arXiv subjects

Michael F. Crommie

Publications and source records attributed to Michael F. Crommie.

At least 55 records · Page 3Linked to original sources

arXiv2020

Tunable ferromagnetism at non-integer filling of a moiré superlattice

The flat bands resulting from moiré superlattices in magic-angle twisted bilayer graphene (MATBG) and ABC-trilayer graphene aligned with hexagonal boron nitride (ABC-TLG/hBN) have been shown to give rise to fascinating correlated electron phenomena such as correlated insulators and superconductivity. More recently, orbital magnetism associated with correlated Chern insulators was found in this class of layered structures centered at integer multiples of n0, the density corresponding to one electron per moiré superlattice unit cell. Here we report the experimental observation of ferromagnetism at fractional filling of a flat Chern band in an ABC-TLG/hBN moirésuperlattice. The ferromagnetic state exhibits prominent ferromagnetic hysteresis behavior with large anomalous Hall resistivity in a broad region of densities, centered in the valence miniband at n = -2.3 n0. This ferromagnetism depends very sensitively on the control parameters in the moiré system: not only the magnitude of the anomalous Hall signal, but also the sign of the hysteretic ferromagnetic response can be modulated by tuning the carrier density and displacement field. Our discovery of electrically tunable ferromagnetism in a moiré Chern band at non-integer filling highlights the opportunities for exploring new correlated ferromagnetic states in moiré heterostructures.

cond-mat.mes-hall↗

arXiv2020

Non-Covalent Dimerization after Enediyne Cyclization on Au(111)

We investigate the thermally-induced cyclization of 1,2 - bis(2 - phenylethynyl)benzene on Au(111) using scanning tunneling microscopy and computer simulations. Cyclization of sterically hindered enediynes is known to proceed via two competing mechanisms in solution: a classic C1 - C6 or a C1 - C5 cyclization pathway. On Au(111) we find that the C1 - C5 cyclization is suppressed and that the C1 - C6 cyclization yields a highly strained bicyclic olefin whose surface chemistry was hitherto unknown. The C1 - C6 product self-assembles into discrete non-covalently bound dimers on the surface. The reaction mechanism and driving forces behind non-covalent association are discussed in light of density functional theory calculations.

cond-mat.mtrl-sci↗

arXiv2020

Imaging spinon density modulations in a 2D quantum spin liquid

Two-dimensional triangular-lattice antiferromagnets are predicted under some conditions to exhibit a quantum spin liquid ground state whose low-energy behavior is described by a spinon Fermi surface. Directly imaging the resulting spinons, however, is difficult due to their fractional, chargeless nature. Here we use scanning tunneling spectroscopy to image spinon density modulations arising from a spinon Fermi surface instability in single-layer 1T-TaSe$_2$, a two-dimensional Mott insulator. We first demonstrate the existence of localized spins arranged on a triangular lattice in single-layer 1T-TaSe$_2$ by contacting it to a metallic 1H-TaSe$_2$ layer and measuring the Kondo effect. Subsequent spectroscopic imaging of isolated, single-layer 1T-TaSe$_2$ reveals long-wavelength modulations at Hubbard band energies that reflect spinon density modulations. This allows direct experimental measurement of the spinon Fermi wavevector, in good agreement with theoretical predictions for a 2D quantum spin liquid. These results establish single-layer 1T-TaSe$_2$ as a new platform for studying novel two-dimensional quantum-spin-liquid phenomena.

cond-mat.str-el↗

arXiv2020

Imaging moiré flat bands in 3D reconstructed WSe2/WS2 superlattices

Moiré superlattices in transition metal dichalcogenide (TMD) heterostructures can host novel correlated quantum phenomena due to the interplay of narrow moiré flat bands and strong, long-range Coulomb interactions1-5. However, microscopic knowledge of the atomically-reconstructed moiré superlattice and resulting flat bands is still lacking, which is critical for fundamental understanding and control of the correlated moiré phenomena. Here we quantitatively study the moiré flat bands in three-dimensional (3D) reconstructed WSe2/WS2 moiré superlattices by comparing scanning tunneling spectroscopy (STS) of high quality exfoliated TMD heterostructure devices with ab initio simulations of TMD moiré superlattices. A strong 3D buckling reconstruction accompanied by large in-plane strain redistribution is identified in our WSe2/WS2 moiré heterostructures. STS imaging demonstrates that this results in a remarkably narrow and highly localized K-point moiré flat band at the valence band edge of the heterostructure. A series of moiré flat bands are observed at different energies that exhibit varying degrees of localization. Our observations contradict previous simplified theoretical models but agree quantitatively with ab initio simulations that fully capture the 3D structural reconstruction. Here the strain redistribution and 3D buckling dominate the effective moiré potential and result in moiré flat bands at the Brillouin zone K points.

cond-mat.mes-hall↗

arXiv2020

Identifying substitutional oxygen as a prolific point defect in monolayer transition metal dichalcogenides with experiment and theory

Chalcogen vacancies are considered to be the most abundant point defects in two-dimensional (2D) transition-metal dichalcogenide (TMD) semiconductors, and predicted to result in deep in-gap states (IGS). As a result, important features in the optical response of 2D-TMDs have typically been attributed to chalcogen vacancies, with indirect support from Transmission Electron Microscopy (TEM) and Scanning Tunneling Microscopy (STM) images. However, TEM imaging measurements do not provide direct access to the electronic structure of individual defects; and while Scanning Tunneling Spectroscopy (STS) is a direct probe of local electronic structure, the interpretation of the chemical nature of atomically-resolved STM images of point defects in 2D-TMDs can be ambiguous. As a result, the assignment of point defects as vacancies or substitutional atoms of different kinds in 2D-TMDs, and their influence on their electronic properties, has been inconsistent and lacks consensus. Here, we combine low-temperature non-contact atomic force microscopy (nc-AFM), STS, and state-of-the-art ab initio density functional theory (DFT) and GW calculations to determine both the structure and electronic properties of the most abundant individual chalcogen-site defects common to 2D-TMDs. Surprisingly, we observe no IGS for any of the chalcogen defects probed. Our results and analysis strongly suggest that the common chalcogen defects in our 2D-TMDs, prepared and measured in standard environments, are substitutional oxygen rather than vacancies.

cond-mat.mtrl-sci↗

arXiv2019

Imaging electric field dynamics with graphene optoelectronics

The use of electric fields for signalling and control in liquids is widespread, spanning bioelectric activity in cells to electrical manipulation of microstructures in lab-on-a-chip devices. However, an appropriate tool to resolve the spatio-temporal distribution of electric fields over a large dynamic range has yet to be developed. Here we present a label-free method to image local electric fields in real time and under ambient conditions. Our technique combines the unique gate-variable optical transitions of graphene with a critically coupled planar waveguide platform that enables highly sensitive detection of local electric fields with a voltage sensitivity of a few microvolts, a spatial resolution of tens of micrometres and a frequency response over tens of kilohertz. Our imaging platform enables parallel detection of electric fields over a large field of view and can be tailored to broad applications spanning lab-on-a-chip device engineering to analysis of bioelectric phenomena.

cond-mat.mes-hall↗

arXiv2019

Inducing Metallicity in Graphene Nanoribbons via Zero-Mode Superlattices

The design and fabrication of robust metallic states in graphene nanoribbons (GNRs) is a significant challenge since lateral quantum confinement and many-electron interactions tend to induce electronic band gaps when graphene is patterned at nanometer length scales. Recent developments in bottom-up synthesis have enabled the design and characterization of atomically-precise GNRs, but strategies for realizing GNR metallicity have been elusive. Here we demonstrate a general technique for inducing metallicity in GNRs by inserting a symmetric superlattice of zero-energy modes into otherwise semiconducting GNRs. We verify the resulting metallicity using scanning tunneling spectroscopy as well as first-principles density-functional theory and tight binding calculations. Our results reveal that the metallic bandwidth in GNRs can be tuned over a wide range by controlling the overlap of zero-mode wavefunctions through intentional sublattice symmetry-breaking.

cond-mat.mtrl-sci↗

arXiv2019

Visualizing Exotic Orbital Texture in the Single-Layer Mott Insulator 1T-TaSe2

Mott insulating behavior is induced by strong electron correlation and can lead to exotic states of matter such as unconventional superconductivity and quantum spin liquids. Recent advances in van der Waals material synthesis enable the exploration of novel Mott systems in the two-dimensional limit. Here we report characterization of the local electronic properties of single- and few-layer 1T-TaSe2 via spatial- and momentum-resolved spectroscopy involving scanning tunneling microscopy and angle-resolved photoemission. Our combined experimental and theoretical study indicates that electron correlation induces a robust Mott insulator state in single-layer 1T-TaSe2 that is accompanied by novel orbital texture. Inclusion of interlayer coupling weakens the insulating phase in 1T-TaSe2, as seen by strong reduction of its energy gap and quenching of its correlation-driven orbital texture in bilayer and trilayer 1T-TaSe2. Our results establish single-layer 1T-TaSe2 as a useful new platform for investigating strong correlation physics in two dimensions.

cond-mat.str-el↗

arXiv2018

Electrons imitating light: Frustrated supercritical collapse in charged arrays on graphene

The photon-like electronic dispersion of graphene bestows its charge carriers with unusual confinement properties that depend strongly on the geometry and strength of the surrounding potential. Here we report bottom-up synthesis of atomically-precise one-dimensional (1D) arrays of point charges aimed at exploring supercritical confinement of carriers in graphene for new geometries. The arrays were synthesized by arranging F4TCNQ molecules into a 1D lattice on back-gated graphene devices, allowing precise tuning of both the molecular charge state and the array periodicity. Dilute arrays of ionized F4TCNQ molecules are seen to behave like isolated subcritical charges but dense arrays show emergent supercriticality. In contrast to compact supercritical clusters, extended 1D charge arrays exhibit both supercritical and subcritical characteristics and belong to a new physical regime termed frustrated supercritical collapse. Here carriers in the far-field are attracted by a supercritical charge distribution, but have their fall to the center frustrated by subcritical potentials in the near-field, similar to the trapping of light by a dense cluster of stars in general relativity.

cond-mat.mes-hall↗

arXiv2018

Observation of Topologically Protected States at Crystalline Phase Boundaries in Single-layer WSe2

Transition metal dichalcogenide (TMD) materials are unique in the wide variety of structural and electronic phases they exhibit in the two-dimensional (2D) single-layer limit. Here we show how such polymorphic flexibility can be used to achieve topological states at highly ordered phase boundaries in a new quantum spin Hall insulator (QSHI), 1T'-WSe2. We observe helical states at the crystallographically-aligned interface between quantum a spin Hall insulating domain of 1T'-WSe2 and a semiconducting domain of 1H-WSe2 in contiguous single layers grown using molecular beam epitaxy (MBE). The QSHI nature of single-layer 1T'-WSe2 was verified using ARPES to determine band inversion around a 120 meV energy gap, as well as STM spectroscopy to directly image helical edge-state formation. Using this new edge-state geometry we are able to directly confirm the predicted penetration depth of a helical interface state into the 2D bulk of a QSHI for a well-specified crystallographic direction. The clean, well-ordered topological/trivial interfaces observed here create new opportunities for testing predictions of the microscopic behavior of topologically protected boundary states without the complication of structural disorder.

cond-mat.mtrl-sci↗

arXiv2018

Microscopy of hydrogen and hydrogen-vacancy defect structures on graphene devices

We have used scanning tunneling microscopy (STM) to investigate two types of hydrogen defect structures on monolayer graphene supported by hexagonal boron nitride (h-BN) in a gated field-effect transistor configuration. The first H-defect type is created by bombarding graphene with 1-keV ionized hydrogen and is identified as two hydrogen atoms bonded to a graphene vacancy via comparison of experimental data to first-principles calculations. The second type of H defect is identified as dimerized hydrogen and is created by depositing atomic hydrogen having only thermal energy onto a graphene surface. Scanning tunneling spectroscopy (STS) measurements reveal that hydrogen dimers formed in this way open a new elastic channel in the tunneling conductance between an STM tip and graphene.

cond-mat.mes-hall↗

arXiv2018

Simulating the nanomechanical response of cyclooctatetraene molecules on a graphene device

We investigate the atomic and electronic structures of cyclooctatetraene (COT) molecules on graphene and analyze their dependence on external gate voltage using first-principles calculations. The external gate voltage is simulated by adding or removing electrons using density functional theory (DFT) calculations. This allows us to investigate how changes in carrier density modify the molecular shape, orientation, adsorption site, diffusion barrier, and diffusion path. For increased hole doping COT molecules gradually change their shape to a more flattened conformation and the distance between the molecules and graphene increases while the diffusion barrier drastically decreases. For increased electron doping an abrupt transition to a planar conformation at a carrier density of -8$\times$10$^{13}$ e/cm$^2$ is observed. These calculations imply that the shape and mobility of adsorbed COT molecules can be controlled by externally gating graphene devices.

cond-mat.mtrl-sci↗

arXiv2018

Visualization and Control of Single Electron Charging in Bilayer Graphene Quantum Dots

Graphene p-n junctions provide an ideal platform for investigating novel behavior at the boundary between electronics and optics that arise from massless Dirac fermions, such as whispering gallery modes and Veselago lensing. Bilayer graphene also hosts Dirac fermions, but they differ from single-layer graphene charge carriers because they are massive, can be gapped by an applied perpendicular electric field, and have very different pseudospin selection rules across a p-n junction. Novel phenomena predicted for these massive Dirac fermions at p-n junctions include anti-Klein tunneling, oscillatory Zener tunneling, and electron cloaked states. Despite these predictions there has been little experimental focus on the microscopic spatial behavior of massive Dirac fermions in the presence of p-n junctions. Here we report the experimental manipulation and characterization of massive Dirac fermions within bilayer graphene quantum dots defined by circular p-n junctions through the use of scanning tunneling microscopy-based (STM) methods. Our p-n junctions are created via a flexible technique that enables realization of exposed quantum dots in bilayer graphene/hBN heterostructures. These quantum dots exhibit sharp spectroscopic resonances that disperse in energy as a function of applied gate voltage. Spatial maps of these features show prominent concentric rings with diameters that can be tuned by an electrostatic gate. This behavior is explained by single-electron charging of localized states that arise from the quantum confinement of massive Dirac fermions within our exposed bilayer graphene quantum dots.

cond-mat.mes-hall↗

arXiv2017

Hierarchical On-Surface Synthesis of Deterministic Graphene Nanoribbon Heterojunctions

Bottom-up graphene nanoribbon (GNR) heterojunctions are nanoscale strips of graphene whose electronic structure abruptly changes across a covalently bonded interface. Their rational design offers opportunities for profound technological advancements enabled by their extraordinary structural and electronic properties. Thus far the most critical aspect of their synthesis, the control over sequence and position of heterojunctions along the length of a ribbon, has been plagued by randomness in monomer sequences emerging from step-growth copolymerization of distinct monomers. All bottom-up GNR heterojunction structures created so far have exhibited random sequences of heterojunctions and, while useful for fundamental scientific studies, are difficult to incorporate into functional nanodevices as a result. Here we describe a new hierarchical fabrication strategy that allows deterministic growth of bottom-up GNRs that preferentially exhibit a single heterojunction interface rather than a random statistical sequence of junctions along the ribbon. Such heterojunctions provide a viable new platform that could be directly used in functional GNR-based device applications at the molecular scale. Our hierarchical GNR fabrication strategy is based on differences in the dissociation energies of C-Br and C-I bonds that allow control over the growth sequence of the block-copolymers from which GNRs are formed, and consequently yields a significantly higher proportion of single-junction GNR heterostructures. Scanning tunnelling spectroscopy and density functional theory calculations confirm that hierarchically-grown heterojunctions between chevron GNR (cGNR) and binaphthyl-cGNR segments exhibit straddling Type I band alignment in structures that are only one atomic layer thick and 3 nm in width.

cond-mat.mtrl-sci↗

arXiv2017

Spatially resolving density-dependent screening around a single charged atom in graphene

Electrons in two-dimensional graphene sheets behave as interacting chiral Dirac fermions and have unique screening properties due to their symmetry and reduced dimensionality. By using a combination of scanning tunneling spectroscopy (STM/STS) measurements and theoretical modeling we have characterized how graphene's massless charge carriers screen individual charged calcium atoms. A back-gated graphene device configuration has allowed us to directly visualize how the screening length for this system can be tuned with carrier density. Our results provide insight into electron-impurity and electron-electron interactions in a relativistic setting with important consequences for other graphene-based electronic devices.

cond-mat.mes-hall↗

arXiv2017

Iodine versus Bromine Functionalization for Bottom-Up Graphene Nanoribbon Growth: Role of Diffusion

Deterministic bottom-up approaches for synthesizing atomically well-defined graphene nanoribbons (GNRs) largely rely on the surface-catalyzed activation of selected labile bonds in a molecular precursor followed by step growth polymerization and cyclodehydrogenation. While the majority of successful GNR precursors rely on the homolytic cleavage of thermally labile C-Br bonds, the introduction of weaker C-I bonds provides access to monomers that can be polymerized at significantly lower temperatures, thus helping to increase the flexibility of the GNR synthesis process. Scanning tunneling microscopy (STM) imaging of molecular precursors, activated intermediates, and polymers resulting from stepwise thermal annealing of both Br and I substituted precursors for chevron GNRs reveals that the polymerization of both precursors proceeds at similar temperatures on Au(111). This observation is consistent with diffusion-limited polymerization of the surface-stabilized radical intermediates that emerge from homolytic cleavage of either the C-Br or the C-I bonds.

cond-mat.mes-hall↗

arXiv2017

Realization of Quantum Spin Hall State in Monolayer 1T'-WTe2

A quantum spin Hall (QSH) insulator is a novel two-dimensional quantum state of matter that features quantized Hall conductance in the absence of magnetic field, resulting from topologically protected dissipationless edge states that bridge the energy gap opened by band inversion and strong spin-orbit coupling. By investigating electronic structure of epitaxially grown monolayer 1T'-WTe2 using angle-resolved photoemission (ARPES) and first principle calculations, we observe clear signatures of the topological band inversion and the band gap opening, which are the hallmarks of a QSH state. Scanning tunneling microscopy measurements further confirm the correct crystal structure and the existence of a bulk band gap, and provide evidence for a modified electronic structure near the edge that is consistent with the expectations for a QSH insulator. Our results establish monolayer 1T'-WTe2 as a new class of QSH insulator with large band gap in a robust two-dimensional materials family of transition metal dichalcogenides (TMDCs).

cond-mat.mtrl-sci↗

arXiv2017

Imaging structural transitions in organometallic molecules on Ag(100) for solar thermal energy storage

The use of opto-thermal molecular energy storage at the nanoscale creates new opportunities for powering future microdevices with flexible synthetic tailorability. Practical application of these molecular materials, however, requires a deeper microscopic understanding of how their behavior is altered by the presence of different types of substrates. Here we present single-molecule resolved scanning tunneling microscopy imaging of thermally- and optically-induced structural transitions in (fulvalene)tetracarbonyldiruthenium molecules adsorbed onto a Ag(100) surface as a prototype system. Both the parent complex and the photoisomer display distinct thermally-driven phase transformations when they are in contact with a Ag(100) surface. This behavior is consistent with the loss of carbonyl ligands due to strong molecule-surface coupling. Ultraviolet radiation induces marked structural changes only in the intact parent complex, thus indicating a photoisomerization reaction. These results demonstrate how stimuli-induced structural transitions in this class of molecule depend on the nature of the underlying substrate.

cond-mat.mtrl-sci↗