Ferroelectric and spontaneous quantum Hall states in intrinsic rhombohedral trilayer graphene
F. Winterer, F. R. Geisenhof, N. Fernandez, A. M. Seiler, F. Zhang, R. T. Weitz
Nature Physics 20 (2), 8 (2024).
Non-trivial interacting phases can emerge in elementary materials. As a prime example, continuing advances in device quality have facilitated the observation of a variety of spontaneously ordered quantum states in bilayer graphene. Its natural extension, rhombohedral trilayer graphene-in which the layers are stacked in an ABC fashion-is predicted to host stronger electron-electron interactions than bilayer graphene because of its flatter low-energy bands and larger winding number. Theoretically, five spontaneous quantum Hall phases have been proposed to be candidate electronic ground states. Here we observe evidence for four of the five competing ordered states in interaction-maximized, dual-gated, rhombohedral trilayer graphene. In particular, at small magnetic fields, two states with Chern numbers 3 and 6 can be stabilized at elevated and low perpendicular electric fields, respectively, and both exhibit clear magnetic hysteresis. We also show that the quantum Hall ferromagnets of the zero-energy Landau levels are ferroelectrics with spontaneous layer polarizations even at zero electric field, as evidenced by electric hysteresis. Bilayer graphene is known to host states where interactions dominate the electronic behaviour. Now, transport measurements show that this is also true for trilayer graphene and give evidence for ferroelectric states and states with high Chern number.
Impact of Electric Field Disorder on Broken-Symmetry States in Ultraclean Bilayer Graphene
F. R. Geisenhof, F. Winterer, A. M. Seiler, J. Lenz, F. Zhang, R. T. Weitz
Nano Letters 8 (2022).
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.
Quantum cascade of correlated phases in trigonally warped bilayer graphene
A. M. Seiler, F. R. Geisenhof, F. Winterer, K. Watanabe, T. Taniguchi, T. Y. Xu, F. Zhang, R. T. Weitz
Nature 608 (7922), 298-+ (2022).
Divergent density of states offers an opportunity to explore a wide variety of correlated electron physics. In the thinnest limit, this has been predicted and verified in the ultraflat bands of magic-angle twisted bilayer graphene(1-5), the band touching points of few-layer rhombohedral graphite(6-8) and the lightly doped rhombohedral trilayer graphene(9-11). The simpler and seemingly better understood Bernal bilayer graphene is also susceptible to orbital magnetism at charge neutrality(7) leading to layer antiferromagnetic states(12) or quantum anomalous Hall states(13). Here we report the observation of a cascade of correlated phases in the vicinity of electric-field-controlled Lifshitz transitions(14,15) and van Hove singularities(16) in Bernal bilayer graphene. We provide evidence for the observation of Stoner ferromagnets in the form of half and quarter metals(10,11). Furthermore, we identify signatures consistent with a topologically non-trivial Wigner-Hall crystal(17) at zero magnetic field and its transition to a trivial Wigner crystal, as well as two correlated metals whose behaviour deviates from that of standard Fermi liquids. Our results in this reproducible, tunable, simple system open up new horizons for studying strongly correlated electrons.
Interplay between topological valley and quantum Hall edge transport
F. R. Geisenhof, F. Winterer, A. M. Seiler, J. Lenz, I. Martin, R. T. Weitz
Nature Communications 13 (1), 4187 (2022).
In electrostatically-gapped bilayer graphene, topologically-protected states can emerge at naturally occurring stacking domain walls even in the absence of a magnetic field. Here, the authors describe the interplay between such domain wall states and quantum Hall edge transport within the eight-fold degenerate zeroth Landau level of suspended bilayer graphene. An established way of realising topologically protected states in a two-dimensional electron gas is by applying a perpendicular magnetic field thus creating quantum Hall edge channels. In electrostatically gapped bilayer graphene intriguingly, even in the absence of a magnetic field, topologically protected electronic states can emerge at naturally occurring stacking domain walls. While individually both types of topologically protected states have been investigated, their intriguing interplay remains poorly understood. Here, we focus on the interplay between topological domain wall states and quantum Hall edge transport within the eight-fold degenerate zeroth Landau level of high-quality suspended bilayer graphene. We find that the two-terminal conductance remains approximately constant for low magnetic fields throughout the distinct quantum Hall states since the conduction channels are traded between domain wall and device edges. For high magnetic fields, however, we observe evidence of transport suppression at the domain wall, which can be attributed to the emergence of spectral minigaps. This indicates that stacking domain walls potentially do not correspond to a topological domain wall in the order parameter.
Spontaneous Gully-Polarized Quantum Hall States in ABA Trilayer Graphene
F. Winterer, A. M. Seiler, A. Ghazaryan, F. R. Geisenhof, K. Watanabe, T. Taniguchi, M. Serbyn, R. T. Weitz
Nano Letters 22 (8), 3317-3322 (2022).
Bernal-stacked multilayer graphene is a versatileplatform to explore quantum transport phenomena and interactionphysics due to its exceptional tunability via electrostatic gating. Forinstance, upon applying a perpendicular electricfield, its bandstructure exhibits several off-center Dirac points (so-called Diracgullies) in each valley. Here, the formation of Dirac gullies and theinteraction-induced breakdown of gully coherence is explored viamagnetotransport measurements in high-quality Bernal-stacked(ABA) trilayer graphene. At zero magneticfield, multiple Lifshitztransitions indicating the formation of Dirac gullies are identified.In the quantum Hall regime, the emergence of Dirac gullies isevident as an increase in Landau level degeneracy. When tuningboth electric and magneticfields, electron-electron interactionscan be controllably enhanced until, beyond critical electric and magneticfields, the gully degeneracy is eventually lifted. The arisingcorrelated ground state is consistent with a previously predicted nematic phase that spontaneously breaks the rotational gully symmetry
Quantum anomalous Hall octet driven by orbital magnetism in bilayer graphene
F. R. Geisenhof, F. Winterer, A. M. Seiler, J. Lenz, T. Y. Xu, F. Zhang, R. T. Weitz
Nature 598 (7879), 53-+ (2021).
The quantum anomalous Hall (QAH) effect-a macroscopic manifestation of chiral band topology at zero magnetic field-has been experimentally realized only by the magnetic doping of topological insulators(1-3) and the delicate design of moire heterostructures(4-8). However, the seemingly simple bilayer graphene without magnetic doping or moire engineering has long been predicted to host competing ordered states with QAH effects(9-11). Here we explore states in bilayer graphene with a conductance of 2 e(2) h(-1) (where e is the electronic charge and h is Planck's constant) that not only survive down to anomalously small magnetic fields and up to temperatures of five kelvin but also exhibit magnetic hysteresis. Together, the experimental signatures provide compelling evidence for orbital-magnetism-driven QAH behaviour that is tunable via electric and magnetic fields as well as carrier sign. The observed octet of QAH phases is distinct from previous observations owing to its peculiar ferrimagnetic and ferrielectric order that is characterized by quantized anomalous charge, spin, valley and spin-valley Hall behaviour(9).
Interfacial Synthesis of Layer-Oriented 2D Conjugated Metal-Organic Framework Films toward Directional Charge Transport
Z. Y. Wang, L. S. Walter, M. Wang, P. St Petkov, B. K. Liang, H. Y. Qi, N. N. Nguyen, M. Hambsch, H. X. Zhong, M. C. Wang, S. Park, L. Renn, K. Watanabe, T. Taniguchi, S. C. B. Mannsfeld, T. Heine, U. Kaiser, S. Q. Zhou, R. T. Weitz, X. L. Feng, R. H. Dong
Journal of the American Chemical Society 143 (34), 13624-13632 (2021).
The development of layer-oriented two-dimensional conjugated metal-organic frameworks (2D c-MOFs) enables access to direct charge transport, dial-in lateral/vertical electronic devices, and the unveiling of transport mechanisms but remains a significant synthetic challenge. Here we report the novel synthesis of metal-phthalocyanine-based p-type semiconducting 2D c-MOF films (Cu-2[PcM-O-8], M = Cu or Fe) with an unprecedented edge-on layer orientation at the air/water interface. The edge-on structure formation is guided by the preorganization of metal-phthalocyanine ligands, whose basal plane is perpendicular to the water surface due to their pi-pi interaction and hydrophobicity. Benefiting from the unique layer orientation, we are able to investigate the lateral and vertical conductivities by DC methods and thus demonstrate an anisotropic charge transport in the resulting Cu-2[PcCu-O-8] film. The directional conductivity studies combined with theoretical calculation identify that the intrinsic conductivity is dominated by charge transfer along the interlayer pathway. Moreover, a macroscopic (cm(2) size) Hall-effect measurement reveals a Hall mobility of similar to 4.4 cm(2) V-1 s(-1 )91 for the obtained Cu-2[PcCu-O-8] film. The orientation control in semiconducting 2D c-MOFs will enable the development of various optoelectronic applications and the exploration of unique transport properties.
Synthesis of large-area rhombohedral few-layer graphene by chemical vapor deposition on copper
C. Bouhafs, S. Pezzini, F. R. Geisenhof, N. Mishra, V. Miseikis, Y. R. Niu, C. Struzzi, R. T. Weitz, A. A. Zakharov, S. Forti, C. Coletti
Carbon 177, 282-290 (2021).
Rhombohedral-stacked few-layer graphene (FLG) displays peculiar electronic properties that could lead to phenomena such as high-temperature superconductivity and magnetic ordering. To date, experimental studies have been mainly limited by the difficulty in isolating rhombohedral FLG with thickness exceeding 3 layers and device-compatible size. In this work, we demonstrate the synthesis and transfer of rhombohedral graphene with thickness up to 9 layers and areas up to similar to 50 mu m(2). The domains of rhombohedral FLG are identified by Raman spectroscopy and are found to alternate with Bernal regions within the same crystal in a stripe-like configuration. Near-field nano-imaging further confirms the structural integrity of the respective stacking orders. Combined spectroscopic and microscopic analyses indicate that rhombohedral-stacking formation is strongly correlated to the underlying copper step-bunching and emerges as a consequence of interlayer displacement along preferential crystallographic orientations. The growth and transfer of rhombohedral FLG with the reported thickness and size shall facilitate the observation of predicted unconventional physics and ultimately add to its technological relevance. (c) 2021 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
Charge Traps in All-Inorganic CsPbBr3 Perovskite Nanowire Field-Effect Phototransistors
F. Winterer, L. S. Walter, J. Lenz, S. Seebauer, Y. Tong, L. Polavarapu, R. T. Weitz
Advanced Electronic Materials 7 (6), 2100105 (2021).
"All-inorganic halide perovskite materials have recently emerged as outstanding materials for optoelectronic applications. However, although critical for developing novel technologies, the influence of charge traps on charge transport in all-inorganic systems still remains elusive. Here, the charge transport properties in cesium lead bromide, nanowire films are probed using a field-effect transistor geometry. Field-effect mobilities of mu(FET) = 4 x 10(-3) cm(-2) V-1 s(-1) and photoresponsivities in the range of R = 25 A W-1 are demonstrated. Furthermore, charge transport both with and without illumination is investigated down to cryogenic temperatures. Without illumination, deep traps dominate transport and the mobility freezes out at low temperatures. Despite the presence of deep traps, when illuminating the sample, the field-effect mobility increases by several orders of magnitude and even phonon-limited transport characteristics are visible. This can be seen as an extension to the notion of ""defect tolerance"" of perovskite materials that has solely been associated with shallow traps. These findings provide further insight in understanding charge transport in perovskite materials and underlines that managing deep traps can open up a route to optimizing optoelectronic devices such as solar cells or phototransistors operable also at low light intensities."
High-Performance Vertical Organic Transistors of Sub-5 nm Channel Length
J. Lenz, A. M. Seiler, F. R. Geisenhof, F. Winterer, K. Watanabe, T. Taniguchi, R. T. Weitz
Nano Letters 21 (10), 4430-4436 (2021).
Miniaturization of electronic circuits increases their overall performance. So far, electronics based on organic semiconductors has not played an important role in the miniaturization race. Here, we show the fabrication of liquid electrolyte gated vertical organic field effect transistors with channel lengths down to 2.4 nm. These ultrashort channel lengths are enabled by using insulating hexagonal boron nitride with atomically precise thickness and flatness as a spacer separating the vertically aligned source and drain electrodes. The transistors reveal promising electrical characteristics with output current densities of up to 2.95 MA cm(-2) at -0.4 V bias, on-off ratios of up to 10(6), a steep subthreshold swing of down to 65 mV dec(-1) and a transconductance of up to 714 S m(-1). Realizing channel lengths in the sub-5 nm regime and operation voltages down to 100 mu V proves the potential of organic semiconductors for future highly integrated or low power electronics.
Ionic liquid gating of single-walled carbon nanotube devices with ultra-short channel length down to 10nm
A. Janissek, J. Lenz, F. del Giudice, M. Gaulke, F. Pyatkov, S. Dehm, F. Hennrich, L. Wei, Y. Chen, A. Fediai, M. Kappes, W. Wenzel, R. Krupke, R. T. Weitz
Applied Physics Letters 118 (6), 63101 (2021).
Ionic liquids enable efficient gating of materials with nanoscale morphology due to the formation of a nanoscale double layer that can also follow strongly vaulted surfaces. On carbon nanotubes, this can lead to the formation of a cylindrical gate layer, allowing an ideal control of the drain current even at small gate voltages. In this work, we apply ionic liquid gating to chirality-sorted (9, 8) carbon nanotubes bridging metallic electrodes with gap sizes of 20nm and 10nm. The single-tube devices exhibit diameter-normalized current densities of up to 2.57mA/mu m, on-off ratios up to 10(4), and a subthreshold swing down to 100mV/dec. Measurements after long vacuum storage indicate that the hysteresis of ionic liquid gated devices depends not only on the gate voltage sweep rate and the polarization dynamics but also on charge traps in the vicinity of the carbon nanotube, which, in turn, might act as trap states for the ionic liquid ions. The ambipolar transfer characteristics are compared with calculations based on the Landauer-Buttiker formalism. Qualitative agreement is demonstrated, and the possible reasons for quantitative deviations and possible improvements to the model are discussed. Besides being of fundamental interest, the results have potential relevance for biosensing applications employing high-density device arrays.
Locally-triggered hydrophobic collapse induces global interface self-cleaning in van-der-Waals heterostructures at room-temperature
S. Wakolbinger, F. R. Geisenhof, F. Winterer, S. Palmer, J. G. Crimmann, K. Watanabe, T. Taniguchi, F. Trixler, R. T. Weitz
2d Materials 7 (3), 35002 (2020).
Mutual relative orientation and well defined, uncontaminated interfaces are the key to obtain van-der-Waals heterostacks with defined properties. Even though the van-der-Waals forces are known to promote the 'self-cleaning' of interfaces, residue from the stamping process, which is often found to be trapped between the heterostructure constituents, can interrupt the interlayer interaction and therefore the coupling. Established interfacial cleaning methods usually involve high-temperature steps, which are in turn known to lead to uncontrolled rotations of layers within fragile heterostructures. Here, we present an alternative method feasible at room temperature. Using the tip of an atomic force microscope (AFM), we locally control the activation of interlayer attractive forces, resulting in the global removal of contaminants from the interface (i.e. the contaminants are also removed in regions several mu m away from the line touched by the AFM tip). By testing combinations of various hydrophobic van-der-Waals materials, mild temperature treatments, and by observing the temporal evolution of the contaminant removal process, we identify that the AFM tip triggers a dewetting-induced hydrophobic collapse and the van-der-Waals interaction is driving the cleaning process. We anticipate that this process is at the heart of the known 'self-cleaning' mechanism. Our technique can be utilized to controllably establish interlayer close coupling between a stack of van-der-Waals layers, and additionally allows to pattern and manipulate heterostructures locally for example to confine material into nanoscopic pockets between two van-der-Waals materials.
Flexible low-voltage high-frequency organic thin-film transistors
J. W. Borchert, U. Zschieschang, F. Letzkus, M. Giorgio, R. T. Weitz, M. Caironi, J. N. Burghartz, S. Ludwigs, H. Klauk
Science Advances 6 (21), eaaz5156 (2020).
The primary driver for the development of organic thin-film transistors (TFTs) over the past few decades has been the prospect of electronics applications on unconventional substrates requiring low-temperature processing. A key requirement for many such applications is high-frequency switching or amplification at the low operating voltages provided by lithium-ion batteries (similar to 3 V). To date, however, most organic-TFT technologies show limited dynamic performance unless high operating voltages are applied to mitigate high contact resistances and large parasitic capacitances. Here, we present flexible low-voltage organic TFTs with record static and dynamic performance, including contact resistance as small as 10 Omega.cm, on/off current ratios as large as 10(10), subthreshold swing as small as 59 mV/decade, signal delays below 80 ns in inverters and ring oscillators, and transit frequencies as high as 21 MHz, all while using an inverted coplanar TFT structure that can be readily adapted to industry-standard lithographic techniques.
Anisotropic Strain-Induced Soliton Movement Changes Stacking Order and Band Structure of Graphene Multilayers: Implications for Charge Transport
F. R. Geisenhof, F. Winterer, S. Wakolbinger, T. D. Gokus, Y. C. Durmaz, D. Priesack, J. Lenz, F. Keilmann, K. Watanabe, T. Taniguchi, R. Guerrero-Aviles, M. Pelc, A. Ayuela, R. T. Weitz
Acs Applied Nano Materials 2 (9), 6067-6075 (2019).
The crystal structure of solid-state matter greatly affects its electronic properties. For example, in multilayer graphene, precise knowledge of the lateral layer arrangement is crucial, since the most stable configurations, Bernal and rhombohedral stacking, exhibit very different electronic properties. Nevertheless, both stacking orders can coexist within one flake, separated by a strain soliton that can host topologically protected states. Clearly, accessing the transport properties of the two stackings and the soliton is of high interest. However, the stacking orders can transform into one another, and therefore, the seemingly trivial question of how reliable electrical contact can be made to either stacking order can a priori not be answered easily. Here, we show that manufacturing metal contacts to multilayer graphene can move solitons by several ism, unidirectionally enlarging Bernal domains due to arising mechanical strain. Furthermore, we also find that during dry transfer of multilayer graphene onto hexagonal boron nitride, such a transformation can happen. Using density functional theory modeling, we corroborate that anisotropic deformations of the multilayer graphene lattice decrease the rhombohedral stacking stability. Finally, we have devised systematics to avoid soliton movement, and how to reliably realize contacts to both stacking configurations, which will aid to reliably access charge transport in both stacking configurations.