Search NASA⌕ Search

Engineering topics

Sykora, Milan

Publications and source records attributed to Sykora, Milan.

15 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

PbS/CdS Quantum Dot Room-Temperature Single-Emitter Spectroscopy Reaches the Telecom O and S Bands via an Engineered Stability

We synthesized PbS/CdS core/shell quantum dots (QDs) to have functional single-emitter properties for room-temperature, solid-state operation in the telecom O and S bands. Two shell-growth methods–cation exchange and successive ionic layer adsorption and reaction (SILAR)–were employed to prepare QD heterostructures with shells of 2–16 monolayers. PbS/CdS QDs were sufficiently bright and stable to resolve photoluminescence (PL) spectra representing both bands from single nanocrystals using standard detection methods, and for a QD emitting in the O-band a second-order correlation function showed strong photon antibunching, important steps toward demonstrating the utility of lead chalcogenide QDs as single-photon emitters (SPEs). Irrespective of type, few telecom-SPEs exist that are capable of such room-temperature operation. Access to single-QD spectra enabled a direct assessment of spectral line width, which was ~70–90 meV compared to much broader ensemble spectra (~300 meV). We show inhomogeneous broadening results from dispersity in PbS core sizes that increases dramatically with extended cation exchange. Quantum yields (QYs) are negatively impacted at thick shells (>6 monolayers) and, especially, by SILAR-growth conditions. Time-resolved PL measurements revealed that, with SILAR, initially single-exponential PL-decays transition to biexponential, with opening of nonradiative carrier-recombination channels. Radiative decay times are, overall, longer for core/shell QDs compared to PbS cores, which we demonstrate can be partially attributed to some core/shell sizes occupying a quasi-type II electron–hole localization regime. Finally, we demonstrate that shell engineering and the use of lower laser-excitation powers can afford significantly suppressed blinking and photobleaching. However, dependence on shell thickness comes at a cost of less-than-optimal brightness, with implications for both materials and experimental design

36 MATERIALS SCIENCE↗
DOE OSTI2019

Raman spectroscopy of bottom-up synthesized graphene quantum dots: size and structure dependence

Graphene quantum dots (GQDs) have attracted significant interest as synthetically tunable optoelectronic and photonic materials that can also serve as model systems for understanding size-dependent behaviors of related graphene structures such as nanoribbons. Here, we present a Raman spectroscopy study of bottom-up synthesized GQDs with lateral dimensions between 0.97 to 1.62 nm, well-defined (armchair) edge type, and fully benzenoid structures. For a better understanding of observed size-dependent trends, the study is extended to larger graphene structures including nano-graphene platelets (>25 nm) and large-area graphene.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Role of Interface Chemistry in Opening New Radiative Pathways in InP/CdSe Giant Quantum Dots with Blinking-Suppressed Two-Color Emission

InP/CdSe core/thick–shell “giant” quantum dots (gQDs) that exhibit blinking–suppressed two–color excitonic emission have been synthesized and optically characterized. These type II heterostructures exhibit photoluminescence from both a charge–separated, near–infrared type II excitonic state, and a shell–localized visible–color excitonic state. Infrared emission is intrinsic to the type II QD, while visible emission can either be eliminated or enhanced through chemical modification of the InP surface prior to CdSe shell growth. Single–QD photoluminescence measurements confirm that the dual color emission is from individual nanocrystals. Here, the probability of observing dual emission from individual QDs and the extent of blinking suppression increases with shell thickness. Visible emission can be stabilized by the addition of a second shell of CdS, where the resulting InP/CdSe/CdS core/shell/shell nanocrystals afford the strongest blinking suppression, determined by analysis of the Mandel Q parameter. Transient absorption spectroscopy verifies that dual emission arises when hole relaxation from the shell to the core is impeded, possibly as a result of enhanced interfacial hole trapping at F – or O 2– defect sites. Electron–hole recombination in the shell then competes with slower type II recombination, providing a different mechanism for breaking Kasha's rule and allowing two colors of light to be emitted from one nanostructure.

36 MATERIALS SCIENCE↗
DOE OSTI2018

High-Temperature Refractory Metasurfaces for Solar Thermophotovoltaic Energy Harvesting

Solar energy promises a viable solution to meet the ever-increasing power demand by providing a clean, renewable energy alternative to fossil fuels. For solar thermophotovoltaics (STPV), high-temperature absorbers and emitters with strong spectral selectivity are imperative to efficiently couple solar radiation into photovoltaic cells. We demonstrate refractory metasurfaces for STPV with tailored absorptance and emittance characterized by in situ high-temperature measurements, featuring thermal stability up to at least 1200 °C. Our tungsten-based metasurface absorbers have close-to-unity absorption from visible to near-infrared and strongly suppressed emission at longer wavelengths, while our metasurface emitters provide wavelength-selective emission spectrally matched to the band-edge of InGaAsSb photovoltaic cells. The projected overall STPV efficiency is as high as 18% when a fully integrated absorber/emitter metasurface structure is employed, which is comparable to the efficiencies of the best currently available commercial single-junction PV cells and can be further improved to potentially exceed those in mainstream photovoltaic technologies. Finally, our work opens a path forward for high-performance STPV systems based on refractory metasurface structures.

14 SOLAR ENERGY↗
DOE OSTI2017

Actinide oxide photodiode and nuclear battery

Photodiodes and nuclear batteries may utilize actinide oxides, such a uranium oxide. An actinide oxide photodiode may include a first actinide oxide layer and a second actinide oxide layer deposited on the first actinide oxide layer. The first actinide oxide layer may be n-doped or p-doped. The second actinide oxide layer may be p-doped when the first actinide oxide layer is n-doped, and the second actinide oxide layer may be n-doped when the first actinide oxide layer is p-doped. The first actinide oxide layer and the second actinide oxide layer may form a p/n junction therebetween. Photodiodes including actinide oxides are better light absorbers, can be used in thinner films, and are more thermally stable than silicon, germanium, and gallium arsenide.

25 ENERGY STORAGE↗
DOE OSTI2017

Giant PbSe/CdSe/CdSe Quantum Dots: Crystal-Structure-Defined Ultrastable Near-Infrared Photoluminescence from Single Nanocrystals

Toward a truly photostable PbSe quantum dot (QD), we apply the thick-shell or “giant” QD structural motif to this notoriously environmentally sensitive nanocrystal system. Namely, using a sequential application of two shell-growth techniques—partial-cation exchange and successive ionic layer adsorption and reaction (SILAR)—we are able to overcoat the PbSe QDs with sufficiently thick CdSe shells to impart new single-QD-level photostability, as evidenced by suppression of both photobleaching and blinking behavior. Here, we further reveal that the crystal structure of the CdSe shell (cubic zinc-blende or hexagonal wurtzite) plays a key role in determining the photoluminescence properties of these giant QDs, with only cubic nanocrystals sufficiently bright and stable to be observed as single emitters. Moreover, we demonstrate that crystal structure and particle shape (cubic, spherical, or tetrapodal) and, thereby, emission properties can be synthetically tuned by either withholding or including the coordinating ligand, trioctylphosphine, in the SILAR component of the shell-growth process.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Using shape to turn off blinking for two-colour multiexciton emission in CdSe/CdS tetrapods

Here, semiconductor nanostructures capable of emitting from two excited states and thereby of producing two photoluminescence colours are of fundamental and potential technological significance. In this limited class of nanocrystals, CdSe/CdS core/arm tetrapods exhibit the unusual trait of two-colour (red and green) multiexcitonic emission, with green emission from the CdS arms emerging only at high excitation fluences. Here we show that by synthetic shape-tuning, both this multi-colour emission process, and blinking and photobleaching behaviours of single tetrapods can be controlled. Specifically, we find that the properties of dual emission and single-nanostructure photostability depend on different structural parameters—arm length and arm diameter, respectively—but that both properties can be realized in the same nanostructure. Furthermore, based on results of correlated photoluminescence and transient absorption measurements, we conclude that hole-trap filling in the arms and partial state-filling in the core are necessary preconditions for the observation of multiexciton multi-colour emission.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

MaRIE: Probing Dynamic Processes in Soft Materials Using Advanced Light Sources

Los Alamos National Laboratory has developed a concept for a new research facility, MaRIE: Matter-Radiation Interactions in Extremes. The key motivation for MaRIE is to develop new experimental capabilities needed to fill the existing gaps in our fundamental understanding of materials important for key National Nuclear Security Agency (NNSA) goals. MaRIE will bring two major new capabilities: (a) the ability to characterize the meso- and microstructure of materials in bulk as well as local dynamic response characteristics, and (b) the ability to characterize how this microstructure evolves under NNSA-relevant conditions and impacts the material’s performance in this regime.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Metasurface Broadband Solar Absorber

Here, we demonstrate a broadband, polarization independent, wide-angle absorber based on a metallic metasurface architecture, which accomplishes greater than 90% absorptance in the visible and near-infrared range of the solar spectrum, and exhibits low absorptivity (emissivity) at mid- and far-infrared wavelengths. The complex unit cell of the metasurface solar absorber consists of eight pairs of gold nano-resonators that are separated from a gold ground plane by a thin silicon dioxide spacer. Moreover, our experimental measurements reveal high-performance absorption over a wide range of incidence angles for both s- and p-polarizations. We also investigate numerically the frequency-dependent field and current distributions to elucidate how the absorption occurs within the metasurface structure.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Electrochromic Graphene Molecules

Polyclic aromatic hydrocarbons, also called Graphene Molecules (GMs), with chemical composition C 132 H 36 (COOH) 2 were synthesized in-situ on the surface of transparent nanocrystaline indium tin oxide (nc-ITO) electrodes. Their electronic structure was studied electrochemically and spectro-electrochemically. Variations in the potential applied onto the nc-ITO/GM electrodes induce only small changes in the observed current but they produce dramatic changes in the absorption of the GMs, which are associated with their oxidation and reduction. Analysis of the absorption changes using modified Nernst equation is used to determine standard potentials associated with the individual charge transfer processes. For the GMs prepared here these were found to be E 1,ox 0 = 0.77± 0.01 V and E 2,ox 0 = 1.24 ± 0.02 V vs. NHE for the first and second oxidation and E 1,red 0 = -1.50 ± 0.04 V for the first reduction. The charge transfer processes are found to be non-ideal. The non-ideality factors associated with the oxidation and reduction processes suggest presence of strong interactions between the GM redox centers. Under the conditions of potential cycling GMs show rapid (seconds) color change with high contrast and stability. An electrochromic application is demonstrated wherein the GMs are used as the optically active component.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2015

Surface treatment of nanocrystal quantum dots after film deposition

Provided are methods of surface treatment of nanocrystal quantum dots after film deposition so as to exchange the native ligands of the quantum dots for exchange ligands that result in improvement in charge extraction from the nanocrystals.

77 NANOSCIENCE AND NANOTECHNOLOGY↗