Visualizing nanoscale excitonic relaxation properties of disordered edges and grain boundaries in monolayer molybdenum disulfide

Bao, Wei; Borys, Nicholas J.; Ko, Changhyun; Suh, Joonki; Fan, Wen; Thron, Andrew M.; Zhang, Yingjie; Buyanin, Alexander; Zhang, Jie; Cabrini, Stefano; Ashby, Paul D.; Weber‐Bargioni, Alexander; Tongay, Sefaattin; Aloni, Shaul; Ogletree, D. Frank; Wu, Junqiao; Salmerón, Miquel; Schuck, P. James

doi:10.1038/ncomms8993

Cited by 226 publications

(319 citation statements)

References 34 publications

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“…The flakes are equilateral triangles, as it is a commonly synthesized shape. [40][41][42][43] In this case, carriers are confined in the two directions of space and we must numerically solve the coupled differential equations in two variables in order to find eigenvalues and eigenfunctions of the Hamiltonian. In the results that follow, Fig.…”

Section: B Mos2 Triangular Quantum Dotsmentioning

confidence: 99%

Edge states in dichalcogenide nanoribbons and triangular quantum dots

2016

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The electronic structure of monolayer MoS2 nanoribbons and quantum dots have been investigated by means of an effective k · p two-band model. Both systems with borders exhibit states spatially localized on the edges and with energies lying in the band gap. We show that the conduction and valence band curvatures determine the presence/absence of these states whose origin has been related to the marginal topological properties of the MoS2 single-valley Hamiltonian.

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Section: B Mos2 Triangular Quantum Dotsmentioning

confidence: 99%

Edge states in dichalcogenide nanoribbons and triangular quantum dots

2016

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“…This process is commonly referred to as chemical vapor deposition (CVD) or powder vaporization [11][12][13][14]. Due to its simplicity, CVD is extensively used by the TMD community to produce high quality, micron-sized single crystals [11][12][13][15][16][17][18][19]. Understanding the vaporization chemistry of solid transition metal precursors and vapor transport of volatilized precursors, particularly with respect to the influence of water vapor, is critical.…”

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confidence: 99%

The important role of water in growth of monolayer transition metal dichalcogenides

et al. 2017

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The important role of water in growth of monolayer transition metal dichalcogenides Interest in transition metal dichalcogenides (TMDs) has been renewed by the discovery of emergent properties when reduced to single, two-dimensional (2D) layers. The transition to direct band gap [1,2], emerging charge density waves [3,4], high mobility [5][6][7], and valley polarization [8][9][10] are some of the many exciting properties that have been reported in the TMD literature recently. A major bottleneck to this research is the lack of reproducible and large scale synthetic methods for high quality, consistent monolayer TMD samples. The dominant growth method is the vaporization and subsequent chalcogenization of solid metal oxides in the presence of gaseous chalcogen precursors. This process is commonly referred to as chemical vapor deposition (CVD) or powder vaporization [11][12][13][14]. Due to its simplicity, CVD is extensively used by the TMD community to produce high quality, micron-sized single crystals [11][12][13][15][16][17][18][19]. Understanding the vaporization chemistry of solid transition metal precursors and vapor transport of volatilized precursors, particularly with respect to the influence of water vapor, is critical. Humidity, i.e. water content of the reaction environment, is an important parameter in the gas phase synthesis of inorganic materials, and while it is typically thought of as a contaminant, water is also an effective transport agent [20][21][22][23]. In this communication, we describe the synthesis of luminescent monolayer TMD islands by introducing water vapor as a simple means of controlling the volatilization and transport of the metal oxide precursor. Our experiments demonstrate a direct correlation between gas phase water content and the morphology of the resulting films. In particular, explicit control of the in situ water vapor concentration allows us to switch between two modes of growth: one in an effectively dry environment, in which the transition metal oxide source is converted directly to TMD material through a solid state reaction with the chalcogen source, and another in which the transition metal oxide undergoes vapor transport followed by reaction with the chalcogen source. We show that a small amount of water enhances the volatilization, and hence vapor transport, of the oxides of tungsten and molybdenum at the elevated temperatures (500-800 °C) used in the conversion or growth of their TMD counterparts. We attribute this effect to the enhanced vaporization of WO 3 and MoO 3 in the presence of water, first demonstrated in the 1930s and Our results show a direct correlation between gas phase water content and the morphology of TMD films. In particular, we show that the presence of water enhances volatilization, and therefore the vapor transport of tungsten and molybdenum oxide. Surprisingly, we find that water not only plays an important role in volatilization but is also compatible with TMD growth. In fact, carefully controlled humidity can consistently produce high qual...

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“…2D TMD semiconductors are particularly interesting because they exhibit direct bandgaps in the visible range [13][14][15] , high charge-carrier mobility 16,17 , extraordinarily enhanced light-matter interactions [18][19][20][21] and potential applications in novel optoelectronic devices 22,23 . Individual atomic-scale defects in 2D TMDs are expected to modify charge transport 24 or introduce ferromagnetism 25 , whereas one-dimensional defects such as grain boundaries and edges may alter electronic 1 and optical properties 1,26 , and introduce magnetic 27 or catalytic 28,29 functionality. Here we report the direct observation of one-dimensional (1D) charge density waves (CDWs) intrinsic to the conducting MTBs of monolayer MoSe 2 .…”

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Charge density wave order in 1D mirror twin boundaries of single-layer MoSe2

et al. 2016

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We provide direct evidence for the existence of isolated, one-dimensional charge density waves at mirror twin boundaries (MTBs) of single-layer semiconducting MoSe 2 . Such MTBs have been previously observed by transmission electron microscopy and have been predicted to be metallic in MoSe 2 and MoS 2 1-7. Our low-temperature scanning tunnelling microscopy/spectroscopy measurements revealed a substantial bandgap of 100 meV opening at the Fermi energy in the otherwise metallic one-dimensional structures. We found a periodic modulation in the density of states along the MTB, with a wavelength of approximately three lattice constants. In addition to mapping the energy-dependent density of states, we determined the atomic structure and bonding of the MTB through simultaneous high-resolution non-contact atomic force microscopy. Density functional theory calculations based on the observed structure reproduced both the gap opening and the spatially resolved density of states.Properties of two-dimensional (2D) transition metal dichalcogenides (TMDs) are highly sensitive to the presence of defects, and a detailed understanding of their structure may lead to tailoring of material properties through 'defect engineering' . Intrinsic defects have been studied extensively in graphene [8][9][10][11][12] . Defects in 2D semiconductors have been explored to a lesser extent, but are expected to substantially modify material properties. 2D TMD semiconductors are particularly interesting because they exhibit direct bandgaps in the visible range [13][14][15] , high charge-carrier mobility 16,17 , extraordinarily enhanced light-matter interactions [18][19][20][21] and potential applications in novel optoelectronic devices 22,23 . Individual atomic-scale defects in 2D TMDs are expected to modify charge transport 24 or introduce ferromagnetism 25 , whereas one-dimensional defects such as grain boundaries and edges may alter electronic 1 and optical properties 1,26 , and introduce magnetic 27 or catalytic 28,29 functionality. Here we report the direct observation of one-dimensional (1D) charge density waves (CDWs) intrinsic to the conducting MTBs of monolayer MoSe 2 . A 1D CDW is a macroscopic quantum state, where atoms in a 1D metallic system relax and break translational symmetry to reduce total energy by opening a small bandgap at the Fermi energy (E F ) and modulating the charge density at the periodicity of the lattice distortion 30,31 . Although CDW order has been observed in 2D TMD metals such as NbSe 2 and TiSe 2 at low temperature 32,33 , CDWs have not previously been associated with 2D TMD semiconductors.Most studies of 1D CDWs have been performed on ensembles of CDWs in conducting polymers, quasi-one-dimensional metals or self-assembled atomic chains adsorbed on semiconducting surfaces, where inter-CDW coupling can significantly impact CDW properties [34][35][36][37][38] . The CDWs observed here are electronically isolated from one another, and have truly one-dimensional character, forming an atomically precise model system t...

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Visualizing nanoscale excitonic relaxation properties of disordered edges and grain boundaries in monolayer molybdenum disulfide

Cited by 226 publications

References 34 publications

Edge states in dichalcogenide nanoribbons and triangular quantum dots

Edge states in dichalcogenide nanoribbons and triangular quantum dots

The important role of water in growth of monolayer transition metal dichalcogenides

Charge density wave order in 1D mirror twin boundaries of single-layer MoSe2

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