Vol. 27, No.

12 | 10 Jun 2019 | OPTICS EXPRESS A890

Precise size distribution measurement of

aerosol particles and fog droplets in the open
atmosphere
HUIGE DI, ZHIXIANG WANG, AND DENGXIN HUA*
School of Mechanical and Precision Instrument Engineering, Xi’an University of Technology, Xi’an
710048, China
*dengxinhua@xaut.edu.cn

Abstract: A precise measurement for the aerosol particle size distribution and fog droplet size
distribution simultaneously in the open atmosphere is proposed. The extinction coefficient and
small-angle forward scattering measurement are integrated into the detection for particle size
distribution in the open atmosphere, and can achieve the fine detection of the particles in the
atmosphere with radius between 0.1 to 30 μm. The key technology including optimal scattering
angle in small-angle forward scattering measurement and optimal wavelengths selection are
discussed and solved in detail. The fourteen different particle size distributions including
aerosol size distributions and fog droplet size distributions are used for the determination of
optimal forward scattering angle and wavelengths. The optimal forward scattering angle is
calculated to be 1.1°. Seven wavelengths for extinction coefficients and five wavelengths for
forward scattering coefficients are chosen for the retrieval of particle size distribution in the
measurement. The regularization inversion of optical parameters for the retrieval of particle
size distribution is described. The aerosol particle size distributions measured by particle
spectrometer and actual fog particle size distributions are used for the method test and the
reconstructions of particle size distributions. The inversion results show that the method can
achieve the precise measurements of aerosol particle size distribution and fog droplet size
distribution. The error influence on the inversion results of distributions is discussed. Based on
the sensitivity analysis of inversion results, the feasibility of measurement in the real
atmosphere is analyzed and discussed, and the scheme of detection system is provided.

© 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

1. Introduction
Aerosols are solid or liquid particles with the radius of 0.001-50 μm suspended in the
atmosphere, and most particle radius range from 0.01 to 5 μm. Aerosols play an important role
in many atmospheric processes. Fog is an aerosol system consisting of a large number of tiny
droplets of water or ice crystals suspended in the atmosphere near the ground [1], and the radius
of fog droplet is mainly distributed between 2 and 15 μm, with a maximum of 50 μm. Due to
the strong scattering or absorption of fog droplets or aerosol particles, the horizontal visibility
is usually less than several kilometers when fog or haze/smog occurs [2]. In North China, fog
and haze weathers often occur, and the microphysical properties of particles in the atmosphere
are prone to change with atmospheric environment (temperature and relative humidity).
Although fog and haze are different weather phenomena, while they often occur
simultaneously, and change each other. Because fog and haze weather have an important impact
on the atmospheric environment, climate change and residents' health, it is necessary to study
fog droplet size distribution (FDSD) and aerosol particle size distribution (APSD). In this paper,
particle size distribution (PSD) is used to represent the total particle size distribution of fog
droplet and aerosol. The simultaneous detection of FDSD and APSD cannot be achieved using
the current instruments.
At present, the measurements of PSD mainly include in situ measurements and remote
sensing measurement for profiles. FDSD is usually detected using the three-purpose droplet

#363390 https://doi.org/10.1364/OE.27.00A890
Journal © 2019 Received 26 Mar 2019; revised 3 May 2019; accepted 7 May 2019; published 20 May 2019
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A891

spectrometer and the droplet spectrometer [3]. The principle of the three-purpose drop
spectrometer is to use inertia to drop the droplets on the glass coated with the oil, and then the
droplet size and number can be directly counted by using a microscope or count on the
photomicrograph. The shortcoming of this method is the collection of droplet samples takes a
long time, and continuous real-time observation cannot be performed. At the same time, the
mechanical counting is an error-prone process [4]. The droplet spectrometer is capable of
continuous observation and producing one FDSD per minute, but the air is sampled into the
instrument by an air pump, the real atmospheric condition such as temperature and humidity is
changed during this process. There are many apparatus for APSD such as wide-range particle
spectrometer (WPS) [5] and optical particle counters [6]. WPS is a recently introduced
commercial instrument with the unique capability to measure APSD from 0.005 to 5 µm of
radius. The instrument includes a scanning mobility spectrometer (SMS) comprised of a
differential mobility analyzer (DMA), a condensation particle counter (CPC) for particle
measurement from 0.005 to 0.25 µm and a laser particle spectrometer (LPS) for measurement
in the range from 0.2 to 5 µm. Air is pumped into the instrument by a sampling pump. As for
the optical particle counter, the sampled air is drawn into the scattering cavity, the particle is
illuminated by the incident radiation, and the detector quantifies the intensity of the scattered
light in an angular range [7]. Then the particle size is determined by the amplitude of the electric
pulse, and the number by counting the electric pulse [8].
Besides WPS and optical particle counters, some equipment or technology based on the
principle of forward scattering is used for the measurement of aerosol or cloud [9–13]. M.
Bouvier, et al. provided a novel approach for in situ soot size distribution measurement based
on spectrally resolved light scattering. The two-angle (90° and 7°) optical technique was
proposed to enable the measurement of the two parameters of a given size distribution [9].The
size distribution of semitransparent irregularly shaped mineral dust aerosol samples was
determined using a commonly used laser particle-sizing technique in the Ref [10]. The size
distribution was derived from intensity measurements of singly scattered light at various
scattering angles close to the forward-scattering direction at a wavelength of 632.8 nm.
The multi-wavelength lidar [14] and sun- photometer [15] can also detect APSD in the
atmosphere with high spatial or temporal resolution. Lidar receives the backscattering signal of
particles at the multiple wavelengths for the retrieval of APSD. The solar photometer is also a
widely used instrument for the aerosol remote sensing. The aerosol optical thickness at different
wavelengths can be obtained by measuring the direct Sun radiation. The APSD in the total
atmosphere can be obtained from the solar photometer.
There are various deficiencies for the above measurements. The disadvantage of the three-
purpose droplet spectrometer is that the APSD cannot be continuously observed. For the droplet
spectrometer, the wide-range particle spectrometer and the optical particle counter, the
disadvantages are the actual atmospheric environment such as temperature and humidity is
changed by the air pump. And all of them cannot detect APSD and FDSD simultaneously. As
for lidar and solar photometer, the optical parameters for the retrieval of APSD are limited, and
the information about the large particle (radius is larger than 5 μm) is not so much [16]. When
fog weather occurs, these two instruments can hardly work. And, it is difficult to achieve fine
detection and retrieval of PSD with a radius of 0.1μm to several microns (including the aerosol
particle and fog droplet) [16,17].
In order to measure the precise APSD and FDSD simultaneously in the open atmosphere, a
photoelectric detection measurement based on forward scattering of a wide-spectrum light is
proposed in this paper. Based on the principles of lidar and solar photometer for APSD,
extinction method and small-angle forward scattering method are integrated into the detection
of PSD. Different particle information can be obtained from the extinction and small-angle
forward scattering signal, extinction for small particles, and forward signal for large particles
such as fog droplets or sand dust. The key technology of this method including the
determination of scattering angle and the wavelengths are discussed and optimized. The
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A892

regularization inversion of photoelectric detection data for retrieval of PSD is described. The
known APSDs and FDSDs are used for the method test and the reconstructions of PSD.
2. APSD and FDSD
There are distinctly different distribution models in the atmosphere. Usually the aerosol number
size distribution is used to represent the different sizes of the particle group [18]. APSD can
generally be described by several lognormal distributions. It can be described by the following
Eqs [16,19]:

n(r )= ∑
k
Ni (
 lnr -lnr n 2 
exp  - mi
)
 , k =1,2, , (1)
i =1 2π ⋅ lnσ i ⋅ r 
 2 ( lnσ i ) 
2

 
Here, n(r) denotes the number concentration distribution, k is the number of modes, Ni is
the total particle number of the ith mode, rmi describes the mode radius of APSD, and lnσi is the
mode width of the ith mode. Usually four main types of aerosol in the troposphere can be
distinguished: urban industrial aerosol, biomass burning aerosol, desert dust, and marine origin
aerosol. The same distribution can be written for volume concentration distribution v(r), which
is preferred, because in volume concentration representation both fine and coarse modes are
relatively easy to distinguish [16]. Both n(r) and v(r) have the same standard deviation σ and
the relationships between radius and concentration for each mode are [20]:
ri v = ri n exp[3(ln σ ) 2 ], (2)

4 9 2
Vi = N i π (ri n )3 exp  ( ln σ )  . (3)
3  2 
The parameters for these typical aerosols are shown in the Table 1 [16]. Besides v(r), the
volume concentration distribution is often expressed in terms of dV/dln(r), and dV/dln(r) = r ×
v(r).
FDSD is usually the generalized gamma distribution proposed by Deirmendjian [21]. It can
be written as:

( )
vF ( r ) =ar c exp -br d . (4)

Here a, b, c and d are the parameters describing the FDSD.

Table 1. The Typical Parameters of Bimodal Distribution of Different Types of Aerosol
Aerosol Urban Biomass Desert Dust
Parameter Industrial Burning and Oceanic
rm1(μm) 0.14-0.18 0.13-0.16 0.12-0.16
rm2(μm) 2.70-3.20 3.20-3.70 1.90-2.70
lnσ1 0.38-0.46 0.40-0.47 0.40-0.53
lnσ2 0.60-0.80 0.70-0.80 0.60-0.70
V1/V2 0.80-2.00 1.30-2.50 0.10-0.50
mr 1.40-1.47 1.47-1.52 1.36-1.56
mi 0.003-0.015 0.01-0.02 0.0015-0.003

3. The measurement of APSD and FDSD simultaneously

In the multi-wavelength lidar, the combined use of extinction and backscatter coefficients is
important for the retrieval of APDS and aerosol microphysical propertie [16,22,23]. The
extinction and backscatter efficiencies at different wavelength are sensitive to the particles of
different diameters. The wavelength of laser is limited and the most commonly used
wavelengths are 0.355 μm, 0.532 μm and 1.064 μm, so the corresponding kernel functions are
not sensitive to size variations of big particles with radius greater than 5μm and small particles
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A893

with radius less than 0.1 μm [16]. According to the Mie theory, the first peak of the extinction
efficiency corresponds to the diameter of the particle [24] and it is generally applicable to the
range of particle radius from 0.01 to 4 μm when light is visible beam. However, the small-angle
forward scattering coefficient, which is sensitive to large particles in the air, can reflect particle
radius of approximately 1 μm to several tens of microns [17]. Therefore, combined with the
method of remote sensing for APSDs, it is proposed to use multi-wavelengths’ photoelectric
detection methods to realize the precise detection of PSD simultaneously. If the extinction and
forward scattering coefficients at the wide wavelength range are obtained, PSD can be retrieved
by using the inversion technology. The air pumping and drying in this method are not required,
and the PSD in the real environment can be obtained. The schematic diagram of PSD
measurement in open environment is shown in Fig. 1.

Fig. 1. The schematic diagram of PSD measurement.

The basic principle of this detection system is as follows: a wide-spectrum light beam
(wavelength is in the range of 0.2 to 3 μm) collimated by a lens with long focal length emits a
beam into the atmosphere. The light is scattered by the aerosol particles or fog droplets in the
atmosphere. After light travels a distance L in the atmosphere, a lens collects the attenuated
scattered light at different directions to the focal plane. The optical fibers placed on the focal
plane transmit the forward scattered light into the spectrometer. The measured air can be
considered to be uniform in a short distance. So the energy received at the wavelength of λ by
the spectrometer are
Jα (λ ) = J 0 (λ ) ⋅ T (λ ) ⋅ exp [ - L ⋅ (α a (λ ) + α m (λ )) ] , (5)

J β (θ , λ ) = J 0 (λ ) ⋅ T (λ ) ⋅ ( β a (θ , λ ) + β m (θ , λ ) ) ⋅ exp - L ⋅ (α a (λ ) + α m (λ ) )  . (6)

Here Jα(λ) is the power received by the spectrometer at the direction of light transmission, J0(λ)
is the emitted power of wavelength λ at the exit of light source, T(λ) is the optical transmittance
of detection system, αa(λ) is the extinction coefficient of the aerosol particles or fog droplets at
the wavelength of λ, αm(λ) is the extinction coefficient of air molecule which can be obtained
by the standard model [25], Jβ(θ, λ) is the power at the angle of θ, βa(θ, λ) is the forward
scattering coefficient of particles at the angle of θ and at the wavelength of λ, βm(θ, λ) is the
forward scattering coefficient of air molecule, L is the optical path length in the atmosphere.
The extinction coefficient and the forward scattering coefficient at the angle of θ can be
expressed from the above Eqs. as follows:

1   J α (λ )  
α a (λ ) =
− ln   − α m (λ )  , (7)
L   J 0 (λ ) ⋅ T (λ )  

J β (θ , λ )
β=
a (θ , λ ) − β m (θ , λ ). (8)
J α (λ )
The optical data αa(λ) and βa(θ, λ) are related to the physical quantities of PSD by the
Fredholm integral Eqs. of the first kind, and can be expressed as [16,26]:
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A894

 α ( λ ) = rmax K ( r,m, λ ) v ( r ) dr
 a 1 ∫rmin a 1


α a ( λ2 ) = ∫r K a ( r,m, λ2 ) v ( r ) dr
rmax

 min , (9)
 

α a ( λn ) = ∫ max K a ( r,m, λn ) v ( r ) dr
r

 rmin

 β (θ , λ ) = rmax K ( r,θ , m, λ ) P(r,θ , m, λ )v ( r ) dr

 a 1 ∫rmin β 1 1


 β a (θ , λ2 ) = ∫r K β ( r,θ , m, λ2 ) P(r,θ , m, λ2 )v ( r ) dr
rmax

 min . (10)
 

 β a (θ , λn ) = ∫ K β ( r,θ , m, λn ) P(r,θ , m, λn )v ( r ) dr
rmax

 rmin

Here αa(λn) denote the extinction coefficient of particles at the wavelength of λn, βa(θ, λn) denote
the forward scattering coefficient at the angle of θ and at the wavelength of λn, v(r) describes
the volume concentration distribution, the lower integration limit is defined by rmin, and the
upper limit is determined by rmax, Kα(r, m, λn) is the extinction kernel function, Kβ(r, θ, m, λn) is
the forward scattering kernel at the angle of θ and the refractive index of m, and P(r, θ, m, λn)
is the phase function of a single particle. The scattering coefficients change with wavelength
and the scatter angles. The key problem in this method for PSD is the determination of the
forward scattering angle and the selection of the optimal wavelength for extinction and forward
scatter.
The PSD can be retrieved from the extinction coefficient and forward scattering coefficient
of the spectrometers using the regularization algorithm or the principal component analysis
technique [27,28]. In this method, no air pumps are needed, so the actual state of the air detected
is not changed. Besides, its’ detection speed is fast, and real-time non-interference detection
can be realized.
Figure 2 shows the extinction efficiencies [29] and the kernels as the function of particle
diameter at the wavelengths of 0.2 μm, 1.06 μm and 3 μm when the refractive index m is 1.50-
0.01i. The kernels are calculated from the extinction efficiencies and the geometric cross
section πr2 as
3
Kα (r , m, λ ) = Qi (r , m, λ ). (11)
4r

Fig. 2. Extinction efficiencies (a) and the kernels (b) at the wavelengths of 0.2 μm, 1.06 μm and
3 μm.
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A895

From the Fig. 2, the extinction efficiency strongly depends on particle size, and it gradually
converges to 2 with the increase of particle size. The maximum peak diameters of extinction
efficiencies change with the wavelength, and balance it [29]. Therefore, the extinction
coefficient can better reflect the particle size characteristics of this region [17]. The detection
of large particles can be realized by obtaining the extinction at longer wavelength. However, it
is difficult to obtain and detect the light at mid-infrared wavelength or longer-band beams.
Therefore, we propose to use small-angle forward scattering coefficients combined with the
extinction coefficients to achieve the detection of large particles in the air. Figure 3 shows the
variation of the scattering phase function of the particle with the diameter of particles at 0.3
μm, 0.55 μm and 1.06 μm at the angle of 2° and the refractive index is 1.50-0.01i. From Fig. 3,
the maximum peak of the scattering phase function is greater than the extinction efficiency, and
it can reflect the characteristics of large particles.

Fig. 3. Phase function (a) and scattering kernel function (b) at the wavelength of 0.3 μm, 0.55
μm and 1.06 μm and at the angle of 2°.

4. The selection of the scattering angle and the wavelengths

4.1 The determination of the forward scattering angle
According to the Mie theory, the intensity distribution of the scattered light is the function of
the angle [29]. The angle, at which the scattering coefficient is the most sensitive to PSDs
difference, should be chosen in the measurement for improving the detection accuracy and
sensitivity.
The scattering phase function Pʹ(λ, θ, m) of PSD is a weighted superposition of the scattering
phase function of a single particle on the particle swarm:
3
Qsca (r ) P ( r, λ ,θ ,m ) v ( r )dr
rmax
∫
P ′ ( λ ,θ ,m ) = 4r
rmin
, (12)
rmax 3
∫rmin 4r sca
Q ( r ) v ( r )dr

where Qsca(r) is the aerosol scattering efficiency at the radius of r.

The scattering phase functions of 14 different PSDs, which represent most aerosol
distributions in the atmosphere, are chosen to calculate the optimal scattering angle. These 14
distributions include 10 APSDs in different atmospheric humidity conditions and 4 FDSDs.
According to the ref [30], the parameters of 5 typical APSDs are chosen and shown in Table 2
and Fig. 4(a). These distributions are basically obtained by optical particle counter, representing
the APSD at low relative humidity.
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A896

Table 2. The parameters of 5 APSDs in low humidity

type rm1 lnσ1 V1 rm2 lnσ2 V2 rm3 lnσ3 V3
1 0.42 0.50 29.0 1.90 0.32 26.0
2 0.32 0.40 19.0 2.90 0.60 18.0
3 0.37 0.45 46.0 1.70 0.32 6.40 3.80 0.38 15.5
4 0.37 0.20 3.70 0.58 0.23 14.0 2.63 0.30 30.0
5 0.32 0.40 15.0 2.35 0.50 7.50
When the relative humidity increases in the atmosphere, the hygroscopic growth of aerosols
would occur. Because of the lack of measured data, the APSDs under high relative humidity
are obtained by the theoretical calculation. The radius of aerosol particles under high relative
humility (RH) can be calculated by the formula (13) and the distributions of wet haze after
moisture absorption can be estimated [31]:
r ( RH ) - (1 d ) - (1 d )
= (1-RH ) - (1-60% ) +1. (13)
r0

Here r0 denotes the radius of aerosol particles, r(RH) denotes the radius after hygroscopic
growth, RH denotes the relative humidity, and d is 3.5 generally [31]. 5 new APSDs are
obtained from the Table 2 and the Eq. (12). They are shown in Fig. 4(b). Four FDSDs are
selected from the Ref [3,32]. for our analysis, and their parameters are shown in Table 3. The
four FDSDs are shown in Fig. 4(c).

Fig. 4. The APSDs and FDSDs for the simulation, (a) APSDs with low relative humidity, (b)
APSDs with high relative humidity, and (c) FDSDs

The scattering phase functions of above 14 PSDs with the scattering angle are calculated
and shown in Fig. 5. We can see that the scattering phase functions change with the PSDs and
angles and there are large variations among the scattering phase functions when the angles are
between 0~2°.
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A897

Table 3. The parameters of FDSDs

Type A b c d
1 381.987 3.019 0.593 0.84
2 74553.269 8.21 8.21 0.4
3 10848.967 −0.4 0 −50.624
4 5.508 5 0.425 1

Fig. 5. The scattering phase functions of 14 PSDs at the angle from 0° to 180°.

In order to select the optimal scattering angle with the highest sensitivity to the PSDs (i.e.,
the difference in the scattering phase function of different PSDs is the largest), the standard
deviation coefficient CV is calculated for the dispersion degree of the particle phase function at
different angles, which is expressed as:
σ
CV = , (14)
µ
Here σ is the standard deviation of 14 curves in Fig. 5, μ is their average value. The curve of
CV with respect to θ is shown in Fig. 6. From the Fig. 6, the value of CV change greatly with
the angle θ, the large value can be found in the range of 0.1°~1.2° and 157°~178°. The angle
where the standard deviation coefficient CV is greater than 1(i.e., 0.1 to 1.1 degrees) is selected
in our design.

Fig. 6. The standard deviation coefficient CV with respect to the scattering angle of θ.

In order to find the optimal angle for the PSD measurement, the overlapping area of the
scattering phase function and PSDs are also calculated. Define the overlapping area as the value
of the normalized particle spectrum and the phase function intersecting in the same coordinate
system. Its’ schematic diagram is shown in Fig. 7. The value reflects the amount of information
about PSD.
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A898

Fig. 7. The overlapping area of scattering phase function P(r, θ, m, λn) and PSDs v(r)

The overlapping area of 14 PSDs and the scattering phase function at 0.1° to 1.1° are
calculated, and shown in Fig. 7. The overlapping area increases with the scattering angle and
reach the largest at 1.1°. The optimal forward scattering angle is chosen at 1.1° for the PSD
measurement.

Fig. 8. The overlapping areas between the scattering phase functions and the PSDs at different
scattering angles (0.1°-1.1°).

4.2 The selection of wavelengths

The detection system designed in our method can theoretically obtain extinction coefficients
and forward scattering coefficients of many wavelengths. It is not necessary to use the optical
parameters of all wavelengths for the PSDs. Quite a number of wavelength signals are useless
in this method. The optimal wavelengths need be singled out for the inversion. The retrieval of
PSD can be realized by the selected multi-wavelengths extinction coefficient and forward
scattering coefficient combined with the inversion algorithm. The APSDs varies greatly with
time and location, which may be the superposition of single lognormal model, two lognormal
models, three lognormal models or four lognormal models [22]. FDSD is usually the
generalized gamma distribution. The single lognormal distribution contains three unknown and
gamma distribution contains four unknowns, so three or four independent extinction
coefficients and forward scatter coefficients are needed to accurately obtain the parameters of
one mode. 12-16 optical parameters are needed to accurately reconstruct the PSD in the
atmosphere.
4.2.1 The selection of wavelengths for extinction coefficients
To select the optimal wavelengths, the extinction coefficients of above 14 PSDs are calculated
at the intervals of 50 nm in the range of 0.2 to 3 μm according to the Mie scattering theory.
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A899

Figure 9 shows the extinction coefficients of these APSDs (Fig. 9(a)) and FDSDs (Fig. 9(b)) at
the wavelengths of 0.2 to 3 μm.

Fig. 9. The extinction coefficients of 14 different PSDs at the wavelengths of 0.2 to 3 μm. (a)
aerosol particles, and (b) fog droplets

According to Fig. 9, the extinction coefficients vary greatly with the PSDs. The extinction
coefficient in foggy days is much larger than that in hazy days and it increases with the increase
of relative humidity in air when haze occurs. Extinction coefficients of aerosol particle change
greatly with the wavelength, especially in the range of 0.2 to 1.5 μm, while they hardly change
with wavelength for fog droplets, as shown in Fig. 8, which indicates that the extinction
coefficients from large particles are not sensitive to the variation of wavelength. According to
the above section, the first peak of the extinction efficiency corresponds to the diameter of the
particle. And APSDs can generally be described by lognormal distribution. The APSDs are
more complex when the diameter of particle is less than 1.5 μm, which means that more
information in this range needed to be obtained for the retrieval of PSD. Five wavelengths in
this range are chosen for the retrieval of APSD, and the intervals between these five
wavelengths are logarithmic equidistances. Since the extinction coefficients of 0.2 −1.5 μm
mainly reflect the particle radius up to about 1 μm, the extinctions of two infrared wavelengths
of 2 μm and 3 μm are also chosen for the retrieval of particles larger than 1 μm. The seven
wavelengths are selected for extinction coefficient, and they are 0.2 μm, 0.337 μm, 0.525 μm,
0.88 μm, 1.45 μm, 2 μm and 3 μm.
4.2.2 The selection of the forward scattering wavelengths
Since it is necessary to simultaneously invert the size distribution of particles with radius of 0-
30 μm, the forward small-angle scattering coefficient is added to achieve accurate inversion of
large particles. Figure 10 shows the forward scattering coefficients of these APSDs (Fig. 10(a))
and FDSDs (Fig. 10(b)) at the wavelength of 0.2-3 μm. There are great differences between the
extinction coefficients and forward scattering coefficients from Fig. 9 and Fig. 10. Similar to
the Fig. 9, the forward scattering coefficients vary greatly with the PSDs, the values of fogs are
greater than aerosols, and the forward scattering coefficients at wet haze day are also greater
than the values at dry haze day. For APSD, the changing trends of forward scattering
coefficients with wavelength are similar. As the wavelength increases, the forward scattering
coefficients decrease rapidly. There are great changes for FDSD with wavelength, especially
within 0.2 to 1 μm. These indicate that the forward scattering coefficients are sensitive to large
particles. The method used in selecting the forward wavelength is the same as that of the
extinction. For the forward kernel function, five wavelengths of equal logarithmic spacing
between 0.3 and 1.06 μm are selected to be 0.3 μm, 0.41 μm, 0.56 μm, 0.78 μm, and 1.06 μm,
respectively.
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A900

Fig. 10. The forward scattering coefficients of 14 PSDs at the wavelengths of 0.2 to 3 μm. (a)
aerosol particles, and (b) fog droplets

The extinction coefficients of 7 wavelengths and the forward scattering coefficients of 5

wavelengths are chosen for the measurement of PSDs. Supposed that the refractive index is
1.50-0.01i, these extinction and the forward scattering kernel functions at the angle of 1.1° are
calculated and shown in Fig. 10. According to these kernels, their first peaks at those
wavelengths cover the range of 0.1 to 30 μm, which means that the particles with the radius of
0.1 to 30 μm can be retrieved.

Fig. 11. The extinction and forward scattering kernel functions at the selected wavelengths.

5. The retrieval algorithm and simulations for PSD

The possibility of using optical parameters to estimate the size distribution of stratospheric
aerosols has been previously discussed by a number of researchers [27]. The regularization
algorithm [23], the principal component analysis technique [27] and linear estimation algorithm
[28] have been used for the aerosol bulk properties. The regularization algorithm is used most
commonly for inverting multi-wavelength measurements, allowing the retrieval of particle size,
concentration, and the main features of the particle size distribution [24]. Using the regularized
inversion algorithm, the particle size distribution of aerosols can be obtained without assuming
the initial complex refractive index and aerosol distribution. In previous research, the
regularization algorithm is mainly used for the inversion of lidar data, and has been discussed
elsewhere [16,24]. The inversion error of microphysical parameters from lidar data can reach
20% to 60% due to the limited optical parameters. In our method, the regularization algorithm
is also selected for the retrieval of the PSD.
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A901

5.1 The regularization algorithm

The solution v(r) of Eq. (9) and Eq. (10) can be approximated by the superposition of base
functions Bj(r):
n
=v(r ) ∑ W B (r ) + ε
j =1
j j
math
(r ), (15)

where Wj are weight coefficients. εmath (r) is the error in the solution. According to the Eqs. (7)
(8) and (14), the optical coefficients can be rewritten as
=g (α , β ) ∑ Aα β
j
( , )j (m)W j + ε math (r ). (16)

Here A(α,β)j(m) is the kernel function matrix, it is a 12 × 12 matrix in our method, and they can
be calculated from the following Eqs.
rmax

Aα i (m) = ∫ Kα ( r , m, λ ) Bi ( r ) dr , (17)
rmin

rmax

Aβ j (m) = ∫ K β ( r , θ , m, λ ) P (r , θ , m, λ ) B j ( r ) dr. (18)

rmin

Representing Wj and gp as vectors, the weight coefficients can be derived from the following
relation:

(A A + γ H ) AT g .
−1
=
W T
(19)

Here γ is the Lagrange multiplier, H is the smoothing matrix, and AT is the transpose of matrix
A. The value of γ was decided by the minimum discrepancy principle [16]. And the logarithmic
normal distribution function was selected as the base function for the inversion. According to
our method, 12 optical parameters including the extinction and forward scattering coefficients
were used for the retrieval of PSD. The extinction coefficients at the wide spectrum of 0.2-3
μm and forward scatter coefficients at 0.3-1.06 μm covering the ultraviolet to infrared range
are combined with the regularized inversion algorithm to invert APSDs and FDSDs.
5.2 Simulation
Four typical APSDs are selected to test our method and verify the rationality of wavelength and
scattering angle selection. Figures 12(a) and 12(b) show the typical urban industrial APSDs
from the Ref [11], Figs. 12(c) and 12(d) is the actual APSD measured by a Particle size
spectrometer in haze day in Xi’an, China, and Fig. 12 (d) show the distribution after
hygroscopic growth from Fig. 12(c). Their extinction coefficients at seven wavelengths (0.2
μm, 0.337 μm, 0.525 μm, 0.88 μm, 1.45 μm, 2 μm, 3 μm) and forward scattering coefficients
at five wavelengths (0.3 μm, 0.41 μm, 0.56 μm, 0.78 μm, 1.06 μm) are calculated from the Eqs.
(3) and (4). The selected complex refractive index of APSD1 and APSD2 in Fig. 11 is 1.50-
0.01i, and the value of APSD3 and APSD4 is 1.40-0.03i.
Besides the APSDs, the complex refractive index is also the unknown quantity in the
inversion. One of the most remarkable features of this regularization approach is that it does
not need the a priori knowledge of the complex refractive index. The regularization algorithm
is performed for the reconstructions of APSDs. All possible complex refractive indices are
chosen for the inversion. The real parts of the refractive index varied from 1.3 to 1.7 in steps of
0.01, the imaginary parts varied from 0 to 0.03 in steps of 0.001. The inversion results of the
complex refractive indices are 1.50-0.01i for APSD1, 1.52-0.011i for APSD2, 1.40-0.022i for
APSD3 and 1.40-0.028i for APSD4. There is a small inversion error for complex refractive
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A902

index. The four initial APSDs (black solid lines) and their retrievals (red dash lines) are
illustrated in Fig. 12, and the corresponding error distributions (blue solid lines) with the
particle radius are also calculated and shown in Fig. 12.

Fig. 12. The retrieval of four APSDs and their error distributions. (a) typical urban APSD1, (b)
typical urban APSD2, (c) measured APSD1, (d) measured APSD2

From the inversion results and their error curves, the APSDs in dry-haze day and wet-haze
day with radius ranging from 0.1 μm to 13 μm can be well reconstructed using the data from
the extinctions and forward scattering coefficients. The maximum point-to-point relative error
is less than 10%, and their mean error is less than 5% for Figs. 12(a) and 12(b). The retrieval
errors of measured distribution in Figs. 12(c) and 12(d) are larger than the models in Figs. 12(a)
and 12(b). The measured distributions are not smooth curves, and the small peaks can be found.
Great errors often occur at peak locations, while the basic distribution characteristics can be
well retrieved. The maximum point-to-point error can reach 20% or worse, while the mean
error is less than 15%. The microphysical parameters are the mean and integral properties of
the particle ensemble, and they can be calculated from the APSD. The effective radius reff,
volume concentration V and number concentration N are chosen for the error analysis [33]:

∫ n(r )r dr ,
3

reff = (20)
∫ n ( r ) r dr
2

N = ∫ n(r )dr , (21)

4π
3 ∫
V= n(r )r 3 dr. (22)

Their error is less than the above point-to-point error of distribution. The retrieval errors are
all less than 8%. The errors of effective radius and volume concentration are less than 5%.
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A903

These error values are far less than inversion error (20% to 60%) from multi-wavelength lidar
data [16,24].
Two FDSDs [2,3] measured by the fog drop spectrometer are also chosen for the test. Fog
drops are much larger than general aerosol particles, so the volume concentrations are much
larger than them. The complex refractive index of fog is chosen as 1.33-0i [34]. The initial,
retrieval FDSDs and their corresponding inversion error are shown in Fig. 13. From them,
FDSDs can also be well reconstructed using the data in our method. The maximum point-to-
point errors are less than 5% at the range of 0 to 30 μm. The large error often occurs at the range
of low concentration. The retrieval errors of microphysical parameters are also calculated. The
retrieval errors of microphysical parameters are less than 1%.

Fig. 13. The retrieval of two FDSDs and their error distributions. (a) typical FDSD1, (b) typical
FDSD2

Besides the above APSDs and FDSDs, more APSDs and FDSDs are also simulated and
reconstructed. The results show that they can be well retrieved using the selected optical
parameters, and there are smaller inversion errors for FDSDs than the APSDs. From the above
analysis, the method proposed can measure PSDs in the open atmosphere. Figure 14 shows a
series of PSDs before and during a haze process (Fig. 14 (a)) and their reconstruction results
(Fig. 14 (b)). The x-axis is the particle diameter, the y-axis is the time and the z-axis is the size
distribution. The PSDs in Fig. 14 (a) were measured in Xi’an in inland China from March 9 to
14, 2018, during which a haze episode occurred. Compared with the sunny day, the volume
concentrations of fine and coarse particles increased simultaneously in haze day. The inversion
can well reconstruct the initial APSDs from Fig. 14 no matter that it's sunny or hazy, which
indicates that our inversion is stable.

Fig. 14. A series of PSDs and their retrievals before and during a haze process. (a) Measured
APSDs, (b) Retrieved APSDs
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A904

5.3 Effects on the retrievals of errors in the optical data

The extinctions and forward scattering coefficients for the inversion of PSD can be obtained
from the scattering signals Jα(λ) and Jβ(θ, λ). The optical parameters may be affected by the
systematic and random errors. From the Eqs. (5) and (6), systematic error in this measurement
comes from different sources and need to be considered. Systematic errors can be due to
nonlinearity of a photodetector, errors of calibration of the system constants and errors in the
assumed atmospheric molecule density. Random errors arise naturally from the measurement
process. In order to study the effect of optical parameter errors on the inversion results, two
important microphysical parameters (effective radius and volume concentration) are selected
to characterize the inversion results. The typical urban APSD in Fig. 12 (a) is used for the
analysis of inversion sensitivity. The initial refractive index is chosen as 1.5-0.001i. The optical
parameters are generated from the Eqs. (7) and (8). We assume that the errors of optical
parameters are −2% to 2%. The next step consists of applying a systematic bias to one optical
datum at a time. For each of these induced biases, the inversion is performed and a new size
distribution and set of microphysical parameters are then obtained. This procedure is applied
to each of the fifteen optical data used in our measurement. Figure 15 and Fig. 16 present the
sensitivity analysis for the retrieval of effective radius and volume concentration.
Figure 15 and Fig. 16 reveal that the retrievals of V are more sensitive to biases than reff. It
is quite apparent that the retrievals are more sensitive to biases in the forward scattering
coefficients. The low sensitivities are to biases in αa(0.2 μm), αa(1.06 μm), αa(2 μm), αa(3 μm),
βa(1.1, 1.06 μm), the high sensitivities are to biases in βa(1.1, 0.41 μm), βa(1.1, 0.56 μm). The
positive slopes indicate higher values of reff and V when the optical data are affected by positive
biases than when they are not affected by biases, while for negative slopes just the opposite
occurs. According to Fig. 15 and Fig. 16, in order to obtain inversion error less than 20%, the
error of optical parameters should be controlled within 2%.

Fig. 15. Percentage deviation of the effective radius as a function of systematic bias in the optical
data. (a) the error induced by the extinction coefficients, and (b) the error induced by the forward
scattering coefficients.
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A905

Fig. 16. Percentage deviation of the volume concentration as a function of systematic bias in the
optical data. (a) the error induced by the extinction coefficients, and (b) the error induced by the
forward scattering coefficients.

6. The feasibility of the measurement in the real atmosphere

From the above simulations, the precise size distribution of aerosol particles and fog droplets
in the open atmosphere can be obtained using the optical signals at the optimal forward
scattering angle of 0° and 1.1° (~19 mrad) in the detection of a wide-spectrum light with the
wavelength between 0.2 and 3 μm. The collimation of the light beam and the light propagation
distance in the atmosphere are very important for our scattering measurement. From the section
3, the scattering phase functions of particles are sensitive to the angles. In order to make the
change of CV less than 3%, the divergence angle of the light beam need be controlled within
1mrad. According to our system scheme in Fig. 1, Lens1 is a collimator, and the transmission
lenses are not suitable due to the existence of chromatic aberration. Reflective lenses with long
focal length can be used for the collimation of light beam with wide spectrum. The combination
of the Cassegrain telescope with a focal length greater than 1 m and a fiber with a core diameter
of 1 mm can ensure that the divergence angle is less than 1 mrad. Similarly, reflective lenses
need be used for the convergence of beams. The light propagation distance in this method
should not be too short in order to obtain sufficient detection sensitivity. Meanwhile, the optical
path distance cannot be too long. Too long optical path distance not only increases the volume
of the measurement instrument, but also affects the optical signals due to the atmospheric
turbulence. The optimal distance would be different for aerosol and fog particles with different
concentrations. It is considered that the optical path between Len1 and Len2 in Fig. 1 is folded
by using two mirrors.
The designed optical system schematic diagram is shown in Fig. 17. Tungsten halide lamp
with wide spectral range can be used as light source. The light beam is transmitted to the focal
point of Cassegrain telescope1 (focal length = 2 m) through an optical fiber with 1mm core
diameter. Fiber attenuator can be used to adjust the energy of output beam. The collimated light
with a divergence angle of 0.5 mrad is emitted into the atmosphere after the Cassegrain
telescope1. A variable diaphragm is used to control beam aperture. Two mirrors with high
reflectivity are used to control the optical path length in the atmosphere. Adjust slightly the
angle between the two mirrors, and the optical path length will change accordingly. By
changing the aperture of the beam and the angle between the two mirrors, the path of the beam
can be controlled to change from 1m to 1000 m. When the severe haze / fog occurs, short optical
path length is needed. When the aerosol concentration in the air is low, long optical path length
is needed. The Cassegrain telescope2 (focal length = 2m) is used to collect the attenuated and
scattered light. Two fibers with 1mm core diameter placed on the focal plane of Cassegrain
telescopes2 are used to receive the forward scattered light at angles of 0° and 1.1°. Adjust the
optical axes of telescopes 1 and 2 so that they are parallel to each other. The fiber placed on the
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A906

focal plane receives the attenuated light at the angle of 0°. Considering the divergence angle,
the fiber receives all the transmitted beams with divergence angle of 0.5mrad. Another optical
fiber is placed on the focal plane with a distance of 38.4 mm from the focal point, and it receives
the 1.1°forward scattered light. Considering the receiving field of view, the second fiber
receives the forward scattered light of 1.1° ± 0.0144°. These designs are feasible in real
atmosphere.

Fig. 17. The designed optical system schematic diagram of PSD measurement.

In order to induce the inversion error of PSD, the optical parameters with high precision
need be measured. According to the Eq. (5), the error of the extinction coefficient is determined
by the error of optical path length L, the emitted power of light source J0(λ), the detected power
Jα(λ), the transmittance of optical system T(λ) and the extinction coefficient of air molecule
αm(λ). L and T(λ)are system constants, and they can be calibrated precisely. The fluctuation of
the light intensity will not affect the result, because the term of intensity is a ratio. When haze
or fog occurs in the atmosphere, the value of αm(λ) is far less than aerosol extinction. So the
error of αm(λ) can be neglected. The error of the forward scattering coefficient comes from the
error of the detected power at the angle of θ Jβ(θ, λ) and Jα(λ). Similarly, the value is also a
ratio, so the effect of the light intensity fluctuation can be neglected. According to the above
discussion, the measurement accuracy of system will be high if the system constants can be
accurately calibrated. And the calibration of system constants is not a difficult task.
7. Conclusion and discussion
A photoelectric detection method for APSDs and FDSDs of fog/haze/smog simultaneously in
the open atmosphere is presented and described in this paper. Extinction measurement and
small-angle forward scattering measurement are adopted for the retrieval of PSD in our method.
The key technology including optimal scattering angle and optimal wavelengths selection is
discussed and solved. The optimal forward scattering angle is calculated to be 1.1°, and seven
wavelengths for extinction coefficients and five wavelengths for forward scattering coefficients
are chosen for the measurement of PSD. The regularized inversion algorithm is used for the
retrieval of APSDs and FDSDs. The six known APSDs and FDSDs were used for method test
and the reconstructions of PSD. The simulation results show that the method can achieve the
measurement of APSDs and FDSDs. The worst cases often occur at the radius less than 0.1μm
for APSDs, the maximum relative error may reach 25%. The basic distribution characteristics
can be well retrieved. For FDSDs, high precision results can be obtained. The optical
parameters at several fixed wavelengths in the above method are chosen for the detection of
PSD, and the optical parameters of these wavelengths can basically satisfy the detection of
APSDs and FDSDs simultaneously. The urban industrial aerosol and fog are discussed in this
paper, they can be thought of as spherical, so Mie theory are used for the calculation of optical
coefficients. If there are non-spherical particles such as dust, the Mie theory will induce error.
The kernels need to be generated in the range of size parameters 0.012 ≤ x= 2π r ≤ 625 using
λ
the T-matrix method or DDA method. These contents will be discussed in future work.
 Vol. 27, No. 12 | 10 Jun 2019 | OPTICS EXPRESS A907

Funding
National Natural Science Foundation of China (NSFC) (41627807, 61575160 and 61875163).
Acknowledgments
Thanks to the professor Mao Jietai from Peking University for giving the good suggestion about
the aerosol size distribution measurement.
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