Abstract

Dynamic light scattering (DLS) is a popular method of particle size measurement, but at ultra-low particle concentrations, the occurrence of number concentration fluctuations limits the use of the technique. Number fluctuations add a non-Gaussian term to the scattered light intensity autocorrelation function (ACF). This leads to an inaccurate particle size distribution (PSD) being recovered if the normal DLS analysis model is used. We propose two methods for inverting the DLS data and recovering the PSDs when number fluctuations are apparent. One is to directly establish the relationship between the non-Gaussian ACF and the PSD by the kernel function reconstruction (KFR) method while including the non-Gaussian term to recover the PSD. The other is to remove the effect of the non-Gaussian term in the ACF by the baseline reset (BR) method. By including the number fluctuation term, the ideal recovered PSD can be obtained from the simulated data, but this will not happen in the experimental measurement data. This is because the measured intensity ACF contains more noise than the simulated ACF at ultra-low concentration. In particular, the baseline noise at the tail of long delay time of ACF overwhelms the number fluctuation term, making it difficult to recover reliable PSD data. Resetting the baseline can effectively remove the digital fluctuation term in ACF, which is also a feasible method to improve PSD recovery under ultra-low concentration. However, increasing noise at ultra-low concentrations can lead to errors in determining an effective baseline. This greatly reduces the accuracy of inversion results. Results from simulated and measured ACF data show that, for both methods, noise on the ACF limits reliable PSD recovery.

Highlights

  • Dynamic light scattering (DLS) was pioneered in the 1960s [1,2,3] and is commonly called photon correlation spectroscopy (PCS) because the experiment is done using digital correlation of photon count signals [4,5]

  • Particle size and particle size distribution (PSD) determination essentially occurs by measuring the diffusion coefficients of the particles undergoing Brownian motion in a small scattering volume

  • The usual method, the kernel function reconstruction (KFR) method, and the baseline reset (BR) method were compared using eight samples of simulated data consisting of two unimodal PSDs at ultra-low concentration

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Summary

Introduction

Dynamic light scattering (DLS) was pioneered in the 1960s [1,2,3] and is commonly called photon correlation spectroscopy (PCS) because the experiment is done using digital correlation of photon count signals [4,5] This technique has been widely applied to measure particle size in many fields such as materials, chemical industry, food, biology and medicine [6,7,8,9,10]. Particle size and particle size distribution (PSD) determination essentially occurs by measuring the diffusion coefficients of the particles undergoing Brownian motion in a small scattering volume This is done by analyzing the timescale of the fluctuations in the intensity of the light scattered from the particles. These fluctuation components will occur on different timescales and with different amplitudes

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