Quantum Photon Sources in WSe₂ Monolayers Induced by Weakly Localized Strain Fields

Quantum emitters in semiconductor transition metal dichalcogenide (TMD) monolayers hold great promise for many quantum optics applications due to the intriguing properties afforded by the host materials. The creation of localized excitonic states in two-dimensional semiconductors is also fundamentally interesting. Local strain engineering of TMD monolayers has been attested to be a viable approach for creating quantum emitters. However, despite the ubiquitous existence of local topography variations in the structures used to create strain gradients in the TMD monolayers, an understanding of their influence on the strain fields and exciton trapping is notably lacking, especially on the nanoscale. In this study, we investigate WSe2 monolayers deposited on the edges of as-fabricated trenches, which are deemed to induce 1D delocalized strain profiles in the monolayers, and observe optical signatures of weakly confined excitonic states supporting biexciton emission. Our numerical simulations of the strain distributions suggest that the quantum emitters originate from quasi-1D like localized strain profiles induced by local topography variations at the trench edges. These findings have strong implications toward the controlled creation of quantum emitters in TMD monolayers and their efficient coupling to photonic structures

Metal-Lined Semiconductor Nanotubes for Surface Plasmon-Mediated Luminescence Enhancement

Highly efficient solid-state light-emitting devices require semiconductor architectures equipped with high quantum efficiency and integratability on conductive substrates. Surface plasmon (SP)-mediated luminescence enhancement has been considered as one of the most promising solutions, because SP resonance can greatly improve the radiative recombination rate and be achieved using metal entities compatible with the electrode fabrication process. Nevertheless, metal/semiconductor heterostructures have had several fabrication-compatible issues due to metal as a potential contaminant of the semiconductor. We present here a simple fabrication scheme for a metal-lined semiconductor nanotube heterostructure, in which a metal layer is selectively formed on the inner wall of the semiconductor nanotube. The Ag-lining process in a ZnO nanotube resulted in 7.5-fold enhancement of the photoluminescence intensity at 11 K. This SP fabrication technique looks promising for highly efficient solid-state lighting based on semiconductor nanostructures without detrimental effects

Anisotropic Cracking of Nanocrystal Superlattices

The synthesis colloidal nanocrystals in nonpolar organic solvents has led to exceptional size- and shape-control, enabling the formation of nanocrystal superlattices isostructural to atomic lattices built with nanocrystals rather than atoms. The long aliphatic ligands (e.g., oleic acid) used to achieve this control separate nanocrystals too far in the solid state for most charge-transporting devices. Solid-state ligand exchange, which brings particles closer together and enhances conductivity, necessitates large changes in the total volume of the solid (compressive stress), which leads to film cracking. In this work, truncate octahedral lead selenide nanocrystals are shown to self-assemble into body-centered cubic superlattices in which the atomic axes of the individual nanocrystals are coaligned with the crystal axes of the superlattice. Due to this coalignment, upon ligand exchange of the superlattices, cracking is preferentially observed on ⟨011⟩ superlattice directions. This observation is related to differences in the ligand binding to exposed {100} and {111} planes of the PbSe nanocrystal surfaces. This result has implications for binary and more complex structures in which differential reactivity of the constituent elements can lead to disruption of the desired structure. In addition, cracks in PbSe superlattices occur in a semiregular spacings inversely related to the superlattice domain size and strongly influenced by the presence of twin boundaries, which serve as both emission centers and propagation barriers for fractures. This work shows that defects, similar to behavior in nanotwinned metals, could be used to engineer enhanced mechanical strength and electrical conductivity in nanocrystal superlattices

Influence of Exciton Dimensionality on Spectral Diffusion of Single-Walled Carbon Nanotubes

We study temporal evolution of photoluminescence (PL) spectra from individual single-walled carbon nanotubes (SWCNTs) at cryogenic and room temperatures. Sublinear and superlinear correlations between fluctuating PL spectral positions and line widths are observed at cryogenic and room temperatures, respectively. We develop a simple model to explain these two different spectral diffusion behaviors in the framework of quantum-confined Stark effect (QCSE) caused by surface charges trapped in the vicinity of SWCNTs. We show that the wave function properties of excitons, namely, localization at cryogenic temperature and delocalization at room temperature, play a critical role in defining sub- and superlinear correlations. Room temperature PL spectral positions and line widths of SWCNTs coupled to gold dimer nanoantennas on the other hand exhibit sublinear correlations, indicating that excitonic emission mainly originates from nanometer range regions and excitons appear to be localized. Our numerical simulations show that such apparent localization of excitons results from plasmonic confinement of excitation and an enhancement of decay rates in the gap of the dimer nanoantennas

Electronic Structure and Chemical Nature of Oxygen Dopant States in Carbon Nanotubes

We performed low temperature photoluminescence (PL) studies on individual oxygen-doped single-walled carbon nanotubes (SWCNTs) and correlated our observations to electronic structure simulations. Our experiment reveals multiple sharp asymmetric emission peaks at energies 50–300 meV red-shifted from that of the <i>E</i>₁₁ bright exciton peak. Our simulation suggests an association of these peaks with deep trap states tied to different specific chemical adducts. In addition, oxygen doping is also observed to split the <i>E</i>₁₁ exciton into two or more states with an energy splitting <40 meV. We attribute these states to dark states that are brightened through defect-induced symmetry breaking. While the wave functions of these brightened states are delocalized, those of the deep-trap states are strongly localized and pinned to the dopants. These findings are consistent with our experimental observation of asymmetric broadening of the deep trap emission peaks, which can result from interaction between pinned excitons and one-dimensional phonons. Exciton pinning also increases the sensitivity of the deep traps to the local dielectric environment, leading to a large inhomogeneous broadening. Observations of multiple spectral features on single nanotubes indicate the possibility of different chemical adducts coexisting on a given nanotube

Anisotropic Photoluminescence from Isotropic Optical Transition Dipoles in Semiconductor Nanoplatelets

Many important light-matter coupling and energy-transfer processes depend critically on the dimensionality and orientation of optical transition dipoles in emitters. We investigate individual quasi-two-dimensional nanoplatelets (NPLs) using higher-order laser scanning microscopy and find that absorption dipoles in NPLs are isotropic in three dimensions at the excitation wavelength. Correlated polarization studies of the NPLs reveal that their emission polarization is strongly dependent on the aspect ratio of the lateral dimensions. Our simulations reveal that this emission anisotropy can be readily explained by the electric field renormalization effect caused by the dielectric contrast between the NPLs and the surrounding medium, and we conclude that emission dipoles in NPLs are isotropic in the plane of the NPLs. Our study presents an approach for disentangling the effects of dipole degeneracy and electric field renormalization on emission anisotropy and can be adapted for studying the intrinsic optical transition dipoles of various nanostructures

Photoluminescence Dynamics of Aryl sp³ Defect States in Single-Walled Carbon Nanotubes

Photoluminescent defect states introduced by sp³ functionalization of semiconducting carbon nanotubes are rapidly emerging as important routes for boosting emission quantum yields and introducing new functionality. Knowledge of the relaxation dynamics of these states is required for understanding how functionalizing agents (molecular dopants) may be designed to access specific behaviors. We measure photoluminescence (PL) decay dynamics of sp³ defect states introduced by aryl functionalization of the carbon nanotube surface. Results are given for five different nanotube chiralities, each doped with a range of aryl functionality. We find that the PL decays of these sp³ defect states are biexponential, with both components relaxing on time scales of ∼100 ps. Exciton trapping at defects is found to increases PL lifetimes by a factor of 5–10, in comparison to those for the free exciton. A significant chirality dependence is observed in the decay times, ranging from 77 ps for (7,5) nanotubes to >600 ps for (5,4) structures. The strong correlation of time constants with emission energy indicates relaxation occurs <i>via</i> multiphonon decay processes, with close agreement to theoretical expectations. Variation of the aryl dopant further modulates decay times by 10–15%. The aryl defects also affect PL lifetimes of the free <i>E</i>₁₁ exciton. Shortening of the <i>E</i>₁₁ bright state lifetime as defect density increases provides further confirmation that defects act as exciton traps. A similar shortening of the <i>E</i>₁₁ dark exciton lifetime is found as defect density increases, providing strong experimental evidence that dark excitons are also trapped at such defect sites

Thermal Hysteresis and Ordering Behavior of Magnetic Skyrmion Lattices

The physics of phase transitions in two-dimensional (2D) systems underpins research in diverse fields including statistical mechanics, nanomagnetism, and soft condensed matter. However, many aspects of 2D phase transitions are still not well understood, including the effects of interparticle potential, polydispersity, and particle shape. Magnetic skyrmions are chiral spin-structure quasi-particles that form two-dimensional lattices. Here, we show, by real-space imaging using in situ cryo-Lorentz transmission electron microscopy coupled with machine learning image analysis, the ordering behavior of Néel skyrmion lattices in van der Waals Fe3GeTe2. We demonstrate a distinct change in the skyrmion size distribution during field-cooling, which leads to a loss of lattice order and an evolution of the skyrmion liquid phase. Remarkably, the lattice order is restored during field heating and demonstrates a thermal hysteresis. This behavior is explained by the skyrmion energy landscape and demonstrates the potential to control the lattice order in 2D phase transitions

Thermal Hysteresis and Ordering Behavior of Magnetic Skyrmion Lattices

The physics of phase transitions in two-dimensional (2D) systems underpins research in diverse fields including statistical mechanics, nanomagnetism, and soft condensed matter. However, many aspects of 2D phase transitions are still not well understood, including the effects of interparticle potential, polydispersity, and particle shape. Magnetic skyrmions are chiral spin-structure quasi-particles that form two-dimensional lattices. Here, we show, by real-space imaging using in situ cryo-Lorentz transmission electron microscopy coupled with machine learning image analysis, the ordering behavior of Néel skyrmion lattices in van der Waals Fe3GeTe2. We demonstrate a distinct change in the skyrmion size distribution during field-cooling, which leads to a loss of lattice order and an evolution of the skyrmion liquid phase. Remarkably, the lattice order is restored during field heating and demonstrates a thermal hysteresis. This behavior is explained by the skyrmion energy landscape and demonstrates the potential to control the lattice order in 2D phase transitions

Thermal Hysteresis and Ordering Behavior of Magnetic Skyrmion Lattices

The physics of phase transitions in two-dimensional (2D) systems underpins research in diverse fields including statistical mechanics, nanomagnetism, and soft condensed matter. However, many aspects of 2D phase transitions are still not well understood, including the effects of interparticle potential, polydispersity, and particle shape. Magnetic skyrmions are chiral spin-structure quasi-particles that form two-dimensional lattices. Here, we show, by real-space imaging using in situ cryo-Lorentz transmission electron microscopy coupled with machine learning image analysis, the ordering behavior of Néel skyrmion lattices in van der Waals Fe3GeTe2. We demonstrate a distinct change in the skyrmion size distribution during field-cooling, which leads to a loss of lattice order and an evolution of the skyrmion liquid phase. Remarkably, the lattice order is restored during field heating and demonstrates a thermal hysteresis. This behavior is explained by the skyrmion energy landscape and demonstrates the potential to control the lattice order in 2D phase transitions