum oscillations (QOs) in the correlated insulators with valley anisotropy of twisted double bilayer graphene (TDBG). The anomalous QOs are best captured in the magneto resistivity oscillations of the insulators at v = −2, with a period of 1/B and an oscillation amplitude as high as 150 kΩ. The QOs can survive up to ∼10 K, and above 12 K, the insulating behaviors are dominant. The QOs of the insulator are strongly D dependent: the carrier density extracted from the 1/B periodicity decreases almost linearly with D from −0.7 to −1.1 V/nm, suggesting a reduced Fermi surface; the effective mass from Lifshitz-Kosevich analysis depends nonlinearly on D, reaching a minimal value of 0.1 me at D = ∼ −1.0 V/nm. Similar observations of QOs are also found at v = 2, as well as in other devices without graphite gate. We interpret the D sensitive QOs of the correlated insulators in the picture of band inversion. By reconstructing an inverted band model with the measured effective mass and Fermi surface, the density of state at the gap, calculated from thermal broadened Landau levels, agrees qualitatively with the observed QOs in the insulators. While more theoretical understandings are needed in the future to fully account for the anomalous QOs in this moiré system, our study suggests that TDBG is an excellent platform to discover exotic phases where correlation and topology are at play.

Analytical model of the energy spectrum and Landau levels of a twisted double bilayer graphene

Motivated by recent experiments Adak et al. (2020) and Szentpéter et al. (2021), in this work we have considered a twisted double bilayer graphene system. Within the low energy effective theory, the bandwidth expression of the moire flatbands (with weak dispersion and diverging effective mass) and Landau level spectrum of the Bernal stacked twisted double bilayer graphene are obtained analytically. We analyze the dependence of the bandwidth, effective mass, and Landau level spectrum on twist angle, inter layer tunneling, and interlayer potential difference. Also, we have investigated the phase diagram of the effective mass as a function of the twist angle and interlayer tunneling strength to seek the parameter space with diverging effective mass. We find that the magic angle at which the flat bands exist is increasing with increasing inter layer tunneling strength. • In this work, in this work we have considered a twisted double bilayer graphene system. • Within the low energy effective theory, the bandwidth expression of the moiré flatbands (with weak dispersion and diverging effective mass) and Landau level spectrum of the Bernal stacked twisted double bilayer graphene are obtained analytically. • We analyze the dependence of the bandwidth, effective mass, and Landau level spectrum on twist angle, inter layer tunneling, and interlayer potential difference. • Also, we have investigated the phase diagram of the effective mass as a function of the twist angle and interlayer tunneling strength to seek the parameter space with diverging effective mass. • We find that the magic angle at which the flat bands exist is increasing with increasing inter layer tunneling strength. • The results presented in this work will be useful for the experimental investigation of the tDBG system.

Quantifying the local mechanical properties of twisted double bilayer graphene.

Nanomechanical measurements of minimally twisted van der Waals materials remained elusive despite their fundamental importance for device realisation. Here, we use Ultrasonic Force Microscopy (UFM) to locally quantify the variation of out-of-plane Young's modulus in minimally twisted double bilayer graphene (TDBG). We reveal a softening of the Young's modulus by 7% and 17% along single and double domain walls, respectively. Our experimental results are confirmed by force-field relaxation models. This study highlights the strong tunability of nanomechanical properties in engineered twisted materials, and paves the way for future applications of designer 2D nanomechanical systems.

Perpendicular electric field drives Chern transitions and layer polarization changes in Hofstadter bands

Moiré superlattices engineer band properties and enable observation of fractal energy spectra of Hofstadter butterfly. Recently, correlated-electron physics hosted by flat bands in small-angle moiré systems has been at the foreground. However, the implications of moiré band topology within the single-particle framework are little explored experimentally. An outstanding problem is understanding the effect of band topology on Hofstadter physics, which does not require electron correlations. Our work experimentally studies Chern state switching in the Hofstadter regime using twisted double bilayer graphene (TDBG), which offers electric field tunable topological bands, unlike twisted bilayer graphene. Here we show that the nontrivial topology reflects in the Hofstadter spectra, in particular, by displaying a cascade of Hofstadter gaps that switch their Chern numbers sequentially while varying the perpendicular electric field. Our experiments together with theoretical calculations suggest a crucial role of charge polarization changing concomitantly with topological transitions in this system. Layer polarization is likely to play an important role in the topological states in few-layer twisted systems. Moreover, our work establishes TDBG as a novel Hofstadter platform with nontrivial magnetoelectric coupling.

Spontaneous time-reversal symmetry breaking in twisted double bilayer graphene

Twisted double bilayer graphene (tDBG) comprises two Bernal-stacked bilayer graphene sheets with a twist between them. Gate voltages applied to top and back gates of a tDBG device tune both the flatness and topology of the electronic bands, enabling an unusual level of experimental control. Metallic states with broken spin and valley symmetries have been observed in tDBG devices with twist angles in the range 1.2–1.3°, but the topologies and order parameters of these states have remained unclear. We report the observation of an anomalous Hall effect in the correlated metal state of tDBG, with hysteresis loops spanning hundreds of mT in out-of-plane magnetic field (B⊥) that demonstrate spontaneously broken time-reversal symmetry. The B⊥ hysteresis persists for in-plane fields up to several Tesla, suggesting valley (orbital) ferromagnetism. At the same time, the resistivity is strongly affected by even mT-scale values of in-plane magnetic field, pointing to spin-valley coupling or to a direct orbital coupling between in-plane field and the valley degree of freedom.

Weak localization on moiré superlattice in twisted double bilayer graphene

Negative magnetoresistance owing to weak localization (WL) was investigated in twisted double bilayer graphene (TDBG) as a function of the twist angle. The ratio of the intervalley scattering time to the intravalley scattering time, estimated using the WL formula for bilayer graphene, tended to decrease as the twist angle increased. This feature is qualitatively explained by the enhancement of intervalley scattering due to the reduction of the intervalley distance in the moiré Brillouin zone (BZ). This indicates that WL in the TDBG occurs with the reconstructed BZ and originates from the scattering process owing to the disorder in moiré superlattice.

Tunable quantum criticalities in an isospin extended Hubbard model simulator

Studying strong electron correlations has been an essential driving force for pushing the frontiers of condensed matter physics. In particular, in the vicinity of correlation-driven quantum phase transitions (QPTs), quantum critical fluctuations of multiple degrees of freedom facilitate exotic many-body states and quantum critical behaviours beyond Landau’s framework1. Recently, moiré heterostructures of van der Waals materials have been demonstrated as highly tunable quantum platforms for exploring fascinating, strongly correlated quantum physics2–22. Here we report the observation of tunable quantum criticalities in an experimental simulator of the extended Hubbard model with spin–valley isospins arising in chiral-stacked twisted double bilayer graphene (cTDBG). Scaling analysis shows a quantum two-stage criticality manifesting two distinct quantum critical points as the generalized Wigner crystal transits to a Fermi liquid by varying the displacement field, suggesting the emergence of a critical intermediate phase. The quantum two-stage criticality evolves into a quantum pseudo criticality as a high parallel magnetic field is applied. In such a pseudo criticality, we find that the quantum critical scaling is only valid above a critical temperature, indicating a weak first-order QPT therein. Our results demonstrate a highly tunable solid-state simulator with intricate interplay of multiple degrees of freedom for exploring exotic quantum critical states and behaviours.

Nonlinear anomalous Hall effects probe topological phase-transitions in twisted double bilayer graphene

Nonlinear anomalous (NLA) Hall effect is the Berry curvature dipole induced second-order Hall voltage or temperature difference induced by a longitudinal electric field or temperature gradient. These are the prominent Hall responses in time-reversal symmetric systems. These band-geometry induced responses in recently realized twistronic platforms can probe their novel electronic band structure and topology. Here, we investigate the family (electrical, thermoelectric, and thermal) of second-order NLA Hall effects in the moiré system of twisted double bilayer graphene (TDBG). We combine the semiclassical transport framework with the continuum model of TDBG to demonstrate that the NLA Hall signals can probe topological phase transitions in moiré systems. We show that the whole family of NLA Hall responses undergo a sign reversal across a topological phase transition. Our study establishes a deeper connection between valley topology and nonlinear Hall effects in time-reversal symmetric systems.

Temperature-linear resistivity in twisted double bilayer graphene

We report an experimental study of carrier density ($n$), displacement field, and twist angle (\ensuremath{\theta}) dependence of temperature ($T$)-linear resistivity in twisted double-bilayer graphene (TDBG). For a large twist angle ($\ensuremath{\theta}>1.{5}^{\ensuremath{\circ}}$) where correlated insulating states are absent, we observe a $T$-linear resistivity (with a slope on the order of $\ensuremath{\sim}10\phantom{\rule{0.28em}{0ex}}\mathrm{\ensuremath{\Omega}}/\mathrm{K}$) over a wide range of carrier densities, and its slope decreases with increasing $n$, which is in agreement with the acoustic phonon scattering model semiquantitatively. The slope of $T$-linear resistivity is nonmonotonically dependent on the displacement field with a single peak structure. For a device with $\ensuremath{\theta}\ensuremath{\sim}1.{23}^{\ensuremath{\circ}}$ at which correlated states emerge, the slope of $T$-linear resistivity is found to be a maximum ($\ensuremath{\sim}100\phantom{\rule{0.28em}{0ex}}\mathrm{\ensuremath{\Omega}}/\mathrm{K}$) at the boundary of the halo structure where phase transition occurs, with signatures of continuous phase transition, Planckian dissipation, and diverging effective mass. These observations are in line with quantum critical behaviors, which might be due to symmetry-breaking instability at the critical points. Our results shed new light on correlated physics in TDBG and other twisted moir\'e systems.

Isospin competitions and valley polarized correlated insulators in twisted double bilayer graphene

New phase of matter usually emerges when a given symmetry breaks spontaneously, which can involve charge, spin, and valley degree of freedoms. Here, we report an observation of new correlated insulators evolved from spin-polarized states to valley-polarized states in twisted double bilayer graphene (TDBG) driven by the displacement field (D). At a high field |D | > 0.7 V/nm, we observe valley polarized correlated insulators with a big Zeeman g factor of ~10, both at v = 2 in the moiré conduction band and more surprisingly at v = −2 in the moiré valence band. Moreover, we observe a valley polarized Chern insulator with C = 2 emanating at v = 2 in the electron side and a valley polarized Fermi surface around v = −2 in the hole side. Our results demonstrate a feasible way to realize isospin control and to obtain new phases of matter in TDBG by the displacement field, and might benefit other twisted or non-twisted multilayer systems.