Fermi-Level Pinning in ErAs Nanoparticles Embedded in III-V Semiconductors.

Embedding rare-earth monopnictide nanoparticles into III-V semiconductors enables unique optical, electrical, and thermal properties for THz photoconductive switches, tunnel junctions, and thermoelectric devices. Despite the high structural quality and control over growth, particle size (<3 nm), and density, the underlying electronic structure of these nanocomposite materials has only been hypothesized. Structural and electronic properties of ErAs nanoparticles with different shapes and sizes (cubic to spherical, 1.14, 1.71, and 2.28 nm) in AlAs, GaAs, InAs, and their alloys are investigated using first-principles calculations, revealing that spherical nanoparticles have lower formation energies. For the lowest-energy nanoparticles, the Fermi level is pinned near midgap in GaAs and AlAs but resonant in the conduction band in InAs. The Fermi level is shifted down as the particle size increases and is pinned on an absolute energy scale considering the band alignment at AlAs/GaAs/InAs interfaces, offering insights into the rational design of these nanomaterials.

Emerging Nontrivial Topology in Ultrathin Films of Rare-Earth Pnictides.

Thin films of rare-earth monopnictide (RE-V) semimetals are expected to turn into semiconductors due to quantum confinement effects (QCE), lifting the overlap between electron pockets at Brillouin zone edges (X) and hole pockets at the zone center (Γ). Instead, using LaSb as an example, we find the emergence of the quantum spin Hall (QSH) insulator phase in (001)-oriented films as the thickness is reduced to 7, 5, or 3 monolayers (MLs). This is attributed to a strong QCE on the in-plane electron pockets and the lack of quantum confinement on the out-of-plane pocket projected onto the zone center, resulting in a band inversion. Spin-orbit coupling (SOC) opens a sizable nontrivial gap in the band structure of ultrathin films. Such effect is anticipated to be general in rare-earth monopnictides and may lead to interesting phenomena when coupled with the 4f magnetic moments present in other members of this family of materials.

Evaluating Glyph Design for Showing Large-Magnitude-Range Quantum Spins.

We present experimental results to explore a form of bivariate glyphs for representing large-magnitude-range vectors. The glyphs meet two conditions: (1) two visual dimensions are separable; and (2) one of the two visual dimensions uses a categorical representation (e.g., a categorical colormap). We evaluate how much these two conditions determine the bivariate glyphs' effectiveness. The first experiment asks participants to perform three local tasks requiring reading no more than two glyphs. The second experiment scales up the search space in global tasks when participants must look at the entire scene of hundreds of vector glyphs to get an answer. Our results support that the first condition is necessary for local tasks when a few items are compared. But it is not enough for understanding a large amount of data. The second condition is necessary for perceiving global structures of examining very complex datasets. Participants' comments reveal that the categorical features in the bivariate glyphs trigger emergent optimal viewers' behaviors. This work contributes to perceptually accurate glyph representations for revealing patterns from large scientific results. We release source code, quantum physics data, training documents, participants' answers, and statistical analyses for reproducible science at https : //osf:io/4xcf5/?viewonly = 94123139df9c4ac984a1e0df811cd580.

From single-particle-like to interaction-mediated plasmonic resonances in graphene nanoantennas.

Plasmonic nanostructures attract tremendous attention as they confine electromagnetic fields well below the diffraction limit while simultaneously sustaining extreme local field enhancements. To fully exploit these properties, the identification and classification of resonances in such nanostructures is crucial. Recently, a novel figure of merit for resonance classification has been proposed1 and its applicability was demonstrated mostly to toy model systems. This novel measure, the energy-based plasmonicity index (EPI), characterizes the nature of resonances in molecular nanostructures. The EPI distinguishes between either a single-particle-like or a plasmonic nature of resonances based on the energy space coherence dynamics of the excitation. To advance the further development of this newly established measure, we present here its exemplary application to characterize the resonances of graphene nanoantennas. In particular, we focus on resonances in a doped nanoantenna. The structure is of interest, as a consideration of the electron dynamics in real space might suggest a plasmonic nature of selected resonances in the low doping limit but our analysis reveals the opposite. We find that in the undoped and moderately doped nanoantenna, the EPI classifies all emerging resonances as predominantly single-particle-like and only after doping the structure heavily, the EPI observes plasmonic response.

Controlling the layer localization of gapless states in bilayer graphene with a gate voltage.

Experiments in gated bilayer graphene with stacking domain walls present topological gapless states protected by no-valley mixing. Here we research these states under gate voltages using atomistic models, which allow us to elucidate their origin. We find that the gate potential controls the layer localization of the two states, which switches non-trivially between layers depending on the applied gate voltage magnitude. We also show how these bilayer gapless states arise from bands of single-layer graphene by analyzing the formation of carbon bonds between layers. Based on this analysis we provide a model Hamiltonian with analytical solutions, which explains the layer localization as a function of the ratio between the applied potential and interlayer hopping. Our results open a route for the manipulation of gapless states in electronic devices, analogous to the proposed writing and reading memories in topological insulators.

Validation of SplitVectors Encoding for Quantitative Visualization of Large-Magnitude-Range Vector Fields.

We designed and evaluated SplitVectors, a new vector field display approach to help scientists perform new discrimination tasks on large-magnitude-range scientific data shown in three-dimensional (3D) visualization environments. SplitVectors uses scientific notation to display vector magnitude, thus improving legibility. We present an empirical study comparing the SplitVectors approach with three other approaches - direct linear representation, logarithmic, and text display commonly used in scientific visualizations. Twenty participants performed three domain analysis tasks: reading numerical values (a discrimination task), finding the ratio between values (a discrimination task), and finding the larger of two vectors (a pattern detection task). Participants used both mono and stereo conditions. Our results suggest the following: (1) SplitVectors improve accuracy by about 10 times compared to linear mapping and by four times to logarithmic in discrimination tasks; (2) SplitVectors have no significant differences from the textual display approach, but reduce cluttering in the scene; (3) SplitVectors and textual display are less sensitive to data scale than linear and logarithmic approaches; (4) using logarithmic can be problematic as participants' confidence was as high as directly reading from the textual display, but their accuracy was poor; and (5) Stereoscopy improved performance, especially in more challenging discrimination tasks.

Approaching the quantum limit for plasmonics: linear atomic chains.

Optical excitations in atomic-scale materials can be strongly mixed, with contributions from both single-particle transitions and collective response. This complicates the quantum description of these excitations, because there is no clear way to define their quantization. To develop a quantum theory for these optical excitations, they must first be characterized so that single-particle-like and collective excitations can be identified. Linear atomic chains, such as atom chains on surfaces, linear arrays of dopant atoms in semiconductors, or linear molecules, provide ideal testbeds for studying collective excitations in small atomic-scale systems. We use exact diagonalization to study the many-body excitations of finite (10 to 25) linear atomic chains described by a simplified model Hamiltonian. Exact diagonalization results can be very different from the density functional theory (DFT) results usually obtained. Highly correlated, multiexcitonic states, strongly dependent on the electron-electron interaction strength, dominate the exact spectral and optical response but are not present in DFT excitation spectra. The ubiquitous presence of excitonic many-body states in the spectra makes it hard to identify plasmonic excitations. A combination of criteria involving a many-body state's transfer dipole moment, balance, transfer charge, dynamical response, and induced-charge distribution do strongly suggest which many-body states should be considered as plasmonic. This analysis can be used to reveal the few plasmonic many-body states hidden in the dense spectrum of low-energy single-particle-like states and many higher-energy excitonic-like states. These excitonic states are the predominant excitation because of the many possible ways to develop local correlations.

Hole spins in an InAs/GaAs quantum dot molecule subject to lateral electric fields.

There has been tremendous progress in manipulating electron and hole-spin states in quantum dots or quantum dot molecules (QDMs) with growth-direction (vertical) electric fields and optical excitations. However, the response of carriers in QDMs to an in-plane (lateral) electric field remains largely unexplored. We computationally explore spin-mixing interactions in the molecular states of single holes confined in vertically stacked InAs/GaAs QDMs using atomistic tight-binding simulations. We systematically investigate QDMs with different geometric structure parameters and local piezoelectric fields. We observe both a relatively large Stark shift and a change in the Zeeman splitting as the magnitude of the lateral electric field increases. Most importantly, we observe that lateral electric fields induce hole-spin mixing with a magnitude that increases with increasing lateral electric field over a moderate range. These results suggest that applied lateral electric fields could be used to fine tune and manipulate, in situ, the energy levels and spin properties of single holes confined in QDMs.

Exciton-plasmon interactions in quantum dot-gold nanoparticle structures.

We present a self-assembly method to construct CdSe/ZnS quantum dot-gold nanoparticle complexes. This method allows us to form complexes with relatively good control of the composition and structure that can be used for detailed study of the exciton-plasmon interactions. We determine the contribution of the polarization-dependent near-field enhancement, which may enhance the absorption by nearly two orders of magnitude and that of the exciton coupling to plasmon modes, which modifies the exciton decay rate.

Superresolution four-wave mixing microscopy.

We report on the development of a superresolution four-wave mixing microscope with spatial resolution approaching 130 nm which represents better than twice the diffraction limit at 800 nm while retaining the ability to acquire materials- and chemical- specific contrast. The resolution enhancement is achieved by narrowing the microscope's excitation volume in the focal plane through the combined use of a Toraldo-style pupil phase filter with the multiplicative nature of four-wave mixing.

Plasmonic properties of metallic nanoparticles: the effects of size quantization.

We examine the size quantization of plasmons in metallic nanoparticles using time-dependent density functional theory. For small particles in the quantum limit, we identify "quantum core plasmons" and "classical surface plasmons", both of which are collective oscillations comprised of multiple single-particle transitions. As particle size increases, the response of the classical surface plasmons becomes much larger than that of the quantum core plasmons.

Coherent stokes scattering from gold nanorods: critical dimensions and multicolor near-resonant plasmon excitation.

In this study, we detail the coherent Stokes scattering from gold nanorods in ensemble and single particle measurements. An increase of more than an order of magnitude was observed in the surface plasmon resonance enhancement of coherent Stokes scattering by gold nanorods for small changes in nanorod dimensions. The impact of this dimensional change is, in general, smaller when probed by single color linear and non-linear techniques. We find that the size sensitivity and associated wavelength dependence of the enhanced coherent Stokes scattering from individual gold nanorods is consistent with predictions based on local surface plasmon resonances found from exact solutions obtained using boundary element methods.

Comparison of the sensitivity and image contrast in spontaneous Raman and coherent Stokes Raman scattering microscopy of geometry-controlled samples.

We experimentally compare the performance and image contrast of spontaneous Raman and coherent Stokes Raman scattering microscopy. We demonstrate the differences between these techniques on a series of geometry-controlled samples that range in complexity from a point (array of tips) to one-dimensional (line grating) and, lastly, two-dimensional (checkereboard) microstructure. Through the use of this sample series, a comparison of the focal volume, achievable signal-to-noise, and resulting image contrast is made. The results demonstrate the efficiency and spatial resolution attainable in coherent Raman microscopy relative to spontaneous Raman microscopy. Additionally, we detail potential complications in the interpretation of coherent Raman images of sample fine structure, where contrast is no longer based solely on oscillator concentration but can be influenced by sample microstructure.

Effect of mechanical strain on the optical properties of quantum dots: controlling exciton shape, orientation, and phase with a mechanical strain.

We show how a nanomechanical strain can be used to dynamically reengineer the optics of quantum dots, giving a tool to manipulate mechanoexciton shape, orientation, fine structure splitting, and optical transitions, transfer carriers between dots, and interact qubits for quantum processing. Most importantly, a nanomechanical strain reengineers both the magnitude and phase of the exciton exchange coupling to tune exchange splittings, change the phase of spin mixing, and rotate the polarization of mechanoexcitons, providing phase and energy control of excitons.

Discrete dipole approximation for the study of radiation dynamics in a magnetodielectric environment.

We develop a general computational approach, based on the discrete dipole approximation, for the study of radiation dynamics near or inside an object with arbitrary linear dielectric permittivity, and magnetic permeability tensors. Our method can account for dispersion and losses and provides insight on the role of local-field corrections in discrete magnetodielectric structures. We illustrate our method in the case of a source inside a magneto-dielectric, isotropic sphere for which the spontaneous emission rate of a source can be computed analytically. We show that our approach is in excellent agreement with the exact result, providing an approach capable of handling both the electric and magnetic response of advanced metamaterials.

Effects of inhomogeneous fields in superresolving structured-illumination microscopy.

The increased resolution attained by structured illumination is based on the degree to which high spatial frequencies can be down converted into the passband of the imaging system. To effectively do this, a high contrast high-frequency illumination pattern is required. We show how the use of high numerical aperture (1.42 NA and 1.65 NA) microscope objectives in structured-illumination microscopy can provide relatively high-frequency illumination patterns. However, a consequence of this is that the resulting illumination pattern can become evanescently decaying and thus becomes inhomogeneous within a microscopically extended sample medium. We demonstrate how these inhomogeneous fields impact the superresolved imaging of the microscope and how these adverse effects can be avoided.

Optical response of strongly coupled quantum dot-metal nanoparticle systems: double peaked Fano structure and bistability.

In this communication, we study the optical response of a semiconductor quantum dot (SQD) coupled with a metal nanoparticle (MNP). In particular, we explore the relationship between the size of the constituents and the response of the system. We identify, here, three distinct regimes of behavior in the strong field limit that each exhibit novel properties. In the first regime, we find that the energy absorption spectrum displays an asymmetrical Fano shape (as previously predicted). It occurs when there is interference between the applied field and the induced field produced by the SQD at the MNP. When the coupling is increased by increasing the size of the SQD, we find a double peaked Fano structure in the response. This second peak occurs when the induced field becomes stronger than the external field. As the coupling is further increased by increasing the sizes of both the SQD and the MNP, we find a regime of bistability. This originates when the self-interaction of the SQD becomes significant. We explore these three regimes in detail and set bounds on each.

Mapping the plasmon resonances of metallic nanoantennas.

We study the light scattering and surface plasmon resonances of Au nanorods that are commonly used as optical nanoantennas in analogy to dipole radio antennas for chemical and biodetection field-enhanced spectroscopies and scanned-probe microscopies. With the use of the boundary element method, we calculate the nanorod near-field and far-field response to show how the nanorod shape and dimensions determine its optical response. A full mapping of the size (length and radius) dependence for Au nanorods is obtained. The dipolar plasmon resonance wavelength lambda shows a nearly linear dependence on total rod length L out to the largest lengths that we study. However, L is always substantially less than lambda/2, indicating the difference between optical nanoantennas and long-wavelength traditional lambda/2 antennas. Although it is often assumed that the plasmon wavelength scales with the nanorod aspect ratio, we find that this scaling does not apply except in the extreme limit of very small, spherical nanoparticles. The plasmon response depends critically on both the rod length and radius. Large (500 nm) differences in resonance wavelength are found for structures with different sizes but with the same aspect ratio. In addition, the plasmon resonance deduced from the near-field enhancement can be significantly red-shifted due to retardation from the resonance in far-field scattering. Large differences in near-field and far-field response, together with the breakdown of the simple scaling law must be accounted for in the choice and design of metallic lambda/2 nanoantennas. We provide a general, practical map of the resonances for use in locating the desired response for gold nanoantennas.

Accelerating Scientific Discovery Through Computation and Visualization III. Tight-Binding Wave Functions for Quantum Dots.

This is the third in a series of articles that describe, through examples, how the Scientific Applications and Visualization Group (SAVG) at NIST has utilized high performance parallel computing, visualization, and machine learning to accelerate scientific discovery. In this article we focus on the use of high performance computing and visualization for simulations of nanotechnology.

Semiconductor-metal nanoparticle molecules: hybrid excitons and the nonlinear fano effect.

Modern nanotechnology opens the possibility of combining nanocrystals of various materials with very different characteristics in one superstructure. Here we study theoretically the optical properties of hybrid molecules composed of semiconductor and metal nanoparticles. Excitons and plasmons in such a hybrid molecule become strongly coupled and demonstrate novel properties. At low incident light intensity, the exciton peak in the absorption spectrum is broadened and shifted due to incoherent and coherent interactions between metal and semiconductor nanoparticles. At high light intensity, the absorption spectrum demonstrates a surprising, strongly asymmetric shape. This shape originates from the coherent internanoparticle Coulomb interaction and can be viewed as a nonlinear Fano effect which is quite different from the usual linear Fano resonance.