arXiv subjects

Michael F. Crommie

Publications and source records attributed to Michael F. Crommie.

At least 37 records · Page 2Linked to original sources

arXiv2023

Wigner Molecular Crystals from Multi-electron Moiré Artificial Atoms

Semiconductor moiré superlattices provide a versatile platform to engineer new quantum solids composed of artificial atoms on moiré sites. Previous studies have mostly focused on the simplest correlated quantum solid - the Fermi-Hubbard model - where intra-atom interactions are simplified to a single onsite repulsion energy U. These studies have revealed novel quantum phases ranging from Mott insulators to quantum anomalous Hall insulators at a filling of one electron per moiré unit cell. New types of quantum solids should arise at even higher filling factors where the multi-electron configuration of moiré artificial atoms provides new degrees of freedom. Here we report the experimental observation of Wigner molecular crystals emerging from multi-electron artificial atoms in twisted bilayer WS2 moiré superlattices. Moiré artificial atoms, unlike natural atoms, can host qualitatively different electron states due to the interplay between quantized energy levels and Coulomb interactions. Using scanning tunneling microscopy (STM), we demonstrate that Wigner molecules appear in multi-electron artificial atoms when Coulomb interactions dominate. Three-electron Wigner molecules, for example, are seen to exhibit a characteristic trimer pattern. The array of Wigner molecules observed in a moiré superlattice comprises a new crystalline phase of electrons: the Wigner molecular crystal. We show that these Wigner molecular crystals are highly tunable through mechanical strain, moiré period, and carrier charge type. Our study presents new opportunities for exploring quantum phenomena in moiré quantum solids composed of multi-electron artificial atoms.

cond-mat.mes-hall↗

arXiv2023

Visualizing and manipulating chiral interface states in a moiré quantum anomalous Hall insulator

Moiré systems made from stacked two-dimensional materials host novel correlated and topological states that can be electrically controlled via applied gate voltages. We have used this technique to manipulate Chern domains in an interaction-driven quantum anomalous Hall insulator made from twisted monolayer-bilayer graphene (tMBLG). This has allowed the wavefunction of chiral interface states to be directly imaged using a scanning tunneling microscope (STM). To accomplish this tMBLG carrier concentration was tuned to stabilize neighboring domains of opposite Chern number, thus providing topological interfaces completely devoid of any structural boundaries. STM tip pulse-induced quantum dots were utilized to induce new Chern domains and thereby create new chiral interface states with tunable chirality at predetermined locations. Theoretical analysis confirms the chiral nature of observed interface states and enables the determination of the characteristic length scale of valley polarization reversal across neighboring tMBLG Chern domains. tMBLG is shown to be a useful platform for imaging the exotic topological properties of correlated moiré systems.

cond-mat.mes-hall↗

arXiv2023

Thermodynamic behavior of correlated electron-hole fluids in van der Waals heterostructures

Coupled two-dimensional electron-hole bilayers provide a unique platform to study strongly correlated Bose-Fermi mixtures in condensed matter. Electrons and holes in spatially separated layers can bind to form interlayer excitons, composite Bosons expected to support high-temperature exciton superfluids. The interlayer excitons can also interact strongly with excess charge carriers when electron and hole densities are unequal. Here, we use optical spectroscopy to quantitatively probe the local thermodynamic properties of strongly correlated electron-hole fluids in MoSe2/hBN/WSe2 heterostructures. We observe a discontinuity in the electron and hole chemical potentials at matched electron and hole densities, a definitive signature of an excitonic insulator ground state. The excitonic insulator is stable up to a Mott density of ~$0.8\times {10}^{12} \mathrm{cm}^{-2}$ and has a thermal ionization temperature of ~70 K. The density dependence of the electron, hole, and exciton chemical potentials reveals strong correlation effects across the phase diagram. Compared with a non-interacting uniform charge distribution, the correlation effects lead to significant attractive exciton-exciton and exciton-charge interactions in the electron-hole fluid. Our work highlights the unique quantum behavior that can emerge in strongly correlated electron-hole systems.

cond-mat.str-el↗

arXiv2023

Imaging Moiré Excited States with Photocurrent Tunneling Microscopy

Moiré superlattices provide a highly tunable and versatile platform to explore novel quantum phases and exotic excited states ranging from correlated insulators1-17 to moiré excitons7-10,18. Scanning tunneling microscopy has played a key role in probing microscopic behaviors of the moiré correlated ground states at the atomic scale1,11-15,19. Atomic-resolution imaging of quantum excited state in moiré heterostructures, however, has been an outstanding experimental challenge. Here we develop a novel photocurrent tunneling microscopy by combining laser excitation and scanning tunneling spectroscopy (laser-STM) to directly visualize the electron and hole distribution within the photoexcited moiré exciton in a twisted bilayer WS2 (t-WS2). We observe that the tunneling photocurrent alternates between positive and negative polarities at different locations within a single moiré unit cell. This alternating photocurrent originates from the exotic in-plane charge-transfer (ICT) moiré exciton in the t-WS2 that emerges from the competition between the electron-hole Coulomb interaction and the moiré potential landscape. Our photocurrent maps are in excellent agreement with our GW-BSE calculations for excitonic states in t-WS2. The photocurrent tunneling microscopy creates new opportunities for exploring photoexcited non-equilibrium moiré phenomena at the atomic scale.

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arXiv2023

Local spectroscopy of a gate-switchable moiré quantum anomalous Hall insulator

In recent years, correlated insulating states, unconventional superconductivity, and topologically non-trivial phases have all been observed in several moiré heterostructures. However, understanding of the physical mechanisms behind these phenomena is hampered by the lack of local electronic structure data. Here, we use scanning tunnelling microscopy and spectroscopy to demonstrate how the interplay between correlation, topology, and local atomic structure determines the behaviour of electron-doped twisted monolayer-bilayer graphene. Through gate- and magnetic field-dependent measurements, we observe local spectroscopic signatures indicating a quantum anomalous Hall insulating state with a total Chern number of $\pm 2$ at a doping level of three electrons per moiré unit cell. We show that the sign of the Chern number and associated magnetism can be electrostatically switched only over a limited range of twist angle and sample hetero-strain values. This results from a competition between the orbital magnetization of filled bulk bands and chiral edge states, which is sensitive to strain-induced distortions in the moiré superlattice.

cond-mat.mes-hall↗

arXiv2022

Imaging gate-induced molecular melting on a graphene field-effect transistor

Solid-liquid phase transitions are fundamental physical processes, but atomically-resolved microscopy has yet to capture both the solid and liquid dynamics for such a transition. We have developed a new technique for controlling the melting and freezing of 2D molecular layers on a graphene field-effect transistor (FET) that allows us to image phase transition dynamics via atomically-resolved scanning tunneling microscopy. Back-gate voltages applied to a F4TCNQ-decorated graphene FET induce reversible transitions between a charge-neutral solid phase and a negatively charged liquid phase. Nonequilibrium molecular melting dynamics are visualized by rapidly heating the graphene surface with electrical current and imaging the resulting evolution toward new equilibrium states. An analytical model has been developed that explains the observed equilibrium mixed-state phases based on spectroscopic measurement of both solid and liquid molecular energy levels. Observed non-equilibrium melting dynamics are consistent with Monte Carlo simulations.

cond-mat.mes-hall↗

arXiv2022

A novel $\sqrt{19}\times\sqrt{19}$ superstructure in epitaxially grown 1T-TaTe$_2$

The spontaneous formation of electronic orders is a crucial element for understanding complex quantum states and engineering heterostructures in two-dimensional materials. We report a novel $\sqrt{19}\times\sqrt{19}$ charge order in few-layer thick 1T-TaTe$_2$ transition metal dichalcogenide films grown by molecular beam epitaxy, which has not been realized. Our photoemission and scanning probe measurements demonstrate that monolayer 1T-TaTe$_2$ exhibits a variety of metastable charge density wave orders, including the $\sqrt{19}\times\sqrt{19}$ superstructure, which can be selectively stabilized by controlling the post-growth annealing temperature. Moreover, we find that only the $\sqrt{19}\times\sqrt{19}$ order persists in 1T-TaTe$_2$ films thicker than a monolayer, up to 8 layers. Our findings identify the previously unrealized novel electronic order in a much-studied transition metal dichalcogenide and provide a viable route to control it within the epitaxial growth process.

cond-mat.mtrl-sci↗

arXiv2022

Mapping Charge Excitations in Generalized Wigner Crystals

Transition metal dichalcogenide-based moire superlattices exhibit very strong electron-electron correlations, thus giving rise to strongly correlated quantum phenomena such as generalized Wigner crystal states. Theoretical studies predict that unusual quasiparticle excitations across the correlated gap between upper and lower Hubbard bands can arise due to long-range Coulomb interactions in generalized Wigner crystal states. Here we describe a new scanning single-electron charging (SSEC) spectroscopy technique with nanometer spatial resolution and single-electron charge resolution that enables us to directly image electron and hole wavefunctions and to determine the thermodynamic gap of generalized Wigner crystal states in twisted WS2 moire heterostructures. High-resolution SSEC spectroscopy was achieved by combining scanning tunneling microscopy (STM) with a monolayer graphene sensing layer, thus enabling the generation of individual electron and hole quasiparticles in generalized Wigner crystals. We show that electron and hole quasiparticles have complementary wavefunction distributions and that thermodynamic gaps of order 50meV exist for the 1/3 and 2/3 generalized Wigner crystal states.

cond-mat.mes-hall↗

arXiv2022

Observation of a multitude of correlated states at the surface of bulk 1T-TaSe$_2$ crystals

The interplay between electron-electron interactions and structural ordering can yield exceptionally rich correlated electronic phases. We have used scanning tunneling microscopy to investigate bulk 1T-TaSe2 and have uncovered surprisingly diverse correlated surface states thereof. These surface states exhibit the same in-plane charge density wave ordering but dramatically different electronic ground states ranging from insulating to metallic. The insulating variety of surface state shows signatures of a decoupled surface Mott layer. The metallic surface states, on the other hand, exhibit zero-bias peaks of varying strength that suggest Kondo phases arising from coupling between the Mott surface layer and the metallic bulk of 1T-TaSe2. The surface of bulk 1T-TaSe2 thus constitutes a rare realization of the periodic Anderson model covering a wide parameter regime, thereby providing a model system for accessing different correlated phenomena in the same crystal. Our results highlight the central role played by strong correlations in this material family.

cond-mat.str-el↗

arXiv2022

Imaging Quantum Interference in Stadium-Shaped Monolayer and Bilayer Graphene Quantum Dots

Experimental realization of graphene-based stadium-shaped quantum dots (QDs) have been few and incompatible with scanned probe microscopy. Yet, direct visualization of electronic states within these QDs is crucial for determining the existence of quantum chaos in these systems. We report the fabrication and characterization of electrostatically defined stadium-shaped QDs in heterostructure devices composed of monolayer graphene (MLG) and bilayer graphene (BLG). To realize a stadium-shaped QD, we utilized the tip of a scanning tunneling microscope to charge defects in a supporting hexagonal boron nitride flake. The stadium states visualized are consistent with tight-binding-based simulations, but lack clear quantum chaos signatures. The absence of quantum chaos features in MLG-based stadium QDs is attributed to the leaky nature of the confinement potential due to Klein tunneling. In contrast, for BLG-based stadium QDs (which have stronger confinement) quantum chaos is precluded by the smooth confinement potential which reduces interference and mixing between states.

cond-mat.mes-hall↗

arXiv2022

Large-gap insulating dimer ground state in monolayer IrTe2

Monolayers of two-dimensional van der Waals materials exhibit novel electronic phases distinct from their bulk due to the symmetry breaking and reduced screening in the absence of the interlayer coupling. In this work, we combine angle-resolved photoemission spectroscopy and scanning tunneling microscopy/spectroscopy to demonstrate the emergence of a unique insulating 2 x 1 dimer ground state in monolayer 1T-IrTe2 that has a large band gap in contrast to the metallic bilayer-to-bulk forms of this material. First-principles calculations reveal that phonon and charge instabilities as well as local bond formation collectively enhance and stabilize a charge-ordered ground state. Our findings provide important insights into the subtle balance of interactions having similar energy scales that occurs in the absence of strong interlayer coupling, which offers new opportunities to engineer the properties of 2D monolayers.

cond-mat.mtrl-sci↗

arXiv2022

Evidence for a spinon Kondo effect in cobalt atoms on single-layer 1T-TaSe$_2$

Quantum spin liquids (QSLs) are highly entangled, disordered magnetic states that arise in frustrated Mott insulators and host exotic fractional excitations such as spinons and chargons. Despite being charge insulators some QSLs are predicted to exhibit gapless itinerant spinons that yield metallic behavior in the spin channel. We have deposited isolated magnetic atoms onto single-layer (SL) 1T-TaSe$_2$, a gapless QSL candidate, to experimentally probe how itinerant spinons couple to impurity spin centers. Using scanning tunneling spectroscopy we observe the emergence of new, impurity-induced resonance peaks at the 1T-TaSe$_2$ Hubbard band edges when cobalt adatoms are positioned to have maximal spatial overlap with the Hubbard band charge distribution. These resonance peaks disappear when the spatial overlap is reduced or when the magnetic impurities are replaced with non-magnetic impurities. Theoretical simulations using a modified Anderson impurity model integrated with a gapless quantum spin liquid show that these resonance peaks are consistent with a Kondo resonance induced by spinons combined with spinon-chargon binding effects that arise due to QSL gauge-field fluctuations.

cond-mat.str-el↗

arXiv2021

Gate-tunable artificial nucleus in graphene

We report an atomically-precise integration of individual nitrogen (N) dopant as an in-plane artificial nucleus in a graphene device by atomic implantation to probe its gate-tunable quantum states and correlation effects. The N dopant creates the characteristic resonance state in the conduction band, revealing a giant carrier-dependent energetic renormalization up to 350 meV with respect to the Dirac point, accompanied by the observation of long-range screening effects. Joint density functional theory and tight-binding calculations with modified perturbation potential corroborate experimental findings and highlight the short-range character of N-induced perturbation.

cond-mat.mtrl-sci↗

arXiv2021

Imaging reconfigurable molecular concentration on a graphene field-effect transistor

The spatial arrangement of adsorbates deposited onto a clean surface in vacuum typically cannot be reversibly tuned. Here we use scanning tunneling microscopy to demonstrate that molecules deposited onto graphene field-effect transistors exhibit reversible, electrically-tunable surface concentration. Continuous gate-tunable control over the surface concentration of charged F4TCNQ molecules was achieved on a graphene FET at T = 4.5K. This capability enables precisely controlled impurity doping of graphene devices and also provides a new method for determining molecular energy level alignment based on the gate-dependence of molecular concentration. The gate-tunable molecular concentration can be explained by a dynamical molecular rearrangement process that reduces total electronic energy by maintaining Fermi level pinning in the device substrate. Molecular surface concentration in this case is fully determined by the device back-gate voltage, its geometric capacitance, and the energy difference between the graphene Dirac point and the molecular LUMO level.

cond-mat.mes-hall↗

arXiv2021

Imaging gate-tunable Tomonaga-Luttinger liquids in 1H-MoSe$_2$ mirror twin boundaries

One-dimensional electron systems (1DESs) exhibit properties that are fundamentally different from higher-dimensional systems. For example, electron-electron interactions in 1DESs have been predicted to induce Tomonaga-Luttinger liquid behavior. Naturally-occurring grain boundaries in single-layer semiconducting transition metal dichalcogenides provide 1D conducting channels that have been proposed to host Tomonaga-Luttinger liquids, but charge density wave physics has also been suggested to explain their behavior. Clear identification of the electronic ground state of this system has been hampered by an inability to electrostatically gate such boundaries and thereby tune their charge carrier concentration. Here we present a scanning tunneling microscopy/spectroscopy study of gate-tunable mirror twin boundaries (MTBs) in single-layer 1H-MoSe$_2$ devices. Gating here enables STM spectroscopy to be performed for different MTB electron densities, thus allowing precise characterization of electron-electron interaction effects. Visualization of MTB electronic structure under these conditions allows unambiguous identification of collective density wave excitations having two distinct velocities, in quantitative agreement with the spin-charge separation predicted by finite-length Tomonaga-Luttinger-liquid theory.

cond-mat.str-el↗

arXiv2021

Imaging Generalized Wigner Crystal States in a WSe2/WS2 Moiré Superlattice

The Wigner crystal state, first predicted by Eugene Wigner in 1934, has fascinated condensed matter physicists for nearly 90 years2-14. Studies of two-dimensional (2D) electron gases first revealed signatures of the Wigner crystal in electrical transport measurements at high magnetic fields2-4. More recently optical spectroscopy has provided evidence of generalized Wigner crystal states in transition metal dichalcogenide (TMDC) moiré superlattices. Direct observation of the 2D Wigner crystal lattice in real space, however, has remained an outstanding challenge. Scanning tunneling microscopy (STM) in principle has sufficient spatial resolution to image a Wigner crystal, but conventional STM measurements can potentially alter fragile Wigner crystal states in the process of measurement. Here we demonstrate real-space imaging of 2D Wigner crystals in WSe2/WS2 moiré heterostructures using a novel non-invasive STM spectroscopy technique. We employ a graphene sensing layer in close proximity to the WSe2/WS2 moiré superlattice for Wigner crystal imaging, where local STM tunneling current into the graphene sensing layer is modulated by the underlying electron lattice of the Wigner crystal in the WSe2/WS2 heterostructure. Our measurement directly visualizes different lattice configurations associated with Wigner crystal states at fractional electron fillings of n = 1/3, 1/2, and 2/3, where n is the electron number per site. The n=1/3 and n=2/3 Wigner crystals are observed to exhibit a triangle and a honeycomb lattice, respectively, in order to minimize nearest-neighbor occupations. The n = 1/2 state, on the other hand, spontaneously breaks the original C3 symmetry and forms a stripe structure in real space. Our study lays a solid foundation toward the fundamental understanding of rich Wigner crystal states in WSe2/WS2 moiré heterostructures.

cond-mat.mes-hall↗

arXiv2021

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.

cond-mat.str-el↗

arXiv2021

Imaging local discharge cascades for correlated electrons in WS2/WSe2 moiré superlattices

Transition metal dichalcogenide (TMD) moiré heterostructures provide an ideal platform to explore the extended Hubbard model1 where long-range Coulomb interactions play a critical role in determining strongly correlated electron states. This has led to experimental observations of Mott insulator states at half filling2-4 as well as a variety of extended Wigner crystal states at different fractional fillings5-9. Microscopic understanding of these emerging quantum phases, however, is still lacking. Here we describe a novel scanning tunneling microscopy (STM) technique for local sensing and manipulation of correlated electrons in a gated WS2/WSe2 moiré superlattice that enables experimental extraction of fundamental extended Hubbard model parameters. We demonstrate that the charge state of local moiré sites can be imaged by their influence on STM tunneling current, analogous to the charge-sensing mechanism in a single-electron transistor. In addition to imaging, we are also able to manipulate the charge state of correlated electrons. Discharge cascades of correlated electrons in the moiré superlattice are locally induced by ramping the STM bias, thus enabling the nearest-neighbor Coulomb interaction (UNN) to be estimated. 2D mapping of the moiré electron charge states also enables us to determine onsite energy fluctuations at different moiré sites. Our technique should be broadly applicable to many semiconductor moiré systems, offering a powerful new tool for microscopic characterization and control of strongly correlated states in moiré superlattices.

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