Regularized Inversion of Aerosol Hygroscopic Growth Factor Probability Density Function: Application to Humidity-Controlled Fast Integrated Mobility Spectrometer Measurements

WashU affiliated authors: Jiaoshi Zhang; Jian Wang (Center for Aerosol Science and Engineering)

Abstract:  Aerosol hygroscopic growth plays an important role in atmospheric particle chemistry and the effects of aerosol on radiation and hence climate. The hygroscopic growth is often characterized by a growth factor probability density function (GF-PDF), where the growth factor is defined as the ratio of the particle size at a specified relative humidity to its dry size. Parametric, least-square methods are the most widely used algorithms for inverting the GF-PDF from measurements of humidified tandem differential mobility analyzers (HTDMA) and have been recently applied to the GF-PDF inversion from measurements of the humidity-controlled fast integrated mobility spectrometer (HFIMS). However, these least square methods suffer from noise amplification due to the lack of regularization in solving the ill-posed problem, resulting in significant fluctuations in the retrieved GF-PDF and even occasional failures of convergence. In this study, we introduce nonparametric, regularized methods to invert aerosol GF-PDF and apply them to HFIMS measurements. Based on the HFIMS kernel function, the forward convolution is transformed into a matrix-based form, which facilitates the application of the nonparametric inversion methods with regularizations, including Tikhonov regularization and Twomey’s iterative regularization. Inversions of the GF-PDF using the nonparameteric methods with regularization are demonstrated using HFIMS measurements simulated from representative GF-PDFs of ambient aerosols. The characteristics of reconstructed GF-PDFs resulting from different inversion methods, including previously developed least-square methods, are quantitively compared. The result shows that Twomey’s method generally outperforms other inversion methods. The capabilities of the Twomey’s method in reconstructing the pre-defined GF-PDFs and recovering the mode parameters are validated.

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