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At least 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Measurement of minority-carrier diffusion lengths using wedge-shaped semiconductor photoelectrodes

Measurement of the photocurrent as a function of the thickness of a light absorber has been shown herein both theoretically and experimentally to provide a method for determination of the minority-carrier diffusion length of a sample. To perform the measurement, an illuminated spot of photons with an energy well above the band gap of the material was scanned along the thickness gradient of a wedge-shaped, rear-illuminated semiconducting light absorber. Photogenerated majority carriers were collected through a back-side transparent ohmic contact, and a front-side liquid or Schottky junction collected the photogenerated minority carriers. Calculations showed that the diffusion length could be evaluated from the exponential variation in photocurrent as a function of the thickness of the sample. Good agreement was observed between experiment and theory for a solid-state silicon Schottky junction measured using this method. As an example for the application of the technique to semiconductor/liquid-junction photoelectrodes, the minority-carrier diffusion length was determined for graded thickness, sputtered tungsten trioxide and polished bismuth vanadate films under back-illumination in contact with an aqueous electrolyte. Furthermore, this wedge technique does not require knowledge of the spectral absorption coefficient, doping, or surface recombination velocity of the sample.

42 ENGINEERING↗
DOE OSTI2014

A surface plasmon enabled liquid-junction photovoltaic cell

Plasmonic nanosystems have recently been shown to be capable of functioning as photovoltaics and of carrying out redox photochemistry, purportedly using the energetic electrons and holes created following plasmonic decay as charge carriers. Although such devices currently have low efficiency, they already manifest a number of favorable characteristics, such as their tunability over the entire solar spectrum and a remarkable resistance to photocorrosion. Here, we report a plasmonic photovoltaic using a 25 μm thick electrolytic liquid junction which supports the iodide/triiodide (I - /I 3 - ) redox couple. The device produces photocurrent densities in excess of 40 μA cm -2 , an open circuit voltage ( V oc ) of ~0.24 V and a fill factor of ~0.5 using AM 1.5 G solar radiation at 100 mW cm -2 . The photocurrent and the power conversion efficiency are primarily limited by the low light absorption in the 2-D gold nanoparticle arrays. The use of a liquid junction greatly reduces dielectric breakdown in the oxide layers utilized, which must be very thin for optimal performance, leading to a great improvement in the long-term stability of the cell's performance.

Lee, Woo-ram↗
DOE OSTI2015

A scanning probe investigation of the role of surface motifs in the behavior of p-WSe 2 photocathodes

The spatial variation in the photoelectrochemical performance for the reduction of an aqueous one-electron redox couple, Ru(NH 3 ) 6 3+/2+ , and for the evolution of H 2 (g) from 0.5 M H 2 SO 4 (aq) at the surface of bare or Pt-decorated p-type WSe 2 photocathodes has been investigated in situ using scanning photocurrent microscopy (SPCM). The measurements revealed significant differences in the charge-collection performance (quantified by the values of external quantum yields, Φ ext ) on various macroscopic terraces. Local spectral response measurements indicated a variation in the local electronic structure among the terraces, which was consistent with a non-uniform spatial distribution of sub-band-gap states within the crystals. The photoconversion efficiencies of Pt-decorated p-WSe2 photocathodes were greater for the evolution of H 2 (g) from 0.5 M H 2 SO 4 than for the reduction of Ru(NH 3 ) 6 3+/2+ , and terraces that exhibited relatively low values of Φext for the reduction of Ru(NH 3 ) 6 3+/2+ could in some cases yield values of Φ ext for the evolution of H 2 (g) comparable to the values of Φ ext yielded by the highest-performing terraces. In conclusion, although the spatial resolution of the techniques used in this work frequently did not result in observation of the effect of edge sites on photocurrent efficiency, some edge effects were observed in the measurements; however the observed edge effects differed among edges, and did not appear to determine the performance of the electrodes.

36 MATERIALS SCIENCE↗
DOE OSTI2015

The role of the domain size and titanium dopant in nanocrystalline hematite thin films for water photolysis

In this study, we develop a novel technique for preparing high quality Ti-doped hematite thin films for photoelectrochemical (PEC) water splitting, through sputtering deposition of metallic iron films from an iron target embedded with titanium (dopants) pellets, followed by a thermal oxidation step that turns the metal films into doped hematite. It is found that the hematite domain size can be tuned from ~10 nm to over 100 nm by adjusting the sputtering atmosphere from more oxidative to mostly inert. The better crystallinity at a larger domain size ensures excellent PEC water splitting performance, leading to record high photocurrent from pure planar hematite thin films on FTO substrates. Titanium doping further enhances the PEC performance of hematite photoanodes. The photocurrent is improved by 50%, with a titanium dopant concentration as low as 0.5 atom%. It is also found that the role of the titanium dopant in improving the PEC performance is not apparently related to the films’ electrical conductivity which had been widely believed, but is more likely due to the passivation of surface defects by the titanium dopants.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2015

Vertical and lateral morphology effects on solar cell performance for a thiophene–quinoxaline copolymer:PC 70 BM blend

The distribution of electron donor and acceptor in the active layer is known to strongly influence the electrical performance of polymer solar cells for most of the high performance polymer:fullerene systems. The formulation of the solution from which the active layer is spincoated plays an important role in the quest for morphology control. We have studied how the choice of solvent and the use of small amounts of a low vapour pressure additive in the coating solution influence the film morphology and the solar cell performance for blends of poly[2,3-bis-(3-octyloxyphenyl)quinoxaline-5,8-diyl-alt-thiophene-2,5-diyl] (TQ1) and [6,6]-phenyl C 71 -butyric acid methyl ester (PC 70 BM). We have investigated the lateral morphology using atomic force microscopy (AFM) and scanning transmission X-ray microscopy (STXM), the vertical morphology using dynamic secondary ion mass spectrometry (d-SIMS) and variable-angle spectroscopic ellipsometry (VASE), and the surface composition using near-edge X-ray absorption fine structure (NEXAFS). The lateral phase-separated domains observed in films spincoated from single solvents, increase in size with increasing solvent vapour pressure and decreasing PC 70 BM solubility, but are not observed when 1-chloronaphthalene (CN) is added. A strongly TQ1-enriched surface layer is formed in all TQ1:PC 70 BM blend films and rationalized by surface energy differences. The photocurrent and power conversion efficiency strongly increased upon the addition of CN, while the leakage current decreased by one to two orders of magnitude. The higher photocurrent correlates with the finer lateral structure and stronger TQ1-enrichment at the interface with the electron-collecting electrode. This indicates that the charge transport and collection are not hindered by this polymer-enriched surface layer. Neither the open-circuit voltage nor the series resistance of the devices are sensitive to the differences in morphology.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Synthesis and characterization of (Ga 1-x Zn x )(N 1-x O x ) nanocrystals with a wide range of compositions

We describe the synthesis and characterization of wurtzite (Ga 1-x Zn x )(N 1-x O x ) nanocrystals with a wide range of compositions and a focus on properties relevant for solar fuel generation. (Ga 1-x Zn x )(N 1-x O x ), a solid solution of GaN and ZnO, is an intriguing material because it exhibits composition-dependent visible absorption even though the parent semiconductors absorb in the UV. When functionalized with co-catalysts, (Ga 1-x Zn x )(N 1-x O x ) is also capable of water splitting under visible irradiation. Here, we examine the synthesis of (Ga 1-x Zn x )(N 1-x O x ) nanocrystals to understand how they form by nitridation of ZnO and ZnGa 2 O 4 nanocrystalline precursors. We find that the ZnO precursor is critical for the formation of crystalline (Ga 1-x Zn x )(N 1-x O x ) at 650 °C, consistent with a mechanism in which wurtzite (Ga 1-x Zn x )(N 1-x O x ) nucleates topotactically on wurtzite ZnO at an interface with ZnGa 2 O 4 . Using this information, we expand the range of compositions from previously reported 0.30 ≤ x ≤ 0.87 to include the low-x and high-x ends of the range. The resulting compositions, 0.06 ≤ x ≤ 0.98, constitute the widest range of (Ga 1-x Zn x )(N 1-x O x ) compositions obtained by one synthetic method. We then examine how the band gap depends on sample composition and find a minimum of 2.25 eV at x = 0.87, corresponding to a maximum possible solar-to-H 2 power conversion efficiency of 12%. Finally, we examine the photoelectrochemical (PEC) oxidation behavior of thick films of (Ga 1-x Zn x )(N 1-x O x ) nanocrystals with x = 0.40, 0.52, and 0.87 under visible illumination. (Ga 1-x Zn x )(N 1-x O x ) nanocrystals with x = 0.40 exhibit solar PEC oxidation activity that, while too low for practical applications, is higher than that of bulk (Ga 1-x Zn x )(N 1-x O x ) of the same composition. The highest photocurrents are observed at x = 0.52, even though x = 0.87 absorbs more visible light, illustrating that the observed photocurrents are a result of an interplay of multiple parameters which remain to be elucidated. This set of characterizations provides information useful for future studies of composition-dependent PEC properties of nanoscale (Ga 1-x Zn x )(N 1-x O x ).

36 MATERIALS SCIENCE↗
DOE OSTI2016

Methylammonium lead iodide grain boundaries exhibit depth-dependent electrical properties

In this paper, the nanoscale through-film and lateral photo-response and conductivity of large-grained methylammonium lead iodide (MAPbI 3 ) thin films are studied. In perovskite solar cells (PSC), these films result in efficiencies >17%. The grain boundaries (GBs) show high resistance at the top surface of the film, and act as an impediment to photocurrent collection. However, lower resistance pathways between grains exist below the top surface of the film, indicating that there exists a depth-dependent resistance of GBs (R GB (z)). Furthermore, lateral conductivity measurements indicate that R GB (z) exhibits GB-to-GB heterogeneity. These results indicate that increased photocurrent collection along GBs is not a prerequisite for high-efficiency PSCs. Rather, better control of depth-dependent GB electrical properties, and an improvement in the homogeneity of the GB-to-GB electrical properties, must be managed to enable further improvements in PSC efficiency. Finally, these results refute the implicit assumption seen in the literature that the electrical properties of GBs, as measured at the top surface of the perovskite film, necessarily reflect the electrical properties of GBs within the thickness of the film.

14 SOLAR ENERGY↗
DOE OSTI2016

Photogeneration of Hydrogen from Water by a Robust Dye-Sensitized Photocathode

We report here on a novel photocathode with a “donor-dye-catalyst” assembly structure for water reduction. The photoelectrocatalytic performance of the photocathode under mild conditions, with a photocurrent of -56 µA/cm2 and a Faradaic yield of 53%, is superior relative to other reported photocathodes with surface attached molecular catalysts. Detailed electron transfer analyses, based on transient absorption measurements, show that the successful application of this photocathode originates mainly from the slow back electron transfer following light excitation. The results also demonstrate that addition of the long-chain assembly to the macro-mesoporous electrode surface plays a fundamental role in providing sufficient catalyst for water reduction.

catalysis, hydrogen↗
DOE OSTI2019

New aspects of improving the performance of WO 3 thin films for photoelectrochemical water splitting by tuning the ultrathin depletion region

In this paper, we explored a facile, scalable and effective method for substantially enhancing photocurrent and incident-photon-to-current efficiency of WO 3 thin-film photoanodes by a mild reduction treatment under low oxygen pressure. Experimental data from photoelectrochemical and electrochemical impedance spectroscopies have shown that such treatment can increase the charge carrier density on WO 3 photoanode surfaces resulting in improvements in hole collection efficiency and reduction in charge recombination. Despite a much thinner layer of WO 3 (about 500 nm) compared to those in other published studies, the electrodes exhibited an ultra-high photocurrent density of 1.81 mA cm –2 at 1.23 V vs . RHE. This current density is one of the highest ones among WO 3 -based photoanodes described in literature. As a result, the proposed surface modulation approach offers an effective and scalable method to prepare high-performance thin film photoanodes for photoelectrochemical water splitting.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Atomic Layer Deposition of Vanadium Oxide to Reduce Parasitic Absorption and Improve Stability in n-i-p Perovskite Solar Cells for Tandems

Two critical issues associated with semi-transparent, n-i-p perovskite solar cells for 2-terminal tandem devices are parasitic absorption and long-term instability associated with the widely used spiro-OMeTAD and MoOx hole transport and buffer layers, respectively. In this work, we present an alternative hole contact bilayer that consists of a 30 nm undoped layer of spiro-TTB in conjunction with 9 nm of air-stable vanadium oxide (VOx) deposited via atomic layer deposition. The low absorption of UV and visible light in this bilayer results in the fabrication of a semi-transparent perovskite cell with 18.9 mA cm-2 of photocurrent, a 14% increase compared to the 16.6 mA cm-2 generated in a control device with 150 nm of doped spiro-OMeTAD. The ALD VOx buffer layer shows promise as a stable alternative to MoOx; an unencapsulated Cs0.17FA0.83Pb(Br0.17I0.83)3 device with ALD VOx and ITO as the top contact maintains its efficiency following 1000 hours at 85 degrees C in a N2 environment. Lastly, we use transfer matrix modeling of the optimized perovskite stack to predict its optical performance in a monolithic tandem cell with heterojunction silicon.

14 SOLAR ENERGY↗
DOE OSTI2022

Surmounting the interband threshold limit by the hot electron excitation of multi-metallic plasmonic AgAuCu NPs for UV photodetector application

We report multi-metallic alloy NPs composed of various elemental compositions can surmount the interband threshold limit of mono-metallic NPs and thus can offer a promising route to boost up the performance limit of conventional ultraviolet photodetectors (PDs). In this work, a hybrid UV-PD configuration has been demonstrated by combining the multi-metallic plasmonic alloy NPs of AgCu, AuCu, and AgAuCu on a GaN photoactive layer in order to exploit the improved photo carrier injection by the strong hot electrons and LSPR. Among various devices, the tri-metallic AgAuCu NP PD demonstrates the highest performance with a remarkably high photocurrent of 1.47 x 10 -2 A at 1 V with fast rise (T r ) and fall (T f ) times of 170 and 700 ms with a very stable current. This leads to the superior figure-of-merit parameters of the PD with a photoresponsivity of 4.3 x 10 6 mA W-1, detectivity of 3.52 x 10 12 Jones and EQE of 1.39 x 10 6 %, which is ~16 times higher than the bare GaN PD. This ranks the AgAuCu PD as one of the best GaN based UV photodetectors. The photocurrent enhancement and excellent figure-of-merit can be attributed to the significantly increased photo carrier injection by the efficient hot electron generation via the LSPR and improved interfacial barrier characteristics by the tri-metallic elemental synergy.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Aliovalent gallium dopants remove Ti 3+ defects and improve photocatalytic and photoelectrochemical water oxidation properties of LaTiO 2 N

LaTiO 2 N is a promising semiconductor for the water splitting reaction due to its 2.1 eV band gap and stability against corrosion. However, its solar energy conversion is limited by Ti 3+ recombination defects introduced during ammonolysis. Here we show for the first time that Ti 3+ defects in LaTiO 2 N can be suppressed with incorporation of 2, 5, and 10% aliovalent gallium (Ga 3+ ) dopants during synthesis via the layered La 2 Ti 2 O 7 intermediate. Electron paramagnetic resonance (EPR) spectroscopy on the solid powders confirms a reduction in the Ti 3+ donor density from 2.97 × 10 17 cm −3 for the non-doped material to ∼6.24 × 10 16 cm −3 for 5% Ga-doped LaTiO 2 N. The remaining Ti 3+ defects are concentrated near the LaTiO 2 N surface, according to X-ray photoelectron spectroscopy. The defect reduction shifts the optical absorption edge from 2.02 to 2.09 eV and eliminates a broad absorption band at 1050 nm from the optical absorption spectra. It also removes a 1.0–1.7 eV sub-band gap photovoltage signal from surface photovoltage spectra. This suggests that empty Ti 3+ d-orbitals are located 1.0–1.7 eV above the LaTiO 2 N valence band edge. Removing these recombination states with increasing Ga 3+ content enhances the photoconversion efficiency of LaTiO 2 N during water oxidation. The optimized 2 wt% CoO x -loaded 5% Ga-doped LaTi O2 N material has a 16% AQE (400 nm) for O 2 production from aqueous silver nitrate solution and a ∼2.1 mA cm −2 water oxidation photocurrent at 1.23 V under 100 mW cm −2 Xe arc lamp illumination. The water oxidation photocurrent is stable during a 50 min test, and the Faraday efficiency for O 2 generation is 97%, confirming short-term corrosion stability of LaTiO 2 N. Altogether, these results provide a better understanding of the distribution, concentration, and impact of Ti 3+ defects on the optical, photovoltage, and photoelectrochemical properties of LaTiO 2 N. In combination with other defect control strategies, aliovalent Ga 3+ doping can help bring the solar energy conversion efficiency of LaTiO 2 N closer to the theoretical limit.

Wang, Li [University of California, Davis, CA (Uni↗
DOE OSTI2011

Optimization on photoelectric detection based on stacked La{sub 0.9}Sr{sub 0.1}MnO{sub 3-{delta}}/LaAlO{sub 3-{delta}} multijunctions

Three multijunctions consisting of La{sub 0.9}Sr{sub 0.1}MnO{sub 3-{delta}} and LaAlO{sub 3-{delta}} on Si substrate have been fabricated under different oxygen pressures by laser molecular beam epitaxy. They exhibit nonlinear and rectifying current-voltage characteristics and evident photocurrent response to He-Ne laser illumination. Experimental results indicate that the periodically stacked multijunction grown under lower oxygen pressure shows a better rectification behavior and a higher photocurrent. The photovoltaic responsivities of the multijunctions are enhanced greatly at reverse bias and are much higher than that of a similarly grown single p-n junction. Based on the band structure of the multilayers, a possible mechanism of the photovoltaic process was proposed. A high photovoltage responsivity of 168.6 mV/mW has been achieved at - 6 V bias; this demonstrates the potential of the present multijunction configuration for photodetectors operating at room temperature.

36 MATERIALS SCIENCE↗
DOE OSTI2012

Holographic modification of TiO{sub 2} nanostructure for enhanced charge transport in dye-sensitized solar cell

We show that the photocurrent and energy conversion efficiency of dye-sensitized solar cells can be greatly enhanced with holographic modification to the morphology of TiO{sub 2} electrode. The nanoporous electrode coated onto conducting glass was irradiated by three interfering laser beams at 1064 nm incident from the backside of the substrate. This generated two-dimensional periodic pillars of higher density in the electrode, through which the photoexcited electrons could be extracted more effectively. The cells fabricated with modified electrodes exhibited average photocurrent and efficiency of 17.14 mA/cm{sup 2} and 9.03%, while 14.91 mA/cm{sup 2} and 7.83% were obtained from the reference cells. It was attributed to the enhanced charge transport accompanied by the reduction of internal resistance of the electrode.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2014

Influence of surface plasmon resonances of silver nanoparticles on optical and electrical properties of textured silicon solar cell

Here, we report average reflectance reduction of ∼8% in wavelength range of 300–1100 nm after coupling surface plasmon resonances (SPRs) of silver nanoparticles (NPs) to textured silicon (T-Si) surface. The enhancement of photocurrent from T-Si solar cell in off-resonant SPR region observed due to better radiative efficiency of NPs leading to outflow of scattered far-field into silicon maximized power generating electrons. Improvement in series resistance, fill factor, and open-circuit voltage (insensitive NPs size and morphology) are also observed with NPs along with photocurrent enhancement (sensitive to NPs sizes), which resulted cell efficiency enhancement from 4.49% to 6.42% for large area of 12.24 cm{sup 2}.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

GaAs/AlGaAs quantum wells with indirect-gap AlGaAs barriers for solar cell applications

We have fabricated GaAs/AlGaAs quantum well (QW) solar cells in which 3 nm-thick QWs and indirect-gap Al{sub 0.78}Ga{sub 0.22}As barriers are embedded, and we studied extraction processes of photogenerated carriers in this QW system. The photocurrent under 700 nm light illumination at voltages close to the open-circuit voltage shows only a small reduction, indicating that the carrier recombination inside QWs is largely suppressed. We attribute this result to an efficient extraction of electrons from the QWs through the X-valley of AlGaAs. The insertion of QWs is shown to be effective in extending the absorption wavelengths and in enhancing the photocurrent. The use of indirect-gap materials as barriers is found to enhance carrier extraction processes, and result in an improved performance of QW solar cells.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗