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At least 271 records · Page 15

Understanding the optoelectronic properties of doped 2D organic-inorganic halide perovskite quantum wells: towards efficient quantum well IR photodetectors

Metal halide perovskite (MHP) multiple quantum wells which consist of multilayers of alternate organic and inorganic layers exhibit large exciton binding energies due to the dielectric confinement between the inorganic and organic layers. These naturally formed multiple quantum wells have strong spin-orbit coupling (SOC) due to the presence of heavy elements in their crystal structures. Although the fundamental properties of 2D MHPs are far from being entirely understood, it is widely accepted that their band edge absorption coefficient results from strong exciton interactions. However, studies demonstrating how different exciton interactions and doping effects influence electronic traps and disorder on the band edge absorption coefficient of 2D MHPs have not been demonstrated. Understanding these interactions in MHPs will allow us to access low energy optical transitions for the fabrication of solution processable short-to-mid-wavelength IR photodetectors (1 – 8 μm). Moreover, upon doping, it is possible to move the Fermi energy into the conduction band (CB) to favorably promote the transport of charges in a working device. Herein, we study the development of 2D MHPs having strong SOC, high carrier mobility, and tunable quantum well structures. Our studies shed light on the design and modulation of fundamental physical phenomena by carefully elucidating the role of dopants (n-type and p-type), exciton heterogeneity, orientation, structure, and bias stress effects on the performance of MHPs as potential IR photodetectors.

36 MATERIALS SCIENCE↗

InGaAs/InAsSb strained layer superlattices for mid-wave infrared detectors

Investigation of growth and properties of InGaAs/InAsSb strained layer superlattices, identified as ternary strained layer superlattices (ternary SLSs), is reported. The material space for the antimony-based SLS detector development is expanded beyond InAs/InAsSb and InAs/(In)GaSb by incorporating Ga into InAs. It was found that this not only provides support for strain compensation but also enhances the infrared (IR) absorption properties. A unique InGaAs/InAsSb SLS exists when the conduction band of InGaAs aligns with that of InAsSb. The bandgap of this specific InGaAs/InAsSb SLS can then be tuned by adjusting the thickness of both constituents. Due to the enhanced electron-hole wavefunction overlap, a significant increase in the absorption coefficient was theoretically predicted for ternary SLS as compared to current state-of-the-art InAs/InAsSb SLS structures, and an approximately 30%–35% increase in the absorption coefficient was experimentally observed. All the samples examined in this work were designed to have the same bandgap of approximately 0.240 eV (5.6 μm) at 150 K.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Radiation effects on beta 10.6 of pure and europium doped KCl

Changes in the optical absorption coefficient as a result of X-ray and electron bombardment of pure KCl (monocrystalline and polycrystalline), and divalent europium doped polycrystalline KCl were determined. The optical absorption coefficients were measured by a constant heat flow calorimetric method. Both 300 KV X-irradiation and 2 MeV electron irradiation produced significant increases in beta 10.6, measured at room temperature. The X-irradiation of pure moncrystalline KCl increased beta 10.6 by 0.005/cm for a 113 MR dose. For an equivalent dose, 2 MeV electrons were found less efficient in changing beta 10.6. However, electron irradiation of pure and Eu-doped polycrystalline KCl produced marked increases in adsorption. Beta increased to over 0.25/cm in Eu-doped material for a 30 x 10 to the 14th power electrons/sq cm dose, a factor of 20 increase over unirradiated material. Moreover, bleaching the electron irradiated doped KCl with 649 m light produced and additional factor of 1.5 increase. These findings will be discussed in light of known defect-center properties in KCl.

Grimes, H. H.↗

Quasi-Fermi level splitting and sub-bandgap absorptivity from semiconductor photoluminescence

A unified model for the direct gap absorption coefficient (band-edge and sub-bandgap) is developed that encompasses the functional forms of the Urbach, Thomas-Fermi, screened Thomas-Fermi, and Franz-Keldysh models of sub-bandgap absorption as specific cases. We combine this model of absorption with an occupation-corrected non-equilibrium Planck law for the spontaneous emission of photons to yield a model of photoluminescence (PL) with broad applicability to band-band photoluminescence from intrinsic, heavily doped, and strongly compensated semiconductors. The utility of the model is that it is amenable to full-spectrum fitting of absolute intensity PL data and yields: (1) the quasi-Fermi level splitting, (2) the local lattice temperature, (3) the direct bandgap, (4) the functional form of the sub-bandgap absorption, and (5) the energy broadening parameter (Urbach energy, magnitude of potential fluctuations, etc.). The accuracy of the model is demonstrated by fitting the room temperature PL spectrum of GaAs. It is then applied to Cu(In,Ga)(S,Se){sub 2} (CIGSSe) and Cu{sub 2}ZnSn(S,Se){sub 4} (CZTSSe) to reveal the nature of their tail states. For GaAs, the model fit is excellent, and fitted parameters match literature values for the bandgap (1.42 eV), functional form of the sub-bandgap states (purely Urbach in nature), and energy broadening parameter (Urbach energy of 9.4 meV). For CIGSSe and CZTSSe, the model fits yield quasi-Fermi leveling splittings that match well with the open circuit voltages measured on devices made from the same materials and bandgaps that match well with those extracted from EQE measurements on the devices. The power of the exponential decay of the absorption coefficient into the bandgap is found to be in the range of 1.2 to 1.6, suggesting that tunneling in the presence of local electrostatic potential fluctuations is a dominant factor contributing to the sub-bandgap absorption by either purely electrostatic (screened Thomas-Fermi) or a photon-assisted tunneling mechanism (Franz-Keldysh). A Gaussian distribution of bandgaps (local E{sub g} fluctuation) is found to be inconsistent with the data. The sub-bandgap absorption of the CZTSSe absorber is found to be larger than that for CIGSSe for materials that yield roughly equivalent photovoltaic devices (8% efficient). Further, it is shown that fitting only portions of the PL spectrum (e.g., low energy for energy broadening parameter and high energy for quasi-Fermi level splitting) may lead to significant errors for materials with substantial sub-bandgap absorption and emission.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Optical Properties and Aging of Light Absorbing Secondary Organic Aerosol

The light-absorbing organic aerosol (OA), commonly referred to as “brown carbon (BrC)”, has attracted considerable attention in recent years because of its potential to affect atmospheric radiation balance, especially in the ultraviolet region and thus impact photochemical processes. A growing amount of data has indicated that BrC is prevalent in the atmosphere, which has motivated numerous laboratory and field studies; however, our understanding of the relationship between the chemical composition and optical properties of BrC remains limited. We conducted chamber experiments to investigate the effect of various VOC precursors, NOx concentrations, photolysis time and relative humidity (RH) on the light absorption of selected secondary organic aerosols (SOA). Light absorption of chamber generated SOA samples, especially aromatic SOA, was found to increase with NOx concentration, at moderate RH, and for the shortest photolysis aging times. The highest mass absorption coefficients (MAC) value is observed from toluene SOA products formed under high NOx conditions at moderate RH, in which nitro-aromatics were previously identified as the major light absorbing compounds. BrC light absorption is observed to decrease with photolysis time, correlated with a decline of the organonitrate fraction of SOA. SOA formed from mixtures of aromatics and isoprene absorb less visible and UV light than SOA formed from aromatic precursors alone on a mass basis. However, the mixed-SOA absorption was underestimated when optical properties were predicted using a two-product SOA formation model, as done in many current climate models. Further investigation, including analysis on detailed mechanisms, are required to explain the discrepancy.

Brown Carbon↗

Cirrus microphysics observations made during FIRE 2: Small particles, high concentrations, and probe comparisons

Aircraft observations of cirrus cloud microphysics were made near Coffeyville, Kansas during Nov. and Dec. 1991. Cloud microphysics measurements were made using both a PMS 2DC probe and an ice particle replicator, both were mounted on the UND Citation aircraft. Intercomparison is made of the size, area, and ice mass spectra determined from these probes. The PMS 2DC undercounts particles for D less than 70 microns and the replicator oversizes particles for D greater than 150 microns, at least when column rosettes are encountered. High concentrations of particles with D less than 50 microns are noted in selected portions of the 22 Nov. 91 replicator data set. Relations between the maximum dimension of a crystal and its shadow area (known as area dimensional relationships) are computed from the PMS data. Area and mass dimensional relationships are used to give a simple analytical expression for computing the wavelength dependent absorption coefficient averaged over a size bin. Calculations based upon the replicator data show that crystals with D less than 50 microns contribute significantly to the solar extinction and infrared absorption coefficients during some time intervals.

Arnott, W. P.↗

Short-lived species detection of nitrous acid by external-cavity quantum cascade laser based quartz-enhanced photoacoustic absorption spectroscopy

Spectroscopic detection of short-lived gaseous nitrous acid (HONO) at 1254.85 cm{sup −1} was realized by off-beam coupled quartz-enhanced photoacoustic spectroscopy (QEPAS) in conjunction with an external cavity quantum cascade lasers (EC-QCL). High sensitivity monitoring of HONO was performed within a very small gas-sample volume (of ∼40 mm{sup 3}) allowing a significant reduction (of about 4 orders of magnitude) of air sampling residence time which is highly desired for accurate quantification of chemically reactive short-lived species. Calibration of the developed QEPAS-based HONO sensor was carried out by means of lab-generated HONO samples whose concentrations were determined by direct absorption spectroscopy involving a ∼109.5 m multipass cell and a distributed feedback QCL. A minimum detection limit (MDL) of 66 ppbv (1 σ) HONO was achieved at 70 mbar using a laser output power of 50 mW and 1 s integration time, which corresponded to a normalized noise equivalent absorption coefficient of 3.6 × 10{sup −8 }cm{sup −1} W/Hz{sup 1/2}. This MDL was down to 7 ppbv at the optimal integration time of 150 s. The corresponding 1σ minimum detected absorption coefficient is ∼1.1 × 10{sup −7 }cm{sup −1} (MDL ∼ 3 ppbv) in 1 s and ∼1.1 × 10{sup −8 }cm{sup −1} (MDL ∼ 330 pptv) in 150 s, respectively, with 1 W laser power.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

On the errors in measuring the particle density by the light absorption method

The accuracy of absorption measurements of the density of particles in a given quantum state as a function of the light absorption coefficient is analyzed. Errors caused by the finite accuracy in measuring the intensity of the light passing through a medium in the presence of different types of noise in the recorded signal are considered. Optimal values of the absorption coefficient and the factors capable of multiplying errors when deviating from these values are determined.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Some optical properties of KTP, LiIO3, and LiNbO3

Measurements of the absorption coefficient for KTP, LiIO3, and LiNbO3 are discussed. The variation of the refractive index with temperature has been measured for KTP and LiIO3. It is necessary to know both the absorption coefficient beta and the variation in the indexes of refraction with temperature change dn/dT to determine the average power limit of a nonlinear interaction. With the dn/dT information, it is also possible to estimate the temperature half width of any nonlinear interaction by calculating the variation of the phase-matching condition with temperature.

Gettemy, Donald J.↗

Laser absorption spectroscopy - Method for monitoring complex trace gas mixtures

A frequency stabilized CO2 laser was used for accurate determinations of the absorption coefficients of various gases in the wavelength region from 9 to 11 microns. The gases investigated were representative of the types of contaminants expected to build up in recycled atmospheres. These absorption coefficients were then used in determining the presence and amount of the gases in prepared mixtures. The effect of interferences on the minimum detectable concentration of the gases was measured. The accuracies of various methods of solution were also evaluated.

Green, B. D.↗

Two-photon absorption in SiO{sub 2}- and (SiO{sub 2} + GeO{sub 2})-based fibres at a wavelength of 349 nm

The nonlinear two-photon light absorption coefficients have been measured in an optical fibre with a quartz glass (SiO{sub 2}) core and in a fibre with a germanosilicate glass (SiO{sub 2} + GeO{sub 2}) core. The two-photon absorption coefficient β measured at a wavelength of 349 nm in the (SiO{sub 2} + GeO{sub 2})-based fibre (13.7 cm TW{sup -1}) multiply exceeds that for the pure quartz glass optical fibre (0.54 cm TW{sup -1}). (nonlinear optical phenomena)

36 MATERIALS SCIENCE↗

Can Vertical Profiles of Tropospheric Methane on Titan Be Derived from Radio-Occultation Soundings?

The intensity of the received signal at Earth in the radio occultations of Titan is attenuated both by refractive defocusing and pressure-induced absorption from N2-N2 and CH4-N2 pairs. Because the absorption strength is different for the two sets of pairs, matching the retrieved absorptivity profile can in principle yield the vertical variation in gaseous methane in the troposphere. There are two factors that make this difficult. The first is the propagation of noise in the phase and amplitude of the received signal in the absorption retrieval. The phase data is first inverted to retrieve vertical profiles of refractivity, from which the refractive defocusing is calculated. This is then subtracted from the observed. intensity attenuation of the received signal to generate a profile of atmospheric absorption. The second problem is the uncertainty in the pressure-induced absorption coefficients. Laboratory data at radio wavelengths is only available near room temperature (see, e.g., [1] for N2-N2), and the extrapolation to the low temperatures in Titan's troposphere is not well established. Ab initio calculations by Borysow et al. [2, 3] provide absorption coefficients at low temperatures and long wavelengths, but their accuracy has come into question. We present examples from Cassini radio occultations of Titan to illustrate the difficulties. For methane mole fractions in the lower troposphere comparable to that inferred from the Huygens probe (approximately 0.05), it will be difficult to separate the contributions of N2-N2 collisions from those of N2-CH4, collisions to the retrieved absorption. However, higher concentrations of CH4 and/or a higher signal-to-noise ratio from a future uplink experiment could result in a successful separation of the two components. However, key to this are highly accurate estimates of the absorption from a combination of laboratory measurements at love temperatures and long wavelengths, and possibly improved theoretical calculations.

Flasar, F. Michael↗

Wavelength Dependence of the Absorption of Black Carbon Particles: Predictions and Results from the TARFOX Experiment and Implications for the Aerosol Single Scattering Albedo

Measurements are presented of the wavelength dependence of the aerosol absorption coefficient taken during the Tropical Aerosol Radiative Forcing Observational Experiment (TARFOX) over the northern Atlantic. The data show an approximate lamda(exp -1) variation between 0.40 and 1.0 micrometers. The theoretical basis of the wavelength variation of the absorption of solar radiation by elemental carbon [or black carbon (BC)] is explored. For a wavelength independent refractive index the small particle absorption limit simplifies to a lambda(exp -1) variation in relatively good agreement with the data. This result implies that the refractive indices of BC were relatively constant in this wavelength region, in agreement with much of the data on refractive indices of BC. However, the result does not indicate the magnitude of the refractive indices. The implications of the wavelength dependence of BC absorption for the spectral behavior of the aerosol single scattering albedo are discussed. It is shown that the single scattering albedo for a mixture of BC and nonabsorbing material decreases with wavelength in the solar spectrum (i.e., the percentage amount of absorption increases). This decease in the single scattering albedo with wavelength for black carbon mixtures is different from the increase in single scattering allied for most mineral aerosols (dusts). This indicates that, if generally true, the spectral variation of the single- scattering albedo can be used to distinguish aerosol types. It also highlights the importance of measurements of the spectral variation of the aerosol absorption coefficient and single scattering albedo.

Bergstrom, Robert W.↗

Analysis of diffential absorption lidar technique for measurements of anhydrous hydrogen chloride from solid rocket motors using a deuterium fluoride laser

An active optical technique (differential absorption lidar (DIAL)) for detecting, ranging, and quantifying the concentration of anhydrous HCl contained in the ground cloud emitted by solid rocket motors (SRM) is evaluated. Results are presented of an experiment in which absorption coefficients of HCl were measured for several deuterium fluoride (DF) laser transitions demonstrating for the first time that a close overlap exists between the 2-1 P(3) vibrational transition of the DF laser and the 1-0 P(6) absorption line of HCl, with an absorption coefficient of 5.64 (atm-cm) to the -1 power. These measurements show that the DF laser can be an appropriate radiation source for detecting HCl in a DIAL technique. Development of a mathematical computer model to predict the sensitivity of DIAL for detecting anhydrous HCl in the ground cloud is outlined, and results that assume a commercially available DF laser as the radiation source are presented.

Bair, C. H.↗

Infrared spectra and optical constants of astronomical ices: III. Propane, propylene, and propyne

Infrared (IR) spectra of the hydrocarbon ices C3H8 (propane), C3H6 (propylene, propene), and C3H4 (propyne, methylacetylene) are relevant to the study of the low-temperature chemistry and spectroscopy of objects within and beyond the Solar System, but IR band strengths and absorption coefficients are lacking for these compounds. Here we present new IR spectra of crystalline and non-crystalline forms of C3H8, C3H6, and C3H4. Measurements of ice density and refractive index also are reported, two quantities needed to compute IR absorption coefficients, band strengths, optical constants, and, ultimately, abundances of propane, propylene, and propyne in extraterrestrial environments and in laboratory experiments. Suggestions and interpretations are offered regarding the multiple crystalline forms of propane and propylene observed. Applications and extensions are described.

Reggie L. Hudson↗

Infrared Spectra and Optical Constants of Astronomical Ices: III. Propane, Propylene, and Propyne

Infrared (IR) spectra of the hydrocarbon ices C3H8 (propane), C3H6 (propylene, propene), and C3H4 (propyne, methylacetylene) are relevant to the study of the low-temperature chemistry and spectroscopy of objects within and beyond the Solar System, but IR band strengths and absorption coefficients are lacking for these compounds. Here we present new IR spectra of crystalline and non-crystalline forms of C3H8, C3H6, and C3H4. Measurements of ice density and refractive index also are reported, two quantities needed to compute IR absorption coefficients, band strengths, optical constants, and, ultimately, abundances of propane, propylene, and propyne in extraterrestrial environments and in laboratory experiments. Suggestions and interpretations are offered regarding the multiple crystalline forms of propane and propylene observed. Applications and extensions are described.

Ices↗

Infrared spectra and optical constants of astronomical ices: III. Propane, propylene, and propyne

Infrared (IR) spectra of the hydrocarbon ices C3H8 (propane), C3H6 (propylene, propene), and C3H4 (propyne, methylacetylene) are relevant to the study of the low-temperature chemistry and spectroscopy of objects within and beyond the Solar System, but IR band strengths and absorption coefficients are lacking for these compounds. Here we present new IR spectra of crystalline and non-crystalline forms of C3H8, C3H6, and C3H4. Measurements of ice density and refractive index also are reported, two quantities needed to compute IR absorption coefficients, band strengths, optical constants, and, ultimately, abundances of propane, propylene, and propyne in extrater-restrial environments and in laboratory experiments. Suggestions and interpretations are offered regarding the multiple crystalline forms of propane and propylene observed. Applications and extensions are described.

Reggie L. Hudson↗