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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 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

SU-C-201-01: Core/shell and Multishell Colloidal Quantum Dots Nanodosimeters Behaviour Under Repeated MV and KV Irradiations

Purpose: This study intends to characterize the energy dependence of the effect of radiation damage on CdSe multi-shell (MS) (CdS/CdZnS/ZnS) and CdSe core/shell (CS)(ZnS) cQDs. It also aims to investigate irregularities resulting of pauses between subsequent irradiations. Methods: Radioluminescence (RL) measurements were performed with a CCD camera as dose was cumulated by the cQDs (up to 10 kGy), for beam energies 120 kVp, 220 kVp and 6 MV. Repeated expositions of 1999 MU were cumulated. Pauses between subsequent irradiations were varied from 2 to 50 minutes. cQDs photoluminescence (PL) and RL spectral stability was tracked by quantifying the position and FWHM of the luminescence peak. Results: Both types of cQDs showed a clear energy dependence of the RL signal decrease between the kV and the MV beams. For 1.2 kGy of dose cumulated, MS cQDs had 92% of the initial signal left at 6 MV compared to 98% at 120 kVp. The same was observed for CS cQDs: 87% at 6 MV vs 94% at 120 kVp. MS cQDs were found to have a systematic (though small, ∼1%) RL intensity recovery for pauses of 15 minutes or more, while CS cQDs maintain a stable loss regardless of the pause duration. PL and RL spectral measurements revealed a good stability (< 1% variation of the peak position and FWHM) for both types of cQDs. Conclusion: In all, both MS and CS cQDs have a sufficient resistance to large doses of radiation for standard radiation therapy and imaging. Since this resistance is better for lower energy, the utilization of cQDs could be optimized for low energy applications (e.g. theragnostic applications for small animal studies and others). Finally, the ionizing radiation damage mechanisms for this new type of nano-scintillator still have to be identified properly.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2013

Photo- and electroluminescence from semiconductor colloidal quantum dots in organic matrices: QD-OLED

The results are reported of an experimental study of samples of organic light-emitting diodes (OLEDs) with luminescent layers fabricated on the basis of two types of CdSe/CdS/ZnS semiconductor quantum dots (QDs) with average CdSe core diameters of 3.2 and 4.1 nm and the same overall diameters of 6.5 nm. The dependences of the LED efficiency on the applied voltage are determined. Assumptions are made about ways of optimizing the design of high-efficiency LEDs.

36 MATERIALS SCIENCE↗
DOE OSTI2019

On the Synthesis and Photoluminescence and Cathodoluminescence Properties of CdSe, CdTe, PbS, InSb, and GaAs Colloidal Quantum Dots

Quantum dots of the group of wide-gap and narrow-gap semiconductors are synthesized and investigated under identical conditions, which makes it possible to perform the comparative analysis and modeling of the mechanisms of radiative recombination and luminescence, for which a stable exciton bond between the electron and hole has an important role. Exciton states are unstable for quantum dots without a shell and narrow-gap semiconductors, which leads to a substantial decrease in the probability of radiative recombination and, correspondingly, the quantum yield of luminescence. The experimental values of the spectral position of the luminescence maximum for quantum dots with clear manifestation of the exciton recombination mechanism noticeably shift to the long-wavelength region with respect to the calculated ones. In calculations and analysis, we use the effective electron mass for bulk semiconductors. The observed good correspondence of the calculated values of the maximum and spectral band with the experiment can mean that quantum dots have a long-range order crystalline structure similar to that one observed in single crystals and polycrystals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

High Efficiency Colloidal Quantum Dot Phosphors

The project showed that non-Cd containing, InP-based nanocrystals (semiconductor materials with dimensions of ~6 nm) have high potential for enabling next-generation, nanocrystal-based, on chip phosphors for solid state lighting. Typical nanocrystals fall short of the requirements for on chip phosphors due to their loss of quantum efficiency under the operating conditions of LEDs, such as, high temperature (up to 150 °C) and high optical flux (up to 200 W/cm2). The InP-based nanocrystals invented during this project maintain high quantum efficiency (>80%) in polymer-based films under these operating conditions for emission wavelengths ranging from ~530 to 620 nm. These nanocrystals also show other desirable attributes, such as, lack of blinking (a common problem with nanocrystals which limits their performance) and no increase in the emission spectral width from room to 150 °C (emitters with narrower spectral widths enable higher efficiency LEDs). Prior to these nanocrystals, no nanocrystal system (regardless of nanocrystal type) showed this collection of properties; in fact, other nanocrystal systems are typically limited to showing only one desirable trait (such as high temperature stability) but being deficient in other properties (such as high flux stability). The project showed that one can reproducibly obtain these properties by generating a novel compositional structure inside of the nanomaterials; in addition, the project formulated an initial theoretical framework linking the compositional structure to the list of high performance optical properties. Over the course of the project, the synthetic methodology for producing the novel composition was evolved to enable the synthesis of these nanomaterials at a cost approximately equal to that required for forming typical conventional nanocrystals. Given the above results, the last major remaining step prior to scale up of the nanomaterials is to limit the oxidation of these materials during the tens of thousands of hours of LED operation. Once the LED phosphor lifetime specifications are met, these nanocrystals will enable white LEDs for solid state lighting to simultaneously have increased efficiency and improved light quality, in addition to enabling the creation of custom light spectrums. These improvements to white LEDs will help accelerate the adoption of SSL, leading to large savings in US and worldwide energy costs.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2018

Charge-Transport Mechanisms in CuInSe x S 2– x Quantum-Dot Films

Colloidal quantum dots (QDs) have attracted considerable attention as promising materials for solution-processable electronic and optoelectronic devices. Copper indium selenium sulfide (CuInSe x S 2–x or CISeS) QDs are particularly attractive as an environmentally benign alternative to the much more extensively studied QDs containing toxic metals such as Cd and Pb. Carrier transport properties of CISeS-QD films, however, are still poorly understood. Here, we aim to elucidate the factors that control charge conductance in CISeS QD solids and, based on this knowledge, develop practical approaches for controlling the polarity of charge transport and carrier mobilities. To this end, we incorporate CISeS QDs into field-effect transistors (FETs) and perform detailed characterization of these devices as a function of the Se/(Se+S) ratio, surface treatment, thermal annealing, and the identity of source and drain electrodes. We observe that as-synthesized CuInSe x S 2–x QDs exhibit degenerate p-type transport, likely due to metal vacancies and CuIn’’ anti-site defects (Cu 1+ on an In 3+ site) that act as acceptor states. Moderate-temperature annealing of the films in the presence of indium source and drain electrodes leads to switching of the transport polarity to nondegenerate n-type, which can be attributed to the formation of In-related defects such as In Cu •• (an In 3+ cation on a Cu 1+ site) or In i ••• (interstitial In3+) acting as donors. We observe that the carrier mobilities increase dramatically (by 3 orders of magnitude) with increasing Se/(Se+S) ratio in both n- and p-type devices. To explain this observation, we propose a two-state conductance model, which invokes a high-mobility intrinsic band-edge state and a low-mobility defect-related intragap state. These states are thermally coupled, and their relative occupancies depend on both QD composition and temperature. Here, our observations suggest that the increase in the relative fraction of Se moves conduction- and valence band edges closer to low-mobility intragap levels. This results in increased relative occupancy of the intrinsic band-edge states and a corresponding growth of the measured mobility. Further improvement in charge-transport characteristics of the CISeS QD samples as well as their stability is obtained by infilling the QD films with amorphous Al 2 O 3 using atomic layer deposition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2011

All-Inorganic, Efficient Photovoltaic Solid State Devices Utilizing Semiconducting Colloidal Nanocrystal Quantum Dots (Final Report)

We demonstrated robust colloidal quantum dot (QD) photovoltaics with high internal quantum efficiencies. In our structures, device durability is derived from use of all-inorganic atmospherically-stable semiconducting metal-oxide films together with QD photoreceptors. We have shown that both QD and metal-oxide semiconducting films and contacts are amenable to room temperature processing under minimal vacuum conditions, enabling large area processing of PV structures of high internal efficiency. We generated the state of the art devices with power conversion efficiency of more than 4%, and have shown that efficiencies as high as 9% are achievable in the near-term, and as high as 17% in the long-term.

14 SOLAR ENERGY↗
DOE OSTI2020

Solution-processable integrated CMOS circuits based on colloidal CuInSe2 quantum dots

Abstract The emerging technology of colloidal quantum dot electronics provides an opportunity for combining the advantages of well-understood inorganic semiconductors with the chemical processability of molecular systems. So far, most research on quantum dot electronic devices has focused on materials based on Pb- and Cd chalcogenides. In addition to environmental concerns associated with the presence of toxic metals, these quantum dots are not well suited for applications in CMOS circuits due to difficulties in integrating complementary n - and p -channel transistors in a common quantum dot active layer. Here, we demonstrate that by using heavy-metal-free CuInSe 2 quantum dots, we can address the problem of toxicity and simultaneously achieve straightforward integration of complimentary devices to prepare functional CMOS circuits. Specifically, utilizing the same spin-coated layer of CuInSe 2 quantum dots, we realize both p - and n -channel transistors and demonstrate well-behaved integrated logic circuits with low switching voltages compatible with standard CMOS electronics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Red shift in the photoluminescence of colloidal carbon quantum dots induced by photon reabsorption

We synthesize the colloidal carbon/graphene quantum dots 1–9 nm in diameter and study their photoluminescence properties. Surprisingly, the luminescence properties of a fixed collection of colloidal carbon quantum dots can be systematically changed as the concentration varies. A model based on photon reabsorption is proposed which explains well the experiment. Infrared spectral study indicates that the surfaces of the carbon quantum dots are substantially terminated by oxygen atoms, which causes their ultra-high hydrophilicity. Our result clarifies the mystery of distinct emission colors in carbon quantum dots and indicates that photon reabsorption can strongly affect the luminescence properties of colloidal nanocrystals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Origins of low energy-transfer efficiency between patterned GaN quantum well and CdSe quantum dots

For hybrid light emitting devices (LEDs) consisting of GaN quantum wells and colloidal quantum dots, it is necessary to explore the physical mechanisms causing decreases in the quantum efficiencies and the energy transfer efficiency between a GaN quantum well and CdSe quantum dots. This study investigated the electro-luminescence for a hybrid LED consisting of colloidal quantum dots and a GaN quantum well patterned with photonic crystals. It was found that both the quantum efficiency of colloidal quantum dots on a GaN quantum well and the energy transfer efficiency between the patterned GaN quantum well and the colloidal quantum dots decreased with increases in the driving voltage or the driving time. Under high driving voltages, the decreases in the quantum efficiency of the colloidal quantum dots and the energy transfer efficiency can be attributed to Auger recombination, while those decreases under long driving time are due to photo-bleaching and Auger recombination.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Colloidal Germanium Quantum Dots with Broadly Tunable Size and Light Emission

Germanium (Ge) colloidal quantum dots (CQDs) were synthesized by thermal decomposition of GeI 2 using capping ligand mixtures of oleylamine (OAm), octadecene (ODE), and trioctylphosphine (TOP). Average diameters could be tuned across a wide range, from 3 to 18 nm, by adjusting reactant concentrations, heating rates, and reaction temperatures. OAm promotes decomposition of GeI 2 to Ge and serves as a weakly bound capping ligand. ODE displaces OAm during the reaction to terminate particle growth and prevent surface oxidation. TOP is necessary for obtaining nanocrystals larger than 11 nm. In conclusion, the Ge CQDs have relatively narrow size distributions and exhibit size-dependent, band-edge photoluminescence (PL), with peak energies from 0.8 to 1.34 eV, across a wide spectral range in the infrared (IR).

Noh, Jungchul [Univ. of Texas, Austin, TX (United ↗
DOE OSTI2018

Recovery of Active and Efficient Photocatalytic H 2 Production for CdSe Quantum Dots

Recently, colloidal semiconductor quantum dots (QDs) have shown great promise as photocatalysts for the production of chemical fuels by sunlight. Here, the efficiency of photocatalytic hydrogen (H 2 ) production for integrated systems of large diameter (4.4 nm) CdSe QDs as light harvesting nanoparticles with varying concentrations of nickel-dihydrolipoic acid (Ni-DHLA) small molecule catalysts was measured. While exhibiting excellent robustness and longevity, the efficiency of H 2 production for equimolar catalyst and QDs was relatively poor. However, the efficiency was found to increase substantially with increasing Ni-DHLA:QD molar ratios Surprisingly, this high activity was only observed with the use of 3-mercaptopropionic acid (MPA) ligands, while CdSe QDs capped with dihydrolipoic acid (DHLA) exhibited poor performance in comparison, indicating that the QD capping ligand has a substantial impact on the catalytic performance. Finally, ultrafast transient absorption spectroscopic measurements of the electron transfer (ET) dynamics show fast ET to the catalyst. Importantly, an increase in ET efficiency is observed as the catalyst concentration is increased. Together, these results suggest that for these large QDs, tailoring the QD surface environment for facile ET and increasing catalyst concentrations increases the probability of ET from QDs to Ni-DHLA, overcoming the relatively small driving force for ET and decreased surface electron density for large diameter QDs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2011

Charge Transport in a Quantum Dot Supercrystal

Colloidal semiconductor quantum dots connected by organic or inorganic molecules can form periodic supercrystals. These supercrystals can be used for various types of electronic and optical applications with properties superior to those of random quantum dots and organic polymer mixtures. We have used ab initio calculations to study the charge transport and carrier mobility in such supercrystals. Among the different possible charge transport mechanisms, we found that the phonon-assisted hopping is the most likely mechanism. The calculated carrier mobility agrees well with the experimentally measured results. Our predictions of the size and temperature dependences on the mobility are awaiting experimental confirmation.

Chemistry↗
DOE OSTI2019

Coherent single-photon emission from colloidal lead halide perovskite quantum dots

Chemically made colloidal semiconductor quantum dots have long been proposed as scalable and color-tunable single emitters in quantum optics, but they have typically suffered from prohibitively incoherent emission. We now demonstrate that individual colloidal lead halide perovskite quantum dots (PQDs) display highly efficient single-photon emission with optical coherence times as long as 80 picoseconds, an appreciable fraction of their 210-picosecond radiative lifetimes. These measurements suggest that PQDs should be explored as building blocks in sources of indistinguishable single photons and entangled photon pairs. Our results present a starting point for the rational design of lead halide perovskite–based quantum emitters that have fast emission, wide spectral tunability, and scalable production and that benefit from the hybrid integration with nanophotonic components that has been demonstrated for colloidal materials.

solar (photovoltaic), solid state lighting, photos↗