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At least 199 records · Page 11

All sources NASA NTRS DOE OSTI

DOE OSTI2017

Systematic evaluation of structure–property relationships in heteroacene – diketopyrrolopyrrole molecular donors for organic solar cells

Improved understanding of fundamental structure–property relationships, particularly the effects of molecular shape and intermolecular packing on film morphology and active layer charge transport characteristics, enables more rational synthesis of new p-type small molecules. Here we investigate a series of small molecules consisting of an acene-based electron-rich core flanked by one or two electron-deficient diketopyrrolopyrrole (DPP) moieties. Through minor changes in the molecule structures, measurable variations in the crystal structure and sizable differences in macroscopic properties are achieved. The molecular symmetry as well as the conformation of the side chains affects the unit cell packing density and strength of the intermolecular electronic coupling in single crystals of all molecules in this series. Here, the addition of a second DPP unit to the benzodithiophene (BDT) core increases molecular planarity leading to decreased reorganization energy, strong cofacial coupling, and moderate hole mobility (2.7 × 10 –4 cm 2 V –1 s –1 ). Increasing the length of the acene core from benzodithiophene to naphthodithiophene (NDT) results in a further reduction in reorganization energy and formation of smaller crystalline domains (~11 nm) when mixed with PCBM. Decreasing the aspect ratio of the core using a “zig-zag” naphthodithiophene (zNDT) isomer results in the highest hole mobility of 1.3 × 10 –3 cm 2 V –1 s –1 due in part to tight lamellar (d = 13.5 Å) and π–π stacking (d = 3.9 Å). The hole mobility is directly correlated with the short-circuit current (11.7 mA cm –2 ) and solar cell efficiency (4.4%) of the highest performing zNDT:PCBM device. For each of these small molecules the calculated π-coupling constant is correlated with the hole mobility as a function of crystal structure and orientation indicating the importance of designing molecules that create extended crystalline networks with maximal π-orbital overlap.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Diffusion of Hydrophilic to Hydrophobic Forms of Nile Red in Aqueous C 12 EO 10 Gels by Variable Area Fluorescence Correlation Spectroscopy

In this work, solute diffusion within lyotropic liquid crystal gels prepared from a series of water and decaethylene glycol monododecyl ether (C 12 EO 10 ) mixtures was explored by variable area fluorescence correlation spectroscopy. Aqueous C 12 EO 10 gels were prepared in concentrations ranging from 55:45 to 70:30 wt% of surfactant and water. Small angle X-ray scattering revealed that these gels comprise hexagonal mesophases of cylindrical micelles. Micelle spacing was found to decrease with increasing C 12 EO 10 concentration. Three different Nile red (NR) dyes were employed as model solutes and were separately doped into the gels at nanomolar levels. These include a hydrophilic form of NR incorporating an anionic sulfonate group (NRSO 3 - ), a hydrophobic form incorporating a fourteen-carbon alkane tail (NRC 14 ), and commercial NR as an intermediate case. FCS data acquired from the gels revealed that NRSO 3 - diffused primarily in 3D. Its diffusion coefficient exhibited a monotonic decrease with increasing gel concentration and micelle packing density, consistent with confinement of its motions as a result of its exclusion from the micelle cores. NRC 14 exhibited the smallest diffusion coefficient, most likely due to its larger size and enhanced interactions with the micelle cores. NR yielded an intermediate diffusion coefficient and the most anomalous behavior of the three dyes, attributable to its facile partitioning between core and corona regions, and greater participation by 1D diffusion. The results of these studies afford an improved understanding of molecular mass transport through soft-matter nanomaterials like those being developed for use in drug delivery and membrane based chemical separations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2014

Chemical bonding, optical constants, and electrical resistivity of sputter-deposited gallium oxide thin films

Gallium oxide (Ga{sub 2}O{sub 3}) thin films were made by sputter deposition employing a Ga{sub 2}O{sub 3} ceramic target for sputtering. The depositions were made over a wide range of substrate temperatures (T{sub s}), from 25 to 600 °C. The effect of T{sub s} on the chemical bonding, surface morphological characteristics, optical constants, and electrical properties of the grown films was evaluated using X-ray photoelectron spectroscopy (XPS), atomic force microscopy (AFM), spectroscopic ellipsometry (SE), and four-point probe measurements. XPS analyses indicate the binding energies (BE) of the Ga 2p doublet, i.e., the Ga 2p{sub 3/2} and Ga 2p{sub 1/2} peaks, are located at 1118.0 and 1145.0 eV, respectively, characterizing gallium in its highest chemical oxidation state (Ga{sup 3+}) in the grown films. The core level XPS spectra of O 1s indicate that the peak is centered at a BE ∼ 531 eV, which is also characteristic of Ga-O bonds in the Ga{sub 2}O{sub 3} phase. The granular morphology of the nanocrystalline Ga{sub 2}O{sub 3} films was evident from AFM measurements, which also indicate that the surface roughness of the films increases from 0.5 nm to 3.0 nm with increasing T{sub s}. The SE analyses indicate that the index of refraction (n) of Ga{sub 2}O{sub 3} films increases with increasing T{sub s} due to improved structural quality and packing density of the films. The n(λ) of all the Ga{sub 2}O{sub 3} films follows the Cauchy's dispersion relation. The room temperature electrical resistivity was high (∼200 Ω-cm) for amorphous Ga{sub 2}O{sub 3} films grown at T{sub s} = RT-300 °C and decreased to ∼1 Ω-cm for nanocrystalline Ga{sub 2}O{sub 3} films grown at T{sub s} ≥ 500–600 °C. A correlation between growth conditions, microstructure, optical constants, and electrical properties of Ga{sub 2}O{sub 3} films is derived.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2014

Spectroscopic ellipsometry determination of the optical constants of titanium-doped WO{sub 3} films made by co-sputter deposition

Titanium (Ti) doped tungsten oxide (WO{sub 3}) thin films were grown by co-sputter deposition of W and Ti metal targets. The sputtering powers to the W and Ti were kept constant at 100 W and 50 W, respectively, while varying the growth temperature (T{sub s}) in the range of 25–400 °C. The structural quality of Ti-doped WO{sub 3} films is dependent on T{sub s}. Ti-doped WO{sub 3} films grown at T{sub s} < 400 °C were amorphous. A temperature of 400 °C is critical to promote the structural order and formation of monoclinic, nanocrystalline films. The optical constants and their dispersion profiles determined from spectroscopic ellipsometry indicate that there is no significant inter-diffusion at the film-substrate interface for W-Ti oxide film growth of ∼40 nm. The index refraction (n) at λ = 550 nm varies in the range of 2.15–2.40 with a gradual increase in T{sub s}. Lorentz-Lorenz analysis (n{sub (λ)} = 550 nm) of the data indicates the gradual improvement in the packing density coupled with structural transformation accounts for the observed optical quality of the Ti-doped WO{sub 3} films as a function of T{sub s}. A correlation between the growth conditions and optical constants is discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2014

Thermal conductivity of vertically aligned carbon nanotube arrays: Growth conditions and tube inhomogeneity

The thermal conductivity of vertically aligned carbon nanotube arrays (VACNTAs) grown on silicon dioxide substrates via chemical vapor deposition is measured using a 3ω technique. For each sample, the VACNTA layer and substrate are pressed to a heating line at varying pressures to extract the sample's thermophysical properties. The nanotubes' structure is observed via transmission electron microscopy and Raman spectroscopy. The presence of hydrogen and water vapor in the fabrication process is tuned to observe the effect on measured thermal properties. The presence of iron catalyst particles within the individual nanotubes prevents the array from achieving the overall thermal conductivity anticipated based on reported measurements of individual nanotubes and the packing density.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2014

One-dimensional array of point-like light sources based on gold nanoparticles and tetracene: Preparation and possible operation mechanisms

A method of preparation of a linear close-packed array of point-like light sources based on a nanocomposite of gold nanoparticles and tetracene is proposed. Ordered system of microleads to the light sources with packing density up to 1000 mm{sup −1} consists of linear conducting chains of cobalt nanoparticles self-assembled in a magnetic field. The electroluminescence from the gold-tetracene nanocomposite occurs in the visible range typical of organic light-emitting field-effect transistors based on tetracene. A theoretical substantiation of the possibility of excitation of tetracene molecules by hot electrons emitted from the gold nanoparticles is suggested and compared with other possible physical mechanisms.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Effect of oxygen annealing on the multiferroic properties of Ca{sup 2+} doped BiFeO{sub 3} nanoceramics

The high leakage current in divalent ion doped BiFeO{sub 3} systems is limiting their large scale application. It is clearly shown that the methodology of oxygen annealing will prove to be an effective procedure for suppressing the detrimental consequences that originate from the oxygen vacancies. The samples annealed under oxygen also show different particle morphologies and packing density that can help in tuning the relevant physical properties, viz., magnetic, ferroelectric, and magnetoelectric. The difference in magnetic behaviour in samples annealed in air and oxygen can be explained in terms of the modification in the Fe-O-Fe bonds, domain wall pinning centres, and crystal anisotropy. Another important observation is the stabilization of a dielectric anomaly near the magnetic transition temperature. This observation can make this multiferroic system very interesting for application in sensors where the change in the magnetic parameters can be observed by monitoring the electrical parameters. Detailed analysis of the dielectric and impedance curves indicate towards the presence of non-Debye type processes in samples obtained by annealing in air or oxygen. From the calculated activation energy values, the vacancy related relaxation mechanism is predominant in air annealed samples, while the oxygen annealed samples show the presence of two type of relaxation processes, viz., electron hopping mechanism stabilizes at low temperature while, at higher temperatures, the process associated with the diffusion of doubly ionized oxygen ions predominates. The ac-conductivity data suggests that the correlated barrier tunnelling mechanism, where single electron or two electrons hopping through neighbouring lattice sites leads to ac-conduction.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2015

Effect of ambient combinations of argon, oxygen, and hydrogen on the properties of DC magnetron sputtered indium tin oxide films

Sputtering has been well-developed industrially with singular ambient gases including neutral argon (Ar), oxygen (O{sub 2}), hydrogen (H{sub 2}) and nitrogen (N{sub 2}) to enhance the electrical and optical performances of indium tin oxide (ITO) films. Recent preliminary investigation into the use of combined ambient gases such as an Ar+O{sub 2}+H{sub 2} ambient mixture, which was suitable for producing high-quality (low sheet resistance and high optical transmittance) of ITO films. To build on this promising preliminary work and develop deeper insight into the effect of ambient atmospheres on ITO film growth, this study provides a more detailed investigation of the effects of ambient combinations of Ar, O{sub 2}, H{sub 2} on sputtered ITO films. Thin films of ITO were deposited on glass substrates by DC magnetron sputtering using three different ambient combinations: Ar, Ar+O{sub 2} and Ar+O{sub 2}+H{sub 2}. The structural, electrical and optical properties of the three ambient sputtered ITO films were systematically characterized by X-ray diffraction (XRD), atomic force microscopy (AFM), scanning electron microscopy (SEM), Raman spectroscopy, four probe electrical conductivity and optical spectroscopy. The XRD and Raman studies confirmed the cubic indium oxide structure, which is polycrystalline at room temperature for all the samples. AFM shows the minimum surface roughness of 2.7 nm for Ar+O{sub 2}+H{sub 2} sputtered thin film material. The thickness of the films was determined by the cross sectional SEM analysis and its thickness was varied from 920 to 817 nm. The columnar growth of ITO films was also discussed here. The electrical and optical measurements of Ar+O{sub 2}+H{sub 2} ambient combinations shows a decreased sheet resistance (5.06 ohm/□) and increased optical transmittance (69%) than other samples. The refractive index and packing density of the films were projected using optical transmission spectrum. From the observed results the Ar+O{sub 2}+H{sub 2} ambient is a good choice to enhance the total optoelectronic properties of the ITO films. The improved electrical and optical properties of ITO films with respect to the Ar+O{sub 2}+H{sub 2} ambient sample were discussed in detail. In addition, the physical properties were also discussed with the influence of this ambient combination with respect to Ar, Ar+O{sub 2} and Ar+O{sub 2}+H{sub 2}.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Optically resonant magneto-electric cubic nanoantennas for ultra-directional light scattering

Cubic dielectric nanoparticles are promising candidates for futuristic low-loss, ultra-compact, nanophotonic applications owing to their larger optical coefficients, greater packing density, and relative ease of fabrication as compared to spherical nanoparticles; besides possessing negligible heating at nanoscale in contrast to their metallic counterparts. Here, we present the first theoretical demonstration of azimuthally symmetric, ultra-directional Kerker's-type scattering of simple dielectric nanocubes in visible and near-infrared regions via simultaneous excitation and interference of optically induced electric- and magnetic-resonances up to quadrupolar modes. Unidirectional forward-scattering by individual nanocubes is observed at the first generalized-Kerker's condition for backward-scattering suppression, having equal electric- and magnetic-dipolar responses. Both directionality and magnitude of these unidirectional-scattering patterns get enhanced where matching electric- and magnetic-quadrupolar responses spectrally overlap. While preserving azimuthal-symmetry and backscattering suppression, a nanocube homodimer provides further directionality improvement for increasing interparticle gap, but with reduced main-lobe magnitude due to emergence of side-scattering lobes from diffraction-grating effect. We thoroughly investigate the influence of interparticle gap on scattering patterns and propose optimal range of gap for minimizing side-scattering lobes. Besides suppressing undesired side-lobes, significant enhancement in scattering magnitude and directionality is attained with increasing number of nanocubes forming a linear chain. Optimal directionality, i.e., the narrowest main-scattering lobe, is found at the wavelength of interfering quadrupolar resonances; whereas the largest main-lobe magnitude is observed at the wavelength satisfying the first Kerker's condition. These unique optical properties of dielectric nanocubes thus can revolutionize their applications at visible and near-infrared regions in the fields of nanoantennas, nanolasers, photovoltaics, and even in biomedicine.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Processing dependence of mechanical properties of metallic glass nanowires

Compared to their crystalline counterparts, nanowires made of metallic glass have not only superb properties but also remarkable processing ability. They can be processed easily and cheaply like plastics via a wide range of methods. To date, the underlying mechanisms of how these different processing routes affect the wires' properties as well as the atomic structure remains largely unknown. Here, by using atomistic modeling, we show that different processing methods can greatly influence the mechanical properties. The nanowires made via focused ion beam milling and embossing exhibit higher strength but localized plastic deformation, whereas that made by casting from liquid shows excellent ductility with homogeneous deformation but reduced strength. The different responses are reflected sensitively in the underlying atomic structure and packing density, some of which have been observed experimentally. The presence of the gradient of alloy concentration and surface effect will be discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Fast and low-dose computed laminography using compressive sensing based technique

Computed laminography (CL) is well known for inspecting microstructures in the materials, weldments and soldering defects in high density packed components or multilayer printed circuit boards. The overload problem on x-ray tube and gross failure of the radio-sensitive electronics devices during a scan are among important issues in CL which needs to be addressed. The sparse-view CL can be one of the viable option to overcome such issues. In this work a numerical aluminum welding phantom was simulated to collect sparsely sampled projection data at only 40 views using a conventional CL scanning scheme i.e. oblique scan. A compressive-sensing inspired total-variation (TV) minimization algorithm was utilized to reconstruct the images. It is found that the images reconstructed using sparse view data are visually comparable with the images reconstructed using full scan data set i.e. at 360 views on regular interval. We have quantitatively confirmed that tiny structures such as copper and tungsten slags, and copper flakes in the reconstructed images from sparsely sampled data are comparable with the corresponding structure present in the fully sampled data case. A blurring effect can be seen near the edges of few pores at the bottom of the reconstructed images from sparsely sampled data, despite the overall image quality is reasonable for fast and low-dose NDT.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2015

Super-stretchable metallic interconnects on polymer with a linear strain of up to 100%

Metal interconnects in flexible and wearable devices are heterogeneous metal-polymer systems that are expected to sustain large deformation without failure. The principal strategy to make strain tolerant interconnect lines on flexible substrates has comprised of creating serpentine structures of metal films with either in-plane or out-of-plane waves, using porous substrates, or using highly ductile materials such as gold. The wavy and helical serpentine patterns preclude high-density packing of interconnect lines on devices, while ductile materials such as Au are cost prohibitive for real world applications. Ductile copper films can be stretched if bonded to the substrate, but show high level of cracking beyond few tens of % strain. In this paper, we demonstrate a material system consisting of Indium metal film over an elastomer (PDMS) with a discontinuous Cr layer such that the metal interconnect can be stretched to extremely high linear strain (up to 100%) without any visible cracks. Such linear strain in metal interconnects exceeds that reported in literature and is obtained without the use of any geometrical manipulations or porous substrates. Systematic experimentation is carried out to explain the mechanisms that allow the Indium film to sustain the high strain level without failure. The islands forming the discontinuous Cr layer are shown to move apart from each other during stretching without delamination, providing strong adhesion to the Indium film while accommodating the large strain in the system. The Indium film is shown to form surface wrinkles upon release from the large strain, confirming its strong adhesion to PDMS. A model is proposed based upon the observations that can explain the high level of stretch-ability of the Indium metal film over the PDMS substrate.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2015

Irreversible thermochromic response of RF sputtered nanocrystalline BaWO{sub 4} films for smart window applications

We report irreversible thermochromic behaviour of BaWO{sub 4} (BWO) films for the first time. BWO films have been deposited at different substrate temperatures (RT, 200, 400, 600 and 800 °C) using RF magnetron sputtering in pure argon plasma. BWO films deposited at 800 °C exhibit crystalline nature. Also, BWO films deposited in the temperature range of 400 - 600 °C exhibit WO{sub 3} as a secondary phase and its weight percentage decreases with an increase in deposition temperature, whereas the films deposited at 800 °C exhibited pure tetragonal phase. FESEM images revealed that as the average particle sizes of the films are higher as compared with the thickness of the films and is explained based on Avrami type nucleation and growth. The transmittance of the films decreases with an increase in deposition temperature up to 600 °C and increases thereafter. Films deposited at 600 °C show ≤ 20% transmittance, looking at the films deposited at room temperature and 800 °C exhibits 90 and 70%, respectively. The refractive index and extinction coefficient of the films show profound dependence on crystallinity and packing density. The optical bandgap of BWO films increases significantly with an increase in O{sub 2}% during the deposition. The optical bandgap of the BWO films deposited at different temperatures in pure argon plasma, are in the range of 3.7 to 3.94 eV whereas the films deposited at 600 °C under different O{sub 2} plasma are in the range of 3.6 - 4.5 eV. The formations of colour centres are associated with the oxygen vacancies, which are clearly seen from the optical bandgap studies. The observed irreversible thermochromic behaviour in BWO films is attributed to the presence of oxygen vacancies that arises due to the electrons trapped at oxygen vacancies causing an inter valence charge transfer of W{sup 5+} to W{sup 6+} and is confirmed through the change in the optical density (ΔOD). Further, the Raman spectra are being used to quantify the presence of oxygen vacancies and the formation of pure BWO phase. The obtained optical responses of BWO films are promising for solar cell and smart window applications.

36 MATERIALS SCIENCE↗

DOE OSTI2016

A study of physical and optical absorption spectra of VO{sup 2+} ions in potassium and sodium oxide borate glasses

Spectroscopic and physical properties of V{sub 2}O{sub 5} doped mixed alkali borate glasses are investigated. Borate glasses containing fixed concentrations of alkaline earth oxides (MgO and BaO) and alkali oxides (K{sub 2}O and Na{sub 2}O) were changes and are prepared by melt quenching technique. The values of r{sub i}, r{sub p}, R{sub m}, α{sub m} molar volume and Λ{sub th} increase and oxygen packing density, density and dopant ion concentration decrease with increasing of K{sub 2}O content. As a result there shall be an increase in the disorder of the glass network. The optical band gap energies, Urbach energy, boron-boron separation,refractive index, dielectric constant, electronic polarizability and reflection loss values are varies nonlinearly with the K{sub 2}O content which manifests the mixed alkali effect.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2016

Enhanced copper micro/nano-particle mixed paste sintered at low temperature for 3D interconnects

An enhanced copper paste, formulated by copper micro- and nano-particles mixture, is reported to prevent paste cracking and obtain an improved packing density. The particle mixture of two different sizes enables reduction in porosity of the micro-paste and resolves the cracking issue in the nano-paste. In-situ temperature and resistance measurements indicate that the mixed paste has a lower densification temperature. Electrical study also shows a ∼12× lower sheet resistance of 0.27 Ω/sq. In addition, scanning electron microscope image analysis confirms a ∼50% lower porosity, which is consistent with the thermal and electrical results. The 3:1 (micro:nano, wt. %) mixed paste is found to have the strongest synergistic effect. This phenomenon is discussed further. Consequently, the mixed paste is a promising material for potential low temperature 3D interconnects fabrication.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2016

Inorganic-ligand exchanging time effect in PbS quantum dot solar cell

We investigate time-dependent inorganic ligand exchanging effect and photovoltaic performance of lead sulfide (PbS) nanocrystal films. With optimal processing time, volume shrinkage induced by residual oleic acid of the PbS colloidal quantum dot (CQD) was minimized and a crack-free film was obtained with improved flatness. Furthermore, sufficient surface passivation significantly increased the packing density by replacing from long oleic acid to a short iodide molecule. It thus facilities exciton dissociation via enhanced charge carrier transport in PbS CQD films, resulting in the improved power conversion efficiency from 3.39% to 6.62%. We also found that excess iodine ions on the PbS surface rather hinder high photovoltaic performance of the CQD solar cell.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2016

Mechanochemical synthesis of high thermoelectric performance bulk Cu 2 X (X = S, Se) materials

We devised a single-step mechanochemical synthesis/densification procedure for Cu 2 X (X = S, Se) thermoelectric materials via applying a pressure of 3 GPa to a stoichiometric admixture of elemental Cu and X for 3 min at room temperature. The obtained bulk materials were single-phase, nearly stoichiometric structures with a relative packing density of 97% or higher. The structures contained high concentration of atomic scale defects and pores of 20-200 nm diameter. The above attributes gave rise to a high thermoelectric performance: at 873 K, the ZT value of Cu2S reached 1.07, about 2.1 times the value typical of samples grown from the melt. The ZT value of Cu 2 Se samples reached in excess of 1.2, close to the state-of-the-art value.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Secondary electron emission yield from high aspect ratio carbon velvet surfaces

The plasma electrons bombarding a plasma-facing wall surface can induce secondary electron emission (SEE) from the wall. A strong SEE can enhance the power losses by reducing the wall sheath potential and thereby increasing the electron flux from the plasma to the wall. The use of the materials with surface roughness and the engineered materials with surface architecture is known to reduce the effective SEE by trapping the secondary electrons. In this work, we demonstrate a 65% reduction of SEE yield using a velvet material consisting of high aspect ratio carbon fibers. The measurements of SEE yield for different velvet samples using the electron beam in vacuum demonstrate the dependence of the SEE yield on the fiber length and the packing density, which is strongly affected by the alignment of long velvet fibers with respect to the electron beam impinging on the velvet sample. Furthermore, the results of SEE measurements support the previous observations of the reduced SEE measured in Hall thrusters.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗