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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Ti3+-TiO2/Ce3+-CeO2 Nanosheet heterojunctions as efficient visible-light-driven photocatalysts

Highlights: • A novel Ti{sup 3+}-TiO{sub 2}/Ce{sup 3+}-CeO{sub 2} nanosheet heterojunction is fabricated. • It owns the bandgap of 2.6 eV and extends the photoresponse to visible light region. • It exhibits excellent visible-light-driven photocatalytic performance. • It is due to synergy of Ti{sup 3+}, Ce{sup 3+} co-doping and nanosheet heterojunction. - Abstract: Novel Ti{sup 3+}-TiO{sub 2}/Ce{sup 3+}-CeO{sub 2} nanosheet heterojunctions are successfully prepared via a facile hydrothermal approach combined with a wet-chemical deposition precipitation and an in situ solid-state chemical reduction strategy. The structures of the as-prepared samples are characterized in detail by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, atomic force microscopy, X-ray photoelectron spectroscopy and UV–vis diffuse reflectance spectroscopy. The results show that Ti{sup 3+} and Ce{sup 3+} are both doped into the lattice of TiO{sub 2} and CeO{sub 2}, respectively, which narrow the band gap to 2.7 eV and extend the photoresponse to visible light region. The photocatalytic degradation rate of methyl orange and methylene blue are as high as 93.3% and 97.1% under visible-light illumination, respectively. The high degradation rate is attributed to the efficient doping of Ti{sup 3+} and Ce{sup 3+}, formation of surface oxygen vacancy and heterojunction, which favors the absorption of visible light and separation of photogenerated charge carriers.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2014

A design of Si-based nanoplasmonic structure as an antenna and reception amplifier for visible light communication

Visible light communication has been widely investigated due to its larger bandwidth and higher bit rate, and it can combine with the indoor illumination system that makes it more convenient to carry out. Receiving and processing the visible light signal on chip request for nanophotonics devices performing well. However, conventional optical device cannot be used for light-on-chip integration at subwavelength dimensions due to the diffraction limit. Herein, we propose a design of Si-based nanoplasmonic structure as an antenna and reception amplifier for visible light communication based on the interaction between Si nanoparticle and Au nanorod. This device integrates the unique scattering property of high-refractive index dielectric Si nanoparticles, whose scattering spectrum is dependent on the particle size, with the localized surface plasmon resonance of Au nanorod. We calculated the spectra collected by plane detector and near field distribution of nanostructure, and theoretically demonstrate that the proposed device can act as good receiver, amplifier and superlens during the visible light signal receiving and processing. Besides, unlike some other designs of nanoantenna devices focused less on how to detect the signals, our hybrid nanoantenna can realize the transfer between the scattering source and the detector effectively by Au nanorod waveguides. These findings suggest that the designed nanoplasmonic structure is expected to be used in on-chip nanophotonics as antenna, spectral splitter and demultiplexer for visible light communication.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2018

In Situ UV-Visible Assessment of Iron-Based High-Temperature Water-Gas Shift Catalysts Promoted with Lanthana: An Extent of Reduction Study

Here, the extent of reduction of unsupported iron-based high-temperature water-gas shift catalysts with small (<5 wt %) lanthana contents was studied using UV-visible spectroscopy. Temperature- programmed reduction measurements showed that lanthana content higher than 0.5 wt % increased the extent of reduction to metallic Fe, while 0.5 wt % of lanthana facilitated the reduction to Fe 3 O 4 . In situ measurements on the iron oxide catalysts using mass and UV-visible spectroscopies permitted the quantification of the extent of reduction under temperature-programmed reduction and high-temperature water-gas shift conditions. The oxidation states were successfully calibrated against normalized absorbance spectra of visible light using the Kubelka-Munk theory. The normalized absorbance relative to the fully oxidized Fe 2 O 3 increased as the extent of reduction increased. XANES suggested that the average bulk iron oxidation state during the water-gas shift reaction was Fe +2.57 for the catalyst with no lanthana and Fe +2.54 for the catalysts with 1 wt % lanthana. However, the UV-vis spectra suggest that the surface oxidation state of iron would be Fe +2.31 for the catalyst with 1 wt % lanthana if the oxidation state of iron in the catalyst with 0 wt % lanthana were Fe +2.57 . The findings of this paper emphasize the importance of surface sensitive UV-visible spectroscopy for determining the extent of catalyst reduction during operation. Furthermore, the paper highlights the potential to use bench-scale UV-visible spectroscopy to study the surface chemistry of catalysts instead of less-available synchrotron X-ray radiation facilities.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Crystallization of electrically conductive visibly transparent ITO thin films by wavelength-range-specific pulsed Xe arc lamp annealing

Here, the transparent electric conductors made of indium tin oxide (ITO)-doped glass prepared by a flash lamp annealing (FLA) process were compared with ITO-doped glass prepared via a conventional rapid thermal annealing (RTA) process. Stylus surface profilometry was used to determine thicknesses, scanning electron microscopy was used to image surfaces, X-ray diffraction was used to determine film structures, X-ray photoelectron spectroscopy was used to determine oxidation states and film compositions, 4-point probe measurements were used to determine electrical conductivities, UV–Vis spectroscopy was used to determine film transparencies, and selective light filtering was used to determine which wavelengths of light are needed to anneal ITO into a visibly transparent electrically conductive thin film via an FLA process. The results showed that FLA with visible light can be used to nearly instantaneously anneal ITO to create visibly transparent and electrically conductive ITO thin films on glass. The FLA process achieved this by predominately exciting unoxidized indium, unoxidized tin, tin monoxide (SnO), and non-stoichiometric indium oxide (InO x ), appropriately distributed in an electron beam physical vapor-deposited amorphous ITO thin film, to allow their oxidation and crystallization into an electrically conductive visibly transparent ITO. Though it is possible to prepare ITO-doped glass that is more transparent with an RTA process, the FLA process is significantly faster, has comparable electrical conductivity, and can strongly localize heating to areas of the as-deposited ITO thin film that are not electrically conductive and visibly transparent.

36 MATERIALS SCIENCE↗
DOE OSTI2011

Visible light responsive iodine-doped TiO 2 for photocatalytic reduction of CO 2 to fuels

Iodine-doped titanium oxide (I-TiO 2 ) nanoparticles that are photocatalitically responsive to visible light illumination have been synthesized by hydrothermal method. The structure and properties of I-TiO 2 nanocrystals prepared with different iodine doping levels and/or calcination temperatures were characterized by X-ray diffraction, transmission electron microscopy and diffraction, X-ray photoelectron spectroscopy, and UV-vis diffuse reflectance spectra. The three nominal iodine dopant levels (5, 10, 15 wt.%) and the two lower calcination temperatures (375, 450°C) produced mixture of anatase and brookite nanocrystals, with small fraction of rutile found at 550°C. The anatase phase of TiO 2 increased in volume fraction with increased calcination temperature and iodine levels. The photocatalytic activities of the I-TiO 2 powders were investigated by photocatalytic reduction of CO 2 with H 2 O under visible light (λ > 400 nm) and also under UV-vis illumination. CO was found to be the major photoreduction product using both undoped and doped TiO 2 . A high CO 2 reduction activity was observed for I-TiO 2 catalysts (highest CO yield equivalent to 2.4 micro mol g -1 h -1 ) under visible light, and they also had much higher CO 2 photoreduction efficiency than undoped TiO 2 under UV-vis irradiation. I-TiO 2 calcined at 375°C has superior activity to those calcined at higher temperatures. Optimal doping levels of iodine were identified under visible and UV-vis irradiations, respectively. This is the first study that investigates nonmetal doped TiO 2 without other co-catalysts for CO 2 photoreduction to fuels under visible light.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2013

Copper(II) imidazolate frameworks as highly efficient photocatalysts for reduction of CO{sub 2} into methanol under visible light irradiation

Three copper(II) imidazolate frameworks were synthesized by a hydrothermal (or precipitation) reaction. The catalysts were characterized by X-ray diffraction (XRD), nitrogen adsorption, transmission electron microscopy (TEM), ultraviolet–visible spectroscopy (UV–vis), Fourier transform infrared spectra (FTIR), thermogravimetry (TG). Meanwhile, the photocatalytic activities of the samples for reduction of CO{sub 2} into methanol and degradation of methylene blue (MB) under visible light irradiation were also investigated. The results show that the as-prepared samples exhibit better photocatalytic activities for the reduction of carbon dioxide into methanol with water and degradation of MB under visible light irradiation. The orthorhombic copper(II) imidazolate frameworks with a band gap of 2.49 eV and green (G) color has the best photocatalytic activity for reduction of CO{sub 2} into methanol, 1712.7 μmol/g over 5 h, which is about three times as large as that of monoclinic copper(II) imidazolate frameworks with a band gap 2.70 eV and blue (J) color. The degradation kinetics of MB over three photocatalysts fitted well to the apparent first-order rate equation and the apparent rate constants for the degradation of MB over G, J and P (with pink color) are 0.0038, 0.0013 and 0.0016 min{sup −1}, respectively. The synergistic effects of smallest band gap and orthorhombic crystal phase structure are the critical factors for the better photocatalytic activities of G. Moreover, three frameworks can also be stable up to 250 °C. The investigation of Cu-based zeolitic imidazolate frameworks maybe provide a design strategy for a new class of photocatalysts applied in degradation of contaminations, reduction of CO{sub 2}, and even water splitting into hydrogen and oxygen under visible light. - Graphical abstract: Carbon dioxide was reduced into methanol with water over copper(II) imidazolate frameworks under visible light irradiation. - Highlights: • Three copper(II) imidazolate frameworks were first applied in the photo-reduction of CO{sub 2}. • The photocatalytic activities of the frameworks depend on their band gap and phase structures. • The photocatalytic activity of orthorhombic frameworks is 3 times that of monoclinic frameworks. • The degradation kinetics of MB over three photocatalysts followed the first-order rate equation. • The largest yield for reduction of CO{sub 2} into methanol on green framworks was 1712.7 μmol/g over 5 h.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Investigation of the photoactivity of pristine and mixed phase N-doped titania under visible and solar irradiation

Nitrogen doped titania nano-particles were synthesized by sol–gel method with an aim to investigate the impact of doping in titanium matrix and the titania phases on their photocatalytic activity under visible and solar irradiation. The structural, optical and chemical characterization of the prepared materials were done using X-ray diffraction analysis, scanning electron microscopy, UV–visible diffuse reflectance spectroscopy, photoluminescence spectroscopy, and Fourier transform infrared spectroscopy. The samples were calcined at different temperatures (200 °C–600 °C) to obtain different phases. All the samples showed red-shift in the visible region attributable to the doping of nitrogen in the titania matrix. The samples calcined at low temperatures showed high photocatalytic activity compared to the high temperature samples. The enhancement in the visible light activity may be attributed to the large amount of nitrogen present in the surface region of the catalyst and reduced carrier recombination. Among the high temperature samples the high activity may be due to the presence of mixed phase as well. - Highlights: • Pristine and mixed phases of N doped titania synthesized at different temperatures. • High visible light photoactivity exhibited by pristine rutile phase and mixed phase. • Role of surface N in rutile and matrix embedded N in other samples corroborated.

36 MATERIALS SCIENCE↗
DOE OSTI2011

Preparation and characterization of ZnO-TiO{sub 2} nanocomposite for photocatalytic disinfection of bacteria and detoxification of cyanide under visible light

Highlights: {yields} ZnO-TiO{sub 2} nanocomposite, obtained by modified ammonia-evaporation-induced synthetic method, absorbs visible light. {yields} ZnO-TiO{sub 2} nanoparticles catalyze bacteria disinfection and cyanide detoxification under sunlight. {yields} ZnO-TiO{sub 2} nanocomposite is selective in photocatalysis. -- Abstract: ZnO-TiO{sub 2} nanocomposite was prepared by modified ammonia-evaporation-induced synthetic method. It was characterized by powder X-ray diffraction, transmission electron microscopy, selected area electron diffraction, and energy dispersive X-ray, UV-visible diffuse reflectance, photoluminescence and electrochemical impedance spectroscopies. Incorporation of ZnO leads to visible light absorption, larger charge transfer resistance and lower capacitance. The nanocomposite effectively catalyzes the inactivation of E. coli under visible light. Further, the prepared nanocomposite displays selective photocatalysis. While its photocatalytic efficiency to detoxify cyanide with visible light is higher than that of TiO{sub 2} P25, its efficiency to degrade methylene blue, sunset yellow and rhodamine B dyes under UV-A light is less than that of TiO{sub 2} P25.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2012

Effects of aluminum substitution on photocatalytic property of BiVO{sub 4} under visible light irradiation

Graphical abstract: Visible-light-driven Al/BiVO{sub 4} photocatalyst was prepared by a hydrothermal process. After introducing Al, the BiVO{sub 4} particles retain monoclinic scheelite structures and the ability of visible light absorption is enhanced. XPS and FTIR results reveal that the Al ions influence the local structure of the BiVO{sub 4}. The photocatalytic experiments demonstrate that the Al species incorporation can effectively enhance the photocatalytic activity of BiVO{sub 4} due to the existence of distorted VO{sub 4}{sup 3-} tetrahedron and the stronger optical absorption intensity. Highlights: Black-Right-Pointing-Pointer The visible-light-driven Al/BiVO{sub 4} photocatalysts are first prepared in our study. Black-Right-Pointing-Pointer It is found that Al is introduced into the BiVO{sub 4} lattice successfully. Black-Right-Pointing-Pointer The Al-doped BiVO{sub 4} shows a far higher photocatalytic activity than undoped BiVO{sub 4}. Black-Right-Pointing-Pointer One of the reason for the higher activity is the distorted VO{sub 4}{sup 3-} tetrahedron. Black-Right-Pointing-Pointer Another reason for the higher activity is the strong optical absorption intensity. -- Abstract: Novel visible-light-driven Al/BiVO{sub 4} photocatalysts were synthesized via a facile hydrothermal method for the first time. The samples were characterized by X-ray diffraction, N{sub 2}-sorption, UV-vis diffuse reflectance spectra, scanning electron microscopy, high-resolution transmission electron microscopy, Fourier transformed infrared spectra and X-ray photoelectron spectroscopy. The photocatalytic activity of the samples was evaluated by the decomposition of methylene blue under visible light irradiation (400 nm < {lambda} <580 nm) and was compared with that of single-phase BiVO{sub 4}. The results revealed that the introduction of Al can improve photocatalytic performance greatly and different concentration of Al resulted in different photocatalytic activity. The highest activity is obtained by the sample with a doping concentration of 12 at%. The reason for the enhanced photocatalytic activities of Al/BiVO{sub 4} samples was also discussed in this paper.

36 MATERIALS SCIENCE↗
DOE OSTI2012

One-step synthesis of Fe–N–S-tri-doped TiO{sub 2} catalyst and its enhanced visible light photocatalytic activity

Graphical abstract: FeNS-TiO{sub 2} exhibits stronger SPS response than that of pure TiO{sub 2}, indicating that the FeNS-TiO{sub 2} should have a higher separation rates of photoinduced charge carriers. Further, for the sample FeNS-TiO{sub 2} a broad shoulder SPS response can be seen at the wavelength range from 390 to 550 nm, suggesting that the light absorption in visible region of FeNS-TiO{sub 2} was greatly improved, which is beneficial to the enhancement of photocatalytic activity. Display Omitted Highlights: ► FeNS-TiO{sub 2} catalyst has been synthesized in the presence of ammonium ferrous sulfate. ► The light absorption edge of FeNS-TiO{sub 2} catalyst was red-shifted to visible region. ► The separation efficiency of photoinduced charge carriers of FeNS-TiO{sub 2} was improved. ► The activity enhanced mechanism of FeNS-TiO{sub 2} was discussed in detail. -- Abstract: Fe–N–S-tridoped TiO{sub 2} was synthesized through simple one step sol–gel reactions in the presence of ammonium ferrous sulfate. The resulting materials were characterized by X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, diffuse reflectance spectrum and surface photovoltage spectroscopy. Results revealed that Fe and S were incorporated into the lattice of TiO{sub 2} by substituting for some Ti atoms and N for O atoms in the lattice of TiO{sub 2}. Tri-doping with Fe, N and S could inhibit the phase transformation of TiO{sub 2} from anatase to rutile, restrain the growth of crystallite sizes, extended the light absorption into the visible region and separate photoinduced charge carriers. The visible photocatalytic activity of Fe–N–S-tridoped TiO{sub 2} was higher than that of N-TiO{sub 2} and P25 TiO{sub 2}. The enhanced photocatalytic activity was attributed to the small crystallite size, high crystallinity, the intense light absorption in visible region, narrow band gap and high separation efficiency of photoinduced charge carriers.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Preparation, characterization and enhanced visible-light photocatalytic activities of BiPO{sub 4}/BiVO{sub 4} composites

Graphical abstract: - Highlights: • BiPO{sub 4}/BiVO{sub 4} composites were successfully prepared by the hydrothermal method. • BiPO{sub 4}/BiVO{sub 4} composites exhibited broad absorption in the visible region. • Visible-light photocatalytic activities of BiPO{sub 4}/BiVO{sub 4} composites were enhanced. • P/V molar ratio and pH value of the reaction affect photocatalytic activity. • The mechanism of enhanced visible-light photocatalytic activities was discussed. - Abstract: BiPO{sub 4}/BiVO{sub 4} composites with different P/V molar ratios were prepared by the hydrothermal method and the effect of pH values of hydrothermal reaction on photocatalytic activity of BiPO{sub 4}/BiVO{sub 4} composite was investigated. The photocatalysts were characterized by X-ray diffraction, field emission scanning electron microscopy, energy-dispersive spectroscopy, X-ray photoelectron spectroscopy and UV–vis diffuse reflectance spectroscopy. The photocatalytic property of BiPO{sub 4}/BiVO{sub 4} was evaluated by photocatalytic degradation of Methylene blue under visible light irradiation. The results showed that the photocatalytic activity of the composites was much higher than that of pure BiPO{sub 4} and BiVO{sub 4}. The rate constant of Methylene blue degradation over BiPO{sub 4}/BiVO{sub 4} (P/V molar ratio of 5:1 and hydrothermal reaction pH value of 1.5) is 1.7 times that of pure BiVO{sub 4}. The photocatalytic activity enhancement of BiPO{sub 4}/BiVO{sub 4} composite is closely related to the BiVO{sub 4} functioning as a sensitizer to adsorb visible light and the heterojunction of BiPO{sub 4}/BiVO{sub 4} acting as an active center for hindering the rapid recombination of electron–hole pairs during the photocatalytic reaction.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Visible light activated photocatalytic behaviour of rare earth modified commercial TiO{sub 2}

Highlights: • RE gave more surface hydroxyl groups attached to the photocatalyst's surface. • RE gave the modified and fired samples a high specific surface area. • Photocatalytic activity was assessed in gas–solid phase under visible-light exposure. • Thermal treated RE-TiO{sub 2}s showed a superior visible-light photocatalytic activity. • La-TiO{sub 2} was the best performing photocatalyst. - Abstract: A commercial TiO{sub 2} nanopowder, Degussa P25, was modified with several rare earth (RE) elements in order to extend its photocatalytic activity into the visible range. The mixtures were prepared via solid-state reaction of the precursor oxides, and thermally treated at high temperature (900 and 1000 °C), with the aim of investigating the photocatalytic activity of the thermally treated samples. This thermal treatment was chosen for a prospective application as a surface layer in materials that need to be processed at high temperatures. The photocatalytic activity (PCA) of the samples was assessed in gas–solid phase – monitoring the degradation of isopropanol (IPA) – under visible-light irradiation. Results showed that the addition of the REs lanthanum, europium and yttrium to TiO{sub 2} greatly improved its photocatalytic activity, despite the thermal treatment, because of the presence of more surface hydroxyl groups attached to the photocatalyst's surface, together with a higher specific surface area (SSA) of the modified and thermally treated samples, with regard to the unmodified and thermally treated Degussa P25. The samples doped with La, Eu and Y all had excellent PCA under visible-light irradiation, even higher than the untreated Degussa P25 reference sample, despite their thermal treatment at 900 °C, with lanthanum producing the best results (i.e. the La-, Eu- and Y-TiO{sub 2} samples, thermally treated at 900 °C, had, respectively, a PCA equal to 26, 27 and 18 ppm h{sup −1} – in terms of acetone formation – versus 15 ppm h{sup −1} for the 900 °C thermally treated Degussa P25). On the other hand, Ce–TiO{sub 2}s had no significant photocatalytic activity.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Indium oxide thin film as potential photoanodes for corrosion protection of stainless steel under visible light

Graphical abstract: If the conduction band potential of In{sub 2}O{sub 3} is more negative than the corrosion potential of stainless steel, photo-induced electrons will be transferred from In{sub 2}O{sub 3} to the steel, thus shifting the potential of the steel into a corrosion immunity region and preventing the steel from the corrosion. - Highlights: • Indium oxide performed novel application under visible light. • Indium oxide by sol–gel method behaved better photoelectrochemical properties. • Electrons were transferred to stainless steel from indium oxide once light on. - Abstract: This paper reports the photoelectrochemical cathodic protection of 304 stainless steel by In{sub 2}O{sub 3} thin-film under visible-light. The films were fabricated with In{sub 2}O{sub 3} powders, synthesized by both sol–gel (In{sub 2}O{sub 3}-sg) and solid-state (In{sub 2}O{sub 3}-ss) processes. The photo-induced open circuit potential and the photo-to-current efficiency measurements suggested that In{sub 2}O{sub 3} could be a promising candidate material for photoelectrochemical cathodic protection of metallic alloys under visible light. Moreover, the polarization curve experimental results indicated that In{sub 2}O{sub 3}-sg thin-film can mitigate the corrosion potential of 304 stainless steel to much more negative values with a higher photocurrent density than the In{sub 2}O{sub 3}-ss film under visible-light illumination. All the results demonstrated that the In{sub 2}O{sub 3}-sg thin-film provides a better photoelectrochemical cathodic protection for 304 stainless steel than In{sub 2}O{sub 3}-ss thin-film under visible-light illumination. The higher photoelectrochemical efficiency is possibly due to the uniform thin films produced with the smaller particle size of In{sub 2}O{sub 3}-sg, which facilitates the transfer of the photo-induced electrons from bulk to the surface and suppresses the charge recombination of the electrons and holes.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Future Fire Impacts on Smoke Concentrations, Visibility, and Health in the Contiguous United States

Fine particulate matter (PM2.5) from U.S. anthropogenic sources is decreasing. However, previous studies have predicted that PM2.5 emissions from wildfires will increase in the midcentury to next century, potentially offsetting improvements gained by continued reductions in anthropogenic emissions. Therefore, some regions could experience worse air quality, degraded visibility, and increases in population-level exposure. We use global climate model simulations to estimate the impacts of changing fire emissions on air quality, visibility, and premature deaths in the middle and late 21st century. We find that PM2.5 concentrations will decrease overall in the contiguous United States (CONUS) due to decreasing anthropogenic emissions (total PM2.5 decreases by 3% in Representative Concentration Pathway [RCP] 8.5 and 34% in RCP4.5 by 2100), but increasing fire-related PM2.5 (fire-related PM2.5 increases by 55% in RCP4.5 and 190% in RCP8.5 by 2100) offsets these benefits and causes increases in total PM2.5 in some regions. We predict that the average visibility will improve across the CONUS, but fire-related PM2.5 will reduce visibility on the worst days in western and southeastern U.S. regions. We estimate that the number of deaths attributable to total PM2.5 will decrease in both the RCP4.5 and RCP8.5 scenarios (from 6% to 4–5%), but the absolute number of premature deaths attributable to fire-related PM2.5 will double compared to early 21st century. We provide the first estimates of future smoke health and visibility impacts using a prognostic land-fire model. Our results suggest the importance of using realistic fire emissions in future air quality projections.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2013

Cationic (V, Y)-codoped TiO{sub 2} with enhanced visible light induced photocatalytic activity: A combined experimental and theoretical study

To employ TiO{sub 2} as an efficient photocatalyst, high reactivity under visible light and improved separation of photoexcited carriers are required. An effective co-doping approach is applied to modify the photocatalytic properties of TiO{sub 2} by doping vanadium (transition metal) and yttrium (rare earth element). V and/or Y codoped TiO{sub 2} was prepared using hydrothermal method without any post calcination for crystallization. Based on density functional theory, compensated and noncompensated V, Y codoped TiO{sub 2} models were constructed and their structural, electronic, and optical properties were calculated. Through combined experimental characterization and theoretical modeling, V, Y codoped TiO{sub 2} exhibited high absorption coefficient with enhanced visible light absorption. All the prepared samples showed pure anatase phase and spherical morphology with uniform particle distribution. Electronic band structure demonstrates that V, Y codoping drastically reduced the band gap of TiO{sub 2}. It is found that both the doped V and Y exist in the form of substitutional point defects replacing Ti atom in the lattice. The photocatalytic activity, evaluated by the degradation of methyl orange, displays that the codoped TiO{sub 2} sample exhibits enhanced visible light photocatalytic activity. The synergistic effects of V and Y drastically improved the Brunauer-Emmett-Teller specific surface area, visible light absorption, and electron-hole pair's separation leading to the enhanced visible light catalytic activity.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Ultraviolet-visible optical isolators based on CeF{sub 3} Faraday rotator

The first ultraviolet (UV) and visible optical isolators based on CeF{sub 3} are demonstrated. CeF{sub 3} possesses unique properties as Faraday rotator for the UV-visible wavelength region: a wide transparency range (wavelength of >300 nm) and an outstanding Verdet constant. In contrast, currently used terbium-gallium garnets and magneto-optical glasses possess a low transparency in the visible and a small Verdet constant in the UV, respectively. The optical isolator prototypes consist of a CeF{sub 3} rod, a single ring magnet, and a couple of beam splitters. The ring magnets have been designed to guarantee a homogeneous magnetic field; for it, numerical simulations have been carried out. The two prototypes are very compact and operate in the UV at 355 and in the visible at 405 nm, respectively. The performance of these devices indicates the high potential of CeF{sub 3} as a new UV-visible Faraday rotator, specially for shorter wavelengths where at present there are no optical isolators available.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Visible-blind ultraviolet photodiode fabricated by UV oxidation of metallic zinc on p-Si

A UV photodiode fabricated by the UV oxidation of a metallic zinc thin film on p-Si has manifested unique photoresponse characteristics. The electron concentration found by the Hall measurement was 3 × 10{sup 16 }cm{sup −3}, and such a low electron concentration resulted in a low visible photoluminescence. UV illumination enhances the oxidation at low temperatures and decreases the concentration of the oxygen vacancies. The I-V characteristic showed a good rectification with a four-order magnitude difference in the forward and reverse currents at 2 V, and its linear and frequency independent C{sup −2}–V characteristic confirmed an abrupt pn junction. The photoresponse showed a visible blindness with a responsivity ratio of UV and visible light as high as 100. Such a visible-blind photoresponse was attributed to the optimum thickness of the SiO{sub 2} formed on the Si surface during the UV oxidation at 400 °C. A lower potential barrier to holes at the ZnO/SiO{sub 2} interface facilitates Fowler-Nordheim tunneling of the photo-generated holes during the UV illumination, while a higher potential barrier to electrons efficiently blocks transport of the photo-generated electrons to the ZnO during the visible light illumination. The presence of oxide resulted in a slow photoresponse to the turn-on and off of the UV light. A detailed analysis is presented to understand how the photo-generated carriers contribute step by step to the photocurrent. In addition to the slow photoresponse associated with the SiO{sub 2} interfacial layer, the decay of the photocurrent was found extremely slow after turn-off of the UV light. Such a slow decay of the photocurrent is referred to as a persistent photoconductivity, which is caused by metastable deep levels. It is hypothesized that Zn vacancies form such a deep level, and that the photo-generated electrons need to overcome a thermal-energy barrier for capture. The ZnO film by the UV oxidation at 400 °C was found to be rich in oxygen and deficient in zinc.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Temporal light modulation: A phantom array visibility measure

At temporal light modulation (TLM) frequencies between 80 Hz and 20 000 Hz observers may perceive a series of repeated images called the phantom array effect (PAE) when they move their eyes in large saccades across a modulating light source or across a scene lit by the modulating light source. To date, there is no well-established measure for quantifying PAE visibility, but there is growing awareness of the need for one among design professionals and sensitive populations. This paper documents a new measure, the phantom array visibility measure (PAVM), which is based on the results of recent human factors experiments. The measure follows the mathematical underpinning used by the flicker visibility measure and the stroboscopic visibility measure, where the time-domain TLM waveform is converted into its Fourier frequency components; each component is evaluated through a threshold curve of modulation depth, then summed through an equation employing a Minkowski exponent. This scales the PAVM so that a value of 1 indicates a waveform at a threshold visibility in the conditions of the underlying experiment.

Tan, J.↗