Showing papers in "Journal of Quantitative Spectroscopy & Radiative Transfer in 2017"
TL;DR: The pgopher program as discussed by the authors is a general purpose program for simulating and fitting molecular spectra, particularly the rotational structure, which can handle linear molecules, symmetric top and asymmetric top.
Abstract: The pgopher program is a general purpose program for simulating and fitting molecular spectra, particularly the rotational structure. The current version can handle linear molecules, symmetric tops and asymmetric tops and many possible transitions, both allowed and forbidden, including multiphoton and Raman spectra in addition to the common electric dipole absorptions. Many different interactions can be included in the calculation, including those arising from electron and nuclear spin, and external electric and magnetic fields. Multiple states and interactions between them can also be accounted for, limited only by available memory. Fitting of experimental data can be to line positions (in many common formats), intensities or band contours and the parameters determined can be level populations as well as rotational constants. pgopher is provided with a powerful and flexible graphical user interface to simplify many of the tasks required in simulating, understanding and fitting molecular spectra, including Fortrat diagrams and energy level plots in addition to overlaying experimental and simulated spectra. The program is open source, and can be compiled with open source tools. This paper provides a formal description of the operation of version 9.1.
704 citations
TL;DR: Level as mentioned in this paper can automatically locate the bound and/or quasibounded levels of any smooth single- or double-minimum potential, and calculate inertial rotation and centrifugal distortion constants and various expectation values for those levels.
Abstract: This paper describes program LEVEL, which can solve the radial or one-dimensional Schrodinger equation and automatically locate either all of, or a selected number of, the bound and/or quasibound levels of any smooth single- or double-minimum potential, and calculate inertial rotation and centrifugal distortion constants and various expectation values for those levels. It can also calculate Franck–Condon factors and other off-diagonal matrix elements, either between levels of a single potential or between levels of two different potentials. The potential energy function may be defined by any one of a number of analytic functions, or by a set of input potential function values which the code will interpolate over and extrapolate beyond to span the desired range.
674 citations
Harvard University1, Langley Research Center2, University of Alabama in Huntsville3, Goddard Space Flight Center4, Finnish Meteorological Institute5, University of California, Berkeley6, National Center for Atmospheric Research7, Saint Louis University8, National Autonomous University of Mexico9, University of Maryland, Baltimore County10, Rutherford Appleton Laboratory11, Yonsei University12, Dalhousie University13, York University14, Environment Canada15, Jet Propulsion Laboratory16, University of Edinburgh17, National Oceanic and Atmospheric Administration18, Spanish National Research Council19, United States Environmental Protection Agency20, Royal Netherlands Meteorological Institute21, European Space Agency22, University of Nebraska–Lincoln23
TL;DR: TEMPO was selected in 2012 by NASA as the first Earth Venture Instrument, for launch between 2018 and 2021, and it will measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy as mentioned in this paper.
Abstract: TEMPO was selected in 2012 by NASA as the first Earth Venture Instrument, for launch between 2018 and 2021. It will measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO observes from Mexico City, Cuba, and the Bahamas to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution (~2.1 km N/S×4.4 km E/W at 36.5°N, 100°W). TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry, as well as contributing to carbon cycle knowledge. Measurements are made hourly from geostationary (GEO) orbit, to capture the high variability present in the diurnal cycle of emissions and chemistry that are unobservable from current low-Earth orbit (LEO) satellites that measure once per day. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a commercial GEO host spacecraft to provide a modest cost mission that measures the spectra required to retrieve ozone (O3), nitrogen dioxide (NO2), sulfur dioxide (SO2), formaldehyde (H2CO), glyoxal (C2H2O2), bromine monoxide (BrO), IO (iodine monoxide),water vapor, aerosols, cloud parameters, ultraviolet radiation, and foliage properties. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O3 chemistry cycle. Multi-spectral observations provide sensitivity to O3 in the lowermost troposphere, substantially reducing uncertainty in air quality predictions. TEMPO quantifies and tracks the evolution of aerosol loading. It provides these near-real-time air quality products that will be made publicly available. TEMPO will launch at a prime time to be the North American component of the global geostationary constellation of pollution monitoring together with the European Sentinel-4 (S4) and Korean Geostationary Environment Monitoring Spectrometer (GEMS) instruments.
226 citations
TL;DR: In this paper, the authors proposed two approaches for alternative 2D thin film coatings, which can enhance the passive thermal management for application to electronic equipment. And they also showed that the performance of radiative cooling can be enhanced by inserting an Al2O3 film (which has strong absorption in the 8−13µm spectrum, and does not absorb in the visible and near-infrared) within conventional coating structures.
Abstract: The operation of most electronic semiconductor devices suffers from the self-generated heat. In the case of photovoltaic or thermos-photovoltaic cells, their exposure to sun or high temperature sources make them get warm beyond the desired operating conditions. In both incidences, the solution strategy requires effective radiative cooling process, i.e., by selective absorption and emission in predetermined spectral windows. In this study, we outline two approaches for alternative 2D thin film coatings, which can enhance the passive thermal management for application to electronic equipment. Most traditional techniques use a metallic (silver) layer because of their high reflectivity, although they display strong absorption in the visible and near-infrared spectrums. We show that strong absorption in the visible and near-infrared spectrums due to a metallic layer can be avoided by repetitive high index-low index periodic layers and broadband reflection in visible and near-infrared spectrums can still be achieved. These modifications increase the average reflectance in the visible and near-infrared spectrums by 3–4%, which increases the cooling power by at least 35 W/m2. We also show that the performance of radiative cooling can be enhanced by inserting an Al2O3 film (which has strong absorption in the 8–13 µm spectrum, and does not absorb in the visible and near-infrared) within conventional coating structures. These two approaches enhance the cooling power of passive radiative cooling systems from the typical reported values of 40 W/m2–100 W/m2 and 65 W/m2 levels respectively.
144 citations
TL;DR: The Atmospheric Chemistry Experiment (ACE) is a Canadian-led small satellite mission for remote sensing of the Earth's atmosphere as discussed by the authors, which was launched into a low Earth circular orbit by NASA on August 12, 2003 and it continues to function nominally.
Abstract: The Atmospheric Chemistry Experiment (ACE), also called SCISAT, is a Canadian-led small satellite mission for remote sensing of the Earth’s atmosphere. ACE was launched into a low Earth circular orbit by NASA on August 12, 2003 and it continues to function nominally. The ACE instruments are a high spectral resolution (0.02 cm −1 ) Fourier Transform Spectrometer (FTS) operating from 2.2 to 13.3 μm (750–4400 cm −1 ), a spectrophotometer known as Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (MAESTRO) with wavelength coverage of 285–1020 nm and two filtered detector arrays to image the Sun at 0.525 and 1.02 μm. ACE operates in solar occultation mode to provide altitude profiles of temperature, pressure, atmospheric extinction and the volume mixing ratios (VMRs) for several dozen molecules and related isotopologues. This paper presents a mission overview and a summary of selected scientific results.
144 citations
TL;DR: In this paper, the first-order semiclassical Rydberg-Klein-Rees procedure for determining the potential energy function for a diatomic molecule from a knowledge of the dependence of the molecular vibrational energies Gv and inertial rotation constants Bv on the vibrational quantum number v.
Abstract: This paper describes computer program RKR1, which implements the first-order semiclassical Rydberg–Klein–Rees procedure for determining the potential energy function for a diatomic molecule from a knowledge of the dependence of the molecular vibrational energies Gv and inertial rotation constants Bv on the vibrational quantum number v . RKR1 allows the vibrational energies and rotational constants to be defined in terms of: (i) conventional Dunham polynomial expansions, (ii) near-dissociation expansions (NDE׳s), or (iii) the mixed Dunham/NDE “MXR” functions introduced by Tellinghuisen [J Chem Phys 2003; 118: 3532]. Internal convergence tests ascertain and report on the precision of the resulting turning points. For cases in which only vibrational data are available, RKR1 also allows an overall potential to be constructed by combining directly-calculated well widths with inner turning points generated from a Morse function. It can also automatically smooth over irregular or unphysical behavior of the steep inner wall of the potential.
134 citations
TL;DR: In this paper, total internal partition sums (TIPS) are reported for 166 isotopologues of 51 molecules important in planetary atmospheres, including C3H4, CH3, and CS2.
Abstract: Total internal partition sums (TIPS) are reported for 166 isotopologues of 51 molecules important in planetary atmospheres. Molecules 1 to 50 are taken from the HITRAN2016 list, and, in some cases, additional isotopologues are considered for some of the molecules. Molecules 51–53 are C3H4, CH3, and CS2, respectively. TIPS are not reported for the O atom and CF4; thus, while there are 53 species in the list, data are reported for 51 molecules. The TIPS are determined by various methods from 1 K to a Tmax that ensures the TIPS reported have converged. These data are provided with HITRAN2016 and a new version of the TIPS code is available in both FORTRAN and python languages.
125 citations
TL;DR: SpectraPlot as discussed by the authors is a web-based application for simulating spectra of atomic and molecular gases, including absorption spectra, transition linestrengths, and blackbody emission spectra.
Abstract: SpectraPlot is a web-based application for simulating spectra of atomic and molecular gases. At the time this manuscript was written, SpectraPlot consisted of four primary tools for calculating: (1) atomic and molecular absorption spectra, (2) atomic and molecular emission spectra, (3) transition linestrengths, and (4) blackbody emission spectra. These tools currently employ the NIST ASD, HITRAN2012, and HITEMP2010 databases to perform line-by-line simulations of spectra. SpectraPlot employs a modular, integrated architecture, enabling multiple simulations across multiple databases and/or thermodynamic conditions to be visualized in an interactive plot window. The primary objective of this paper is to describe the architecture and spectroscopic models employed by SpectraPlot in order to provide its users with the knowledge required to understand the capabilities and limitations of simulations performed using SpectraPlot. Further, this manuscript discusses the accuracy of several underlying approximations used to decrease computational time, in particular, the use of far-wing cutoff criteria.
102 citations
TL;DR: An asymmetric Fabry-Perot emitter with a lossless dielectric spacer inserted between a vanadium dioxide (VO 2 ) thin film and an opaque aluminum substrate is proposed in this article.
Abstract: An asymmetric Fabry-Perot emitter is proposed with a lossless dielectric spacer inserted between a vanadium dioxide (VO 2 ) thin film and an opaque aluminum substrate. Switchable mid-infrared emittance has been achieved due to the insulator-to-metal transition of VO 2 . When VO 2 is dielectric below 341 K, the structure is highly reflective, thereby minimizing thermal radiation loss. Above 345 K, the VO 2 becomes metallic and forms a Fabry-Perot resonance cavity with high broadband emissivity around 10 µm wavelength, providing a radiative cooling effect due to enhanced thermal emission. The radiative properties are calculated via a uniaxial transfer matrix method and Bruggeman effective medium theory. The physical mechanisms that provide the observed absorption enhancements are elucidated by examining the total phase shift in the multilayer structure and the phonon modes of VO 2. When experiencing the VO 2 phase transition, the radiative power of the proposed coating achieves a 6.5 fold enhancement for extraterrestrial spacecraft systems, and 7.3 fold enhancement for terrestrial systems such as buildings, making it a promising choice for dynamic radiative cooling applications in a variable environment. The findings here will facilitate research and development of novel coating materials for radiative cooling applications.
96 citations
TL;DR: The RFM is designed for robustness, flexibility and ease-of-use (particularly by the non-expert), and no claims are made for superior accuracy, or indeed novelty, compared to other line-by-line codes.
Abstract: The Reference Forward Model (RFM) is a general purpose line-by-line radiative transfer model, currently supported by the UK National Centre for Earth Observation. This paper outlines the algorithms used by the RFM, focusing on standard calculations of terrestrial atmospheric infrared spectra followed by a brief summary of some additional capabilities and extensions to microwave wavelengths and extraterrestrial atmospheres. At its most basic level — the ‘line-by-line’ component — it calculates molecular absorption cross-sections by applying the Voigt lineshape to all transitions up to ±25 cm−1 from line-centre. Alternatively, absorptions can be directly interpolated from various forms of tabulated data. These cross-sections are then used to construct infrared radiance or transmittance spectra for ray paths through homogeneous cells, plane-parallel or circular atmospheres. At a higher level, the RFM can apply instrumental convolutions to simulate measurements from Fourier transform spectrometers. It can also calculate Jacobian spectra and so act as a stand-alone forward model within a retrieval scheme. The RFM is designed for robustness, flexibility and ease-of-use (particularly by the non-expert), and no claims are made for superior accuracy, or indeed novelty, compared to other line-by-line codes. Its main limitations at present are a lack of scattering and simplified modelling of surface reflectance and line-mixing.
81 citations
TL;DR: In this article, a new 626-based Ames-2 PES refinement and Ames-2016 line lists for 13 CO2 isotopologues are reported, with line position deviations reduced by 50% or more, which consequently leads to more reliable intensities.
Abstract: A new 626-based Ames-2 PES refinement and Ames-2016 line lists for 13 CO2 isotopologues are reported. A consistent σRMS = ±0.02 cm−1 is established for hundreds of isotopologue band origins using the Ames-2 PES. Ames-2016 line lists are computed at 296 K, 1000 K and 4000 K using the Ames-2 PES and the same DMS-N2 dipole surface used previously, with J up to 150, E′ up to 24,000 cm−1 or 18,000 cm−1 and appropriate intensity cutoffs. The lists are compared to the CDSD-296, CDSD-4000 databases, UCL line lists, and a few recent highly accurate CO2 intensity measurements. Both agreements and discrepancies are discussed. Compared to the old Ames CO2 lists, the Ames-2016 line lists have line position deviations reduced by 50% or more, which consequently leads to more reliable intensities. The line shape parameters in the Ames-2016 line lists are predicted using the newly assigned conventional vibrational polyad quantum numbers for rovibrational levels below 12,000 cm−1 so the quality of the line shape parameters is similar to that of CDSD or HITRAN. This study further proves that a semi-empirically refined PES (Ames-1 and Ames-2) coupled with a high quality ab initio DMS (DMS-N2 and UCL) may generate IR predictions with consistent accuracy and is thus helpful in the analysis of laboratory spectra and simulations of various isotopologues. The Ames-2016 lists based on DMS-N2 have reached the ∼1% intensity prediction accuracy level for the recent 626 30013-00001 and 20013-00001 bands, but further quantification and improvements require sub-percent or sub-half-percent accurate experimental intensities. The inter-isotopologue consistency of the intensity prediction accuracies should have reached better than 1–3% for regular bands not affected by resonances. Since the Effective Dipole Models (EDM) in CDSD and HITRAN have 1–20% or even larger uncertainties, we show that the Ames lists can provide better alternative IR data for many hard-to-determine isotopologue bands. Comparison at 4000 K suggests that the Ames-4000 K 12C16O2 line list is reliable and consistent within the current cutoffs of J ≤ 150 and E′ ≤ 24,000 cm−1, but intensity contributions involving higher energy levels should not be omitted and future computations need to be converged up to at least 32,000 cm−1 or higher. The remaining issues are discussed regarding the source of energy level discrepancies, intensity underestimations by ∼50% for some weak bands, etc. and also future work.
TL;DR: This paper validate near- and far-field distributions against the well-established multi-sphere T -matrix (MSTM) code and discuss the convergence behavior for ensembles of different sizes, including an exemplary system comprising 10 5 particles.
Abstract: CELES is a freely available MATLAB toolbox to simulate light scattering by many spherical particles. Aiming at high computational performance, CELES leverages block-diagonal preconditioning, a lookup-table approach to evaluate costly functions and massively parallel execution on NVIDIA graphics processing units using the CUDA computing platform. The combination of these techniques allows to efficiently address large electrodynamic problems (>104 scatterers) on inexpensive consumer hardware. In this paper, we validate near- and far-field distributions against the well-established multi-sphere T-matrix (MSTM) code and discuss the convergence behavior for ensembles of different sizes, including an exemplary system comprising 105 particles.
TL;DR: In this paper, a two-dimensional radiative transfer was proposed for the correction of horizontal gradients in profile retrievals from limb observations of the martian atmosphere, which is applied to limb emission measurements from the Mars Climate Sounder instrument on Mars Reconnaissance Orbiter.
Abstract: The remote sounding of infrared emission from planetary atmospheres using limb-viewing geometry is a powerful technique for deriving vertical profiles of structure and composition on a global scale. Compared with nadir viewing, limb geometry provides enhanced vertical resolution and greater sensitivity to atmospheric constituents. However, standard limb profile retrieval techniques assume spherical symmetry and are vulnerable to biases produced by horizontal gradients in atmospheric parameters. We present a scheme for the correction of horizontal gradients in profile retrievals from limb observations of the martian atmosphere. It characterizes horizontal gradients in temperature, pressure, and aerosol extinction along the line-of-sight of a limb view through neighboring measurements, and represents these gradients by means of two-dimensional radiative transfer in the forward model of the retrieval. The scheme is applied to limb emission measurements from the Mars Climate Sounder instrument on Mars Reconnaissance Orbiter. Retrieval simulations using data from numerical models indicate that biases of up to 10 K in the winter polar region, obtained with standard retrievals using spherical symmetry, are reduced to about 2 K in most locations by the retrieval with two-dimensional radiative transfer. Retrievals from Mars atmospheric measurements suggest that the two-dimensional radiative transfer greatly reduces biases in temperature and aerosol opacity caused by observational geometry, predominantly in the polar winter regions.
TL;DR: In this article, an integrated self-consistent model developed to ensure the best accuracy is presented, which is also important to consider multiple sources of spectroscopic data for such a study in order to improve the dynamic range of the model and to minimize effects of instrumentation and associated systematic errors.
Abstract: Retrievals of atmospheric composition from near-infrared measurements require measurements of airmass to better than the desired precision of the composition. The oxygen bands are obvious choices to quantify airmass since the mixing ratio of oxygen is fixed over the full range of atmospheric conditions. The OCO-2 mission is currently retrieving carbon dioxide concentration using the oxygen A-band for airmass normalization. The 0.25% accuracy desired for the carbon dioxide concentration has pushed the required state-of-the-art for oxygen spectroscopy. To measure O2 A-band cross-sections with such accuracy through the full range of atmospheric pressure requires a sophisticated line-shape model (Rautian or Speed-Dependent Voigt) with line mixing (LM) and collision induced absorption (CIA). Models of each of these phenomena exist, however, this work presents an integrated self-consistent model developed to ensure the best accuracy. It is also important to consider multiple sources of spectroscopic data for such a study in order to improve the dynamic range of the model and to minimize effects of instrumentation and associated systematic errors. The techniques of Fourier Transform Spectroscopy (FTS) and Cavity Ring-Down Spectroscopy (CRDS) allow complimentary information for such an analysis. We utilize multispectrum fitting software to generate a comprehensive new database with improved accuracy based on these datasets. The extensive information will be made available as a multi-dimensional cross-section (ABSCO) table and the parameterization will be offered for inclusion in the HITRANonline database.
TL;DR: In this article, the axial and transverse radiation force cross-sections of optical tractor Bessel polarized beams are theoretically investigated for a dielectric sphere with particular emphasis on the beam topological charge (or order), half-cone angle and polarization.
Abstract: Axial and transverse radiation force cross-sections of optical tractor Bessel polarized beams are theoretically investigated for a dielectric sphere with particular emphasis on the beam topological charge (or order), half-cone angle and polarization. The angular spectrum decomposition method (ASDM) is used to derive the non-paraxial electromagnetic (EM) field components of the Bessel beams. The multipole expansion method using vector spherical harmonics is utilized and appropriate beam-shape coefficients are derived in order to compute the radiation force cross-sections. The analysis has no limitation to a particular range of frequencies such that the Rayleigh, Mie or geometrical optics regimes can all be considered effectively using the present rigorous formalism. The focus of this investigation is to identify some of the tractor beam conditions so as to achieve retrograde motion of a dielectric sphere located arbitrarily in space. Numerical computations for the axial and transverse radiation force cross-sections are presented for linear, right-circular, radial, azimuthal and mixed polarizations of the individual plane waves forming the Bessel beams of zeroth- and first-order (with positive or negative helicity), respectively. As the sphere shifts off the beam׳s axis, the axial pulling (tractor) force is weakened. Moreover, the transverse radiation force cross-section field changes with the sphere׳s size factor ka (where k is the wavenumber and a is the sphere radius). Both stable and unstable equilibrium regions around the beam׳s axis are found, depending on the choice of ka and the half-cone angle α0. These results are particularly important in the development of emergent technologies for the photophoretic assembly of optically-engineered (meta)materials with designed properties using optical tractor (vortex) beams, particle manipulation, levitation and positioning, and other applications.
TL;DR: In this paper, a pattern-free noncontact thermal modulator is proposed based on the mechanical rotation between two Van der Waals films with optical axes parallel to the surfaces, which can reach a value higher than 5 for hexagonal Boron Nitride (hBN) films separated by a nanoscale gap distance.
Abstract: Modulating heat flux provides a platform for a plethora of emerging devices such as thermal diodes, thermal transistors, and thermal memories. Here, a pattern-free noncontact thermal modulator is proposed based on the mechanical rotation between two Van der Waals films with optical axes parallel to the surfaces. A modulation contrast can reach a value higher than 5 for hexagonal Boron Nitride (hBN) films separated by a nanoscale gap distance. The dominant radiative heat exchange comes from the excitation of both Type I and Type II hyperbolic surface phonon polaritons (HSPhPs) at the vacuum-hBN interface for different orientations, while the large modulation contrast is mainly attributed to the mismatching Type I HSPhPs induced by rotation. This work opens the possibility to design cheap thermal modulators without relying on nanofabrication techniques, and paves the way to apply natural Van der Waals materials in manipulating heat currents in an active way.
TL;DR: In this paper, a line-by-line (LBL) algorithm was developed for use within the MODTRAN ® 6 1 atmospheric radiative transfer model to solve the 1-D scattering problem.
Abstract: A new line-by-line (LBL) algorithm has been developed for use within the MODTRAN ® 6 1 atmospheric radiative transfer model. The model computes both emitted and scattered line-of-sight radiances utilizing a spherical refractive geometry package and the DISORT discrete ordinate model to solve the 1-D scattering problem. The MODTRAN6 LBL method distinguishes itself from most other monochromatic models in that the radiative transfer problem is solved at arbitrarily fine spectral resolution within disjoint and contiguous 0.1 cm -1 steps, marching through the user-specified band pass. The advantage of this approach is that the predominantly Lorentzian, temperature and pressure dependent contributions to each 0.1 cm -1 spectral bin from molecular transitions centered more than 0.05 cm -1 from the bin can be summed off-line and fit to a simple analytic form. The line-shape of each molecular transition is explicitly modeled on-the-fly only over a narrow 0.2 cm -1 sub-region. The challenge of this approach is to ensure that spectral discontinuities do not arise at spectral bin edges, where the method for modeling absorption from individual molecular lines changes abruptly. Interpolations based on the radiative transfer physics of the pre-computed line tail data are introduced to produce a smooth transition across these edges. Spectral validations against LBLRTM verify the fidelity of the approach. The new MODTRAN LBL algorithm is used to quantify the accuracy of the MODTRAN band model and correlated- k statistical approaches under varying conditions. Future upgrades to the MODTRAN band model, correlated- k and LBL methods are also discussed.
TL;DR: In this article, the authors used the averaged energy difference method and the empirical expression for J ′ J ″ -dependence Voigt profiles based on these widths and the BT2 line list to generate high resolution ( Δ ν ˜ = 001 cm − 1 ) pressure broadened cross sections for a fixed range of temperatures and pressures between 300 and 2000 K and 0001-10 bar.
Abstract: Many atmospheres (cool stars, brown dwarfs, giant planets, extrasolar planets) are predominately composed of molecular hydrogen and helium H216O is one of the best measured molecules in extrasolar planetary atmospheres to date and a major compound in the atmospheres of brown-dwarfs and oxygen-rich cool stars, yet the scope of experimental and theoretical studies on the pressure broadening of water vapour lines by collision with hydrogen and helium remains limited Theoretical H2- and He-broadening parameters of water vapour lines (rotational quantum number J up to 50) are obtained for temperatures in the range 300–2000 K Two approaches for calculation of line widths were used: (i) the averaged energy difference method and (ii) the empirical expression for J ′ J ″ -dependence Voigt profiles based on these widths and the BT2 line list are used to generate high resolution ( Δ ν ˜ = 001 cm − 1 ) pressure broadened cross sections for a fixed range of temperatures and pressures between 300 and 2000 K and 0001–10 bar An interpolation procedure which can be used to determine cross sections at intermediate temperature and pressure is described Pressure broadening parameters and cross sections are presented in new ExoMol format
TL;DR: In this paper, a comprehensive theoretical development of possible reference approaches in modelling of radiation transfer in non-uniform gaseous media is developed within the framework of the Generalized SLW Model.
Abstract: A comprehensive theoretical development of possible reference approaches in modelling of radiation transfer in non-uniform gaseous media is developed within the framework of the Generalized SLW Model. The notion of absorption spectrum “correlation” adopted currently for global methods in gas radiation is critically revisited and replaced by a less restrictive concept of rank correlated spectrum. Within this framework it is shown that eight different reference approaches are possible, of which only three have been reported in the literature. Among the approaches presented is a novel Rank Correlated SLW Model, which is distinguished by the fact that i) it does not require the specification of a reference gas thermodynamic state, and ii) it preserves the emission term in the spectrally integrated Radiative Transfer Equation. Construction of this reference model requires only two absorption line blackbody distribution functions, and subdivision into gray gases can be performed using standard quadratures. Consequently, this new reference approach appears to have significant advantages over all other methods, and is, in general, a significant improvement in the global modelling of gas radiation. All reference approaches are summarized in the present work, and their use in radiative transfer prediction is demonstrated for simple example cases. Further, a detailed rigorous theoretical development of the improved methods is provided.
TL;DR: In this paper, the authors describe program dPotFit, which performs least-squares fits of diatomic molecule spectroscopic data consisting of any combination of microwave, infrared or electronic vibrational bands, fluorescence series, and tunneling predissociation level widths, involving one or more electronic states, and for appropriate systems, second virial coefficient data, to determine analytic potential energy functions defining the observed levels and other properties of each state.
Abstract: This paper describes program dPotFit, which performs least-squares fits of diatomic molecule spectroscopic data consisting of any combination of microwave, infrared or electronic vibrational bands, fluorescence series, and tunneling predissociation level widths, involving one or more electronic states and one or more isotopologs, and for appropriate systems, second virial coefficient data, to determine analytic potential energy functions defining the observed levels and other properties of each state. Four families of analytical potential functions are available for fitting in the current version of dPotFit: the Expanded Morse Oscillator (EMO) function, the Morse/Long-Range (MLR) function, the Double-Exponential/Long-Range (DELR) function, and the ‘Generalized Potential Energy Function׳ (GPEF) of Surkus, which incorporates a variety of polynomial functional forms. In addition, dPotFit allows sets of experimental data to be tested against predictions generated from three other families of analytic functions, namely, the ‘Hannover Polynomial’ (or “X-expansion”) function, and the ‘Tang–Toennies’ and Scoles–Aziz ‘HFD’, exponential-plus-van der Waals functions, and from interpolation-smoothed pointwise potential energies, such as those obtained from ab initio or RKR calculations. dPotFit also allows the fits to determine atomic-mass-dependent Born–Oppenheimer breakdown functions, and singlet-state Λ-doubling, or Σ 2 splitting radial strength functions for one or more electronic states. dPotFit always reports both the 95% confidence limit uncertainty and the “sensitivity” of each fitted parameter; the latter indicates the number of significant digits that must be retained when rounding fitted parameters, in order to ensure that predictions remain in full agreement with experiment. It will also, if requested, apply a “sequential rounding and refitting” procedure to yield a final parameter set defined by a minimum number of significant digits, while ensuring no significant loss of accuracy in the predictions yielded by those parameters.
TL;DR: In this paper, the second part of a series of investigation to develop algorithms for simultaneous retrieval of aerosol parameters and surface reflectance from the future hyperspectral and geostationary satellite sensors such as Tropospheric Emissions: Monitoring of POllution (TEMPO) is described.
Abstract: This paper describes the second part of a series of investigation to develop algorithms for simultaneous retrieval of aerosol parameters and surface reflectance from the future hyperspectral and geostationary satellite sensors such as Tropospheric Emissions: Monitoring of POllution (TEMPO). The information content in these hyperspectral measurements is analyzed for 6 principal components (PCs) of surface spectra and a total of 14 aerosol parameters that describe the columnar aerosol volume V total , fine-mode aerosol volume fraction, and the size distribution and wavelength-dependent index of refraction in both coarse and fine mode aerosols. Forward simulations of atmospheric radiative transfer are conducted for 5 surface types (green vegetation, bare soil, rangeland, concrete and mixed surface case) and a wide range of aerosol mixtures. It is shown that the PCs of surface spectra in the atmospheric window channel could be derived from the top-of-the-atmosphere reflectance in the conditions of low aerosol optical depth (AOD ≤ 0.2 at 550 nm), with a relative error of 1%. With degree freedom for signal analysis and the sequential forward selection method, the common bands for different aerosol mixture types and surface types can be selected for aerosol retrieval. The first 20% of our selected bands accounts for more than 90% of information content for aerosols, and only 4 PCs are needed to reconstruct surface reflectance. However, the information content in these common bands from each TEMPO individual observation is insufficient for the simultaneous retrieval of surface’s PC weight coefficients and multiple aerosol parameters (other than V total ). In contrast, with multiple observations for the same location from TEMPO in multiple consecutive days, 1–3 additional aerosol parameters could be retrieved. Consequently, a self-adjustable aerosol retrieval algorithm to account for surface types, AOD conditions, and multiple-consecutive observations is recommended to derive aerosol parameters and surface reflectance simultaneously from TEMPO.
TL;DR: In this paper, the authors compared ACE-FTS version 3.5 profiles that are collocated with MIPAS and MLS, and analyzed the differences between instrument retrievals for Northern and Southern hemispheres and for local morning and evening data.
Abstract: The atmospheric limb sounders, ACE-FTS on the SCISAT satellite, MIPAS on ESA׳s Envisat satellite, and MLS on NASA׳s Aura satellite, take measurements used to retrieve atmospheric profiles of O3, N2O, H2O, HNO3, and CO. Each was taking measurements between February 2004 and April 2012 (ACE-FTS and MLS are currently operational), providing hundreds of profile coincidences in the Northern and Southern hemispheres, and during local morning and evening. Focusing on determining diurnal and hemispheric biases in the ACE-FTS data, this study compares ACE-FTS version 3.5 profiles that are collocated with MIPAS and MLS, and analyzes the differences between instrument retrievals for Northern and Southern hemispheres and for local morning and evening data. For O3, ACE-FTS is typically within ±5% of mid-stratospheric MIPAS and MLS data and exhibits a positive bias of ~10 to 20% in the upper stratosphere – lower mesosphere. For H2O, ACE-FTS exhibits an average bias of −5% between 20 and 60 km. For N2O, ACE-FTS agrees with MIPAS and MLS within −20 to +10% up to 45 km and 35 km, respectively. For HNO3, ACE-FTS typically agrees within ±10% below 30 km, and exhibits a positive bias of ~10 to 20% above 30 km. With respect to MIPAS CO, ACE-FTS exhibits an average −11% bias between 28 and 50 km, and at higher altitudes a positive bias on the order of 10% (>100%) in the winter (summer). With respect to winter MLS CO, ACE-FTS is typically within ±10% between 25 and 40 km, and has an average bias of −11% above 40 km.
TL;DR: In this article, a fast superposition T-matrix solution for electromagnetic scattering by a collection of arbitrarily-shaped inhomogeneous particles is formulated by expanding the Green's dyadic in the spherical vector wave functions and formulating a volume integral equation.
Abstract: A fast superposition T-matrix solution is formulated for electromagnetic scattering by a collection of arbitrarily-shaped inhomogeneous particles. The T-matrices for individual constituents are computed by expanding the Green's dyadic in the spherical vector wave functions and formulating a volume integral equation, where the equivalent electric current is the unknown and the spherical vector wave functions are treated as excitations. Furthermore, the volume integral equation and the superposition T-matrix are accelerated by the precorrected-FFT algorithm and the fast multipole algorithm, respectively. The approach allows for an efficient scattering analysis of the clusters and aggregates consisting of a large number of arbitrarily-shaped inhomogeneous particles.
TL;DR: In this article, the theory and practical principles of simulation of optical tweezers, including the choice of method of calculation of optical force, numerical solution of the equations of motion of the particle, and finish with a discussion of a range of open problems.
Abstract: Computational modelling has made many useful contributions to the field of optical tweezers. One aspect in which it can be applied is the simulation of the dynamics of particles in optical tweezers. This can be useful for systems with many degrees of freedom, and for the simulation of experiments. While modelling of the optical force is a prerequisite for simulation of the motion of particles in optical traps, non-optical forces must also be included; the most important are usually Brownian motion and viscous drag. We discuss some applications and examples of such simulations. We review the theory and practical principles of simulation of optical tweezers, including the choice of method of calculation of optical force, numerical solution of the equations of motion of the particle, and finish with a discussion of a range of open problems.
TL;DR: In this paper, the impact of morphology on the radiative properties of fractal soot aggregates was investigated using the discrete dipole approximation (DDA) using the optical properties of four different types of aggregates of freshly emitted soot with a fractal dimension D f = 1.65 and a pre-factor k f =1.76 were calculated.
Abstract: The impact of morphology on the radiative properties of fractal soot aggregates was investigated using the discrete dipole approximation (DDA). The optical properties of four different types of aggregates of freshly emitted soot with a fractal dimension D f =1.65 and a fractal pre-factor k f =1.76 were calculated. The four types of aggregates investigated are formed by uniform primary particles in point-touch, by uniform but overlapping primary particles, by uniform but enlarged primary particles in point-touch, and formed by point-touch and polydisperse primary particles. The radiative properties of aggregates consisting of N =20, 56 and 103 primary particles were numerically evaluated for a given refractive index at 0.532 and 1.064 μm. The radiative properties of soot aggregates vary strongly with the volume equivalent radius a eff and wavelength. The accuracy of DDA was evaluated in the first and fourth cases against the generalized multi-sphere Mie (GMM) solution in terms of the vertical–vertical differential scattering cross section ( C vv ). The model predicted the average relative deviations from the base case to be within 15–25% for C vv , depending on the number of particles for the aggregate. The scattering cross sections are only slightly affected by the overlapping but more significantly influenced by primary particle polydispersity. It was also found that the enlargement of primary particles by 20% has a strong effect on soot aggregate radiative properties.
TL;DR: In this paper, the authors computed room temperature line lists for six symmetric isotopologues of carbon dioxide, covering the range 0-8000 cm−1, based on variational nuclear motion calculations and on a reliability analysis of the generated line intensities.
Abstract: Remote sensing experiments require high-accuracy, preferably sub-percent, line intensities and in response to this need we present computed room temperature line lists for six symmetric isotopologues of carbon dioxide: 13C16O2, 14C16O2, 12C17O2, 12C18O2, 13C17O2 and 13C18O2, covering the range 0–8000 cm−1. Our calculation scheme is based on variational nuclear motion calculations and on a reliability analysis of the generated line intensities. Rotation–vibration wavefunctions and energy levels are computed using the DVR3D software suite and a high quality semi-empirical potential energy surface (PES), followed by computation of intensities using an ab initio dipole moment surface (DMS). Four line lists are computed for each isotopologue to quantify sensitivity to minor distortions of the PES/DMS. Reliable lines are benchmarked against recent state-of-the-art measurements and against the HITRAN2012 database, supporting the claim that the majority of line intensities for strong bands are predicted with sub-percent accuracy. Accurate line positions are generated using an effective Hamiltonian. We recommend the use of these line lists for future remote sensing studies and their inclusion in databases.
TL;DR: In this article, a hybrid near-field radiative thermal modulator made of two graphene-covered silicon carbide (SiC) plates separated by a nanometer vacuum gap is proposed.
Abstract: In this work, we propose a hybrid near-field radiative thermal modulator made of two graphene-covered silicon carbide (SiC) plates separated by a nanometer vacuum gap. The near-field photon tunneling between the emitter and receiver is modulated by changing graphene chemical potentials with symmetrically or asymmetrically applied voltage biases. The radiative heat flux calculated from fluctuational electrodynamics significantly varies with graphene chemical potentials due to tunable near-field coupling strength between graphene plasmons across the vacuum gap. Thermal modulation and switching, which are the key functionalities required for a thermal modulator, are theoretically realized and analyzed. Newly introduced quantities of the modulation factor, the sensitivity factor and switching factor are studied quite extensively in a large parameter range for both graphene chemical potential and vacuum gap distance. This opto-electronic device with faster operating mode, which is in principle only limited by electronics and not by the thermal inertia, will facilitate the practical application of active thermal management, thermal circuits, and thermal computing with photon-based near-field thermal transport.
TL;DR: In this paper, the authors improved two-wavelength polarization Mie-scattering lidars at several main sites of the Asian dust and aerosol lidar observation network (AD-Net) by adding a nitrogen Raman scatter measurement channel at 607-nm and have conducted ground-based network observation with the improved Mie−Raman lidars (MRL) in East Asia since 2009.
Abstract: We improved two-wavelength polarization Mie-scattering lidars at several main sites of the Asian dust and aerosol lidar observation network (AD-Net) by adding a nitrogen Raman scatter measurement channel at 607 nm and have conducted ground-based network observation with the improved Mie–Raman lidars (MRL) in East Asia since 2009. This MRL provides 1 α+ 2 β +1 δ data at nighttime: extinction coefficient ( α 532 ), backscatter coefficient ( β 532 ), and depolarization ratio ( δ 532 ) of particles at 532 nm and an attenuated backscatter coefficient at 1064 nm ( β at ,1064 ). Furthermore, we developed a Multi-wavelength Mie-Raman lidar (MMRL) providing 2 α +3 β +2 δ data ( α at 355 and 532 nm; β at 355 and 532; β at at 1064 nm; and δ at 355 and 532 nm) and constructed MMRLs at several main sites of the AD-Net. We identified an aerosol-rich layer and height of the planetary boundary layer (PBL) using β at ,1064 data, and derived aerosol optical properties (AOPs, for example, α a , β a , δ a , and lidar ratio ( S a )). We demonstrated that AOPs cloud be derived with appropriate accuracy. Seasonal means of AOPs in the PBL were evaluated for each MRL observation site using three-year data from 2010 through 2012; the AOPs changed according to each season and region. For example, S a ,532 at Fukue, Japan, were 44±15 sr in winter and 49±17 in summer; those at Seoul, Korea, were 56±18 sr in winter and 62±15 sr in summer. We developed an algorithm to estimate extinction coefficients at 532 nm for black carbon, dust, sea-salt, and air-pollution aerosols consisting of a mixture of sulfate, nitrate, and organic-carbon substances using the 1 α 532 +2 β 532 and 1064 +1 δ 532 data. With this method, we assume an external mixture of aerosol components and prescribe their size distributions, refractive indexes, and particle shapes. We applied the algorithm to the observed data to demonstrate the performance of the algorithm and determined the vertical structure for each aerosol component.
TL;DR: In this paper, first-principle theoretical predictions of methane spectral line intensities that are competitive with (and complementary to) the best laboratory measurements are reported, and a detailed comparison with the most accurate data shows that discrepancies in integrated polyad intensities are in the range of 0.4% −2.3%.
Abstract: In this work, we report first-principle theoretical predictions of methane spectral line intensities that are competitive with (and complementary to) the best laboratory measurements. A detailed comparison with the most accurate data shows that discrepancies in integrated polyad intensities are in the range of 0.4%–2.3%. This corresponds to estimations of the best available accuracy in laboratory Fourier Transform spectra measurements for this quantity. For relatively isolated strong lines the individual intensity deviations are in the same range. A comparison with the most precise laser measurements of the multiplet intensities in the 2ν3 band gives an agreement within the experimental error margins (about 1%). This is achieved for the first time for five-atomic molecules. In the Supplementary Material we provide the lists of theoretical intensities at 269 K for over 5000 strongest transitions in the range below 6166 cm−1. The advantage of the described method is that this offers a possibility to generate fully assigned exhaustive line lists at various temperature conditions. Extensive calculations up to 12,000 cm−1 including high-T predictions will be made freely available through the TheoReTS information system (http://theorets.univ-reims.fr, http://theorets.tsu.ru) that contains ab initio born line lists and provides a user-friendly graphical interface for a fast simulation of the absorption cross-sections and radiance.
TL;DR: In this article, the authors developed an idealized model to account for the effects of non-absorptive coating on the optical properties of black carbon (BC) aggregates, and applied the classic fractal aggregate to represent realistic BC particles, and the coating is assumed to be spherical.
Abstract: This study develops an idealized model to account for the effects of non-absorptive coating on the optical properties of black carbon (BC) aggregates. The classic fractal aggregate is applied to represent realistic BC particles, and the coating is assumed to be spherical. To accelerate the single-scattering simulation, BC monomers that were overlapped with coating sphere (not those completely inside the coating) are slightly moved to avoid overlapping. The multiple-sphere T-matrix method (MSTM) becomes applicable to calculate the optical properties of inhomogeneous particles with any coating amount, and is generally two orders of magnitude faster than the discrete-dipole approximation for particles we considered. Furthermore, the simple spherical coating is found to have similar effects on the optical properties to those based on more complicated coating structure. With the simple particle model and the efficient MSTM, it becomes possible to consider the influence of coating with much more details. The non-absorptive coating of BC aggregates can significantly enhance BC extinction and absorption, which is consistent with previous studies. The absorption of coated aggregates can be over two times stronger than that of BC particles without coating. Besides the coating volume, the relative position between the mass centers of BC aggregate and coating also plays an important role on the optical properties, and should obviously be considered in further studies.