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SPARCLE




Introduction

SPARCLE is an advanced Optical Particle Counter, OPC. In a conventional OPC, an individual particle is illuminated by a light source the scattering intensity is then measured. This measurement is then related to the size of the particle from a calibration curve. Unfortunately the light intensity is also a function of the particles refractive index. For a synthetic aerosol made from one material this is of little consequence but for a mixed aerosols such as those found in the atmosphere errors can be as large as a factor of three (Willeke 1993). SPARCLE turns this dependence on it's head, inferring both the refractive index and particle size, offering a unique concept for aerosol measurement.

No aerosol instrument currently exists with this capability and this makes SPARCLE an ideal instrument to study the radiative impact of aerosols a recognised area of uncertainty in the assessment of climate change (IPCC, 2007). Integration of individual particle quantities can give properties of the aerosol, such as, particle size distribution, the total aerosol phase function and the single scatter albedo.


Instrument history

Phase I instrument

A proof-of-concept Stratospheric Aerosol Composition and Loading Experiment (SPARCLE) instrument was designed and developed by Dr Gareth Thomas to measure the complex refractive index and size of individual aerosol particles. Basic principles were observed and reported during this work at University of Canterbury, New Zealand under the supervision of Dr Grainger. Development the mathematical tools and algorithms for the instrument were also undertake. Much was learned about the basic principles of the instrument. Since this work Dr Thomas and Dr Grainger (his supervisor) moved to Oxford. Detailed information on the phase I instrument can be found in Thomas 2003.

Phase II instrument

In 2007 HEFCE funding was secured to develop the instrument further, the main aim of this project was to move design from a stratospheric instrument into one suitable for use in troposphere studies. Dr Dan Peters then applied the lessons learned on the instrument design by Thomas and building a breadboard implementation of the new design. In addition new design tools were developed to predict the instrument performance, by both Dr Peters and Mr Andrew Smith (as part of his PhD). Detail information on the Phase II instrument can be found in Peters 2009.


Basic principles

The instrument measures both the intensity of the scattered laser light from one particle at a time using a photomultiplier tube, PMT, and the angular light scattering pattern using a linear detector array LDA. The light scattering pattern allows individual particle refractive index and particle size to be derived.

Due to the large amount of data from the LDA signal, the signal is pre-processed to reduce the number of measured parameters (termed the measurement vector) required in the analysis algorithm (to find the particle size and refractive index).

Fig. 1. Example LDA signal.

Fig. 2. Smoothed LDA signal (in black), crosses show the points used in the particle analysis. Red line is the curve fitted by Mie theory to these data points.

Fig. 3. The Fourier transform of the LDA signal is shown in black. The red line shows the Fourier transform of the fitted Mie function from the analysis.

An example LDA signal for the Phase I instrument is shown in Fig.1. To reduce the number of measured parameters passed to the analysis the signal is transformed in the following way to be represented by around 21 parameters rather than all the LDA pixels. First the signal is smoothed to remove the high frequency spatial variations, this is plotted as the black line in Fig.2. From this smoothed curve a 20 points are sampled and these are then used in the analysis, these points are plotted in Fig.2. as crosses.

To represent the high frequency information a Fourier transform is taken of the LDA signal minus the smoothed LDA signal (Fig3. black line). The peak of the Fourier transform is then found, and this spatial frequency is used one the measured parameters. Thus the analysis algorithm input parameters are reduced from the number of LDA pixels to just 21 parameters. These are then fitted to Mie theory. The fits for the example LDA signal when compared to Mie theory as shown as the red line in the above plots. For more detail on the analysis method see Thomas 2003.


Instrument performance

Measurement signal-to-noise

Fig. 4. Predicted Phase II detector performance.

Using modelling software it is possible to obtain size resolved instrument performance plots-these are shown in Fig.4. The PMT detector allows the possibility of detecting the smallest particles, whilst the LDA affords the opportunity to resolve the scattering pattern of the particles.

Fig. 4 shows the LDA is sensitivities to particles 100nm in radius and above. The LDA covers the coarse and fine fraction with the PMT providing sensitivity from 80nm radius. The limiting factor for the LDA performance is the dark noise, for the PMT it is Rayleigh scattering from the surrounding air molecules.

Both detectors are not photon limited. The photon limit for the detectors is 30nm for the LDA and 15nm of the PMT (the radius where the blue and black lines cross in Fig. 9). This indicates that some performance enhancements may be possible with further development of the instrument optics. For further discussion of the instruments performance see Peters 2009.

Refractive index and particle sizing range

Fig. 5. Number of degrees of freedom for the Phase II instrument.

Having sufficient signal to construct a measurement vector is one thing, but what will this mean in terms of the instruments ability to determine refractive index and particle size? To help answerer this question we can compute the number of degrees of freedom of the analysis system. This analysis does not include the signal-to-noise ratio but rather calculates the number of independent parameters that can be retrieved given sufficient signal-to-noise. Thus when interpreting this plot we must also referrer to the signal-to-noise plots to get the complete picture of the instruments performance.

The result of this analysis are shown in Fig. 5 for a number of different refractive index values and particle sizes found in the atmosphere. Were the plot shows three degrees of freedom, the complex refractive index (real and imaginary parts) and the particle size can be determined, these areas are shown in red. The green areas designate were only two independent parameters can be determined, i.e. particle size and the real part of the refractive index. The blue areas show were size only can be obtained.

Thus the instrument can provide the full refractive index and particle size measurements for nearly all refractive index values for particles 200nm radius and above, and there is good signal-to-noise from both the LDA and PMT in this range to make this measurement possible (see Fig. 4.)


Future work

The current LDA signal is not limited by the noise shown in Fig. 4 but rather by the digitization noise of the electronics. Thus additional gain is required to ensure the instrument is limited by shot noise.

In addition to allow extend operation, or operation by inexperience personnel the instruments flow control need to be modified for closed loop control. This will allow high quality number density information to be obtain which is not currently possible as the flows must be monitored and pump flows manually adjusted.


Links and references

IPCC: Climate Change 2007 - The Physical Science Basis, Contribution of Working Group I to the Fourth Assessment Report of the IPCC, Cambridge University Press

Peters D., Grainger R.G., Smith A, Final Report: Characterising near surface aircraft PM, Omega, 2009

Thomas, GE,A new instrument for stratospheric aerosol measurement, PhD Thesis, University of Canterbury, 2003.

Willeke, K., Baron P. A., Aerosol measurement: principles, techniques, and applications, Van Nostrand Reinhold, 1993.

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