LÉNÁRD VÁMOS, SIMULATION MODELS FOR AEROSOL CHARACTERIZATION BY ELASTIC LIGHT SCATTERING WITH

SPECIAL EMPHASIS ON PHOTON CORRELATION EXPERIMENTS IN THE NANO-PARTICLE SIZE RANGE, PHD THESIS, 2010

Summary

Exotic mechanical, optical, biochemical and catalytic properties make nanoparticles (particles
smaller than 100 nanometers) of special interest. The widening application fields require more
and more information about the particles. Very often the optical methods are the only way to
study aerosol properties (astronomic observation, solar photometry, satellite remote sensing,
real-time non intrusive flow or combustion analysis etc.). Elastic light scattering
measurements and the theoretical interpretation of such data yield precise determination of
size, refractive index, shape, orientation etc. The Lorenz-Mie theory as a classical
electromagnetic approach was used for the problem of homogenous spheres, single layered
spheres and cylinders. More than 100 years experience assures the validity of the calculus;
however the applications for nanoparticles were not in the focus till nowadays. Measurement
simulation is a cost effective and fast method for the characterization and optimization of
measurement parameters, developing new characterization methods. Furthermore
measurement simulations can play a central roll in the model-based signal processing
methods.
The central theme of this thesis is the real-time characterization of aerosols especially in the
submicron/nanometer size range (below 500nm) which is extremely required for both the
research area and the industry.
Elastic light scattering properties of water coated carbon spheres as typical rain droplets in
urban atmosphere are studied in the submicron size range illuminated by unpolarized visible
light. I have demonstrated that the scattered intensity measurements on one-layered single
particles of known size or their monodisperse ensemble make possible the rough estimation
(within 10% uncertainty) of the layer thickness smaller than the core radius.
A simple and direct particle counting method is proposed for monodisperse ensembles
independent of the wavelength and refractive index.
Laser Doppler anemometry/velocimetry (LDA/LDV) offers a non-intrusive in-situ single
particle characterization solution among the several particle characterization methods, that’s
why it is commonly used both in scientific and industrial environments, especially in extreme
conditions. The high detection sensitivity required for nanoparticles can be reached by using
the detectors in Geiger-mode with photon correlation method to estimate the flow velocity.
An accurate new method was proposed for timing jitter measurements of single photon
counting detectors. In my diploma work a refined method was developed for the nanoparticle
sizing based on the measurements of the signal visibility, called R parameter method. In this
thesis the scattering amplitude method is proposed due to its high sensitivity. By the complete
simulation of the measurement including particle flow, elastic scattering, data acquisition etc.
a complex signal processing method was developed for simultaneous particle counting, sizing
and velocity estimation by the standard dual-beam LDA system in photon correlation mode.
The particle counting technique is adapted from the Time Correlated Single Photon Counting
method and developed to the particulate requirements of the photon-correlation LDA. Then a
model-based optimization method is proposed for submicron/nanometer particle sizing based
on scattered intensity. Although the method requires calibration, the procedure becomes
simplified by the help of the simulation software package.
The construction of the first prototype is supported by a grant from the Central Hungary
Operational Programme (project number: KMOP-1.1.1-07/1-2008-0056, short name: NANO-
LDA). Several research labs and high-ranking companies in the nanoparticle production area
(such as Degussa AG, Heraus Quartz Glass company) show interest in the NANO-LDA
project.