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1.
Nat Mater ; 2020 Mar 30.
Artigo em Inglês | MEDLINE | ID: mdl-32231241

RESUMO

Interacting electrons confined in one dimension are generally described by the Luttinger liquid formalism, where the low-energy electronic dispersion is assumed to be linear and the resulting plasmonic excitations are non-interacting. Instead, a Luttinger liquid in one-dimensional materials with nonlinear electronic bands is expected to show strong plasmon-plasmon interactions, but an experimental demonstration of this behaviour has been lacking. Here, we combine infrared nano-imaging and electronic transport to investigate the behaviour of plasmonic excitations in semiconducting single-walled carbon nanotubes with carrier density controlled by electrostatic gating. We show that both the propagation velocity and the dynamic damping of plasmons can be tuned continuously, which is well captured by the nonlinear Luttinger liquid theory. These results contrast with the gate-independent plasmons observed in metallic nanotubes, as expected for a linear Luttinger liquid. Our findings provide an experimental demonstration of one-dimensional electron dynamics beyond the conventional linear Luttinger liquid paradigm and are important for understanding excited-state properties in one dimension.

2.
Nano Lett ; 2020 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-32286843

RESUMO

The layer stacking order has profound effects on the physical properties of two-dimensional van der Waals heterostructures. For example, graphene multilayers can have distinct electronic band structures and exhibit completely different behaviors depending on the stacking order. Fascinating physical phenomena, such as correlated insulators, superconductors, and ferromagnetism, can also emerge with a periodic variation of the layer stacking order, which is known as the moiré superlattice in van der Waals materials. In this work, we realize the global phase transition between different graphene layer stacking orders and elucidate its microscopic origin. We experimentally determine the energy difference between different stacking orders with the accuracy of µeV/atom. We reveal that both the carrier doping and the electric field can drive the layer-stacking phase transition through different mechanisms: carrier doping can change the energy difference because of a non-negligible work function difference between different stacking orders; the electric field, on the other hand, induces a band-gap opening in ABC-stacked graphene and hence changes the energy difference. Our findings provide a fundamental understanding of the electrically driven stacking-order phase transition in few-layer graphene and demonstrate a reversible and noninvasive method to globally control the stacking order.

3.
Nature ; 579(7799): 359-363, 2020 03.
Artigo em Inglês | MEDLINE | ID: mdl-32188951

RESUMO

Moiré superlattices can be used to engineer strongly correlated electronic states in two-dimensional van der Waals heterostructures, as recently demonstrated in the correlated insulating and superconducting states observed in magic-angle twisted-bilayer graphene and ABC trilayer graphene/boron nitride moiré superlattices1-4. Transition metal dichalcogenide moiré heterostructures provide another model system for the study of correlated quantum phenomena5 because of their strong light-matter interactions and large spin-orbit coupling. However, experimental observation of correlated insulating states in this system is challenging with traditional transport techniques. Here we report the optical detection of strongly correlated phases in semiconducting WSe2/WS2 moiré superlattices. We use a sensitive optical detection technique and reveal a Mott insulator state at one hole per superlattice site and surprising insulating phases at 1/3 and 2/3 filling of the superlattice, which we assign to generalized Wigner crystallization on the underlying lattice6-11. Furthermore, the spin-valley optical selection rules12-14 of transition metal dichalcogenide heterostructures allow us to optically create and investigate low-energy excited spin states in the Mott insulator. We measure a very long spin relaxation lifetime of many microseconds in the Mott insulating state, orders of magnitude longer than that of charge excitations. Our studies highlight the value of using moiré superlattices beyond graphene to explore correlated physics.

4.
ACS Nano ; 2020 Jan 08.
Artigo em Inglês | MEDLINE | ID: mdl-31891480

RESUMO

Membranes that selectively filter for both anions and cations are central to technological applications from clean energy generation to desalination devices. 2D materials have immense potential as these ion-selective membranes due to their thinness, mechanical strength, and tunable surface chemistry; however, currently, only cation-selective membranes have been reported. Here we demonstrate the controllable cation and anion selectivity of both monolayer graphene and hexagonal boron nitride. In particular, we measure the ionic current through membranes grown by chemical vapor deposition containing well-known defects inherent to scalably produced and wet-transferred 2D materials. We observe a striking change from cation selectivity with monovalent ions to anion selectivity by controlling the concentration of multivalent ions and inducing charge inversion on the 2D membrane. Furthermore, we find good agreement between our experimental data and theoretical predictions from the Goldman-Hodgkin-Katz equation and use this model to extract selectivity ratios. These tunable selective membranes conduct up to 500 anions for each cation and thus show potential for osmotic power generation.

5.
ACS Nano ; 13(11): 12385-12392, 2019 Nov 26.
Artigo em Inglês | MEDLINE | ID: mdl-31593435

RESUMO

The self-assembly of nanoscale materials at the liquid-liquid interface allows for fabrication of three-dimensionally structured liquids with nearly arbitrary geometries and tailored electronic, optical, and magnetic properties. Two-dimensional (2D) materials are highly anisotropic, with thicknesses on the order of a nanometer and lateral dimensions upward of hundreds of nanometers to micrometers. Controlling the assembly of these materials has direct implications for their properties and performance. We here describe the interfacial assembly and jamming of Ti3C2Tx MXene nanosheets at the oil-water interface. Planar, as well as complex, programmed three-dimensional all-liquid objects are realized. Our approach presents potential for the creation of all-liquid 3D-printed devices for possible applications in all-liquid electrochemical and energy storage devices and electrically active, all-liquid fluidics that exploits the versatile structure, functionality, and reconfigurability of liquids.

6.
ACS Nano ; 13(11): 12710-12718, 2019 Nov 26.
Artigo em Inglês | MEDLINE | ID: mdl-31638764

RESUMO

Recent direct experimental observation of multiple highly dispersive C60 valence bands has allowed for a detailed analysis of the unusual photoemission traits of these features through photon energy- and polarization-dependent measurements. Previously obscured dispersions and strong photoemission traits are now revealed by specific light polarizations. The observed intensity effects prove the locking in place of the C60 molecules at low temperatures and the existence of an orientational order imposed by the substrate chosen. Most importantly, photon energy- and polarization-dependent effects are shown to be intimately linked with the orbital character of the C60 band manifolds which allow for a more precise determination of the orbital character within the third highest occupied molecular orbital (HOMO-2). Our observations and analysis provide important considerations for the connection between molecular and crystalline C60 electronic structure, past and future band structure studies, and for increasingly popular C60 electronic device applications, especially those making use of heterostructures.

7.
Nat Mater ; 18(10): 1065-1070, 2019 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-31384030

RESUMO

The Berry phase of Bloch states can have profound effects on electron dynamics1-3 and lead to novel transport phenomena, such as the anomalous Hall effect and the valley Hall effect4-6. Recently, it was predicted that the Berry phase effect can also modify the exciton states in transition metal dichalcogenide monolayers, and lift the energy degeneracy of exciton states with opposite angular momentum through an effective valley-orbital coupling1,7-11. Here, we report the observation and control of the Berry phase-induced splitting of the 2p exciton states in monolayer molybdenum diselenide (MoSe2) using the intraexciton optical Stark spectroscopy. We observe the time-reversal-symmetric analogue of the orbital Zeeman effect resulting from the valley-dependent Berry phase, which leads to energy difference of +14 (-14) meV between the 2p+ and 2p- exciton states in the K (K') valley, consistent with the ordering from our ab initio GW-Bethe-Salpeter equation results. In addition, we show that the light-matter coupling between intraexciton states is remarkably strong, leading to a prominent valley-dependent Autler-Townes doublet under resonant driving. Our study opens up pathways to coherently manipulate the quantum states and excitonic excitation with infrared radiation in two-dimensional semiconductors.

8.
Nature ; 569(7757): E7, 2019 May.
Artigo em Inglês | MEDLINE | ID: mdl-31065056

RESUMO

Change history: In this Letter, the following text has been added to the Acknowledgements section: "the scanning transmission electron microscopy measurements at the Molecular Foundry were supported by the Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under contract number DE-AC02-05CH11231". See accompanying Amendment.

9.
Nano Lett ; 19(3): 1782-1787, 2019 03 13.
Artigo em Inglês | MEDLINE | ID: mdl-30746949

RESUMO

Alloying two-dimensional (2D) semiconductors provides a powerful method to tune their physical properties, especially those relevant to optoelectronic applications. However, as the crystal structure becomes more complex, it becomes increasingly difficult to accurately correlate response characteristics to detailed atomic structure. We investigate, via annular dark-field scanning transmission electron microscopy, electron energy loss spectroscopy, and second harmonic generation, the layered III-VI alloy GaSe0.5Te0.5 as a function of layer number. The local atomic structure and stacking sequence for different layers is explicitly determined. We complement the measurements with first-principles calculations of the total energy and electronic band structure of GaSe0.5Te0.5 for different crystal structures and layer number. The electronic band gap as well as the π and π + σ plasmons are found to be sensitive to layer number.

10.
Nature ; 567(7746): 76-80, 2019 03.
Artigo em Inglês | MEDLINE | ID: mdl-30804525

RESUMO

Moiré superlattices enable the generation of new quantum phenomena in two-dimensional heterostructures, in which the interactions between the atomically thin layers qualitatively change the electronic band structure of the superlattice. For example, mini-Dirac points, tunable Mott insulator states and the Hofstadter butterfly pattern can emerge in different types of graphene/boron nitride moiré superlattices, whereas correlated insulating states and superconductivity have been reported in twisted bilayer graphene moiré superlattices1-12. In addition to their pronounced effects on single-particle states, moiré superlattices have recently been predicted to host excited states such as moiré exciton bands13-15. Here we report the observation of moiré superlattice exciton states in tungsten diselenide/tungsten disulfide (WSe2/WS2) heterostructures in which the layers are closely aligned. These moiré exciton states manifest as multiple emergent peaks around the original WSe2 A exciton resonance in the absorption spectra, and they exhibit gate dependences that are distinct from that of the A exciton in WSe2 monolayers and in WSe2/WS2 heterostructures with large twist angles. These phenomena can be described by a theoretical model in which the periodic moiré potential is much stronger than the exciton kinetic energy and generates multiple flat exciton minibands. The moiré exciton bands provide an attractive platform from which to explore and control excited states of matter, such as topological excitons and a correlated exciton Hubbard model, in transition-metal dichalcogenides.

11.
Nat Commun ; 10(1): 477, 2019 01 29.
Artigo em Inglês | MEDLINE | ID: mdl-30696830

RESUMO

The photon-like behavior of electrons in graphene causes unusual confinement properties that depend strongly on the geometry and strength of the surrounding potential. We report bottom-up synthesis of atomically-precise one-dimensional (1D) arrays of point charges on graphene that allow exploration of a new type of supercritical confinement of graphene carriers. The arrays were synthesized by arranging F4TCNQ molecules into a 1D lattice on back-gated graphene, allowing precise tuning of both the molecular charge and the array periodicity. While dilute arrays of ionized F4TCNQ molecules are seen to behave like isolated subcritical charges, dense arrays show emergent supercriticality. In contrast to compact supercritical clusters, these extended arrays display 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 their fall to the center is frustrated by subcritical potentials in the near-field, similar to trapping of light by a dense cluster of stars in general relativity.

12.
Phys Rev Lett ; 121(4): 047702, 2018 Jul 27.
Artigo em Inglês | MEDLINE | ID: mdl-30095956

RESUMO

Quantum-confined electrons in one dimension behave as a Luttinger liquid. However, unambiguous demonstration of Luttinger liquid phenomena in single-walled carbon nanotubes (SWNTs) has been challenging. Here we investigate well-defined SWNT cross junctions with a point contact between two Luttinger liquids and combine electrical transport and optical nanoscopy measurements to correlate completely different physical properties (i.e., the electron tunneling and the plasmon propagation) in the same Luttinger liquid system. The suppressed electron tunneling at SWNT junctions exhibits a power-law scaling, which yields a Luttinger liquid interaction parameter that agrees quantitatively with that independently determined from the plasmon velocity based on the near-field optical nanoscopy.

13.
Nano Lett ; 18(8): 5104-5110, 2018 08 08.
Artigo em Inglês | MEDLINE | ID: mdl-30035544

RESUMO

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.

14.
Science ; 361(6399): 263-266, 2018 07 20.
Artigo em Inglês | MEDLINE | ID: mdl-30026223

RESUMO

The scientific bounty resulting from the successful isolation of few to single layers of two-dimensional materials suggests that related new physics resides in the few- to single-chain limit of one-dimensional materials. We report the synthesis of the quasi-one-dimensional transition metal trichalcogenide NbSe3 (niobium triselenide) in the few-chain limit, including the realization of isolated single chains. The chains are encapsulated in protective boron nitride or carbon nanotube sheaths to prevent oxidation and to facilitate characterization. Transmission electron microscopy reveals static and dynamic structural torsional waves not found in bulk NbSe3 crystals. Electronic structure calculations indicate that charge transfer drives the torsional wave instability. Very little covalent bonding is found between the chains and the nanotube sheath, leading to relatively unhindered longitudinal and torsional dynamics for the encapsulated chains.

15.
Science ; 360(6391): 893-896, 2018 05 25.
Artigo em Inglês | MEDLINE | ID: mdl-29798880

RESUMO

Transition metal dichalcogenide (TMDC) materials are promising for spintronic and valleytronic applications because valley-polarized excitations can be generated and manipulated with circularly polarized photons and the valley and spin degrees of freedom are locked by strong spin-orbital interactions. In this study we demonstrate efficient generation of a pure and locked spin-valley diffusion current in tungsten disulfide (WS2)-tungsten diselenide (WSe2) heterostructures without any driving electric field. We imaged the propagation of valley current in real time and space by pump-probe spectroscopy. The valley current in the heterostructures can live for more than 20 microseconds and propagate over 20 micrometers; both the lifetime and the diffusion length can be controlled through electrostatic gating. The high-efficiency and electric-field-free generation of a locked spin-valley current in TMDC heterostructures holds promise for applications in spin and valley devices.

16.
Nano Lett ; 18(4): 2683-2688, 2018 04 11.
Artigo em Inglês | MEDLINE | ID: mdl-29583012

RESUMO

Quantum emitters in two-dimensional hexagonal boron nitride (hBN) are attractive for a variety of quantum and photonic technologies because they combine ultra-bright, room-temperature single-photon emission with an atomically thin crystal. However, the emitter's prominence is hindered by large, strain-induced wavelength shifts. We report the discovery of a visible-wavelength, single-photon emitter (SPE) in a zero-dimensional boron nitride allotrope (the boron nitride nanococoon, BNNC) that retains the excellent optical characteristics of few-layer hBN while possessing an emission line variation that is lower by a factor of 5 than the hBN emitter. We determined the emission source to be the nanometer-size BNNC through the cross-correlation of optical confocal microscopy with high-resolution scanning and transmission electron microscopy. Altogether, this discovery enlivens color centers in BN materials and, because of the BN nanococoon's size, opens new and exciting opportunities in nanophotonics, quantum information, biological imaging, and nanoscale sensing.

17.
Nano Lett ; 18(2): 1442-1447, 2018 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-29364679

RESUMO

We report on the self-assembly of semicrystalline [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) nanosheets at the interface between a hydrophobic solvent and water, and utilize this opportunity for the realization of electronically active organic/organic molecular heterostructures. The self-assembled PCBM nanosheets can feature a lateral size of >1 cm2 and be transferred from the water surface to both hydrophobic and hydrophilic surfaces using facile transfer techniques. We employ a transferred single PCBM nanosheet as the active material in a field-effect transistor (FET) and verify semiconductor function by a measured electron mobility of 1.2 × 10-2 cm2 V-1 s-1 and an on-off ratio of ∼1 × 104. We further fabricate a planar organic/organic heterostructure with the p-type organic semiconductor poly(3-hexylthiophene-2,5-diyl) as the bottom layer and the n-type PCBM nanosheet as the top layer and demonstrate ambipolar FET operation with an electron mobility of 8.7 × 10-4 cm2 V-1 s-1 and a hole mobility of 3.1 × 10-4 cm2 V-1 s-1.

18.
Nat Mater ; 17(2): 204, 2018 01 23.
Artigo em Inglês | MEDLINE | ID: mdl-29358774

RESUMO

This corrects the article DOI: 10.1038/nmat4795.

19.
ACS Omega ; 3(10): 12930-12935, 2018 Oct 31.
Artigo em Inglês | MEDLINE | ID: mdl-31458016

RESUMO

We present a theoretical study on the formation of graphene nanoribbons-via polymerization of coronene molecules-inside the inner cavity of boron nitride nanotubes. We examine the electronic property of the hybrid system, and we show that the boron nitride nanotube does not significantly alter the electronic properties of the encapsulated graphene nanoribbon. Motivated by previous experimental works, we examine graphene nanoribbons with two different widths and investigate probable scenarios for defect formation and/or twisting of the resulting graphene nanoribbons and their effect on the electronic properties of the hybrid system.

20.
Sci Rep ; 7(1): 15096, 2017 11 08.
Artigo em Inglês | MEDLINE | ID: mdl-29118413

RESUMO

We demonstrate the fabrication of individual nanopores in hexagonal boron nitride (h-BN) with atomically precise control of the pore shape and size. Previous methods of pore production in other 2D materials typically create pores with irregular geometry and imprecise diameters. In contrast, other studies have shown that with careful control of electron irradiation, defects in h-BN grow with pristine zig-zag edges at quantized triangular sizes, but they have failed to demonstrate production and control of isolated defects. In this work, we combine these techniques to yield a method in which we can create individual size-quantized triangular nanopores through an h-BN sheet. The pores are created using the electron beam of a conventional transmission electron microscope; which can strip away multiple layers of h-BN exposing single-layer regions, introduce single vacancies, and preferentially grow vacancies only in the single-layer region. We further demonstrate how the geometry of these pores can be altered beyond triangular by changing beam conditions. Precisely size- and geometry-tuned nanopores could find application in molecular sensing, DNA sequencing, water desalination, and molecular separation.

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