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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 1,801 records · Page 100
All sourcesNASA NTRSDOE OSTI
DOE OSTI2011

Nanobody-based chimeric receptor gene integration in Jurkat cells mediated by PhiC31 integrase

The crucial role of T lymphocytes in anti-tumor immunity has led to the development of novel strategies that can target and activate T cells against tumor cells. Recombinant DNA technology has been used to generate non-MHC-restricted chimeric antigen receptors (CARs). Here, we constructed a panel of recombinant CAR that harbors the anti-MUC1 nanobody and the signaling and co-signaling moieties (CD3{zeta}/CD28) with different spacer regions derived from human IgG3 with one or two repeats of the hinge sequence or the hinge region of Fc{gamma}RII. The PhiC31 integrase system was employed to investigate if the recombination efficiency could be recruited for high and stable expression of T cell chimeric receptor genes. The effect of nuclear localization signal (NLS) and two different promoters (CMV and CAG) on efficacy of PhiC31 integrase in human T cell lines was evaluated. The presence of integrase in combination with NLS, mediated up to 7.6 and 8.5 fold increases in CAR expression in ZCHN-attB and ZCHHN-attB cassette integrated T cells, respectively. Our results showed that highly efficient and stable transduction of the Jurkat cell line by PhiC31 integrase is a feasible modality for generating anti-cancer chimeric T cells for use in cancer immunotherapy.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2021

Evidence for Field-Dependent Charge Separation Caused by Mixed Phases in Polymer–Fullerene Organic Solar Cells

As organic photovoltaic performance approaches 20% efficiencies, causal structure–performance relationships must be established for devices to realize theoretical limits and become commercially competitive. Here, we reveal evidence of a causal relationship between mixed donor–acceptor interfaces and charge generation in polymer–fullerene solar cells. To do this, we combine a holistic loss analysis of device performance with quantitative synchrotron X-ray nanocharacterization to identify a >98% anticorrelation between field-dependent geminate recombination and nanodomain purity. Importantly, our analysis eliminates other possible explanations of the performance trends, a requirement to establish causality. The unprecedented granular level of our analysis also separates field-dependent and field-independent recombination at the interface, where we find for the first time that this system is free of field-independent recombination, a loss channel that plagues high-performance systems, including those with non-fullerene acceptors. Furthermore, this result broadens the case that minimizing mixed phases to promote sharp interfaces between pure aggregated domains is the ideal nanostructure for realizing theoretical efficiency limits of organic photovoltaics.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2024

Ultrafast Exciton Dynamics of CH 3 NH 3 PbBr 3 Perovskite Nanoclusters

Exciton dynamics of perovskite nanoclusters has been investigated for the first time using femtosecond transient absorption (TA) and time-resolved photoluminescence (TRPL) spectroscopy. The TA results show two photoinduced absorption signals at 420 and 461 nm and a photoinduced bleach (PB) signal at 448 nm. The analysis of the PB recovery kinetic decay and kinetic model uncovered multiple processes contributing to electron-hole recombination. The fast component (~8 ps) is attributed to vibrational relaxation within the initial excited state, and the medium component (~60 ps) is attributed to shallow carrier trapping. The slow component is attributed to deep carrier trapping from the initial conduction band edge (~666 ps) and the shallow trap state (~40 ps). The TRPL reveals longer time dynamics, with modeled lifetimes of 6.6 and 93 ns attributed to recombination through the deep trap state and direct band edge recombination, respectively. In conclusion, the significant role of exciton trapping processes in the dynamics indicates that these highly confined nanoclusters have defect-rich surfaces.

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

Interplay between Interfacial Structures and Device Performance in Organic Solar Cells: A Case Study with the Low Work Function Metal, Calcium

A better understanding of how interfacial structure affects charge carrier recombination would benefit the development of highly efficient organic photovoltaic (OPV) devices. Here, transient photovoltage (TPV) and charge extraction (CE) measurements are used in combination with synchrotron radiation photoemission spectroscopy (SRPES) to gain insight into the correlation between interfacial properties and device performance. OPV devices based on PCDTBT/PC 71 BM with a Ca interlayer were studied as a reference system to investigate the interfacial effects on device performance. Devices with a Ca interlayer exhibit a lower recombination than devices with only an Al cathode at a given charge carrier density (n). Furthermore, the interfacial band structures indicate that the strong dipole moment produced by the Ca interlayer can facilitate the extraction of electrons and drive holes away from the cathode/polymer interface, resulting in beneficial reduction in interfacial recombination losses. These results help explain the higher efficiencies of devices made with Ca interlayers compared to that without the Ca interlayer.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Enabling Efficient Creation of Long-Lived Charge-Separation on Dye-Sensitized NiO Photocathodes

The hole-injection and recombination photophysics for NiO sensitized with RuP ([Ru II (bpy) 2 (4,4'-(PO 3 H 2 ) 2 -bpy)] 2+ ) are explored. Ultrafast transient absorption (TA) measurements performed with an external electrochemical bias reflect the efficiency for productive hole-injection, that is, quenching of the dye excited state that results in a detectable charge-separated electron–hole pair, is linearly dependent on the electronic occupation of intragap states in the NiO film. Population of these states via a negative applied potential increases the efficiency from 0% to 100%. The results indicate the primary loss mechanism for dye-sensitized NiO is rapid nongeminate recombination enabled by the presence of latent holes in the surface of the NiO film. Our results indicate a new design paradigm for NiO photocathodes and devices centered on the avoidance of this recombination pathway.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Uncovering the Role of Hole Traps in Promoting Hole Transfer from Multiexcitonic Quantum Dots to Molecular Acceptors

The understanding of electronic dynamics in multiexcitonic quantum dots (QDs) is important for designing efficient systems useful in high power scenarios, such as solar concentrators and multielectron charge transfer. The multiple charge carriers within a QD can undergo undesired Auger recombination events, which rapidly annihilate carriers on picosecond time scales and generate heat from absorbed photons instead of useful work. Compared to the transfer of multiple electrons, the transfer of multiple holes has proven to be more difficult due to slower hole transfer rates. To probe the competition between Auger recombination and hole transfer in CdSe, CdS, and CdSe/CdS QDs of varying sizes, we synthesized a phenothiazine derivative with optimized functionalities for binding to QDs as a hole accepting ligand and for spectroscopic observation of hole transfer. Transient absorption spectroscopy was used to monitor the photoinduced absorption features from both trapped holes and oxidized ligands under excitation fluences where the averaged initial number of excitons in a QD ranged from ~1 to 19. We observed fluence-dependent hole transfer kinetics that last around 100 ps longer than the predicted Auger recombination lifetimes, and the transfer of up to 3 holes per QD. Theoretical modeling of the kinetics suggests that binding of hole acceptors introduces trapping states significantly different from those in native QDs passivated with oleate ligands. Holes in these modified trap states have prolonged lifetimes, which promotes the hole transfer efficiency. These results highlight the beneficial role of hole-trapping states in devising hole transfer pathways in QD-based systems under multiexcitonic conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Stimulated Emission from Below the Bandgap in Giant Quantum Shells

Colloidal semiconductor nanocrystals (NCs) have emerged as promising candidates for developing solution-processable optical gain media, with potential applications in integrated photonic circuits and lasers. However, the deployment of NCs in these technologies has been hindered by nonradiative Auger recombination of multiexciton states, which shortens the optical gain lifetime and reduces its spectral range. Here, we demonstrate that these limitations can be overcome by using giant colloidal quantum shells (g-QSs), comprising a quantum-confined CdSe shell grown over a large (~14 nm) CdS bulk core. Such bulk-nanoscale architecture minimizes exciton–exciton interactions, leading to suppressed Auger recombination and one of the broadest gain bandwidths reported for colloidal nanomaterials, spanning energies both above and, remarkably, below the bandgap. Ultrafast transient absorption and photoluminescence measurements demonstrate that the high-energy portion of optical gain arises from states containing more than 15 excitons per particle while the unusual sub-bandgap gain behaviour results from an Auger-assisted radiative recombination, a mechanism that has traditionally been viewed as a loss pathway. Altogether, these results reveal a unique gain regime associated with bulk-nanocrystal hybrid systems, which offers a promising path toward solution-processable light sources.

Absorption↗
DOE OSTI2011

Carrier spin relaxation in GaInNAsSb/GaNAsSb/GaAs quantum well

We have investigated the carrier spin relaxation in GaInNAsSb/GaNAsSb/GaAs quantum well (QW) by time-resolved photoluminescence (PL) measurement. The sample consists of an 8-nm-thick GaIn{sub 0.36}N{sub 0.006}AsSb{sub 0.015} well, 5-nm-thick GaN{sub 0.01}AsSb{sub 0.11} intermediate barriers and 100-nm-thick GaAs barriers grown by molecular beam epitaxy on a GaAs(100) substrate. The spin relaxation time and recombination lifetime at 10 K are measured to be 228 ps and 151 ps, respectively. As a reference, we have also obtained a spin relaxation time of 125 ps and a recombination lifetime of 63 ps for GaInNAs/GaNAs/GaAs QW. This result shows that crystal quality is slightly improved by adding Sb, although these short carrier lifetimes mainly originate from a nonradiative recombination. These spin relaxation times are longer than the 36 ps spin relaxation time of InGaAs/InP QWs and shorter than the 2 ns spin relaxation time of GaInNAs/GaAs QW.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2012

Probing the properties of nebular plasmas with optical and infrared spectroscopy

A number of current developments arising from spectroscopic studies of ionized nebulae are reviewed. Until the past decade or so, such studies were generally confined to the analysis of recombination lines from hydrogen and helium, along with collisionally excited forbidden lines from second and third row elements in the periodic table. However, the advent of efficient detectors on 8m-class telescopes has enabled the detection of recombination lines from second and third row elements, along with collisionally excited lines from much less abundant species. Significant discrepancies have been found between ionic abundances derived from collisionally excited lines and those obtained for the same ions from their recombination lines. The existence of 'cold plasma' with T{sub e}{<=} 1000 K has been confirmed for a number of planetary nebulae. Optical and infrared collisionally excited ionic lines from a wide range of 'neutron-capture' elements from beyond the iron abundance peak have also been detected. There is a consequent need for new calculations and experimental measurements of the atomic data needed to interpret these observations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2013

Electronic and optical properties of ScN and (Sc,Mn)N thin films deposited by reactive DC-magnetron sputtering

Scandium nitride (ScN) is a rocksalt semiconductor that has attracted significant attention from various researchers for a diverse range of applications. Motivated by the prospect of using its interesting electronic structure for optoelectronic and dilute magnetic semiconductor applications, we present detailed studies of the electronic transport and optical properties of ScN and its alloys with manganese nitride (MnN). Our results suggest (a) dilute manganese doping in ScN compensates for the high n-type carrier concentrations arising due to oxygen impurities and (b) an n-type to p-type carrier type transition occurs at a composition between 5.8% and 11% Mn on Sc sites. In terms of its optical properties, our analysis clearly indicates direct and indirect bandgap absorption edges of ScN located at 2.04 eV and 1.18 eV, respectively. In addition to the direct gap absorption edge, (Sc,Mn)N samples also show Mn-defect induced electronic absorption. Photoluminescence measurements at room temperature from ScN films exhibit a yellowish-green emission corresponding to direct gap radiative recombination. Direct gap recombination is not expected given the smaller indirect gap. A possible role of high excitation intensities in suppressing relaxation and recombination across the indirect bandgap is suspected. Raman spectroscopic and ellipsometric characterization of the dielectric permittivities of ScN and (Sc,Mn)N are also presented to assist in understanding the potential of ScN for optoelectronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Growth, steady-state, and time-resolved photoluminescence study of CdTe/MgCdTe double heterostructures on InSb substrates using molecular beam epitaxy

CdTe/MgCdTe double heterostructures (DHs) are grown on InSb substrates using molecular beam epitaxy and reveal strong photoluminescence with over double the intensity of a GaAs/AlGaAs DH with an identical layer structure design grown on GaAs. Time-resolved photoluminescence of the CdTe/MgCdTe DH gives a Shockley-Read-Hall recombination lifetime of 86 ns, which is more than one order of magnitude longer than that of typical polycrystalline CdTe films. These findings indicate that monocrystalline CdTe/MgCdTe DHs effectively reduce surface recombination, have limited nonradiative interface recombination, and are promising for solar cells that could reach power conversion efficiencies similar to that of GaAs.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Two-dimensional excitons in three-dimensional hexagonal boron nitride

The recombination processes of excitons in hexagonal boron nitride (hBN) have been probed using time-resolved photoluminescence. It was found that the theory for two-dimensional (2D) exciton recombination describes well the exciton dynamics in three-dimensional hBN. The exciton Bohr radius and binding energy deduced from the temperature dependent exciton recombination lifetime is around 8 Å and 740 meV, respectively. The effective masses of electrons and holes in 2D hBN deduced from the generalized relativistic dispersion relation of 2D systems are 0.54m{sub o}, which are remarkably consistent with the exciton reduced mass deduced from the experimental data. Our results illustrate that hBN represents an ideal platform to study the 2D optical properties as well as the relativistic properties of particles in a condensed matter system.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2013

Layered insulator hexagonal boron nitride for surface passivation in quantum dot solar cell

Single crystalline, two dimensional (2D) layered insulator hexagonal boron nitride (h-BN), is demonstrated as an emerging material candidate for surface passivation on mesoporous TiO{sub 2}. Cadmium selenide (CdSe) quantum dot based bulk heterojunction (BHJ) solar cell employed h-BN passivated TiO{sub 2} as an electron acceptor exhibits photoconversion efficiency ∼46% more than BHJ employed unpassivated TiO{sub 2}. Dominant interfacial recombination pathways such as electron capture by TiO{sub 2} surface states and recombination with hole at valence band of CdSe are efficiently controlled by h-BN enabled surface passivation, leading to improved photovoltaic performance. Highly crystalline, confirmed by transmission electron microscopy, dangling bond-free 2D layered h-BN with self-terminated atomic planes, achieved by chemical exfoliation, enables efficient passivation on TiO{sub 2}, allowing electronic transport at TiO{sub 2}/h-BN/CdSe interface with much lower recombination rate compared to an unpassivated TiO{sub 2}/CdSe interface.

14 SOLAR ENERGY↗
DOE OSTI2014

A numerical simulation study of gallium-phosphide/silicon heterojunction passivated emitter and rear solar cells

The performance of passivated emitter and rear (PERC) solar cells made of p-type Si wafers is often limited by recombination in the phosphorus-doped emitter. To overcome this limitation, a realistic PERC solar cell is simulated, whereby the conventional phosphorus-doped emitter is replaced by a thin, crystalline gallium phosphide (GaP) layer. The resulting GaP/Si PERC cell is compared to Si PERC cells, which have (i) a standard POCl{sub 3} diffused emitter, (ii) a solid-state diffused emitter, or (iii) a high efficiency ion-implanted emitter. The maximum efficiencies for these realistic PERC cells are between 20.5% and 21.2% for the phosphorus-doped emitters (i)–(iii), and up to 21.6% for the GaP emitter. The major advantage of this GaP hetero-emitter is a significantly reduced recombination loss, resulting in a higher V{sub oc}. This is so because the high valence band offset between GaP and Si acts as a nearly ideal minority carrier blocker. This effect is comparable to amorphous Si. However, the GaP layer can be contacted with metal fingers like crystalline Si, so no conductive oxide is necessary. Compared to the conventional PERC structure, the GaP/Si PERC cell requires a lower Si base doping density, which reduces the impact of the boron-oxygen complexes. Despite the lower base doping, fewer rear local contacts are necessary. This is so because the GaP emitter shows reduced recombination, leading to a higher minority electron density in the base and, in turn, to a higher base conductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Role of size and defects in ultrafast broadband emission dynamics of ZnO nanostructures

As wide bandgap materials are nanostructured for optoelectronics and energy technologies, understanding how size and defects modify the carrier dynamics becomes critical. Here, we examine broadband ultraviolet-visible subpicosecond emission dynamics of prototypical ZnO in bulk, nanowire and nanosphere geometries. Using a high-sensitivity transient emission Kerr-based spectrometer, we probe exciton dynamics in the low fluence regime to determine how defects states impact thermalization and recombination rates. In contrast to steady-state measurements, we transiently identify low-energy emission features that originate from localized excitonic states rather than mid-gap states, characterized by distinct recombination kinetics, and correlate to longer thermalization times. These states are critical for understanding the overall excited state lifetime of materials in this size regime, where crystallinity rather than dimensionality plays a primary role in dictating recombination dynamics.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Amorphous silicon passivated contacts for diffused junction silicon solar cells

Carrier recombination at the metal contacts is a major obstacle in the development of high-performance crystalline silicon homojunction solar cells. To address this issue, we insert thin intrinsic hydrogenated amorphous silicon [a-Si:H(i)] passivating films between the dopant-diffused silicon surface and aluminum contacts. We find that with increasing a-Si:H(i) interlayer thickness (from 0 to 16 nm) the recombination loss at metal-contacted phosphorus (n{sup +}) and boron (p{sup +}) diffused surfaces decreases by factors of ∼25 and ∼10, respectively. Conversely, the contact resistivity increases in both cases before saturating to still acceptable values of ∼ 50 mΩ cm{sup 2} for n{sup +} and ∼100 mΩ cm{sup 2} for p{sup +} surfaces. Carrier transport towards the contacts likely occurs by a combination of carrier tunneling and aluminum spiking through the a-Si:H(i) layer, as supported by scanning transmission electron microscopy–energy dispersive x-ray maps. We explain the superior contact selectivity obtained on n{sup +} surfaces by more favorable band offsets and capture cross section ratios of recombination centers at the c-Si/a-Si:H(i) interface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Development and operation of a high-throughput accurate-wavelength lens-based spectrometer

A high-throughput spectrometer for the 400–820 nm wavelength range has been developed for charge exchange recombination spectroscopy or general spectroscopy. A large 2160 mm{sup −1} grating is matched with fast f/1.8 200 mm lenses, which provide stigmatic imaging. A precision optical encoder measures the grating angle with an accuracy ≤0.075 arc sec. A high quantum efficiency low-etaloning CCD detector allows operation at longer wavelengths. A patch panel allows input fibers to interface with interchangeable fiber holders that attach to a kinematic mount at the entrance slit. Computer-controlled hardware allows automated control of wavelength, timing, f-number, automated data collection, and wavelength calibration.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

On the correlation of the Auger generated hot electron emission and efficiency droop in III-N light-emitting diodes

Recent experiments presented in by Iveland et al. [Phys. Rev. Lett. 110, 177406 (2013)] demonstrated that hot electron emission from cesiated p-contacts of III-nitride quantum-well (QW) light-emitting diodes (LEDs) coincides with the onset of the efficiency droop. We have carried out Monte Carlo simulations of hot-electron transport in realistic III-N LEDs. The simulations account for the hole population and all relevant electron scattering and recombination processes. We show that Auger recombination generates a significant hot electron population, which is temporarily trapped in the conduction band side-valleys, without decaying completely before reaching the p-contact. The leakage current due to electron overflow and thermal escape from the QWs is shown to have a minimal impact on the droop. We conclude that the experimentally observed hot electrons are created by Auger recombination in QWs, and that the Auger effect as the origin of the droop is the only consistent explanation for the experimental findings of Iveland et al., [Phys. Rev. Lett. 110, 177406 (2013)].

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

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