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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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12 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Pair distribution function analysis of nano-object assemblies

The atomic pair distribution function (aPDF) analysis technique, also known as the total scattering method, which considers both Bragg and diffuse scattering, has been used extensively to probe local atomic arrangements in crystalline and disordered materials. In contrast, there have been limited applications of the PDF in self-assembled nanomaterials, which represent a class of materials built from nanoscale objects, such as nano-colloids, micelles and proteins. As distinguished from atoms, nano-objects have polydispersity in size and shape, and such form-factor effects complicate the application of PDF analysis to nano-systems. Here, in this paper, the application of the PDF is extended to spherical nano-object assemblies and the formulae for the nano-PDF (nPDF) are derived, showing some differences from the aPDF. By numerical simulations, the properties of the nPDF (peak broadening and pattern profile) are studied systematically as a function of structural features, such as nano-object parameters (size and size polydispersity) and assembly structural features (size, shape, structure type and lattice disorder), and of data processing parameters ( q cut-off and `missing' data in ultra-small-angle regions). The nPDF analysis method is found to provide an effective route to revealing not only nanoscale but also mesoscale structural properties, for example the morphology of a nano-assembly.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

Chapter 4.2 - Preparation of nanoparticles for surface analysis

A variety of methods used to prepare nano-objects for surface analysis are described along with information about when they might be best applied. Intrinsic properties of NPs that complicate their characterization and need to be considered when planning for surface or other analyses of NPs are identified, including challenges associated with reproducible synthesis and functionalization of the particles as well as their dynamic nature. Information about the sample preparation processes, along with analysis data, that need to be added to the collection of material provenance information is identified and examples of protocols that have been successfully used for preparation of nano-objects for surface analysis are included in an annex.

characterization challenges↗
DOE OSTI2023

Enhancing Nanoparticle Detection in Interferometric Scattering (iSCAT) Microscopy Using a Mask R-CNN

Interferometric scattering microscopy (iSCAT) is a label-free optical microscopy technique that enables imaging of individual nano-objects such as nanoparticles, viruses, and proteins. Essential to this technique is the suppression of background scattering and identification of signals from nano-objects. In the presence of substrates with high roughness, scattering heterogeneities in the background, when coupled with tiny stage movements, cause features in the background to be manifested in background-suppressed iSCAT images. Traditional computer vision algorithms detect these background features as particles, limiting the accuracy of object detection in iSCAT experiments. Here, in this paper, we present a pathway to improve particle detection in such situations using supervised machine learning via a mask region-based convolutional neural network (mask R-CNN). Using a model iSCAT experiment of 19.2 nm gold nanoparticles adsorbing to a rough layer-by-layer polyelectrolyte film, we develop a method to generate labeled datasets using experimental background images and simulated particle signals and train the mask R-CNN using limited computational resources via transfer learning. We then compare the performance of the mask R-CNN trained with and without inclusion of experimental backgrounds in the dataset against that of a traditional computer vision object detection algorithm, Haar-like feature detection, by analyzing data from the model experiment. Results demonstrate that including representative backgrounds in training datasets improved the mask R-CNN in differentiating between background and particle signals and elevated performance by markedly reducing false positives. The methodology for creating a labeled dataset with representative experimental backgrounds and simulated signals facilitates the application of machine learning in iSCAT experiments with strong background scattering and thus provides a useful workflow for future researchers to improve their image processing capabilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Phonon-Assisted Intertube Electronic Transport in an Armchair Carbon Nanotube Film

The electrical conductivity of a macroscopic assembly of nanomaterials is determined through a complex interplay of electronic transport within and between constituent nano-objects. Phonons play dual roles in this situation: their increased populations tend to reduce the conductivity via electron scattering, while they can boost the conductivity by assisting electrons to propagate through the potential-energy landscape. Here, we identified a phonon-assisted coherent electron transport process between neighboring nanotubes in temperature-dependent conductivity measurements on a macroscopic film of armchair single-wall carbon nanotubes. Through atomistic modeling of electronic states and calculations of both electronic and phonon-assisted junction conductances, we conclude that phonon-assisted conductance is the dominant mechanism for observed high-temperature transport in armchair carbon nanotubes. The unambiguous manifestation of coherent intertube dynamics proves a single-chirality armchair nanotube film to be a unique macroscopic solid-state ensemble of nano-objects promising for the development of room-temperature coherent electronic devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Polymer Size–Catalytic Activity Relationships in Solution by Fluorescence Correlation Spectroscopy

Measuring the catalytic activity of specific sizes of polymers with active catalysts in solution is typically challenging, due to limited instrument detection sensitivity and/or dynamic range. Here, a fluorescence correlation spectroscopy (FCS) method is developed to determine the catalytic activity of living polymers of a specific apparent size in solution. Deviation from a single-component FCS data fitting, as assessed by χ2, is also introduced and developed as a “speciation index”—a method to evaluate and track changes in the relative amount of distinct polymer sizes with reaction progress. These methods are enabled by incorporating a selectively reactive fluorescent monomer into growing polydicyclopentadiene or polynorbornene during ring-opening metathesis polymerization (ROMP). Compared to polynorbornene, data showed that catalysts in aggregates of polyDCPD retained higher activity for longer—outcomes not directly inferable from simple diffusional-access predictions. Here, the ability to assign catalytic activity to polymers of specific sizes, and then to determine how this activity evolves with reaction progress, support long-term goals in the development and measurement of nano-objects that possess size-dependent catalytic activity.

Active catalyst↗
DOE OSTI2024

Copper(I) photosensitizer-silica nanoparticle assembly towards enhanced aqueous photoluminescence

Harnessing the luminescence potential of Cu(I) complexes in aqueous media is typically hindered by their poor photostability and altered properties. Here, we report the synthesis, engineering and morphological characterization of a hydrophobic homoleptic copper(I) complex entrapped into silica nanoparticles, Cu-I@SiO 2 (where “Cu-I” designates [Cu(2,9-diiodo-1,10-phenanthroline) 2 ] + ), as a promising stabilisation strategy towards water-compatible, Cu(I) complex-based luminescence. The polyether chain-decorated nano-objects are spherical with an average diameter of ca. 10.8 ± 1.9 nm. Upon dispersion in water, clear solution-like suspensions were obtained. Significantly, the aqueous suspensions photo-luminesce (Φ em = 5×10 -4 ) upon excitation through the Metal-to-Ligand Charge-Transfer transition (MLCT) of the embedded copper(I) complexes. In contrast, the corresponding silica-free molecular complex dissolved in an aqueous environment revealed fully quenched emission. Finally, the use of Cu-I@SiO 2 suspensions as luminescent probes is reported, first by assessing their potential use as electrochemiluminescent probes, and second by monitoring the photoluminescence from Cu-I@SiO 2 in the presence of whole blood.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Super-resolution Imaging of Plasmonic Near-Fields: Overcoming Emitter Mislocalizations

Plasmonic nano-objects have shown great potential in enhancing applications like biological/chemical sensing, light harvesting and energy transfer, and optical/quantum computing. Therefore, an extensive effort has been vested in optimizing plasmonic systems and exploiting their field enhancement properties. Super-resolution imaging with quantum dots (QDs) is a promising method to probe plasmonic near-fields but is hindered by the distortion of the QD radiation pattern. Here, we investigate the interaction between QDs and “L-shaped” gold nanoantennas and demonstrate both theoretically and experimentally that this strong interaction can induce polarization-dependent modifications to the apparent QD emission intensity, polarization, and localization. Based on FDTD simulations and polarization-modulated single-molecule microscopy, we show that the displacement of the emitter’s localization is due to the position-dependent interference between the emitter and the induced dipole, and can be up to 100 nm. Our results help pave a pathway for higher precision plasmonic near-field mapping and its underlying applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Tuning the Dimensionality of Excitons in Colloidal Quantum Dot Molecules

Electrically coupled quantum dots (QDs) can support unique optoelectronic properties arising from the superposition of single-particle excited states. Experimental methods for integrating colloidal QDs within the same nano-object, however, have remained elusive to the rational design. Here, we demonstrate a chemical strategy that allows for the assembling of colloidal QDs into coupled composites, where proximal interactions give rise to unique optoelectronic behavior. The assembly method employing “adhesive” surfactants was used to fabricate both homogeneous (e.g., CdS–CdS, PbS–PbS, CdSe–CdSe) and heterogeneous (e.g., PbS–CdS, CdS–CdSe) nanoparticle assemblies, exhibiting quasi-one-dimensional exciton fine structure. In addition, tunable mixing of single-particle exciton states was achieved for dimer-like assemblies of CdSe/CdS core–shell nanocrystals. The nanoparticle assembly mechanism was explained within the viscoelastic interaction theory adapted for molten-surface colloids. Furthermore, we expect that the present work will provide the synthetic and theoretical foundation needed for building assemblies of many inorganic nanocrystals.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Real-Time In Situ Observation of CsPbBr 3 Perovskite Nanoplatelets Transforming into Nanosheets

The manipulation of nano-objects through heating is an effective strategy for inducing structural modifications and therefore changing the optoelectronic properties of semiconducting materials. Despite its potential, the underlying mechanism of the structural transformations remains elusive, largely due to the challenges associated with their in situ observations. To address these issues, we synthesize temperature-sensitive CsPbBr 3 perovskite nanoplatelets and investigate their structural evolution at the nanoscale using in situ heating transmission electron microscopy. We observe the morphological changes that start from the self-assembly of the nanoplatelets into ribbons on a substrate. We identify several paths of merging nanoplates within ribbons that ultimately lead to the formation of nanosheets dispersed randomly on the substrate. These observations are supported by molecular dynamics simulations. We correlate the various paths for merging to the random orientation of the initial ribbons along with the ligand mobility (especially from the edges of the nanoplatelets). This leads to the preferential growth of individual nanosheets and the merging of neighboring ones. These processes enable the creation of structures with tunable emission, ranging from blue to green, all from a single material. Our real-time observations of the transformation of perovskite 2D nanocrystals reveal a route to achieve large-area nanosheets by controlling the initial orientation of the self-assembled objects with potential for large-scale applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Selectively accessing the hotspots of optical nanoantennas by self-aligned dry laser ablation

Plasmonic nanostructures serve as optical antennas for concentrating the energy of incoming light in localized hotspots close to their surface. By positioning nanoemitters in the antenna hotspots, energy transfer is enabled, leading to novel hybrid antenna-emitter-systems, where the antenna can be used to manipulate the optical properties of the nano-objects. The challenge remains how to precisely position emitters within the hotspots. We report a self-aligned process based on dry laser ablation of a calixarene that enables the attachment of molecules within the electromagnetic hotspots at the tips of gold nanocones. Within the laser focus, the ablation threshold is exceeded in nanoscale volumes, leading to selective access of the hotspot areas. A first indication of the site-selective functionalization process is given by attaching fluorescently labelled proteins to the nanocones. In a second example, Raman-active molecules are selectively attached only to nanocones that were previously exposed in the laser focus, which is verified by surface enhanced Raman spectroscopy. Enabling selective functionalization is an important prerequisite e.g. for preparing single photon sources for quantum optical technologies, or multiplexed Raman sensing platforms.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Optical Forces on an Oscillating Dipole Near VO2 Phase Transition

We investigate optical forces on oscillating dipoles close to a phase change vanadium dioxide (VO2) film, which exhibits a metal-insulator transition around 340 K and low thermal hysteresis. This configuration emulates the interaction between an illuminated nanosphere and an interface and we employ a classical description to capture its important aspects. We consider both electric and magnetic dipoles for two different configurations, namely with the dipole moments parallel and perpendicular to the VO2 film. By using Bruggeman theory to describe the effective optical response of the material, we show that the thermal hysteresis present in the VO2 transition clearly shows up in the behavior of optical forces. In the near-field regime, the force on both dipoles can change from attractive to repulsive just by heating (or cooling) the film for a selected frequency range. We also verified that the optical forces are comparable to the Casimir-Polder force in a similar system, revealing the possibility of modulating or even changing the sign of the resultant force on an illuminated nano-object due to the presence of a thermochromic material. We hope that this work contributes to set the grounds for alternative approaches to control light-matter interactions using phase-change materials.

36 MATERIALS SCIENCE↗