scholarly journals High-resolution optical constants of crystalline ammonium nitrate for infrared remote sensing of the Asian Tropopause Aerosol Layer

2021 ◽  
Vol 14 (3) ◽  
pp. 1977-1991
Author(s):  
Robert Wagner ◽  
Baptiste Testa ◽  
Michael Höpfner ◽  
Alexei Kiselev ◽  
Ottmar Möhler ◽  
...  

Abstract. Infrared spectroscopic observations have shown that crystalline ammonium nitrate (AN) particles are an abundant constituent of the upper tropospheric aerosol layer which is formed during the Asian summer monsoon period, the so-called Asian Tropopause Aerosol Layer (ATAL). At upper tropospheric temperatures, the thermodynamically stable phase of AN is different from that at 298 K, meaning that presently available room-temperature optical constants of AN, that is, the real and imaginary parts of the complex refractive index, cannot be applied for the quantitative analysis of these infrared measurements. In this work, we have retrieved the first low-temperature data set of optical constants for crystalline AN in the 800–6000 cm−1 wavenumber range with a spectral resolution of 0.5 cm−1. The optical constants were iteratively derived from an infrared extinction spectrum of 1 µm sized AN particles suspended in a cloud chamber at 223 K. The uncertainties of the new data set were carefully assessed in a comprehensive sensitivity analysis. We show that our data accurately fit aircraft-borne infrared measurements of ammonium nitrate particles in the ATAL.

2020 ◽  
Author(s):  
Robert Wagner ◽  
Baptiste Testa ◽  
Michael Höpfner ◽  
Alexei Kiselev ◽  
Ottmar Möhler ◽  
...  

Abstract. Infrared spectroscopic observations have shown that crystalline ammonium nitrate (AN) particles are an abundant constituent of the upper tropospheric aerosol layer which is formed during the Asian summer monsoon period, the so-called Asian Tropopause Aerosol Layer (ATAL). At upper tropospheric temperatures, the thermodynamically stable phase of AN is different from that at 298 K, meaning that presently available room-temperature optical constants of AN, that is, the real and imaginary parts of the complex refractive index, cannot be applied for the quantitative analysis of these infrared measurements. In this work, we have retrieved the first low-temperature data set of optical constants for crystalline AN in the 800–6000 cm−1 wavenumber range with a spectral resolution of 0.5 cm−1. The optical constants were iteratively derived from an infrared extinction spectrum of 1 micrometer-sized AN particles suspended in a cloud chamber at 223 K. The uncertainties of the new data set were carefully assessed in a comprehensive sensitivity analysis. We show that our data accurately fit aircraft-borne infrared measurements of ammonium nitrate particles in the ATAL.


2020 ◽  
Vol 74 (8) ◽  
pp. 868-882
Author(s):  
Tanya L. Myers ◽  
Thomas A. Blake ◽  
Michael O. Yokosuk ◽  
Gilles Fortin ◽  
Timothy J. Johnson

Infrared reflectance analysis is facilitated via the comparison of spectra recorded in situ to a databank of actual or synthetic infrared reflectance spectra. It has recently been shown that reference spectra corresponding to the many different morphological forms of the same chemical can be generated synthetically using the imaginary, k, and real, n, components of the complex refractive index, [Formula: see text] =  n + i k. One method to obtain the n and k vectors is infrared ellipsometry, which measures the changes in amplitude, tan Ψ, and phase, Δ, of polarized light reflected from the sample both as a function of wavenumber and angle of incidence. The method requires specularly reflected light, so best results are usually obtained with polished planar samples of large surface area. Due to the difficulties of obtaining such samples, however, we investigate the possibility of pressing powders of neat materials and obtaining the corresponding optical constants from the pellets. In this paper, variability in the sample pellet and preparation method is investigated, as is variability in the fitting procedure for the derived optical constants. The n/k vectors are derived from the measured ellipsometric parameters, tan ψ and Δ, as they are fit by an oscillator model which yield n([Formula: see text]) and k([Formula: see text]) vectors as a function of wavenumber, [Formula: see text]. Construction of the oscillator model is not automatic and depends on significant input from the analyst as well as the sample’s physical characteristics. For pellet pressing, the experimental variability was found to be minimized for size-selected powdered samples as gauged by the minimal variance in ψ and Δ for three different pellets; similarly, the analytical precision for multiple measurements of the same pellet was also quite good, suggesting that a pressed pellet is a viable sample preparation method. Experimental variabilities were comparatively small; the greatest variability came in the analytic fitting procedure with differences in the k-peak values up to 10% for only the sharpest bands arising from four different fits to the same data set. The final ellipsometric n/k data are compared to literature values obtained from crystalline ammonium sulfate ((NH4)2SO4) samples as well as single-angle reflectance measurements that also used pressed pellets. Comparison with the previous literature values shows generally good agreement, although larger k-values are observed for the independent sets of data derived from pressed pellets. These data are suggested as an improved set of optical constants for (NH4)2SO4.


2017 ◽  
Vol 114 (27) ◽  
pp. 6972-6977 ◽  
Author(s):  
Pengfei Yu ◽  
Karen H. Rosenlof ◽  
Shang Liu ◽  
Hagen Telg ◽  
Troy D. Thornberry ◽  
...  

An enhanced aerosol layer near the tropopause over Asia during the June–September period of the Asian summer monsoon (ASM) was recently identified using satellite observations. Its sources and climate impact are presently not well-characterized. To improve understanding of this phenomenon, we made in situ aerosol measurements during summer 2015 from Kunming, China, then followed with a modeling study to assess the global significance. The in situ measurements revealed a robust enhancement in aerosol concentration that extended up to 2 km above the tropopause. A climate model simulation demonstrates that the abundant anthropogenic aerosol precursor emissions from Asia coupled with rapid vertical transport associated with monsoon convection leads to significant particle formation in the upper troposphere within the ASM anticyclone. These particles subsequently spread throughout the entire Northern Hemispheric (NH) lower stratosphere and contribute significantly (∼15%) to the NH stratospheric column aerosol surface area on an annual basis. This contribution is comparable to that from the sum of small volcanic eruptions in the period between 2000 and 2015. Although the ASM contribution is smaller than that from tropical upwelling (∼35%), we find that this region is about three times as efficient per unit area and time in populating the NH stratosphere with aerosol. With a substantial amount of organic and sulfur emissions in Asia, the ASM anticyclone serves as an efficient smokestack venting aerosols to the upper troposphere and lower stratosphere. As economic growth continues in Asia, the relative importance of Asian emissions to stratospheric aerosol is likely to increase.


2015 ◽  
Vol 15 (10) ◽  
pp. 5429-5442 ◽  
Author(s):  
E. Giannakaki ◽  
A. Pfüller ◽  
K. Korhonen ◽  
T. Mielonen ◽  
L. Laakso ◽  
...  

Abstract. Raman lidar data obtained over a 1 year period has been analysed in relation to aerosol layers in the free troposphere over the Highveld in South Africa. In total, 375 layers were observed above the boundary layer during the period 30 January 2010 to 31 January 2011. The seasonal behaviour of aerosol layer geometrical characteristics, as well as intensive and extensive optical properties were studied. The highest centre heights of free-tropospheric layers were observed during the South African spring (2520 ± 970 m a.g.l., also elsewhere). The geometrical layer depth was found to be maximum during spring, while it did not show any significant difference for the rest of the seasons. The variability of the analysed intensive and extensive optical properties was high during all seasons. Layers were observed at a mean centre height of 2100 ± 1000 m with an average lidar ratio of 67 ± 25 sr (mean value with 1 standard deviation) at 355 nm and a mean extinction-related Ångström exponent of 1.9 ± 0.8 between 355 and 532 nm during the period under study. Except for the intensive biomass burning period from August to October, the lidar ratios and Ångström exponents are within the range of previous observations for urban/industrial aerosols. During Southern Hemispheric spring, the biomass burning activity is clearly reflected in the optical properties of the observed free-tropospheric layers. Specifically, lidar ratios at 355 nm were 89 ± 21, 57 ± 20, 59 ± 22 and 65 ± 23 sr during spring (September–November), summer (December–February), autumn (March–May) and winter (June–August), respectively. The extinction-related Ångström exponents between 355 and 532 nm measured during spring, summer, autumn and winter were 1.8 ± 0.6, 2.4 ± 0.9, 1.8 ± 0.9 and 1.8 ± 0.6, respectively. The mean columnar aerosol optical depth (AOD) obtained from lidar measurements was found to be 0.46 ± 0.35 at 355 nm and 0.25 ± 0.2 at 532 nm. The contribution of free-tropospheric aerosols on the AOD had a wide range of values with a mean contribution of 46%.


2018 ◽  
Vol 25 (5) ◽  
pp. 1433-1443
Author(s):  
C. Jansing ◽  
H. Wahab ◽  
H. Timmers ◽  
A. Gaupp ◽  
H.-C. Mertins

The complex refractive index of many materials is poorly known in the soft X-ray range across absorption edges. This is due to saturation effects that occur there in total-electron-yield and fluorescence-yield spectroscopy and that are strongest at resonance energies. Aiming to obtain reliable optical constants, a procedure that reconciles electron-yield measurements and reflection spectroscopy by correcting these saturation effects is presented. The procedure takes into account the energy- and polarization-dependence of the photon penetration depth as well as the creation efficiency for secondary electrons and their escape length. From corrected electron-yield spectra the absorption constants and the imaginary parts of the refractive index of the material are determined. The real parts of the index are subsequently obtained through a Kramers–Kronig transformation. These preliminary optical constants are refined by simulating reflection spectra and adapting them, so that measured reflection spectra are reproduced best. The efficacy of the new procedure is demonstrated for graphite. The optical constants that have been determined for linearly polarized synchrotron light incident with p- and s-geometry provide a detailed and reliable representation of the complex refractive index of the material near π- and σ-resonances. They are also suitable for allotropes of graphite such as graphene.


2001 ◽  
Vol 79 (1) ◽  
pp. 61-78 ◽  
Author(s):  
S. Ishii ◽  
T. Shibata ◽  
T. Sakai ◽  
M. Kido ◽  
K. Hara ◽  
...  

Author(s):  
Ruey-Shiang Shaw ◽  
Sheng-Pao Shih ◽  
Ta-Yu Fu ◽  
Chia-Wen Tsai

The software industry faces drastic changes in technology and business operations. The research structure of this study is based on the business model for software industries proposed by Rajala in 2003. The researcher employed an ex post facto research design to conduct a case study of the Galaxy Software Service Co., a company that is representative of the software industry in Taiwan. The main research goal of this study is to explore how this particular company developed into a large software company in the Taiwanese software sector, which is characterized by a prevalence of small- and medium-sized businesses, over a period of 25 years. This study employs a case study design and relies on in-depth participation and interviews to acquire a complete data set of the company’s internal operations. The evolution of the business model from the company’s inception until the present day has been divided into four phases: the entrepreneur phase, the growth phase, the stable phase, and the innovative breakthrough phase. The company developed into a major player in the software industry for 3 reasons: it has always insisted on a product differentiation strategy based on the sole reliance on software products, it started out as a software products dealer and gradually developed its own research and development capability, and it built a large-scale project management capability and received CMMI certification. These factors make the company stand out from other System Integrated businesses in the Taiwanese software sector offering both hardware and software products.


2019 ◽  
Vol 19 (13) ◽  
pp. 8399-8406 ◽  
Author(s):  
Qianshan He ◽  
Jianzhong Ma ◽  
Xiangdong Zheng ◽  
Xiaolu Yan ◽  
Holger Vömel ◽  
...  

Abstract. We measured the vertical profiles of backscatter ratio (BSR) using the balloon-borne, lightweight Compact Optical Backscatter AerosoL Detector (COBALD) instruments above Linzhi, located in the southeastern Tibetan Plateau, in the summer of 2014. An enhanced aerosol layer in the upper troposphere–lower stratosphere (UTLS), with BSR (455 nm) > 1.1 and BSR (940 nm) > 1.4, was observed. The color index (CI) of the enhanced aerosol layer, defined as the ratio of aerosol backscatter ratios (ABSRs) at wavelengths of 940 and 455 nm, varied from 4 to 8, indicating the prevalence of fine particles with a mode radius of less than 0.1 µm. We find that unlike the very small particles (mode radius smaller than 0.04 µm) at low relative humidity (RHi < 40 %), the relatively large particles in the aerosol layer were generally very hydrophilic as their size increased dramatically with relative humidity. This result indicates that water vapor can play a very important role in increasing the size of fine particles in the UTLS over the Tibetan Plateau. Our observations provide observation-based evidence supporting the idea that aerosol particle hygroscopic growth is an important factor influencing the radiative properties of the Asian Tropopause Aerosol Layer (ATAL) during the Asian summer monsoon.


2018 ◽  
Vol 176 ◽  
pp. 05055 ◽  
Author(s):  
S. Samoilova ◽  
M. Sviridenkov ◽  
I. Penner ◽  
G. Kokhanenko ◽  
Yu. Balin

Regular lidar measurements of the vertical distribution of aerosol optical parameters are carried out in Tomsk (56°N, 85°E) since April, 2011. We present the results of retrieval of microphysical characteristics from the data of measurements by means of Raman lidar in 2013. Section 2 is devoted to the theoretical aspects of retrieving the particle size distribution function U(r) (SDF) assuming a known complex refractive index m (CRI). It is shown that the coarse fraction cannot be retrieved unambiguously. When estimating U(r) and m together (section 3), the retrieved refractive index is non-linearly related to the optical coefficients and the distribution function, which leads to appearance of different, including false values of m. The corresponding U(r) differs only slightly, so the inaccuracy in m does not essentially affect the retrieval of the distribution function.


2018 ◽  
Vol 11 (6) ◽  
pp. 3339-3350 ◽  
Author(s):  
Andreas Schneider ◽  
Tobias Borsdorff ◽  
Joost aan de Brugh ◽  
Haili Hu ◽  
Jochen Landgraf

Abstract. A new data set of vertical column densities of the water vapour isotopologues H2O and HDO from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) instrument for the whole of the mission period from January 2003 to April 2012 is presented. The data are retrieved from reflectance measurements in the spectral range 2339 to 2383 nm with the Shortwave Infrared CO Retrieval (SICOR) algorithm, ignoring atmospheric light scattering in the measurement simulation. The retrievals are validated with ground-based Fourier transform infrared measurements obtained within the Multi-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water (MUSICA) project. A good agreement for low-altitude stations is found with an average bias of −3.6×1021 for H2O and −1.0×1018 molec cm−2 for HDO. The a posteriori computed δD shows an average bias of −8 ‰, even though polar stations have a larger negative bias. The latter is due to the large amount of sensor noise in SCIAMACHY in combination with low albedo and high solar zenith angles. To demonstrate the benefit of accounting for light scattering in the retrieval, the quality of the data product fitting effective cloud parameters simultaneously with trace gas columns is evaluated in a dedicated case study for measurements round high-altitude stations. Due to a large altitude difference between the satellite ground pixel and the mountain station, clear-sky scenes yield a large bias, resulting in a δD bias of 125 ‰. When selecting scenes with optically thick clouds within 1000 m above or below the station altitude, the bias in a posteriori δD is reduced from 125 to 44 ‰. The insights from the present study will also benefit the analysis of the data from the new Sentinel-5 Precursor mission.


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