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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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At least 721 records · Page 40
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Quantum funneling in blended multi-band gap core/shell colloidal quantum dot solar cells

Multi-band gap heterojunction solar cells fabricated from a blend of 1.2 eV and 1.4 eV PbS colloidal quantum dots (CQDs) show poor device performance due to non-radiative recombination. To overcome this, a CdS shell is epitaxially formed around the PbS core using cation exchange. From steady state and transient photoluminescence measurements, we understand the nature of charge transfer between these quantum dots. Photoluminescence decay lifetimes are much longer in the PbS/CdS core/shell blend compared to PbS only, explained by a reduction in non-radiative recombination resulting from CdS surface passivation. PbS/CdS heterojunction devices sustain a higher open-circuit voltage and lower reverse saturation current as compared to PbS-only devices, implying lower recombination rates. Further device performance enhancement is attained by modifying the composition profile of the CQD species in the absorbing layer resulting in a three dimensional quantum cascade structure.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Suppression of dark current through barrier engineer for solution-processed colloidal quantum-dots infrared photodetectors

In an attempt to suppress the dark current, the barrier layer engineer for solution-processed PbSe colloidal quantum-dot (CQD) photodetectors has been investigated in the present study. It was found that the dark current can be significantly suppressed by implementing two types of carrier blocking layers, namely, hole blocking layer and electron blocking layer, sandwiched in between two active PbSe CQD layers. Meanwhile no adverse impact has been observed for the photo current. Our study suggests that this improvement resides on the transport pathway created via carrier recombination at intermediate layer, which provides wide implications for the suppression of dark current for infrared photodetectors.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Local structure of temperature and pH-sensitive colloidal microgels

The temperature dependence of the local intra-particle structure of colloidal microgel particles, composed of interpenetrated polymer networks, has been investigated by small-angle neutron scattering at different pH and concentrations, in the range (299÷315) K, where a volume phase transition from a swollen to a shrunken state takes place. Data are well described by a theoretical model that takes into account the presence of both interpenetrated polymer networks and cross-linkers. Two different behaviors are found across the volume phase transition. At neutral pH and T ≈ 307 K, a sharp change of the local structure from a water rich open inhomogeneous interpenetrated polymer network to a homogeneous porous solid-like structure after expelling water is observed. Differently, at acidic pH, the local structure changes almost continuously. These findings demonstrate that a fine control of the pH of the system allows to tune the sharpness of the volume-phase transition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Background limited mid-infrared photodetection with photovoltaic HgTe colloidal quantum dots

The photovoltaic response of thin films of HgTe colloidal quantum dots in the 3–5 μm range is observed. With no applied bias, internal quantum efficiency exceeding 40%, specific detectivity above 10{sup 10} Jones and microseconds response times are obtained at 140 K. The cooled devices detect the ambient thermal radiation. A detector with 5.25 μm cut-off achieves Background Limited Infrared Photodetection at 90 K.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Excited-state dynamics of size-dependent colloidal TiO{sub 2}-Au nanocomposites

The ultrafast excited-state dynamics of size-dependent TiO{sub 2}-Au nanocomposites synthesized by reducing gold nanoclusters to the surface of colloidal TiO{sub 2} nanoparticles are studied using pump-probe transient absorption spectroscopy with 400 nm excitation pulses. The results show that the relaxation processes of the plasmon depletion band, which are described by electron-phonon and phonon-phonon scattering lifetimes, are independent of the gold nanocluster shell size surrounding the TiO{sub 2} nanoparticle core. The dynamics corresponding to interfacial electron transfer between the gold nanoclusters and the TiO{sub 2} bandgap are observed to spectrally overlap with the gold interband transition signal, and the electron transfer lifetimes are shown to significantly decrease as the nanocluster shell size increases. Additionally, size-dependent periodic oscillations are observed and are attributed to acoustic phonons of a porous shell composed of aggregated gold nanoclusters around the TiO{sub 2} core, with frequencies that decrease and damping times that remain constant as the nanocluster shell size increases. These results are important for the development of improved catalytic nanomaterial applications.

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

Cobalt ferrite nanoparticles with improved aqueous colloidal stability and electrophoretic mobility

We have synthesized CoFe{sub 2}O{sub 4} (CFO) nanoparticles of size ∼ 12.2 nm by hydrothermal synthesis method. To control the size of these CFO nanoparticles, oleic acid was used as a surfactant. The inverse spinel phase of the synthesized nanoparticles was confirmed by X-ray diffraction method. As synthesized oleic acid coated CFO (OA@CFO) nanoparticles has very less electrophoretic mobility in the water and are not water dispersible. These OA@CFO nanoparticles were successfully turned into water soluble phase with a better colloidal aqueous stability, through a chemical treatment using citric acid. The modified citric acid coated CFO (CA@CFO) nanoparticles were dispersible in water and form a stable aqueous solution with high electrophoretic mobility.

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

An on-chip colloidal magneto-optical grating

Interacting nano- and micro-particles provide opportunities to create a wide range of useful colloidal and soft matter constructs. In this letter, we examine interacting superparamagnetic polymeric particles residing on designed permalloy (Ni{sub 0.8} Fe{sub 0.2}) shapes that are subject to weak time-orbiting magnetic fields. The precessing field and magnetic barriers that ensue along the outer perimeter of the shapes allow for containment concurrent with independent field-tunable ordering of the dipole-coupled particles. These remotely activated arrays with inter-particle spacing comparable to the wavelength of light yield microscopic on-chip surface gratings for beam steering and magnetically regulated light diffraction applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Optical and electrical characterizations of a single step ion beam milling mesa devices of chloride passivated PbS colloidal quantum dots based film

Colloidal Quantum Dots (CQDs) are of increasing interest, thanks to their quantum size effect that gives rise to their usage in various applications, such as biological tagging, solar cells and as the sensitizing layer of night vision devices. Here, we analyze the optical absorbance of chloride passivated PbS CQDs as well as revealing a correlation between their photoluminescence and sizes distribution, using theoretical models and experimental results from the literature. Next, we calculate the CQDs resistivity as a film. Although resistivity can be calculated from sheet resistance measurement using four point probes, such measurement is usually carried-out on the layer’s surface that in most cases has dangling bonds and surface states, which might affect the charges flow and modify the resistivity. Therefore; our approach, which was applied in this work, is to extract the actual resistivity from measurements that are performed along the film’s thickness (z-direction). For this intent, we fabricated gold capped PbS mesas devices using a single step Ion Beam Milling (IBM) process where we milled the gold and the PbS film continually, and then measured the vertical resistance. Knowing the mesas’ dimensions, we calculate the resistivity. To the best of our knowledge, no previous work has extracted, vertically, the resistivity of chloride passivated PbS CQDs using the above method.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Optimization schemes for efficient multiple exciton generation and extraction in colloidal quantum dots

Multiple exciton generation (MEG) is a process in which more than one electron hole pair is generated per absorbed photon. It allows us to increase the efficiency of solar energy harvesting. Experimental studies have shown the multiple exciton generation yield of 1.2 in isolated colloidal quantum dots. However real photoelectric devices require the extraction of electron hole pairs to electric contacts. We provide a systematic study of the corresponding quantum coherent processes including extraction and injection and show that a proper design of extraction and injection rates enhances the yield significantly up to values around 1.6.

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

Utilization of machine learning to accelerate colloidal synthesis and discovery

Machine learning techniques are seeing increased usage for predicting new materials with targeted properties. However, widespread adoption of these techniques is hindered by the relatively greater experimental efforts required to test the predictions. Furthermore, because failed synthesis pathways are rarely communicated, it is difficult to find prior datasets that are sufficient for modeling. This work presents a closed-loop machine learning-based strategy for colloidal synthesis of nanoparticles, assuming no prior knowledge of the synthetic process, in order to show that synthetic discovery can be accelerated despite limited data availability.

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

Voltage-controlled reversible modulation of colloidal quantum dot thin film photoluminescence

Active modulation of quantum dot thin film photoluminescence (PL) has been far-reaching potential applications in biomedical and optoelectronic systems, but challenges remain in achieving large PL modulation depth and fast temporal response. Here, we report an efficient voltage-controlled optical down-converter by optically exciting a colloidal quantum dot thin film within a quantum dot light-emitting diode under reverse bias. Utilizing field-induced luminescence quenching, we show that a large electric field can strongly modify carrier dynamics in this nanostructured device, resulting in stable and reversible photoluminescence quenching. The device exhibits photoluminescence reduction of up to 99.5%, corresponding to a contrast ratio of 200:1 under the applied electric field of 3 MV cm -1 with a 300 ns response time. Using excitation wavelength dependent and transient PL spectroscopy, we further show that the high degree of quenching is achieved by a synergistic interplay of quantum-confined Stark effect and field-induced exciton dissociation.

42 ENGINEERING↗
DOE OSTI2024

The surface chemistry of colloidal lead halide perovskite nanowires

This study explored the interplay between the ligand–surface chemistry of colloidal CsPbBr 3 nanowires (NWs) and their optical properties. The ligand equilibrium was probed using nuclear magnetic resonance spectroscopy, and by perturbing the equilibrium via dilution, the gradual removal of ligands from the CsPbBr 3 surface was observed. This removal was correlated with an increase in the surface defect density, as suggested by a broadening of the photoluminescence (PL) spectrum, a decrease in the PL quantum yield (PLQY), and quenching of the PL decay. These results highlight similar surface binding between the traditional CsPbBr 3 quantum dots and our NWs, thereby expanding the scope of well-established ligand chemistry to a relatively unexplored nanocrystal morphology. In conclusion, by controlling the dilution factor, it was revealed that CsPbBr 3 NWs achieve a PLQY of 72% ± 2% and a relatively long average PL lifetime of 400 ± 10 ns, without relying on additional surface passivation techniques, such as ligand exchange.

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

Spectral features of colloidal solutions of elongated gold nanoparticles produced by laser ablation in aqueous solutions

The extinction spectra of colloidal solutions of gold nanoparticles produced by laser ablation in water and aqueous solutions of salts using two near-IR lasers with pulse durations of 200 ns and 1 ps are experimentally investigated. The extinction spectrum of the particles formed by ablation in aqueous solutions is characterised by enhanced optical density in the red and IR regions. This feature is due to the formation of elongated gold nanoparticles, as confirmed by transmission electron microscopy. The surface images of a gold target subjected to multipulse laser ablation exhibit micron and submicron structures. (nanophotonics)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

Biaxial ferromagnetic liquid crystal colloids

Significance We introduce a soft-matter system with fluidity coexisting with long-range biaxial and ferromagnetic ordering of anisotropic molecular and magnetic colloidal building blocks. The facile polar switching of this complex fluid promises technological applications and rich physical behavior arising from the properties of solid magnetic nanoparticles and their long-range ordering prompted by interactions with the host medium.

Liu, Qingkun↗
DOE OSTI2023

Molecular surface programming of rectifying junctions between InAs colloidal quantum dot solids

Heavy-metal-free III–V colloidal quantum dots (CQDs) show promise in optoelectronics: Recent advancements in the synthesis of large-diameter indium arsenide (InAs) CQDs provide access to short-wave infrared (IR) wavelengths for three-dimensional ranging and imaging. In early studies, however, we were unable to achieve a rectifying photodiode using CQDs and molybdenum oxide/polymer hole transport layers, as the shallow valence bandedge (5.0 eV) was misaligned with the ionization potentials of the widely used transport layers. This occurred when increasing CQD diameter to decrease the bandgap below 1.1 eV. Here, we develop a rectifying junction among InAs CQD layers, where we use molecular surface modifiers to tune the energy levels of InAs CQDs electrostatically. Previously developed bifunctional dithiol ligands, established for II-VI and IV-VI CQDs, exhibit slow reaction kinetics with III-V surfaces, causing the exchange to fail. Here, we study carboxylate and thiolate binding groups, united with electron-donating free end groups, that shift upward the valence bandedge of InAs CQDs, producing valence band energies as shallow as 4.8 eV. Photophysical studies combined with density functional theory show that carboxylate-based passivants participate in strong bidentate bridging with both In and As on the CQD surface. The tuned CQD layer incorporated into a photodiode structure achieves improved performance with EQE (external quantum efficiency) of 35% (>1 μm) and dark current density < 400 nA cm -2 , a >25% increase in EQE and >90% reduced dark current density compared to the reference device. This work represents an advance over previous III-V CQD short-wavelength IR photodetectors (EQE < 5%, dark current > 10,000 nA cm -2 ).

36 MATERIALS SCIENCE↗
DOE OSTI2024

Quantifying electron transport in aggregated colloidal suspensions in the strong flow regime

Electron transport in complex fluids, biology, and soft matter is a valuable characteristic in processes ranging from redox reactions to electrochemical energy storage. These processes often employ conductor–insulator composites in which electron transport properties are fundamentally linked to the microstructure and dynamics of the conductive phase. While microstructure and dynamics are well recognized as key determinants of the electrical properties, a unified description of their effect has yet to be determined, especially under flowing conditions. In this work, the conductivity and shear viscosity are measured for conductive colloidal suspensions to build a unified description by exploiting both recent quantification of the effect of flow-induced dynamics on electron transport and well-established relationships between electrical properties, microstructure, and flow. These model suspensions consist of conductive carbon black (CB) particles dispersed in fluids of varying viscosities and dielectric constants. In a stable, well-characterized shear rate regime where all suspensions undergo self-similar agglomerate breakup, competing relationships between conductivity and shear rate were observed. To account for the role of variable agglomerate size, equivalent microstructural states were identified using a dimensionless fluid Mason number, Mn f , which allowed for isolation of the role of dynamics on the flow-induced electron transport rate. At equivalent microstructural states, shear-enhanced particle–particle collisions are found to dominate the electron transport rate. This work rationalizes seemingly contradictory experimental observations in literature concerning the shear-dependent electrical properties of CB suspensions and can be extended to other flowing composite systems.

Science & Technology - Other Topics↗
DOE OSTI2024

Active doping controls the mode of failure in dense colloidal gels

Mechanical properties of disordered materials are governed by their underlying free energy landscape. In contrast to external fields, embedding a small fraction of active particles within a disordered material generates nonequilibrium internal fields, which can help to circumvent kinetic barriers and modulate the free energy landscape. In this work, we investigate through computer simulations how the activity of active particles alters the mechanical response of deeply annealed polydisperse colloidal gels. We show that the “swim force” generated by the embedded active particles is responsible for determining the mode of mechanical failure, i.e., brittle vs. ductile. We find, and theoretically justify, that at a critical swim force the mechanical properties of the gel decrease abruptly, signaling a change in the mode of mechanical failure. The weakening of the elastic modulus above the critical swim force results from the change in gel porosity and distribution of attractive forces among gel particles, while below the critical swim force, the ductility enhancement is caused by an increase of gel structural disorder. Above the critical swim force, the gel develops a pronounced heterogeneous structure characterized by multiple pore spaces, and the mechanical response is controlled by dynamical heterogeneities. We contrast these results with those of a simulated monodisperse gel that exhibits a nonmonotonic trend of ductility modulation with increasing swim force, revealing a complex interplay between the gel energy landscape and embedded activity.

Zhou, Tingtao (ORCID:000000021766719X)↗
DOE OSTI2025

Bridging microscopic dynamics and rheology in the yielding of charged colloidal suspensions

The yielding of soft materials is critical to many natural and industrial processes, yet experimental insights into microscopic aspects of yielding are limited. This study combines angle X-ray scattering, X-ray photon correlation spectroscopy, and in situ rheology (Rheo-SAXS-XPCS) with fast lubrication dynamics simulations to examine how interparticle interactions influence yielding in charged colloidal suspensions. By tuning attraction through salt addition, we compare repulsive and attractive systems under deformation. Repulsive suspensions yield uniformly with Andrade-like creep and minimal structural change. In contrast, attractive suspensions show complex behaviors, including shear banding, delayed yielding, and resolidification, governed by transient dynamics at shear band interfaces. These results directly link microscopic particle dynamics to macroscopic flow and demonstrate how interaction potentials control rheological behavior. This work offers a framework for designing soft materials with tailored properties for applications in coatings, food processing, drug delivery, and other technologies requiring precise mechanical control.

Molecular Dynamics Simulation↗