Time Dependence of Ultra-Short Laser Pulses Scattering by Atom in High Frequency Limit

We investigated theoretically the time dependence of ultra-short laser pulse scattering by an atom at the high-frequency limit for the spectral and total probability of the process using new expression which we derived in this paper. We established that the time dependence of spectral scattering is presented by the curve with the maximum for sufficiently large detuning of scattering frequency from the carrier frequency of the pulse, while the total scattering probability is always the monotonically increasing function of time. We also studied the dependence of scattering probability on pulse duration at the long-time limit. It was shown that, at the long-pulse limit, the scattering probability is a linear function of pulse duration, while in the opposite case, it is a function with maximum. The position of this maximum is determined by the detuning of the scattering frequency from the carrier frequency of the pulse.

The CU 2-D-MAX-DOAS instrument – Part 2: Raman scattering probability measurements and retrieval of aerosol optical properties

The multiannual global mean of aerosol optical depth at 550 nm (AOD550) over land is ∼ 0.19, and that over oceans is ∼ 0.13. About 45 % of the Earth surface shows AOD550 smaller than 0.1. There is a need for measurement techniques that are optimized to measure aerosol optical properties under low AOD conditions. We present an inherently calibrated retrieval (i.e., no need for radiance calibration) to simultaneously measure AOD and the aerosol phase function parameter, g, based on measurements of azimuth distributions of the Raman scattering probability (RSP), the near-absolute rotational Raman scattering (RRS) intensity. We employ radiative transfer model simulations to show that for solar azimuth RSP measurements at solar elevation and solar zenith angle (SZA) smaller than 80°, RSP is insensitive to the vertical distribution of aerosols and maximally sensitive to changes in AOD and g under near-molecular scattering conditions. The University of Colorado two-dimensional Multi-AXis Differential Optical Absorption Spectroscopy (CU 2-D-MAX-DOAS) instrument was deployed as part of the Two Column Aerosol Project (TCAP) at Cape Cod, MA, during the summer of 2012 to measure direct sun spectra and RSP from scattered light spectra at solar relative azimuth angles (SRAAs) between 5 and 170°. During two case study days with (1) high aerosol load (17 July, 0.3 < AOD430 < 0.6) and (2) near-molecular scattering conditions (22 July, AOD430 < 0.13) we compare RSP-based retrievals of AOD430 and g with data from a co-located CIMEL sun photometer, Multi-Filter Rotating Shadowband Radiometer (MFRSR), and an airborne High Spectral Resolution Lidar (HSRL-2). The average difference (relative to DOAS) for AOD430 is +0.012 ± 0.023 (CIMEL), −0.012 ± 0.024 (MFRSR), −0.011 ± 0.014 (HSRL-2), and +0.023 ± 0.013 (CIMELAOD − MFRSRAOD) and yields the following expressions for correlations between different instruments: DOASAOD = −(0.019 ± 0.006) + (1.03 ± 0.02) × CIMELAOD (R2 = 0.98), DOASAOD = −(0.006 ± 0.005) + (1.08 ± 0.02) × MFRSRAOD (R2 = 0.98), and CIMELAOD = (0.013 ± 0.004) + (1.05 ± 0.01) × MFRSRAOD (R2 = 0.99). The average g measured by DOAS on both days was 0.66 ± 0.03, with a difference of 0.014 ± 0.05 compared to CIMEL. Active steps to minimize the error in the RSP help to reduce the uncertainty in retrievals of AOD and g. As AOD decreases and SZA increases, the RSP signal-to-noise ratio increases. At AOD430 ∼ 0.4 and 0.10 the absolute AOD errors are ∼ 0.014 and 0.003 at 70° SZA and 0.02 and 0.004 at 35° SZA. Inherently calibrated, precise AOD and g measurements are useful to better characterize the aerosol direct effect in urban polluted and remote pristine environments.

The CU 2D-MAX-DOAS instrument - part 2: Raman Scattering Probability Measurements and Retrieval of Aerosol Optical Properties

The multiannual global mean of aerosol optical depth at 550 nm (AOD550) over land is ~0.19, and that over oceans is ~0.13. About 45% of the Earth surface shows AOD550 smaller than 0.1. There is a need for measurement techniques that are optimized to measure aerosol optical properties under low AOD conditions. We present an inherently calibrated retrieval (i.e., no need for radiance calibration) to simultaneously measure AOD and the aerosol phase function parameter, g, based on measurements of azimuth distributions of the Raman Scattering Probability (RSP), the near-absolute Rotational Raman Scattering (RRS) intensity. We employ Radiative Transfer Model simulations to show that solar azimuth RSP measurements are insensitive to the vertical distribution of aerosols, and maximally sensitive to changes in AOD and g under near molecular scattering conditions. The University of Colorado two dimensional Multi-AXis Differential Optical Absorption Spectroscopy (CU 2D-MAX-DOAS) instrument was deployed as part of the Two Column Aerosol Project (TCAP) at Cape Cod, MA, during the summer of 2012 to measure direct sun spectra, and RSP from scattered light spectra at solar relative azimuth angles (SRAA) between 5° and 170°. During two case study days with (1) high aerosol load (17 July, 0.3 < AOD430 < 0.6) and (2) near-molecular scattering conditions (22 July, AOD430 < 0.13) we compare RSP based retrievals of AOD430 and g with data from a co-located CIMEL sun photometer, Multi-Filter Rotating Shadowband Radiometer (MFRSR), and airborne High Spectral Resolution Lidar (HSRL-2). The average difference (relative to DOAS) for AOD430 is: +0.012 ± 0.023 (CIMEL), –0.012 ± 0.024 (MFRSR), –0.011 ± 0.014 (HSRL-2), and +0.023 ± 0.013 (CIMEL – MFSRS); and yields the following expressions for correlations between different instruments: DOASAOD = –(0.019 ± 0.006) + (1.03 ± 0.02)·CIMELAOD (R2 = 0.98), DOAS = –(0.006 ± 0.005) + (1.08 ± 0.02)·MFRSRAOD (R2 = 0.98), and CIMELAOD = (0.013 ± 0.004) + (1.05 ± 0.01)·MFRSR = 0.99). The average g measured by DOAS on both days was 0.66 ± 0.03, with a difference of 0.014 ± 0.05 compared to CIMEL. Active steps to minimize RSP in the reference spectrum help to reduce the uncertainty in RSP retrievals of AOD and g. As AOD decreases, and solar zenith angle (SZA) increases the RSP signal-to-noise ratio increases. At AOD430 ~ 0.4 and 0.10 the absolute AOD errors are ~0.014 and 0.003 at 70° SZA, and 0.02 and 0.004 at 35° SZA. Inherently calibrated, precise AOD and g measurements are useful to better characterize the aerosol direct effect in urban polluted and remote pristine environments.

Three-dimensional simulation of the Ring effect in observations of scattered sun light using Monte Carlo radiative transfer models

We present a new technique for the quantitative simulation of the "Ring effect" for scattered light observations from various platforms and under different atmospheric situations. The method is based on radiative transfer calculations at only one wavelength λ0 in the wavelength range under consideration, and is thus computationally fast. The strength of the Ring effect is calculated from statistical properties of the photon paths for a given situation, which makes Monte Carlo radiative transfer models in particular appropriate. We quantify the Ring effect by the so called rotational Raman scattering probability, the probability that an observed photon has undergone a rotational Raman scattering event. The Raman scattering probability is independent from the spectral resolution of the instrument and can easily be converted into various definitions used to characterise the strength of the Ring effect. We compare the results of our method to the results of previous studies and in general good quantitative agreement is found. In addition to the simulation of the Ring effect, we developed a detailed retrieval strategy for the analysis of the Ring effect based on DOAS retrievals, which allows the precise determination of the strength of the Ring effect for a specific wavelength while using the spectral information within a larger spectral interval around the selected wavelength. Using our technique, we simulated synthetic satellite observation of an atmospheric scenario with a finite cloud illuminated from different sun positions. The strength of the Ring effect depends systematically on the measurement geometry, and is strongest if the satellite points to the side of the cloud which lies in the shadow of the sun.