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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Origin of Broad Emission Spectra in InP Quantum Dots: Contributions from Structural and Electronic Disorder

The ensemble emission spectra of colloidal InP quantum dots are broader than achievable spectra of cadmium- and lead-based quantum dots, despite similar single-particle line widths and significant efforts invested in the improvement of synthetic protocols. Here, we seek to explain the origin of persistently broad ensemble emission spectra of colloidal InP quantum dots by investigating the nature of the electronic states responsible for luminescence. We identify a correlation between red-shifted emission spectra and anomalous broadening of the excitation spectra of luminescent InP colloids, suggesting a trap-associated emission pathway in highly emissive core shell quantum dots. Time-resolved pump probe experiments find that s are largely untrapped on photoluminescence relevant time scales pointing to emission from recombination of localized holes with free electrons. Two-dimensional electronic spectroscopy on InP quantum dots reveals multiple emissive states and increased electron phonon coupling associated with hole localization. These localized hole states near the valence band edge are hypothesized to arise from incomplete surface passivation and structural disorder associated with lattice defects. We confirm the presence and effect of lattice disorder by X-ray absorption spectroscopy and Raman scattering measurements. Participation of localized electronic states that are associated with various classes of lattice defects gives rise to phonon-coupled defect related emission. These findings explain the origins of the persistently broad emission spectra of colloidal InP quantum dots and suggest future strategies to narrow ensemble emission lines comparable to what is observed for cadmium-based materials.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Nanostructured silicon substrates of nanopore morphology for buffer-layer free nanoheteroepitaxial growth of InP films

To reduce the cost of III–V solar cells, a buffer-layer free method of depositing high-quality III–V thin films onto low-cost silicon nanostructured substrates is proposed that is enabled by stress relaxation due to the nanopore morphology of the silicon substrate. As a proof-of-concept test of the proposed method, the nanoheteroepitaxial deposition of high quality InP thin film is examined. By comparing the deposition of InP (under conditions optimized for InP deposition onto InP substrates) onto nanostructured Si(100) substrates with nanopore and nanopillar morphologies, the morphology of nanopores is found to be preferred for the nanoheteroepitaxial deposition of InP films.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Production of ice-nucleating particles (INPs) by fast-growing phytoplankton

Sea spray aerosol contains ice-nucleating particles (INPs), which affect the formation and proper ties of clouds. Here, we show that aerosols emitted from fast-growing marine phytoplankton produce effective immersion INPs, which nucleate at temperatures significantly warmer than the atmospheric homogeneous freezing (-38.0 °C) of pure water. Aerosol sampled over phytoplankton cultures grown in a Marine Aerosol Ref erence Tank (MART) induced nucleation and freezing at temperatures as high as -15.0 °C during exponential phytoplankton growth. This was observed in monospecific cultures representative of two major groups of phy toplankton, namely a cyanobacterium (Synechococcus elongatus) and a diatom (Thalassiosira weissflogii). Ice nucleation occurred at colder temperatures (-28.5 °C and below), which were not different from the freezing temperatures of procedural blanks, when the cultures were in the stationary or death phases of growth. Ice nucleation at warmer temperatures was associated with relatively high values of the maximum quantum yield of photosystem II ( Φ PSII ), an indicator of the physiological status of phytoplankton. High values of Φ PSII indicate the presence of cells with efficient photochemistry and greater potential for photosynthesis. For comparison, field measurements in the North Atlantic Ocean showed that high net growth rates of natural phytoplankton assemblages were associated with marine aerosol that acted as effective immersion INPs at relatively warm temperatures. Data were collected over 4 d at a sampling station maintained in the same water mass as the water column stabilized after deep mixing by a storm. Phytoplankton biomass and net phytoplankton growth rate (0.56 d -1 ) were greatest over the 24 h preceding the warmest mean ice nucleation temperature (-25.5 °C). Collectively, our laboratory and field observations indicate that phytoplankton physiological status is a useful predictor of effective INPs and more reliable than biomass or taxonomic affiliation. Ocean regions associated with fast phytoplankton growth, such as the North Atlantic during the annual spring bloom, may be significant sources of atmospheric INPs.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Annual cycle of aerosol properties over the central Arctic during MOSAiC 2019–2020 – light-extinction, CCN, and INP levels from the boundary layer to the tropopause

Abstract. The MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition was the largest Arctic field campaign ever conducted. MOSAiC offered the unique opportunity to monitor and characterize aerosols and clouds with high vertical resolution up to 30 km height at latitudes from 80 to 90∘ N over an entire year (October 2019 to September 2020). Without a clear knowledge of the complex aerosol layering, vertical structures, and dominant aerosol types and their impact on cloud formation, a full understanding of the meteorological processes in the Arctic, and thus advanced climate change research, is impossible. Widespread ground-based in situ observations in the Arctic are insufficient to provide these required aerosol and cloud data. In this article, a summary of our MOSAiC observations of tropospheric aerosol profiles with a state-of-the-art multiwavelength polarization Raman lidar aboard the icebreaker Polarstern is presented. Particle optical properties, i.e., light-extinction profiles and aerosol optical thickness (AOT), and estimates of cloud-relevant aerosol properties such as the number concentration of cloud condensation nuclei (CCN) and ice-nucleating particles (INPs) are discussed, separately for the lowest part of the troposphere (atmospheric boundary layer, ABL), within the lower free troposphere (around 2000 m height), and at the cirrus level close to the tropopause. In situ observations of the particle number concentration and INPs aboard Polarstern are included in the study. A strong decrease in the aerosol amount with height in winter and moderate vertical variations in summer were observed in terms of the particle extinction coefficient. The 532 nm light-extinction values dropped from >50 Mm−1 close to the surface to <5 Mm−1 at 4–6 km height in the winter months. Lofted, aged wildfire smoke layers caused a re-increase in the aerosol concentration towards the tropopause. In summer (June to August 2020), much lower particle extinction coefficients, frequently as low as 1–5 Mm−1, were observed in the ABL. Aerosol removal, controlled by in-cloud and below-cloud scavenging processes (widely suppressed in winter and very efficient in summer) in the lowermost 1–2 km of the atmosphere, seems to be the main reason for the strong differences between winter and summer aerosol conditions. A complete annual cycle of the AOT in the central Arctic could be measured. This is a valuable addition to the summertime observations with the sun photometers of the Arctic Aerosol Robotic Network (AERONET). In line with the pronounced annual cycle in the aerosol optical properties, typical CCN number concentrations (0.2 % supersaturation level) ranged from 50–500 cm−3 in winter to 10–100 cm−3 in summer in the ABL. In the lower free troposphere (at 2000 m), however, the CCN level was roughly constant throughout the year, with values mostly from 30 to 100 cm−3. A strong contrast between winter and summer was also given in terms of ABL INPs which control ice production in low-level clouds. While soil dust (from surrounding continents) is probably the main INP type during the autumn, winter, and spring months, local sea spray aerosol (with a biogenic aerosol component) seems to dominate the ice nucleation in the ABL during the summer months (June–August). The strong winter vs. summer contrast in the INP number concentration by roughly 2–3 orders of magnitude in the lower troposphere is, however, mainly caused by the strong cloud temperature contrast. A unique event of the MOSAiC expedition was the occurrence of a long-lasting wildfire smoke layer in the upper troposphere and lower stratosphere. Our observations suggest that the smoke particles frequently triggered cirrus formation close to the tropopause from October 2019 to May 2020.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1991

Photoluminescence lifetime measurements in InP wafers

A simple apparatus to measure the minority carrier lifetime in InP has been developed. The technique stimulates the sample with a short pulse of light from a diode laser and measures the photoluminescence decay to extract the minority carrier lifetime. The photoluminescence lifetime in InP as a function of doping on both n- and p-type material is examined. The results also show a marked difference in the lifetime of n-type InP and p-type InP of similar doping levels. N-type InP shows a lifetime considerably longer than the expected radiative limited lifetime.

Landis, Geoffrey A.↗
NASA NTRS1993

Electrochemical characterization of p(+)n and n(+)p diffused InP structures

The relatively well documented and widely used electrolytes for characterization and processing of Si and GaAs-related materials and structures by electrochemical methods are of little or no use with InP because the electrolytes presently used either dissolve the surface preferentially at the defect areas or form residual oxides and introduce a large density of surface states. Using an electrolyte which was newly developed for anodic dissolution of InP, and was named the 'FAP' electrolyte, accurate characterization of InP related structures including nature and density of surface states, defect density, and net majority carrier concentration, all as functions of depth was performed. A step-by-step optimization of n(+)p and p(+)n InP structures made by thermal diffusion was done using the electrochemical techniques, and resulted in high performance homojunction InP structures.

Wilt, David M.↗
NASA NTRS1994

Summary of Workshop on InP: Status and Prospects

The primary objective of most of the programs in InP solar cells is the development of the most radiation hard solar cell technology. In the workshop, it was generally agreed that the goal is a cell which displays high radiation tolerance in a radiation environment equivalent to a 1 MeV electron fluence of about 10(exp 16)/sq cm. Furthermore, it is desired that the radiation response of the cell be essentially flat out to this fluence - i.e. that the power output of the cell not decrease from its beginning of life (BOL) value in this radiation environment. It was also agreed in the workshop that the manufacturability of InP solar cells needs to be improved. In particular, since InP wafers are relatively dense and brittle, alternative substrates need to be developed. Research on hetero-epitaxial InP cells grown on Si, Ge, and GaAs substrates is currently underway. The ultimate goal is to develop hetero-epitaxial InP solar cells using a cheap, strong, and lightweight substrate.

Walters, R. J.↗
DOE OSTI2024

InP- and GaAs-Based 0.6 eV GaInAs Devices for Thermophotovoltaics and Laser Power Conversion

Emerging applications such as thermal energy grid storage, waste heat recovery and portable power generation require efficient thermophotovoltaic (TPV) converters tuned to temperatures near 1000 Degrees Celsius or below. Metamorphic GaInAs with larger lattice constants than InP present a promising option for these needs. The ability to grow these devices on GaAs substrates instead of more expensive InP would enhance the scalability of these devices. In this talk, we present inverted metamorphic Ga0.3In0.7As photovoltaic converters with sub-0.60 eV bandgaps grown on InP and GaAs substrates. These devices are realized using InAsP or GaInP/InAsP compositionally graded buffers which exhibit threading dislocation densities of 1.3 +/- 0.6 x 106 cm-2 and 8.9 +/- 1.7 x 106 cm-2 on InP and GaAs, respectively. Despite this difference in defect density, the devices generate similar open-circuit voltages of 0.386 V and 0.383 V, respectively, under irradiance producing a short-circuit current density of -10 A/cm2, with bandgap-voltage offsets of 0.20 and 0.21 V. We estimate their thermophotovoltaic efficiency using these measurements coupled with broadband reflectance measurments. The InP-based cell is estimated to yield 1.09 W/cm2 at 1100 Degrees Celsius vs. 0.92 W/cm2 for the GaAs-based cell, with TPV efficiencies of 16.8 vs. 9.2%. Both devices are limited by sub-bandgap absorption, which we assess largely occurs in the graded buffers. We estimate that the 1100 Degrees Celsius thermophotovoltaic efficiencies would increase to 24.0% and 20.7% in structures with the graded buffer removed, if previously demonstrated reflectance is achieved. These devices also have application as laser power converters in the 2.0-2.3 um atmospheric window. We estimate efficiencies of 36.8% and 32.5% under 2.0 um monochromatic irradiance of 1.86 W/cm2 and 2.81 W/cm2, respectively.

ENGINEERING,MATERIALS SCIENCE,SOLAR ENERGY↗
DOE OSTI2025

Nb 2 O 5 Protection Layers for Hydrogen Evolution by p-InP Photocathodes in Acidic Electrolytes

Coatings of HfO 2 , Ta 2 O 5 , TiO 2 , and Nb 2 O 5 were evaluated as protection layers for p-InP photocathodes in aqueous acidic electrolytes. Each candidate protection layer was characterized based on interfacial conduction of photogenerated electrons, the thermodynamic and kinetic stability of the overlayer over the relevant potential and pH range for cathodic fuel-forming half-reactions, and inhibition of the primary anodic and/or chemical dissolution processes that limit electrode stability. The conduction of photogenerated electrons and inhibition of anodic oxidation was evaluated using V 3+ / 2+ in 5.0 M HCl(aq) as a one-electron redox couple with a potential close to that of hydrogen evolution in acidic media. Failure modes due to cathodic plating of metal, as well as anodic dissolution and chemical dissolution processes, were evaluated for photocathodes made from etched p-InP, platinized p-InP, and p-InP photoelectrodes that had been coated with the various oxide films and then platinized for use in photoelectrochemical hydrogen evolution in acidic aqueous electrolytes. Nb 2 O 5 best met all of the criteria, contrasting with TiO 2 , which is thermodynamically and kinetically unstable in acid over the potential range relevant for the hydrogen evolution and/or CO 2 reduction electrochemical half-reactions. Furthermore, these protocols should be useful for other materials and semiconductors to determine the effectiveness of protection layers for photocathodes.

Electrodes↗
DOE OSTI2016

Crystallinity, Surface Morphology, and Photoelectrochemical Effects in Conical InP and InN Nanowires Grown on Silicon

The growth conditions of two types of indium-based III–V nanowires, InP and InN, are tailored such that instead of yielding conventional wire-type morphologies, single-crystal conical structures are formed with an enlarged diameter either near the base or near the tip. By using indium droplets as a growth catalyst, combined with an excess indium supply during growth, “ice cream cone” type structures are formed with a nanowire “cone” and an indium-based “ice cream” droplet on top for both InP and InN. Surface polycrystallinity and annihilation of the catalyst tip of the conical InP nanowires are observed when the indium supply is turned off during the growth process. This growth design technique is extended to create single-crystal InN nanowires with the same morphology. Conical InN nanowires with an enlarged base are obtained through the use of an excess combined Au–In growth catalyst. Electrochemical studies of the InP nanowires on silicon demonstrate a reduction photocurrent as a proof of photovolatic behavior and offer insight as to how the observed surface polycrystallinity and the resulting interface affect these device-level properties. Furthermore, a photovoltage is induced in both types of conical InN nanowires on silicon, which is not replicated in epitaxial InN thin films.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Front-Surface Potential of Platinized p -InP Photocathodes Probed by Dual-Working-Electrode Measurements

The front-surface potential (E fr ) of p-InP/Pt photocathodes performing the hydrogen-evolution reaction has been probed under operating conditions using a dual-workingelectrode (DWE) method. The DWE data are consistent with expectations for proposed stability mechanisms for p-InP photocathodes. Specifically, E fr for Pt-modified p-InP adopts a value near the reversible hydrogen electrode (RHE) potential, consistent with kinetic suppression of metallic In 0 formation. The data provide a rapid, operando metric of interfacial catalyst activity, and indicate that E fr for the p-InP/Pt junction is governed by surface catalytic kinetics rather than by the applied back-contact potential (E b ).

Catalysts↗
DOE OSTI2015

Role of TiO 2 Surface Passivation on Improving the Performance of p-InP Photocathodes

The role of TiO 2 thin films deposited by atomic layer deposition on p-InP photocathodes used for solar hydrogen generation was examined. It was found that, in addition to its previously reported corrosion protection role, the large valence band offset between TiO 2 and InP creates an energy barrier for holes reaching the surface. Also, the conduction band of TiO 2 is well-aligned with that of InP. The combination of these two effects creates an electronselective contact with low interface recombination. Under simulated solar illumination in HClO 4 aqueous electrolyte, an onset potential of >800 mV vs RHE was achieved, which is the highest yet reported for an InP photocathode.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Enrichment of Phosphates, Lead, and Mixed Soil–Organic Particles in INPs at the Southern Great Plains Site

Ice nucleating particles (INPs) are rare particles that initiate primary ice formation, a critical step required for subsequent important cloud microphysical processes that ultimately govern cloud phase and cloud radiative properties. Laboratory studies have found that organic-rich dusts, such as those found in soils, are more efficient INPs compared to mineral dust. However, the atmospheric relevance of these organic-rich dusts are not well understood, particularly in regions with significant agricultural activity. The Agricultural Ice nuclei at the Southern Great Plains field campaign (AGINSGP) was conducted in rural Oklahoma to investigate how soil dusts contribute to INP populations in the Great Plains. We present chemical characterization of ambient and ice crystal residual particles from a single day of sampling, using single particle mass spectrometry (SPMS) and scanning microscopy. Ambient particles were primarily carbonaceous or secondary aerosol, while the fraction of dust particles was higher in the residual particles. We also observed an unusual particle type consisting of a carbonaceous core mixed with dust fragments on the surface, which was found in higher proportion in residuals. Dust particles measured during residual sampling contained greater proportions of phosphate $(^{63}\text{PO}^-_2$ and $^{79}\text{PO}^-_3)$ and lead ( 206 Pb + ). Strong sulfate signals were not seen in the residual dust particles measured by the SPMS, while nitrate was slightly depleted relative to ambient dust. This study shows that organic-rich soils may be important contributors to the ambient INP population in agricultural regions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Surface characterization of InP trenches embedded in oxide using scanning probe microscopy

Metrology for structural and electrical analyses at device level has been identified as one of the major challenges to be resolved for the sub-14 nm technology nodes. In these advanced nodes, new high mobility semiconductors, such as III–V compounds, are grown in narrow trenches on a Si substrate. Probing the nature of the defects, the defect density, and the role of processing steps on the surface of such structures are prime metrology requirements. In order to enable defect analysis on a (III–V) surface, a proper sample preparation for oxide removal is of primary importance. In this work, the effectiveness of different chemical cleanings and thermal annealing procedures is investigated on both blanket InP and oxide embedded InP trenches by means of scanning probe microscopy techniques. It is found that the most effective approach is a combination of an HCl-based chemical cleaning combined with a low-temperature thermal annealing leading to an oxide free surface with atomically flat areas. Scanning tunneling microscopy (STM) has been the preferred method for such investigations on blanket films due to its intrinsic sub-nm spatial resolution. However, its application on oxide embedded structures is non-trivial. To perform STM on the trenches of interest (generally <20 nm wide), we propose a combination of non-contact atomic force microscopy and STM using the same conductive atomic force microscopy tip Our results prove that with these procedures, it is possible to perform STM in narrow InP trenches showing stacking faults and surface reconstruction. Significant differences in terms of roughness and terrace formation are also observed between the blanket and the oxide embedded InP.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Optical and structural properties of 100 MeV Fe{sup 9+} ion irradiated InP

Single crystal InP samples were irradiated with 100 MeV Fe{sup 9+} ions for ion fluences 1x10{sup 12} and 1x10{sup 13} cm{sup −2}. Optical properties of irradiated InP was investigated by Spectroscopic Ellipsometry and UV-VIS-NIR spectroscopy. The optical parameters like, refractive index, extinction coefficient, absorption coefficient is found to be fluence dependent near the surface as well as near the projected range. Small change in the optical parameters near the surface region as investigated by Spectroscopic Ellipsometry indicatesthat the surfaces of irradiated InP are similar to non-irradiated InP. This is also supported by RBS/C measurements. The UV-VIS-NIR study revealed the decrease in the band gap and increase in the defect concentration in the irradiated sample as a result of nuclear energy loss.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Growing InGaAs quasi-quantum wires inside semi-rhombic shaped planar InP nanowires on exact (001) silicon

We report InGaAs quasi-quantum wires embedded in planar InP nanowires grown on (001) silicon emitting in the 1550 nm communication band. An array of highly ordered InP nanowire with semi-rhombic cross-section was obtained in pre-defined silicon V-grooves through selective-area hetero-epitaxy. The 8% lattice mismatch between InP and Si was accommodated by an ultra-thin stacking disordered InP/GaAs nucleation layer. X-ray diffraction and transmission electron microscope characterizations suggest excellent crystalline quality of the nanowires. By exploiting the morphological evolution of the InP and a self-limiting growth process in the V-grooves, we grew embedded InGaAs quantum-wells and quasi-quantum-wires with tunable shape and position. Room temperature analysis reveals substantially improved photoluminescence in the quasi-quantum wires as compared to the quantum-well reference, due to the reduced intrusion defects and enhanced quantum confinement. These results show great promise for integration of III-V based long wavelength nanowire lasers on the well-established (001) Si platform.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Voc Degradation in TF-VLS Grown InP Solar Cells

Here we consider two hypotheses to explain the open-circuit voltage (VOC) degradation observed in thin-film vapor-liquid-solid (TF-VLS) grown p-type InP photovoltaic cells: bandgap narrowing and local shunting. First, a bandgap (Eg) narrowing effect is hypothesized, based on the surface inhomogeneity of VLS InP captured by the photoluminescence (PL) image. The PL data was used to estimate a spatially-resolved active VOC across surface of the InP sample. Combining this data with the effective Jsc allowed an assessment of the I-V characteristics of individual unit cells. Next, an H-SPICE diode compact model was utilized to reproduce the I-V characteristics of the whole sample. We find a good fit to the I-V performance of TF-VLS grown InP solar cell. Second, a local shunting effect was also considered as an alternative explanation of the VOC degradation effect. Again, PL image data was used, and small local shunt resistance was added in arbitrary elementary unit cells to represent certain dark spots seen in the PL image and dictate the VOC degradation occurred in the sample.

14 SOLAR ENERGY↗
DOE OSTI2012

Effect of Cl{sub 2}- and HBr-based inductively coupled plasma etching on InP surface composition analyzed using in situ x-ray photoelectron spectroscopy

A Cl{sub 2}-HBr-O{sub 2}/Ar inductively coupled plasma (ICP) etching process has been adapted for the processing of InP-based heterostructures in a 300-mm diameter CMOS etching tool. Smooth and anisotropic InP etching is obtained at moderate etch rate ({approx}600 nm/min). Ex situ x-ray energy dispersive analysis of the etched sidewalls shows that the etching anisotropy is obtained through a SiO{sub x} passivation mechanism. The stoichiometry of the etched surface is analyzed in situ using angle-resolved x-ray photoelectron spectroscopy. It is observed that Cl{sub 2}-based ICP etching results in a significantly P-rich surface. The phosphorous layer identified on the top surface is estimated to be {approx}1-1.3-nm thick. On the other hand InP etching in HBr/Ar plasma results in a more stoichiometric surface. In contrast to the etched sidewalls, the etched surface is free from oxides with negligible traces of silicon. Exposure to ambient air of the samples submitted to Cl{sub 2}-based chemistry results in the complete oxidation of the P-rich top layer. It is concluded that a post-etch treatment or a pure HBr plasma step may be necessary after Cl{sub 2}-based ICP etching for the recovery of the InP material.

36 MATERIALS SCIENCE↗