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Domain boundaries in ferroelectric materials exhibit rich and diverse physical properties distinct from their parent materials and have been proposed for novel applications in nanoelectronics and quantum information technology. Due to their complexity and diversity, the internal atomic and electronic structure of domain boundaries that governs the electronic properties as well as the kinetics of domain switching remains far from being elucidated. By using scanning tunneling microscopy and spectroscopy (STM/S) combined with density functional theory (DFT) calculations, we directly visualize the atomic structure of domain boundaries in two-dimensional (2D) ferroelectric beta' In2Se3 down to the monolayer limit and reveal a double-barrier energy potential of the 60{\deg} tail to tail domain boundaries for the first time. We further controllably manipulate the domain boundaries with atomic precision by STM and show that the movements of domain boundaries can be driven by the electric field from an STM tip and proceed by the collective shifting of atoms at the domain boundaries. The results will deepen our understanding of domain boundaries in 2D ferroelectric materials and stimulate innovative applications of these materials., Comment: 26 pages (not including SI), 4 figures

Traditionally, phase transitions are explored using a combination of macroscopic functional characterization and scattering techniques, providing insight into average properties and symmetries of the lattice but local atomic level mechanisms during phase transitions generally remain unknown. Here we explore the mechanisms of a phase transition between the trigonal prismatic and distorted octahedral phases of layered chalogenides in the MoS2 ReS2 system from the observations of local degrees of freedom, namely atomic positions by Scanning Transmission Electron Microscopy (STEM). We employ local crystallographic analysis based on machine learning of atomic environments to build a picture of the transition from the atomic level up and determine local and global variables controlling the local symmetry breaking. In particular, we argue that the dependence of the average symmetry breaking distortion amplitude on global and local concentration can be used to separate local chemical and global electronic effects on transition. This approach allows exploring atomic mechanisms beyond the traditional macroscopic descriptions, utilizing the imaging of compositional fluctuations in solids to explore phase transitions over a range of realized and observed local stoichiometries and atomic configurations., Comment: 5 figures, 20 pages including supplementary

Exploration of structure-property relationships as a function of dopant concentration is commonly based on mean field theories for solid solutions. However, such theories that work well for semiconductors tend to fail in materials with strong correlations, either in electronic behavior or chemical segregation. In these cases, the details of atomic arrangements are generally not explored and analyzed. The knowledge of the generative physics and chemistry of the material can obviate this problem, since defect configuration libraries as stochastic representation of atomic level structures can be generated, or parameters of mesoscopic thermodynamic models can be derived. To obtain such information for improved predictions, we use data from atomically resolved microscopic images that visualize complex structural correlations within the system and translate them into statistical mechanical models of structure formation. Given the significant uncertainties about the microscopic aspects of the material's processing history along with the limited number of available images, we combine model optimization techniques with the principles of statistical hypothesis testing. We demonstrate the approach on data from a series of atomically-resolved scanning transmission electron microscopy images of Mo$_x$Re$_{1-x}$S$_2$ at varying ratios of Mo/Re stoichiometries, for which we propose an effective interaction model that is then used to generate atomic configurations and make testable predictions at a range of concentrations and formation temperatures., Comment: 26 pages, 8 figures

The exceptional electronic, optical and chemical properties of two-dimensional materials strongly depend on the 3D atomic structure and crystal defects. Using Re-doped MoS2 as a model, here we develop scanning atomic electron tomography (sAET) to determine the 3D atomic positions and crystal defects such as dopants, vacancies and ripples with a precision down to 4 picometers. We measure the 3D bond distortion and local strain tensor induced by single dopants for the first time. By directly providing experimental 3D atomic coordinates to density functional theory (DFT), we obtain more truthful electronic band structures than those derived from conventional DFT calculations relying on relaxed 3D atomic models, which is confirmed by photoluminescence measurements. We anticipate that sAET is not only generally applicable to the determination of the 3D atomic coordinates of 2D materials, heterostructures and thin films, but also could transform ab initio calculations by using experimental 3D atomic coordinates as direct input to better predict and discover new physical, chemical and electronic properties., Comment: 44 pages, 18 figures

Charged excitons called trions play an important role in the fundamental valley dynamics in the newly emerging 2D semiconductor materials. We used ultrafast pump- probe spectroscopy to study the valley trion dynamics in a MoSe$_2$ monolayer grown by using chemical vapor deposition. The dynamics display an ultrafast trion formation followed by a non-exponential decay. The measurements at different pump fluences show that the trion decay dynamics become slower as the excitation density increases. The observed trion dynamics and the associated density dependence are a result of the trapping by two defect states as being the dominating decay mechanism. The simulation based on a set of rate equations reproduces the experimental data for different pump fluences. Our results reveal the important trion dynamics and identify the trapping by defect states as the primary trion decay mechanism in monolayer MoSe$_2$ under the excitation densities used in our experiment., Comment: 16 pages, 4 figures

Molybdenum disulfide (MoS2) monolayers have attracted much attention for their novel optical properties and efficient light-matter interactions. When excited by incident laser, the optical response of MoS2 monolayers was effectively modified by elementary photo-excited excitons owing to their large exciton binding energy, which can be facilitated for the optical-controllable exciton-plasmon interactions. Inspired by this concept, we experimentally investigated active light control of surface plasmon resonance (SPR) in MoS2-Ag hybrid nanostructures. The white light spectra of SPR were gradually red-shifted by increasing laser power, which was distinctly different from the one of bare Ag nanostructure. This spectroscopic tunability can be further controlled by near-field coupling strength and polarization state of light, and selectively applied to the control of plasmonic dark mode. An analytical Lorentz model for photo-excited excitons induced modulation of MoS2 dielectric function was developed to explain the insight physics of this SPR tunability. Our study opens new possibilities to the development of all-optical controlled nanophotonic devices based on 2D materials., Comment: 27 pages, 6 figures

Phosphorene, an elemental 2D material, which is the monolayer of black phosphorus, has been mechanically exfoliated recently. In its bulk form, black phosphorus shows high carrier mobility (~10000 cm2/Vs) and a ~0.3 eV direct bandgap. Well-behaved p-type field-effect transistors with mobilities of up to 1000 cm2/Vs, as well as phototransistors, have been demonstrated on few-layer black phosphorus, showing its promise for electronics and optoelectronics applications due to its high hole mobility and thickness-dependence direct bandgap. However, p-n junctions, the basic building blocks of modern electronic and optoelectronic devices, have not yet been realized based on black phosphorus. In this paper, we demonstrate a gate tunable p-n diode based on a p-type black phosphorus/n-type monolayer MoS2 van der Waals p-n heterojunction. Upon illumination, these ultra-thin p-n diodes show a maximum photodetection responsivity of 418 mA/W at the wavelength of 633 nm, and photovoltaic energy conversion with an external quantum efficiency of 0.3%. These p-n diodes show promise for broadband photodetection and solar energy harvesting., Comment: 37 pages