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At least 451 records · Page 25

Optical nonlinear absorption characteristics of Sb{sub 2}Se{sub 3} nanoparticles

In this work, we report for the first time, the nonlinear optical absorption properties of antimony selenide (Sb{sub 2}Se{sub 3}) nanoparticles synthesized through solvothermal route. X-ray diffraction results revealed the crystalline nature of the nanoparticles. Electron microscopy studies revealed that the nanoparticles are in the range of 10 - 40 nm. Elemental analysis was performed using EDAX. By employing open aperture z-scan technique, we have evaluated the effective two-photon absorption coefficient of Sb{sub 2}Se{sub 3} nanoparticles to be 5e-10 m/W at 532 nm. These nanoparticles exhibit strong intensity dependent nonlinear optical absorption and hence could be considered to have optical power limiting applications in the visible range.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

A study of polaritonic transparency in couplers made from excitonic materials

We have studied light matter interaction in quantum dot and exciton-polaritonic coupler hybrid systems. The coupler is made by embedding two slabs of an excitonic material (CdS) into a host excitonic material (ZnO). An ensemble of non-interacting quantum dots is doped in the coupler. The bound exciton polariton states are calculated in the coupler using the transfer matrix method in the presence of the coupling between the external light (photons) and excitons. These bound exciton-polaritons interact with the excitons present in the quantum dots and the coupler is acting as a reservoir. The Schrödinger equation method has been used to calculate the absorption coefficient in quantum dots. It is found that when the distance between two slabs (CdS) is greater than decay length of evanescent waves the absorption spectrum has two peaks and one minimum. The minimum corresponds to a transparent state in the system. However, when the distance between the slabs is smaller than the decay length of evanescent waves, the absorption spectra has three peaks and two transparent states. In other words, one transparent state can be switched to two transparent states when the distance between the two layers is modified. This could be achieved by applying stress and strain fields. It is also found that transparent states can be switched on and off by applying an external control laser field.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Spray pyrolysis deposition of Cu-ZnO and Zn-SnO{sub 2} solar cells

Large-gap metal oxides, such as titanium, tin, and zinc oxides, have attracted great interest because of their remarkable potential in dye-sensitized solar cells (DSSC) and their low cost and simple preparation procedure. In this work, we investigated several Zn-SnO{sub 2} and Cu-ZnO thin films that were sprayed under different experimental conditions. We varied [Zn/[Sn] and [Cu/[Zn] ratios, calculated on atomic percent in the starting solution. We report some structural results of the films using X-ray diffraction. Optical reflection and transmission spectra investigated by an UV/VIS/NIR spectrophotometer permit the determination of optical constants. The direct band gap was deduced from the photon energy dependence of the absorption coefficient.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Extinction of Laser Light Due to Arctic Haze Final Campaign Report

Recent changes in emission patterns may have altered the historical stability of light attenuation strengths within the Arctic and, more specifically, the polar dome. While there have been decades of past and ongoing research on how atmospheric constituents, such as aerosols, affect light absorption, the bulk of this work is focused on the visible region. In recent years, there has been renewed interest in understanding laser light propagation at wavelengths such as 1 and 2 µm in this area. There is a need to evaluate how specific environmental parameters affect the propagation of light in this wavelength region, in particular: the extinction, scattering, and absorption coefficients, and how they relate to particle concentration; cn 2 and refractive index variations. Seasonally dependent variations in particle concentrations and compositions introduce different absorption and scattering characteristics that, in conjunction with varying temperatures, index-of-refraction variations, and wind, can result in laser beam focus and irradiance degradation. Understanding the fundamental influence of these parameters with respect to the propagation of light across a wide spectral band could lead to new insights about the minimal required datastreams required to provide accurate light propagation forecasting.

54 ENVIRONMENTAL SCIENCES↗

Bio-Optical Properties and Ocean Color Algorithms for Coastal Waters Influenced by the Mississippi River During a Cold Front Passage

During the passage of a cold front in March 2002, bio-optical properties examined in coastal waters impacted by the Mississippi River indicated westward advective flows and increasing river discharge containing a larger nonalgal particle content contributed significantly to surface optical variability. A comparison of seasonal data from three cruises indicated spectral models of absorption and scattering to be generally consistent with other coastal environments, while their parameterization in terms of chlorophyll a concentration (Chl) showed seasonal variability. The exponential slope of the colored dissolved organic matter (CDOM) averaged 0.0161 plus or minus 0.00054 per nanometer, and for nonalgal absorption it averaged 0.011 per nanometer with deviations from general trends observed due to anomalous water properties. Although the phytoplankton specific absorption coefficients varied over a wide range (0.02 to 0.1 square meters (mg Chl) sup -1)) being higher in offshore surface waters, values of phytoplankton absorption spectra at the SeaWiFS wavebands were highly correlated to modeled values. The normalized scattering spectral shapes and the mean spectrum were in agreement to observations in other coastal waters, while the backscattering ratios were on average lower in phytoplankton dominated surface waters (0.0101 plus or minus 0.002) and higher in near-bottom waters (0.0191 plus or minus 0.0045) with low Chl. Average percent differences in remote sensing reflectance R (sub rs) derived form modeled and in-eater radiometric measurements were highest in the blue wavebands (52%) and at sampling stations with a ore stratified water column. Estimates of Chl and CDOM absorption derived from SeaWiFS images generated using regional empirical algorithms were highly correlated to in situ data.

D'Sa Eurico J.↗

Size dependent nonlinear optical properties of YCrO{sub 3} nanosystems

We report size-dependent optical limiting response of YCrO{sub 3} nanosystems upon illumination by nanosecond laser pulses at 532 nm. The limiting properties were investigated using the open aperture z-scan technique. Three-photon absorption coefficient is found to increase with particle size within the range of our investigations. We propose that the obtained nonlinearity is caused by two photon absorption, followed by excited state absorption.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Infrared thermometry in high temperature materials processing: influence of liquid water and steam

Here, the capability of four infrared thermometry techniques (2-colour and 1-colour pyrometers, Pyrolaser and IR camera) was evaluated with respect to the impact of water or steam in the line of sight to determine temperature from two heat sources (blackbody calibration source and steel block inside the furnace). The influence of liquid water on the temperature readings was minimal when using 2-colour pyrometry due to comparable absorption coefficients of water for the measured wavelengths. The signals measured using both the Pyrolaser and the 1-colour pyrometer were decreased due to the partial absorption and resulted in an apparent temperature lower than the actual. Water readily absorbed the IR signal in the range of the IR camera operation, resulting in no signal whenever liquid water was present in the line of sight. Steam caused the most deviation and fluctuation of temperature readings for all techniques due to the large level of light scattering in addition to the absorption of the radiant energy. A technique was developed to determine the transmissivity (apparent emissivity) when water or steam is in the line of sight of measurement. An approximate correction to the measurements based on Planck’s law is discussed for both 2-colour and 1-colour pyrometers.

2-colour and 1-colour pyrometry↗

Parameterization of near infrared absorption by atmospheric gases

An absorption coefficient (k) distribution model is presented for fast calculation of atmospheric transmittances based solely on essential data from line-by-line (LBL) calculations. The absorption at any site is summed over the spectra obtained by LBL calculations. Application of the scaling model is illustrated with sample calculations for 0.72 micron emissions and the 1.36 micron water vapor band. LBL absorption spectra are calculated for the pressure levels 260 mb, 400 mb and 1000 mb.

Ridgway, W. L.↗

Optical spectra and intensities of graphene magnetic dot bound to a negatively charged Coulomb impurity

Employing numerical diagonalization, we study the optical properties of an electron in a monolayer-graphene magnetic dot bound to an off-center negatively charged Coulomb impurity based on the massless Dirac-Weyl model. Numerical results show that, since the electron-hole symmetry is broken by the Coulomb potential, the optical absorption spectra of the magnetic dot in the presence of a Coulomb impurity are different between the electron states and the hole states. Effects of both the magnetic field and the dot size on the absorption coefficient are presented as functions of the incident photon energies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ab initio theory of free-carrier absorption in semiconductors

The absorption of light by free carriers in semiconductors results in optical loss for all photon wavelengths. Since free-carrier absorption competes with optical transitions across the band gap, it also reduces the efficiency of optoelectronic devices such as solar cells because it does not generate electron-hole pairs. In this work, we develop a first-principles theory of free-carrier absorption taking into account both single-particle excitations and the collective Drude term, and we demonstrate its application to the case of doped Si. Here, we determine the free-carrier absorption coefficient as a function of carrier concentration and we obtain excellent agreement with experimental data. We identify the dominant processes that contribute to free-carrier absorption at various photon wavelengths, and analyze the results to evaluate the impact of this loss mechanism on the efficiency of Si-based optoelectronic devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Saturation of the two-plasmon parametric decay instability in experiments on the electron cyclotron plasma heating due to the extraordinary pump wave depletion

The saturation level of the low-threshold parametric two-plasmon instability of the extraordinary pump wave decay to two upper hybrid plasmons is analyzed under conditions when the only efficient saturation mechanism is the pump depletion. A closed system of differential equations describing both the instability excitation and saturation is derived. The system is solved numerically and an analytic expression is obtained for the anomalous absorption coefficient of the pump wave caused by the development of this instability. The saturation level of the two-plasmon decay instability and the related anomalous absorption efficiency are estimated from data obtained in experiments on the electron cyclotron resonance heating of the plasma by an extraordinary wave in the TEXTOR tokamak.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Empirical relation between interstellar X-ray absorption and optical extinction

An empirical relation between interstellar X-ray absorption and optical extinction is derived from the correlation of measurements made on objects of large intrinsic diameter. The result is Av = 4.5 times 10 to the -22nd power N(H) mag, with the principal error being largely systematic in origin, where N(H) represents the column density of interstellar matter in the Brown and Gould model for the X-ray absorption coefficient. Applying this ratio to optically identified compact sources, it is concluded that sources in binary systems showing pronounced X-ray occultations have an intrinsic absorption equivalent to about 10 to the 22-nd power atoms per sq cm of interstellar matter and that there are a few compact sources where the absorption seems to be primarily interstellar in origin. The interstellar absorption expected in Cyg X-1 from the extinction of its optical counterpart is much greater than that suggested by X-ray spectra, which may be due to a soft X-ray component greater than that predicted by the power law fitted to higher energy data.

Gorenstein, P.↗

Solvated Electron in Acetonitrile: Radiation Yield, Absorption Spectrum, and Equilibrium between Cavity- and Solvent-Localized States

The equilibrium between a solvent cavity-localized electron, ecav-, and a dimeric solvent anion, (CH 3 CN)$_{2}^{•-}$, which are the two lowest energy states of the solvated electron in acetonitrile, has been investigated by pulse radiolysis at 233-353 K. The enthalpy and entropy for the e$_{cav}^{-}$ to (CH 3 CN)$_{2}^{•-}$ conversion amount to -11.2 ± 0.3 kcal/mol and -39.3 ± 1.2 cal/(mol K), corresponding to a 0.44 ± 0.35 equilibrium constant at 25 °C. The radiation yield of the solvated electron has been quantified using a Co(II) macrocycle that scavenges electrons with a 1.55 × 10 11 M -1 s -1 rate constant. The apparent yield increases without saturation over the attainable scavenger concentration range, reaching 2.8 per 100 eV; this value represents the lower limit for the acetonitrile ionization yield in pulse radiolysis. The apparent molar absorption coefficient of (20.8 ± 1.5) × 10 3 M -1 cm -1 at 1450 nm and 20 °C for the solvated electron and individual vis-near-infrared (NIR) absorption spectra of e$_{cav}^{-}$ and (CH 3 CN)$_{2}^{•-}$ are derived from the data. Variances with previous reports are thoroughly discussed. All together, these results resolve several controversies concerning the solvated electron properties in acetonitrile and furnish requisite data for quantitative pulse radiolysis investigations in this commonly used solvent.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Franz-Keldysh effect in GeSn pin photodetectors

The optical properties and the Franz-Keldysh effect at the direct band gap of GeSn alloys with Sn concentrations up to 4.2% at room temperature were investigated. The GeSn material was embedded in the intrinsic region of a Ge heterojunction photodetector on Si substrates. The layer structure was grown by means of ultra-low temperature molecular beam epitaxy. The absorption coefficient as function of photon energy and the direct bandgap energies were determined. In all investigated samples, the Franz-Keldysh effect can be observed. A maximum absorption ratio of 1.5 was determined for 2% Sn for a voltage swing of 3 V.

36 MATERIALS SCIENCE↗

Simulation of spatial distribution of absorbed laser energy in spherical microcapsules

Specific features of optical field distribution in composite spherical particles consisting of a liquid core and nanocomposite absorbing shell are theoretically studied at different wavelengths of incident radiation. Using the numerical simulation it is shown that the thickness of the shell of the spherical microcapsule particle and its intrinsic absorption coefficient determine the character of the spatial distribution and the absorbed power. The variation of these parameters allows one to change the spatial position of efficient volume absorption regions and peak absorption values. This provides favourable conditions for opening the shells in appropriate spatial zones to release the contents of the microcapsules. (interaction of laser radiation with matter)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Two-photon absorption in arsenic sulfide glasses

The two-photon absorption coefficient of 1047-nm light in As{sub 35}S{sub 65} chalcogenide glass has been measured. CW probe radiation has been used to observe the linear absorption in glass induced by two-photon excitation. The induced absorption lifetime was found to be ∼2 ms. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Combinatorial Platform for Discovery of Nanocrystal-Ink Based Earth Abundant Element PV with Efficiency Greater than 20% (Final Technical Report)

(1) We successfully developed an ultrasonic spray coating system that can be used to deposit thin chalcogenide films with composition gradients. 4 publications under the contract have been published with the instrument. The instrument was used to reveal the effects of intrinsic composition and examine the effects of 25 different dopant elements. Surprisingly, doping with most elements had little to no effect on the quasi- Fermi level splitting of bare films. A few elements were found to be detrimental including Fe, Co, and Ni. However, Li, Ge, and others were discovered to be beneficial. Ge and Li were explored in depth, and our best devices utilize lithium doping. (2) We developed a new model of absorption coefficients, that when combined with absolute intensity photoluminescence, yield the steady-state quasi-Fermi level splitting and a way to quantify the sub-bandgap absorption. This has resulted in 2 publications on the method, with another in preparation. This is a significant development that should impact other PV technologies. We have already received samples from 2 major PV companies to examine. Further, the model shows that tail states (potential fluctuations) in CZTSSe can only explain about 90 mV of loss in the open circuit voltage. (3) We found that lithium doping has several beneficial effects on CZTSSe. It improves the open-circuit voltage, short circuit current, fill factor, and shunt resistance. By using scanning Kelvin probe microscopy (SKPM) and conductive AFM (along with device measurements, DLPC, and XPS), we discovered that lithium acts to increase the p-type doping in both the grain and grain boundaries (GBs). The effect is stronger in the GBs and changes the direction of the electric field at the GB. In lithium doped devices, an electric field repels minority carrier electrons away from the GB. This resulted in a publication and the fabrication of 11.8% efficient devices from a DMSO-thiourea molecular ink. The mechanism of action is most likely due to the formation of Li Cu , which inhibits the formation of the donor defect Zn Cu . This reduces compensation and increases the net p-type doping. (4) By alloying with germanium, we have fabricated CZTGSSSe devices with the best open-circuit voltage (relative the maximum theoretical open-circuit voltage for the bandgap) for any kesterite solar cell. The Voc/Voc,max is 63%, compared to 58% for the record efficiency cell from hydrazine. The origin of the increased voltage efficiency appears to be related to the conduction band off-set and the suppression of a deep defect ($\sim$0.8 eV), most likely due to Cu Sn , but Sn Zn or Sn Cu are also possible. All milestones and go/no-go metrics were met with exception of the device efficiency milestone (15% then 20%). However, under the contract, hydrazine-free CZTSSe device efficiencies increased from 7.2% at the start of the contract to 11.8% upon completion.

14 SOLAR ENERGY↗

Combinatorial Platform for Discovery of Nanocrystal-Ink Based Earth Abundant Element PV with Efficiency Greater than 20%

(1) We successfully developed an ultrasonic spray coating system that can be used to deposit thin chalcogenide films with composition gradients. 4 publications under the contract have been published with the instrument. The instrument was used to reveal the effects of intrinsic composition and examine the effects of 25 different dopant elements. Surprisingly, doping with most elements had little to no effect on the quasi-Fermi level splitting of bare films. Ge and Li were explored in depth, and our best devices utilize lithium doping. (2) We developed a new model of absorption coefficients, that when combined with absolute intensity photoluminescence, yield the steady-state quasi-Fermi level splitting and a way to quantify the sub-bandgap absorption. This has resulted in 2 publications on the method, with another in preparation. This is a significant development that should impact other PV technologies. (3) We found that lithium doping has several beneficial effects on CZTSSe. It improves the open-circuit voltage, short circuit current, fill factor, and shunt resistance. By using scanning Kelvin probe microscopy (SKPM) and conductive AFM (along with device measurements, DLPC, and XPS), we discovered that lithium acts to increase the p-type doping in both the grain and grain boundaries (GBs). The effect is stronger in the GBs and changes the direction of the electric field at the GB. In lithium doped devices, an electric field repels minority carrier electrons away from the GB. This resulted in a publication and the fabrication of 11.8% efficient devices from a DMSO-thiourea molecular ink. The mechanism of action is most likely due to the formation of LiCu, which inhibits the formation of the donor defect ZnCu. This reduces compensation and increases the net p-type doping. (4) By alloying with germanium, we have fabricated CZTGSSe devices with the best open-circuit voltage (relative the maximum theoretical open-circuit voltage for the bandgap) for any kesterite solar cell. The Voc/Voc,max is 63%, compared to 58% for the record efficiency cell from hydrazine. The origin of the increased voltage efficiency appears to be related to the conduction band off-set and the suppression of a deep defect (~0.8 eV), most likely due to CuSn, but SnZn or SnCu are also possible. All milestones and go/no-go metrics were met with exception of the device efficiency milestone (15% then 20%). However, under the contract, hydrazine-free CZTSSe device efficiencies increased from 7.2% at the start of the contract to 11.8% upon completion.

14 SOLAR ENERGY↗