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Atmospheric Research 281 (2023) 106468

Contents lists available at ScienceDirect

Atmospheric Research
journal homepage: www.elsevier.com/locate/atmosres

Impact of Relative Humidity on the vertical distribution of aerosols


over India
P. Prasad , Ghouse Basha , M. Venkat Ratnam *
National Atmospheric Research Laboratory (NARL), Gadanki, India

A R T I C L E I N F O A B S T R A C T

Keywords: Water uptake by aerosol particles significantly changes its light-scattering characteristics, alters the physical and
Aerosols optical properties of aerosols. In this article, we present the effect of ambient relative humidity (RH) on the
Extinction coefficient optical properties of surface and columnar aerosols under different RH conditions during different seasons over
Relative humidity
India. In particular, relation between surface RH and surface aerosol properties, surface RH and aerosol optical
Hygroscopic growth
depth (AOD) and profile of RH on the AOD is presented. An increase in the surface aerosol scattering coefficient
(σscat) and total aerosol number concentration (N(d)) is observed under high humidity (50–100%) condition than
low humidity (0–30%). This is more prominent in the winter and pre-monsoon seasons. An increase in the AOD is
observed as surface RH increase in all the seasons except in monsoon season where it showed an inverse relation.
The profile measurements (Lidar and radiosonde) also showed a consistent increase in AOD (0-6 km) from low to
high RH (0-6 km) conditions. This relationship is significant during winter followed by the post-monsoon, pre-
monsoon, and monsoon seasons. An increase in AOD with RH is observed regardless of altitude in all seasons,
except during the monsoon at higher altitudes (2-6 km). Our findings clearly demonstrated that during the winter
and monsoon (pre- and post-monsoon) seasons, aerosols within (above) the boundary layer are more sensitive to
the RH. This relationship has been tested in different surface conditions across India using CALIPSO and IMD
radiosonde measurements. These measurements also confirmed an increase in AOD with increasing RH in all the
regions except East Coast (EC) region. Irrespective of the region, this feature is more prominent at lower altitudes
(0–1.5 km) during winter and higher altitudes (1.5-6 km) during other seasons. At higher altitudes, only a few
regions (Central India, Indo-Gangetic Plain, and West Coast) showed an inverse relationship between AOD and
RH during the monsoon and post-monsoon seasons. Further, our results illustrated the contribution of hygro­
scopic particles to the RH increases the AOD in a given season. This finding implies that hygroscopic growth
caused by water-soluble particles in the lower troposphere can significantly alter the magnitude of aerosol
radiative forcing both at the surface and at the top of the atmosphere.

1. Introduction of various chemical species such as soot, sulphate, nitrate, organic car­
bon, and mineral dust (Tijjani et al., 2014). As a result, the hygroscopic
In both direct and indirect ways, atmospheric aerosols contribute properties of water-soluble aerosols have a significant impact on their
significantly to the uncertainty in climate change assessments (IPCC, size at ambient RH, altering scattering capability and residence time in
2022). The ambient relative humidity (RH) is an important factor that the atmosphere (Ogren and Charlson, 1992). Furthermore, as RH in­
influences the microphysical and optical properties of aerosols, as well creases to 100%, the amount of water uptake by these aerosols will
as their chemical composition and aerosol loading due to water uptake depend on their chemical composition, as compared to the dry state, and
(Chen et al., 2018a). One of the causes for the uncertainties is the thus changes in their optical properties (Ogren and Charlson, 1992). Sea
interaction between atmospheric water vapour and aerosol (i.e., aerosol salt, for example, is purely hygroscopic and exhibits an increase in
hygroscopicity) (Kuang et al., 2016). The hygroscopicity of aerosols can scattering coefficient as RH increases when compared to dust particles
also influence secondary aerosol formation and visibility (Chen et al., (Zieger et al., 2013). Thus, the mixing state and hygroscopicity of
2018b; Wu et al., 2018a). Tropospheric aerosols are primarily composed aerosol particles are critical because they influence the radiative budget

* Corresponding author.
E-mail address: vratnam@narl.gov.in (M.V. Ratnam).

https://doi.org/10.1016/j.atmosres.2022.106468
Received 1 July 2022; Received in revised form 13 September 2022; Accepted 11 October 2022
Available online 14 October 2022
0169-8095/© 2022 Elsevier B.V. All rights reserved.
P. Prasad et al. Atmospheric Research 281 (2023) 106468

and the activity of cloud condensation nuclei (Twomey, 1977). The in­ (scattering coefficient, absorption coefficient, and total aerosol number
formation on aerosol loadings (e.g., aerosol optical depth) and aerosol concentration) measured by co-located aerosol instruments over
optical properties (e.g., extinction and absorption coefficient, single Gadanki from 2008 to 2015. Using long-term CALIPSO and network of
scattering albedo) are crucial for estimating radiative forcing. These India Meteorological Department (IMD) radiosonde observations, this
parameters, however, are completely dependent on the ambient RH study was also extended to other regions in India. The understanding of
(Tang et al., 1996). As a result, aerosol optical and microphysical the RH effect is critical for validating ground-based measurements with
properties measured at dry state differ significantly from ambient RH optical aerosol measurements (eg. Lidar and satellite retrieval).
conditions. Furthermore, the RH effect is important for satellite retrieval correction
In recent years, different studies have been conducted to investigate (e.g., Remer et al., 2005) and for improving climate models (e.g., Chin
the impact of RH on the optical properties of aerosols from field cam­ et al., 2009).
paigns, laboratory experiments, aircraft measurements and modelling
efforts around the world (eg. Burgos et al., 2019; Jin et al., 2022; Xu 2. Data and Instrumentation
et al., 2020). However, most of the measurements are typically per­
formed under dry conditions by heating air mass samples (Burgos et al., 2.1. Ground-based aerosol measurements
2019). Measurement of RH dependence aerosol optical properties at
various ambient RH conditions is required for climate forcing calcula­ The scattering coefficient (σscat), absorption coefficient (σabs) and
tions in the regional atmosphere (Yu et al., 2018). According to a recent total aerosol number concentration (N(d)) are obtained from the various
study, aerosols can absorb water as the ambient RH rises, which co-located instruments such as Nephelometer, Aethalometer and Aero­
significantly increase the light scattering coefficient by changing parti­ dynamic particle sizer (APS), respectively, over Gadanki (13.5oN,
cle size and shape at surface (Jin et al., 2022). In urban areas over 79.2◦ E) during 2008–2015. Nephelometer (TSI, model 3563) provides
Tehran, the extinction coefficient is found to be smaller at low RH an aerosol scattering coefficient at three different wavelengths (450,
conditions but increases rapidly at high RH conditions (Sabetghadam 550, and 700 nm). Scattering coefficient at 550 nm is used in this
and Ahmadi-Givi, 2014). Several studies have also showed that the analysis. Aethalometer (model AE-31) estimates aerosol absorption co­
growth of the extinction coefficient varies under different humidity efficient at seven wavelengths viz., 370, 470, 520, 590, 660, 880 and
conditions at the surface (Lin et al., 2013; Sun et al., 2013). The effect of 950 nm and is operated since 2008. Data screening procedures and
RH on aerosol optical properties is not only noticed at the surface but estimation of absorption coefficient and other technical details are dis­
also seen on the Aerosol Optical Depth (AOD). Eck et al. (2008) has cussed in Ravi kiran et al. (2018). The absorption coefficient at 550 nm is
reported that an increase in AOD is observed with increasing in the total used in this study which is re-estimated from the 880 nm and 520 nm
column water vapour (CWV). A strong positive correlation is also found (Nandan et al., 2021). APS (TSI model 3321) provides an aerosol size
between AOD and CWV during severe haze episodes in January 2013 distribution at a wavelength of 655 nm. The APS measures size resolved
over Beijing, China (Bi et al., 2014). Previous studies over China also aerosol number concentration whose range of its detection diameter
highlited the relationship between PM2.5 concentrations and visibility (aerodynamic diameter) is from 0.5 to 20 μm and binned into 52
and this relation depends significantly on the ambient RH (Wang et al., channels (Nandan et al., 2021). AOD is obtained from the Sky-
2019; Gui et al., 2019). However, aerosol distribution in the troposphere radiometer (POM-01L, Make: Prede Co. Ltd., Japan) being operated at
is not uniform throughout the altitudes and varies regionally and Gadanki since 2008. It measures the direct and diffuse sky radiance at 5
seasonally. As a result, the RH effect on columnar aerosol properties will wavelengths (400, 500, 675, 870, and 1020 nm) at 1 min. and 10 min.
be complex, necessitating detailed investigations at various background intervals, respectively. Sky-radiometer provides various aerosol optical
conditions (Qiu and Shu, 2018). properties such as Aerosol Optical Depth (AOD), asymmetry parameter,
To investigate the relative impact of RH on columnar aerosol prop­ and single scattering albedo etc., based on the SKYRAD software
erties, we must rely on vertical profiles of RH and aerosol extinction (Nakajima et al., 1996). AOD at 500 nm measured by sky-radiometer
rather than surface RH. Globally, there are very few studies that use during 2008 to 2015 is used in this analysis. More details of this in­
observations to understand the impact of the vertical profile of RH on strument and retrieval methods are described in Madhavan et al. (2021).
the aerosol extinction profiles. Using aircraft measurements, it was re­ Besides these, we also make use of simultaneous measurements from
ported that the variability of aerosol extinction is primarily controlled Automatic Weather Station (AWS) to understand the surface RH impact
by aerosol loading and RH, with less contribution from aerosol on the aerosol optical properties.
composition over the Baltimore–Washington region (Beyersdorf et al.,
2016). Using 27 months of Cloud Aerosol Lidar Infrared Pathfinder 2.2. Ground-based Lidar MPL
Satellite Observations (CALIPSO) measurements at five different surface
conditions across China, Qiu and Shu (2018) found that water vapour in Micro Pulse Lidar (MPL) being operated at NARL, Gadanki is used for
the atmosphere has a significant influence on the aerosol extinction studying the optical properties of aerosols and boundary layer charac­
coefficient. It is well understood from these works that aerosol extinc­ teristics during August 2010 to December 2018. This MPL consists of Nd:
tion coefficient increases under high humidity conditions. However, YAG laser operated at 532 nm wavelength with an energy of 4 μJ and
majority of the studies cited above are primarily concerned with the pulse repetition frequency of 2500 Hz. This Lidar is being operated only
impact of RH on surface aerosol parameters, with little focus on the at night times during clear and partially clear sky conditions due to a
vertical extent of aerosols. The relationship between humidity and the highly sensitive photo-multiplier tube. MPL provides raw backscatter
extinction coefficient in the troposphere, on the other hand, has received signals in the form of photon counts which are integrated over 1-min
more attention but has not been investigated in detail. temporal resolution and stored at 30 m vertical resolution from the
To the best of our knowledge, the effect of RH on the vertical extent surface to 45 km. Background noise correction and range correction has
of aerosols has not yet been reported over the Indian region, which is been taken care before deriving the aerosol extinction profiles as already
one of the most polluted regions. This could be due to a lack of obser­ discussed in the earlier literatures (Gupta et al., 2021; Prasad et al.,
vational data on concurrent vertical profiles of aerosol extinction and 2019). The aerosol extinction has been estimated using Fernald inver­
humidity. We present an approach for assessing the impact of RH on the sion method (Fernald, 1984), by assuming Lidar Ratio as 40 sr and
vertical distribution of aerosol using data from ground-based Micro- reference height at 8 km. The complete technical details of MPL and
Pulse Lidar (MPL) and simultaneous radiosonde observations over methodology of estimating aerosol extinction profiles is provided in the
Gadanki (13.5◦ N, 79.2◦ E) in India collected during 2010 to 2018. We previous studies (Gupta et al., 2021; Prasad et al., 2019). In this study we
also looked at how surface RH affected surface aerosol parameters considered mean aerosol extinction profiles from MPL measurements

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P. Prasad et al. Atmospheric Research 281 (2023) 106468

obtained during 19:00 to 21:00 IST, which is the closest time of radio­ which reflects in the aerosol extinction profile (Guo et al., 2017; Tackett
sonde launching, to understand the influence of vertical profile of RH on et al., 2018; Zeng et al., 2021). Due to this reason, we have considered
the vertical extent of aerosols. We also estimated AOD by integrating the the aerosol extinction profile from ~100 m above from the surface. The
aerosol extinction from surface to the desired altitudes (0–1 km, 1–2 km, CALIPSO measurements have larger bias in the daytime measurements
2–4 km, 4–6 km). than the night time due to contamination from several other sources (eg.
solar background illumination) which causes difficulty in detecting
optically thin layers during daytime (Mamouri et al., 2009; Zeng et al.,
2.3. Space-borne Lidar CALIPSO 2021). The extinction profile derived from CALIPSO matches well with
ground-based Lidar measurements over Gadanki (Gupta et al., 2021;
Ground-based Lidars will provide columnar distribution of aerosols Prasad et al., 2019; Ratnam et al., 2018). Thus, the extinction profiles at
with good vertical and temporal resolution but difficult to get spatially. 532 nm only at night time overpass from the CALIPSO observations are
Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) onboard taken by considering the grid size of ±0.5◦ to the latitude and longitude
Cloud Aerosol Lidar and Infrared Pathfinder Satellite Observations of corresponding radiosonde stations (Fig. 1). Further, in order to un­
(CALIPSO) provides an excellent opportunity to obtain extinction pro­ derstand the aerosol types over Gadanki and other parts of India, we
files spatially. CALIPSO is a dual-polarization elastic backscatter Lidar have taken the Vertical Feature Mask (VFM) data from the CALIPSO
designed to study the vertical extent of aerosols and clouds (Winker measurements.
et al., 2009). It is a nadir viewing satellite inclined at 98◦ at an altitude of
705 km with a 16-day repeat cycle launched in April 2006 (http
://www-calipso.larc.nasa.gov/). In the present study we used Level 2, 2.4. Radiosonde measurements
version 4.20, 5-km aerosol profile products from the CALIPSO during
2006–2020. By applying the Cloud Aerosol Discrimination (CAD) score The high-resolution GPS radiosondes have been launched regularly
ranging from (− 100 to − 20), it discriminates the aerosols from the at 12:00 UTC (17:30 IST) from Gadanki since April 2006. These radio­
clouds and other layers. We followed all the screening procedures and sondes provided profiles of atmospheric meteorological parameters such
applied quality control flags to the Level 2 data prior to use in the as Temperature (T), Pressure (P), Relative Humidity (RH), Wind Speed
analysis (Winker et al., 2013). The major limitation in the space-borne (WS) and Wind Direction (WD) up to an average altitude of ~30 km. The
lidars is the signal contamination mainly within the boundary layer raw data were recorded at a sampling interval of 1 s with vertical

Fig. 1. (a) Map of India showing the radiosonde stations used in this study. The solid circles with different colours represent IMD radiosonde stations considered for 7
different geographic locations and the star denotes observational site Gadanki. The background colour contours show the Aerosol Optical Depth (AOD) observed
using MODIS averaged during 2001–2018. Composite monthly mean profiles of (b) temperature, (c) relative humidity, (d) wind speed, and (e) wind direction
obtained using GPS radiosonde measurements over Gadanki averaged from 2010 to 2018. Black solid line in (b) and (c) represents the composite monthly mean
atmospheric boundary layer (ABL) altitude obtained from radiosonde measurements during 2010–2018.

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P. Prasad et al. Atmospheric Research 281 (2023) 106468

resolution of 5-6 m (Hemanth Kumar et al., 2015; Ratnam et al., 2014). 4. Result and discussion
The quality checks have been applied to maintain continuity and con­
sistency in the measurements (Ratnam et al., 2014). The radiosonde 4.1. Diurnal and annual variation of surface aerosol parameters and
profiles are interpolated to 30 m to remove the outliers and to match relative humidity
with the MPL measurements. In this study, we used T, RH, WS and WD
profiles from the radiosonde during 2010–2018. Further, we have Fig. 2(a-c) show the seasonal mean diurnal variation of scattering
considered data from the 23 IMD radiosonde stations over India coefficient (σscat), total aerosol number concentration (N(d) > 0.5 μm),
covering seven different geographical regions based on the spatial het­ and absorption coefficient (σabs) from the surface observations over
erogeneity of AOD and topography as shown in Fig. 1. This AOD Gadanki, averaged from 2008 to 2015. The surface aerosol parameters
(combined Deep Blue (DB) and Dark Target (DT) product) is obtained (σscat, σabs and N(d)) show a distinguishable peak in the morning hours,
from MODerate resolution Imaging Spectroradiometer (MODIS) satellite thereafter, gradually decrease to a minimum value in the afternoon and
averaged during 2001–2018 (https://giovanni.gsfc.nasa.gov). This then attain a secondary peak around evening. Compared to other sea­
product is MODIS-Terra merged DT and DB at 550 nm for the land and sons, significant diurnal variation has been observed during winter. The
ocean (MOD08_M3) C6.1 Level 3 monthly AOD (Wei et al., 2019). These decrease in the coefficients and concentrations during daytime are pri­
observations have a spatial resolution of 1◦ × 1◦ with a swath of 2330 marily due to strong atmospheric mixing and dilution of pollutants as
km and 36 spectral bands. The available IMD radiosonde stations cover boundary layer height increases (Mehta et al., 2017; Nandan et al.,
most of heterogeneous variability in AOD regions and different surface 2021). After sunset the formation of stable boundary layer leads to
conditions. Since, we have selected CALIPSO night time ~ 20 UTC constrain the aerosol concentrations near to the surface and remain high
(~01:30 IST) overpass observations, we chose the closest time of IMD until early morning hours (Talukdar and Ratnam, 2021). Fig. 2(e)–(g)
radiosonde data is at 00 UTC (05:30 IST). We have obtained quality show the composite monthly mean of scattering coefficient, total aerosol
controlled IMD radiosonde observations data from the Integrated Global number concentration, and absorption coefficient. During the winter
Radiosonde Archive (IGRA) (Durre et al., 2006). (monsoon) season, the maximum (minimum) values are observed in all
surface aerosol parameters (σscat, σabs and N(d)). The boundary layer
3. Location and background meteorological conditions dynamics primarily control the diurnal and seasonal variation of all
surface aerosol parameters (Mehta et al., 2017; Nandan et al., 2021). In
The measurements are being carried out at Gadanki, a tropical rural addition to the boundary layer, wind speed is also responsible for
site located in the southern peninsular India (Fig. 1a). Burning of wood, changes in surface aerosol properties by influencing the transportation
agriculture residue and forest fires are most common events from the and dilution of atmospheric aerosols (Krishnan and Kunhikrishnan,
surrounding villages nearby Gadanki (Jain et al., 2019). A National 2004; Nandan et al., 2021). Furthermore, wet scavenging influences
Highway (NH-18) which passes near the observational site, experiencing aerosol distribution both near the surface and vertically, resulting in
moderate to heavy traffic could be one of the major sources for the higher (lower) aerosol concentrations during the winter (monsoon)
anthropogenic emissions. The climatological monthly mean meteoro­ season (Nandan et al., 2021; Ratnam et al., 2018). However, Prasad et al.
logical parameters (T, RH, WS, and WD) observed over Gadanki using (2021) showed that it is the strong thermal inversions that control the
radiosonde measurements averaged from 2010 to 2018 is also shown in vertical distribution of aerosols rather than boundary layer altitude.
Fig. 1. The vertical profiles of T, RH, WS and WD are shown only up to 6 Few studies have already demonstrated a direct relationship between
km that is relevant to the present study. The temperature has shown ambient RH and aerosol optical properties (e.g., Jin et al., 2022; Lin
large variation mainly below the boundary layer with maximum during et al., 2013). The emissions near the surface over the region, in
pre-monsoon and minimum in winter months (Fig. 1b). The boundary conjunction with the meteorological parameters, play a significant role
layer altitude derived from radiosonde is also superimposed in the same in changing the aerosol distribution. Because of its hygroscopicity,
panel and the details of this estimation are given in Basha and Ratnam studies investigating the effect of RH on aerosols are gaining more
(2009). The RH is mainly restricted to lower altitudes (up to ~2.5 km) attention these days. Thus, detailed investigations have been conducted
during winter (Fig. 1c). In monsoon, higher RH and maximum wind in this study to understand the effect of RH on aerosols both near and far
speed (Fig. 1d) is noticed at higher altitudes (~2-6 km) due to strong from the surface. Therefore, the variability of RH at diurnal and seasonal
low-level jet (LLJ) persisting during monsoon season (Ratnam et al., scales of RH is shown in Fig. 2d & 2h, respectively. It exhibits a distinct
2018). The wind direction (Fig. 1e) observed during monsoon season diurnal cycle, with maximum RH from the evening to early morning
show that winds are mainly coming from southwest direction over hours and minimum RH during the day (Fig. 2d). This feature is prev­
Gadanki. Whereas, other seasons winds are mainly from north and alent, especially during the winter. During the period 2008–2015, the
northeast direction. Gadanki experiences both southwest and northeast maximum RH is observed during the post-monsoon (74 ± 17%), fol­
monsoon which contribute to wet scavenging of aerosols mainly below lowed by the winter (71 ± 21%), monsoon (61 ± 17%), and the mini­
the boundary layer which leads to a clean environment (Ratnam et al., mum during the pre-monsoon (56 ± 23%) (Fig. 2h). Interestingly,
2018). The IMD classified the seasons based on the background wind temporal and seasonal variations in σabs, σscat, and N(d) are closely
conditions over India. The seasons are categorized as winter (Decem­ related to changes in surface RH. Therefore, it is clear that, changes in
ber–February), summer/pre-monsoon (March–May), monsoon/South the ambient RH in the atmosphere can alter the particle size of aerosols
West (SW) monsoon (June–September), and post-monsoon/North East due to their hygroscopic growth, and thus modify the aerosol back­
(NE) monsoon (October–November). The onset of the SW monsoon oc­ scattering (Kuang et al., 2016; Zieger et al., 2013). The changes in sur­
curs in the first week of June (over Trivandrum), and its withdrawal face aerosol parameters under different ambient RH conditions will be
starts in the middle of September (from the central India). Thereafter, quantified in the following sub-section.
NE monsoon prevails during October to November over south-eastern
part of India, until the monsoon front withdraws fully from the Indian 4.2. Impact of ambient RH on aerosol parameters at surface
subcontinent.
The optical properties of aerosols will be influenced by the amount of
water vapour present in the atmosphere, either through absorption at a
specific wavelength or due to their hygroscopic nature (Niranjan and
Babu, 1993). Based on the distribution of RH values observed over
Gadanki, we considered three different ranges (i.e., low RH (0–30%),
medium RH (30–50%), and high RH (50–100%)) to examine the effect of

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Fig. 2. Seasonal mean diurnal variation of (a) Scattering coefficient (σscat), (b) Aerosol number concentration (N(d)), (c) Absorption coefficient (σabs) and (d) Relative
humidity (RH) at surface. (e)-(h) is same as (a)-(d) but for composite monthly mean during 2008–2015 over Gadanki.

RH on surface aerosol parameters. During the winter (pre-monsoon) coefficient (βp) increased slightly under low RH conditions and sharply
season, the mean scattering coefficient (σscat) value increases from 92 under high RH conditions as the fine-mode aerosol mass concentration
Mm− 1 to 202 Mm− 1 (101 Mm− 1 to 145 Mm− 1) as the RH range increases increased. Secondary aerosols with higher aerosol hygroscopicity
from 0-30% to 50–100% (Fig. 3a). The total aerosol number concen­ formed under high RH conditions, contribute significantly to βp via
tration (N(d)) increases in mean values from 54 cm− 3 to 116 cm− 3 (58 aerosol hygroscopic growth at both the ground and 532-m levels (Jin
cm− 3 to 83 cm− 3) as the RH range increases from 0-30% to 50–100% et al., 2022). During the monsoon and post-monsoon seasons, the
during winter (pre-monsoon) (Fig. 3b). In the monsoon and post- southwest and northeast monsoons have the greatest influence on the
monsoon, similar increases in σscat and N(d) are not observed as RH observational site Gadanki (Basha and Ratnam, 2013). Due to strong wet
increases. However, regardless of season, the absorption coefficient scavenging, a very clean atmosphere is observed within the boundary
(σabs) remains more or less constant for varying RH ranges (Fig. 3c). The layer during the monsoon (Prasad et al., 2019; Ratnam et al., 2018).
strong (weak) correlation coefficient is observed between scattering When compared to other seasons, all surface aerosol parameters show
coefficeint, number concentration (absorption coefficient) and RH in all relatively lower concentrations during the monsoon (Fig. 2). Despite the
seasons and the correlation is significant during winter (Fig. S1). The fact that there is a enough moisture at the surface during monsoon
higher scattering coefficient under high RH condition during winter season, no significant changes in the aerosol optical parameters are
could be attributed to the availability of water-soluble particles, which observed under different RH conditions. This could be because of the
could have resulted in an increase in aerosol particle size and, as a result, low aerosol loading near the surface (Ravi kiran et al., 2018) and the
an increase in light scattering. Furthermore, as ambient RH rises, aero­ lack of hygroscopic particles over the Gadanki. This result demonstrates
sols grow due to water uptake, which enhances aerosol hygroscopicity the significant impact of ambient RH on aerosol scattering coefficient
and aids in the formation of secondary aerosols and particle accumu­ and aerosol number concentration, which was primarily observed over
lation (Wu et al., 2018b). Zang et al. (2019) reported that under wet Gadanki during the winter and pre-monsoon seasons. The effect of
2−
conditions, ammonium (NH+ 4 ), sulphate (SO4 ), and nitrate (NO3 )

ambient RH on the optical properties of columnar aerosols is discussed
concentrations were increased by 2.5, 2, and 1.5 times, respectively, and in the following sub-section.
that ammonia-rich conditions in wintertime efficiently promoted the
formation of SO2−4 and NO3 over Wuhan, China. These secondary ions

play an important role in increasing pollution and aerosol light scat­ 4.3. Effect of surface RH on columnar AOD
tering. Jin et al. (2022) also reported that the aerosol scattering
Another important aerosol optical property is aerosol optical depth

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P. Prasad et al. Atmospheric Research 281 (2023) 106468

Fig. 3. Seasonal variation of (a) Scattering coefficient (σscat), (b) Aerosol number concentration (N(d)), (c) Absorption coefficient (σabs), and (d) Aerosol Optical
Depth (AOD) under different ambient relative humidity conditions during 2008–2015 over Gadanki.

(AOD), which indicates the quantitative measure of total columnar


aerosol concentrations from the surface to the top of the atmosphere. To
investigate the effect of surface RH on AOD, we used the hourly aver­
aged AOD from the co-located sky-radiometer measurements and the
corresponding hourly RH data from AWS. Fig. 3d depicts the AOD under
various RH conditions and seasons. Except during monsoon season, an
increase in AOD is observed as surface RH increases from 0-30% to
50–100% (Fig. 3d). Generally, surface RH will have less impact on the
columnar AOD because it represents the integral of total aerosol con­
centrations from the surface to the top of the atmosphere. Surprisingly, it
is observed that surface RH has a significant effect on columnar AOD.
Such systematic increase in columnar AOD is not observed during the
monsoon season. In contrast, we see the inverse relation between AOD
and surface RH. This is expected as in the monsoon months, we have
noticed less surface RH (Fig. 2d) and high RH in 2-6 km (Fig. 1c) over
Gadanki. Moreover, in monsoon season a significant amount of aerosols
(~80–90%) are found above the boundary layer which is contributing to
the total AOD and clean environment below ~2 km (Prasad et al., 2019).
Thus, it is clear that vertical distribution of aerosol and RH is not uni­
form throughout the altitude and it changes from season to season. Thus, Fig. 4. Typical profiles of aerosol extinction, temperature (T), relative hu­
the detailed investigations are required to understand the role of RH on midity (RH) observed over Gadanki during (a) high humidity day on 21
vertical extent of aerosols during different seasons. Nevertheless, using December 2016 and (b) low humidity day on 22 December 2016. Black solid
surface RH to assess the effect of RH on the total vertical extent of line represents the ABL altitude during respective days.
aerosols is difficult. In order to investigate the actual impact of RH on the
columnar aerosols at various altitudes, vertical profiles of RH are interesting to see that the vertical profile of RH closely matches the
required. We used simultaneous RH profiles obtained from radiosonde vertical profile of aerosols. This is observed not only on the specific days,
measurements launched over Gadanki around 12 UTC for this purpose. but also on multiple days and throughout the seasons. These typical
Fig. 4 depicts typical profiles of aerosol extinction and relative humidity profiles exhibits that there is a close relationship between the two. In the
obtained from simultaneous MPL and radiosonde measurements, following sub-section, we will discuss how aerosols are distributed
respectively. We looked at consecutive low and high humidity days to vertically at different relative humidity levels, as well as their
see how the vertical profile of RH affects the aerosol extinction (Fig. 4). relationship.
When compared to a low humidity day (Fig. 4b), the aerosol extinction is
nearly doubled below ~1 km on a high humidity day (Fig. 4a). It is very

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P. Prasad et al. Atmospheric Research 281 (2023) 106468

4.4. Relation between vertical profiles of relative humidity and aerosol the pre-monsoon season, there is a slight increase in extinction at me­
extinction dium (Fig. 5f) and high (Fig. 5g) humidity levels compared to low hu­
midity levels (Fig. 5e) across the profile. High extinction values (~0.05
In general, aerosols in the atmosphere are mostly concentrated in the km− 1) are observed at higher altitudes (above 4 km) during the pre-
lower layers of troposphere. As a result, as altitude increases, the aerosol monsoon (Fig. 5g), but at low humidity, aerosol extinction is
extinction coefficient decreases. This is also true for the RH, except completely restricted to 4 km (Fig. 5e). Interestingly, the aerosol dis­
during monsoon season where higher humidity conditions prevails at tribution altitude increases from 3 to 3.5 km (3 to 4 km) in medium
higher altitudes (Fig. 1c). We examined the aerosol extinction and RH (high) humidity conditions as compared to low RH condition during
profiles from simultaneous MPL and radiosonde measurements from winter. The vertical extent of aerosol increases from 4 km to 5 km (4 km
2010 to 2018 to investigate the influence of RH profile on the vertical to 6 km) in pre-monsoon.
distribution of aerosols. To reduce the bias of higher altitude RH on Further, we took the difference in aerosol extinction profiles between
aerosol extinction, we used mean RH from the surface to 4 km (up to 6 high-low and medium-low level humidity conditions to see how much
km) during winter (pre-monsoon) in this analysis, based on the vertical enhancement in aerosol extinction at different altitudes during high and
extent of aerosols. Furthermore, based on the mean RH values, we medium humidity conditions (Fig. 6). The maximum difference in mean
separated aerosol extinction profiles into three different humidity con­ extinction coefficient between high and low humidity conditions (me­
ditions (i.e., low RH (0–30%), medium RH (30–50%), and high RH dium and low) is approximately 0.12 km− 1 (0.04 km− 1) and is observed
(50–100%)). During the winter (pre-monsoon) season, the number of during winter between the altitudes of 1–1.5 km (0.8-1 km) (Fig. 6a). In
profiles for low, medium, and high RH cases was 83, 91, and 23 (65, 79, the pre-monsoon (Fig. 6b), the maximum difference between high and
and 18), respectively. Fig. 5 depicts the aerosol extinction profiles under low (medium and low) conditions is found to be ~0.075 km− 1 (~0.03
various humidity conditions during the winter and pre-monsoon sea­ km− 1) between the altitudes of 4-6 km (3–4.5 km). This clearly shows
sons. In the same panels, the mean boundary layer (black solid line) that the effect of RH is not uniform across the altitude and varies with
altitude for the corresponding days is superimposed. Under three altitude and season. Aerosols within the boundary layer (black solid line
different humidity conditions, the mean aerosol extinction profiles show in Fig. 6) are more sensitive to humidity during the winter, whereas
a decreasing trend with increasing altitude, with large differences in above the boundary layer aerosols are more sensitive during the pre-
winter (Fig. 5). Fig. 5d and 5h show the mean aerosol extinction and monsoon. The degree to which aerosols are sensitive to humidity is
mean RH profiles for all humidity conditions during the winter and pre- clearly reflected in aerosol extinction at those altitudes.
monsoon seasons, respectively. The extinction coefficient below the
boundary layer is found to be greater during medium (~0.18 km− 1, 4.5. Impact of RH on AOD at different layers over Gadanki
Fig. 5b) and high-humidity (~0.24 km− 1, Fig. 5c) conditions than dur­
ing low humidity (~0.13 km− 1, Fig. 5a) conditions in winter. Aerosol Previous results show that increasing RH causes an increase in
extinction is nearly doubled below ~1 km in high humidity conditions aerosol extinction. However, based on the extinction profiles, it is
(Fig. 5c), compared to low humidity conditions during winter. During difficult to quantify how much concentration has increased at different

Fig. 5. Mean aerosol extinction coefficient profiles under three different humidity conditions (a) Low humidity (0–30%), (b) Medium humidity (30–50%), (c) High
humidity (50–100%), and (d) all humidity conditions during winter. (e)-(h) is same as (a)-(d) but for pre-monsoon. Black solid line represents the mean ABL altitude
for corresponding humidity conditions.

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Fig. 6. Difference in the mean aerosol extinction profiles between high-low


(orange solid line) and medium-low (blue solid line) level humidity condi­
tions during (a) winter and (b) pre-monsoon over Gadanki. Black solid line
represents the mean ABL altitude during respective seasons. (For interpretation
of the references to colour in this figure legend, the reader is referred to the web
Fig. 7. The variation in AOD under different humidity conditions at different
version of this article.)
altitudes during (a) winter and (b) pre-monsoon over Gadanki obtained from
MPL and radiosonde measurements.
altitudes in relation to RH. We calculated AOD for various altitudes,
such as 0–4 km during winter and 0–6 km in other seasons and calcu­ 4 km during winter (Fig. 7a). This pattern is more pronounced in 2-4 km
lated mean RH for those corresponding altitude ranges. Fig. S2 depicts followed by 4-6 km and 1-2 km in the pre-monsoon, but not in 0-1 km
the variation in AOD for different RH ranges (0–30%, 30–50%, and (Fig. 7b). During the winter (pre-monsoon), the maximum availability of
50–100%) during different seasons. The number of points for each hu­ hygroscopic aerosols may be found at 0-2 km (2-6 km). This causes the
midity condition is indicated in the corresponding panels. During the aerosol particles to grow, resulting in strong scattering and, as a result, a
winter season, a consistent increase in AOD (0.13 to 0.27) is observed as high AOD. This feature, however, is not observed at other altitudes,
the RH range increases from 0- 30% to 50–100% (Fig. S2a). When despite the presence of higher aerosol concentrations and RH. This may
compared to low RH conditions in winter, the AOD nearly doubles in be due to the changes in the chemical composition and aerosol species
high RH conditions whereas in the pre-monsoon, a slight increase in with respect to altitude that modifies the hygroscopic behavior of
AOD (0.26 to 0.32) is observed as RH increases from 0- 30% to 30–50%, aerosols and this will be discussed later.
with little variation observed at 50–100% (Fig. S2b). Over Gadanki, as
previously stated, it is influenced by both the northeast and southwest
monsoons. As a result, there are fewer clear sky aerosol extinction 4.6. Influence of RH on AOD over the Indian region
profiles. With the available data, we demonstrated the behavior of AOD
as a function of RH during the monsoon and post-monsoon seasons In previous sections it has been observed that RH has a significant
(Fig. S2c-d). We observed very high RH during the monsoon, primarily impact on aerosol vertical distribution. Using IMD radiosonde and
at higher altitudes between 2 and 6 km from radiosonde observations CALIPSO measurements, we tried to understand the relation between
(Fig. 1c) over Gadanki due to the presence of a low-level jet (Ratnam RH and AOD in other parts of India. As previously stated, the radiosonde
et al., 2018). As a result, we have divided the RH (0-6 km) ranges as stations in India were classified into seven distinct geographical regions
0–60%, 60–70%, and 70–100% only during the monsoon season. During based on the spatial heterogeneity of AOD and topography, which is
the monsoon, such a systematic increase in AOD with RH is not observed illustrated in Fig. 1. The seven different geographical regions are
(Fig. S2c), whereas in post-monsoon, an increase in AOD (0.15 to 0.24) denoted as Indo-Gangetic Plain (IGP), Central India (CI), North East
is observed (Fig. S2d), as shown in Fig. 3d. Further, we have also esti­ India (NEI), North West India (NWI), South India (SI), East Coast (EC)
mated AOD for different altitude ranges under different humidity con­ and West Coast (WC). Fig. 8 depicts the mean aerosol extinction profiles
ditions during monsoon season (Fig. S3). A slight increase in AOD is observed at three different humidity conditions over different regions of
observed between 0 and 2 km as RH range increases which is not noticed India. The vertical extent of aerosols in the seven regions for these three
in 2-6 km. The findings show that varying RH causes a consistent in­ humidity conditions shows different decreasing magnitudes in the
crease in AOD in all seasons except during monsoon season at higher extinction with increasing altitude. Except for the coastal stations (EC
altitudes. However, it is unclear at what altitudes this influence is more and WC), there is a clear difference in the aerosol extinction profiles
pronounced from this analysis. between high and low humidity conditions during the winter (Fig. 8a).
We divided the surface to 6 km into three (four) altitude layers During the pre-monsoon season, this separation is more pronounced
during winter (pre-monsoon) because of the uneven distribution of over the SI, CI, and IGP regions (Fig. 8b). However, during the monsoon
aerosols and humidity in the lower troposphere: 0-1 km, 1-2 km, and 2-4 and post-monsoon seasons, there is no such clear difference in the
km (0-1 km, 1-2 km, 2-4 km, and 4-6 km). To understand the actual extinction profiles in most of the India. During these two seasons, almost
effect of RH on AOD, the mean RH and AOD estimated for these altitude all regions had a significant amount of aerosols persisting at higher al­
ranges were considered. Fig. 7 depicts the variation in AOD under titudes. Certain altitudes exhibit significant differences in the extinction
different RH conditions at different layers during the winter and pre- profiles between low and high humidity conditions, depending on the
monsoon seasons. A systematic increase in AOD is observed in 0-1 km region.
and 1-2 km for RH values ranging from 0- 30% to 50–100%, but not in 2- To examine the effect of RH on AOD, we calculated the AOD for
altitudes of 0-4 km in winter and 0-6 km in other seasons and took the

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P. Prasad et al. Atmospheric Research 281 (2023) 106468

Fig. 8. Seasonal mean profiles of aerosol extinction observed under different relative humidity conditions during (a) winter, (b) pre-monsoon, (c) monsoon, (d) post-
monsoon over different regions over India obtained from CALIPSO and IMD radiosonde observations during 2006–2020.

mean RH for those altitudes. Fig. 9 depicts the variation in AOD for causes washout of aerosols from the atmosphere, so we have not
different RH ranges (0–30%, 30–50%, and 50–100%) across different observed any significant relation between RH and AOD. This feature is
regions in India. Except for the EC region, a consistent increase in AOD more prominent in lower altitudes (0–1.5 km) during winter and at
with increasing RH from 0- 30% to 50–100% is observed in all regions in higher altitudes (1.5–6 km) in other seasons in all the regions. CALIPSO
winter (Fig. 9). During the pre-monsoon season, an increase in AOD is measurements also confirm that, regardless of the season, RH have large
observed up to 30–50%, after which no significant influence is observed influence on the vertical distribution of aerosols in good parity with that
at 50–100% RH in all regions. During winter and pre-monsoon seasons, observed over Gadanki.
similar features can be seen over Gadanki (Fig. S2). In monsoon and
post-monsoon seasons, few regions (CI, IGP and WC) showed an inverse 4.7. Role of Aerosol sub-types on the relation between RH and AOD
relation between AOD and RH whereas other regions (NWI, SI, NEI and
EC) shows a slight increase in AOD with respect to RH. The sources, In order to see the influence of aerosol types on this relation (RH and
distribution and composition of aerosols that change from region to AOD), we make use of CALIPSO Vertical Feature Mask (VFM) data for
region could be one of the reasons for varying this relation over Indian the troposphere over Gadanki during 2010–2018 (Fig. S4). Polluted
region. Complex nature of aerosols over the IGP is mainly because the Continental (PC) is the dominant aerosol species observed over Gadanki
region is very diverse in topography, population distribution, meteo­ during the winter (Fig. S4e) and post-monsoon (Fig. S4h). Whereas, Dust
rology and emission sources (Srivastava et al., 2012). This region is and Polluted Dust (PD) are found higher percentage during pre-monsoon
strongly affected by frequent and intense dust storms through long- (Fig. S4f) and monsoon season (Fig. S4g). The dominance of PD during
range transport from Thar Desert, southwest Asia, and the Arabian pre-monsoon is mainly attributed to the presence of anthropogenic
Sea. Further, IGP region has distinct aerosol composition which is aerosols over the site produced from the local biomass burning activities
characterized as mixed aerosols with the prevalence of coarser particles and dust from long-range transport (Ravi Kiran et al., 2018). In monsoon
(eg. dust) in the upper IGP, while elevated concentrations of finer (post-monsoon) season, mixed aerosol types consisting of PD, Dust, and
aerosols and soot particles over the middle and lower parts of IGP elevated smoke (PD, PC and elevated smoke) is observed. Using cluster
(Kumar et al., 2019). In central India, the dust emissions from the Thar analysis applied to the sky-radiometer measurements over Gadanki, Sai
Desert and emissions from forest fires and open burning of crop waste Krishnaveni et al. (2022) also observed that the polluted continental is
which contributes more biomass aerosol contribution (Ramachandran dominating species of about 44.72% (58.36%) during the winter (post-
and Cherian, 2008). Hence, the changes in the aerosol composition over monsoon) season over Gadanki. Whereas, in pre-monsoon local biomass
different regions may have significant impact on this relation. In the burning activity and forest fires in peninsular India is contributing to the
west coast region, due to extensive rainfall during monsoon season aerosol (41.65%) concentrations over Gadanki. The highest percentage

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P. Prasad et al. Atmospheric Research 281 (2023) 106468

taken place before reaching the observational site. This may be one of
the reasons why AOD does not increase with increase in RH at higher
altitudes (2-6 km) during monsoon over Gadanki.
We have also investigated aerosol types over different radiosonde
stations to cover different parts of India in different seasons during
2006–2020 (Fig. 10). The higher concentration of PC is observed during
winter and post-monsoon season irrespective of the region. The Dust and
PD are found to be higher percentage during pre-monsoon and monsoon
season in majority of the regions. Similar to Gadanki, we have also
estimated the percentage of availability of hygroscopic and non-
hygroscopic particles over different regions (Table 1). The sufficeint
number of hygroscopic particles are found during winter, followed by
post-monsoon, monsoon and pre-monsoon season over Indian region.
However, significant amount of non-hygroscopic particles are also
noticed during pre-monsoon and monsoon season in all the regions.
Thus, the changing in the concentration of hygroscopic and non-
hygroscopic particles from season to season is one of the possible
reason for varying relation between RH and AOD over Indian region.
Lakshmi et al. (2021) also demonstrated that anthropogenic dust sources
dominate dust loading during the winter, whereas natural dust con­
tributes the majority of total dust loading over the Indian region during
the pre-monsoon season using CALIPSO observations. During the
monsoon, marine aerosols and mineral dust are transported by the
monsoon winds over to the Indian landmass, contributing significantly
to aerosol loading (Mishra et al., 2010; Ratnam et al., 2018). Further­
more, during the monsoon, long-range transport and wet-scavenging
will have a greater impact on the vertical distribution of aerosols than
other meteorological and dynamical parameters (Prasad et al., 2021;
Ratnam et al., 2018). During the post-monsoon season, agricultural
residue burning in the north-west parts of the IGP region (Singh et al.,
2014), that is transported along the wind to the observation site, may
Fig. 9. Variation in the AOD under different humidity conditions over different also contribute to the moderate biomass burning (%) during this season
regions in India (a) West Coast (WC), (b) East Coast (EC), (c) South India (SI), (Singh et al., 2014). We need detailed information on the vertical dis­
(d) Central India (CI), (e) North West India (NWI), (f) North East India (NEI), tribution of aerosol composition and aerosol types to understand the
(g) Indo-Gangetic Plain (IGP) and (h) Total during different seasons. relationship between hygroscopic growth and aerosol optical properties
(Jung et al., 2009; Qu et al., 2015). Thereby the impact of RH on aerosol
of polluted marine aerosol (57.43%) are observed during monsoon also changes according to the availability of water soluble and insoluble
season. Jain et al. (2019) also shown the presence of cations (Na+, Li+, species in a particular season over a region.
2+ 2−
Ca+2 , NH4 , K and Mg ) and anions (F , SO4 , Cl and NO3 ) using
+ + − − −

rainwater analysis collected during monsoon season over Gadanki. 5. Summary and conclusions
Based on the cluster analysis (Omar et al., 2005), the likely composition
given in a particular aerosol types is as follows, PC, Dusty Marine (DM) In this communication, the potential impact of relative humidity
and Clean Continental (CC) contains the majority of the water-soluble (RH) on the surface and elevated aerosol optical properties is investi­
species (eg., SO2−
4 , NO3 , NH4 , and NaCl), whereas the Dust, PD and
− + gated using long-term (2010–2018) simultaneous Micro-pulse Lidar
Elevated Smoke (ES) contains water-insoluble components (eg., soot, (MPL) and radiosonde observations over Gadanki, India. In particular,
OC, and mineral dust). Based on the composition given in the literature the effect of surface RH (AWS measurements) on the surface aerosol
for a particular aerosol type, we have segregated into hygrocopic (PC, properties (Aethalometer, Aerodynamic particle sizer (APS) and Neph­
CC, DM) and non-hygroscopic particles (PD, Dust, ES). Then, we have elometer), surface RH on the integrated aerosols (Aerosol Optical Depth
estimated the percentage of availability of hygroscopic and non- (AOD) (sky-radiometer) and profile of RH (radiosonde) on the profile of
hygroscopic particles over Gadanki and found that higher percentage aerosols (MPL) is presented. After establishing the relation between the
of hygroscopic particles during winter (68%), followed by post-monsoon two, study is further extended to other regions covering complete India
(35%), monsoon (12%) and pre-monsoon (9%) season. The significant using satellite (CALIPSO) and IMD radiosonde observations. In this
impact of RH on AOD during winter and post-monsoon may be due to investigation, we provide comprehensive, observation-based evidence
large amount of hygroscopic particles (water-soluble species) are on the relation between the aerosols and different RH conditions over
available compared to other seasons over Gadanki (Sai Krishnaveni the Indian region. The main findings of this study are summarized as
et al., 2022). The PC (PD) is primarily made up of water soluble follows:
(insoluble) aerosols that are strongly (weakly) affected by humidity (Xue
et al., 2011). The existence of maximum concentrations from marine 1. Increase in the surface aerosol parameters (σscat and N(d)) with in­
aerosols (sodium and chloride particles) found over Gadanki could be crease in the surface RH is clearly noticed during winter and pre-
the reason for observing a slight impact of RH on AOD mainly below 2 monsoon seasons. Interestingly, increase in the AOD (sky-radiom­
km during monsoon season (Jain et al., 2019). At higher altitudes, we eter) with increase in surface RH is also observed in all seasons,
have not observed such increase in AOD with respect to humidity. This except in monsoon season where an inverse realtion is observed. This
may be due to aerosols observed at higher altitudes are mainly trans­ result suggests that effect of RH on AOD varies depending on altitude
ported from the Arabian sea through LLJ (Ratnam et al., 2018). The up and season.
take of high moisture in these advected aerosols might have already 2. Irrespective of the season, the profile measurements of AOD (from
MPL) and RH (from radiosonde) also revealed a consistent increase

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P. Prasad et al. Atmospheric Research 281 (2023) 106468

Fig. 10. Pie chart representing the percentage (%) of total aerosol sub-types observed between 0 and 8 km during (a) winter, (b) pre-monsoon, (c) monsoon, and (d)
post-monsoon over different regions in India.

Table 1
The percentage (%) of availability of hygroscopic and non-hygroscopic particles during different seasons over different regions in India.
Region Hygroscopic (%) Non-Hygroscopic (%)

Winter Pre-monsoon Monsoon Post-monsoon Winter Pre-monsoon Monsoon Post-monsoon

WC 65 40 36 52 35 60 64 48
EC 60 36 46 57 40 64 54 43
SI 54 7 8 33 46 93 92 67
CI 22 1 9 19 78 99 91 81
NWI 15 1 3 7 85 99 97 93
NEI 33 6 26 37 67 94 74 63
IGP 27 2 15 22 73 98 85 78

in AOD (0-6 km) from low to high RH (0-6 km) conditions over monsoon seasons over Gadanki and over the Indian region. One
Gadanki. This relation is significant during winter, followed by the possible explanation for the varying relationship between RH and
post-monsoon, pre-monsoon, and monsoon seasons. AOD during different seasons is that the contribution of hygroscopic
3. Regardless of altitude, an increase in AOD with RH is observed in all particles which are more sensitive to RH is changing from season to
seasons except during the monsoon season at higher altitudes (2-6 season.
km). As a result, aerosols below (above) the boundary layer are more
sensitive to changes in humidity during the winter (other seasons). In this study, we quantified the relation between aerosols and RH
Surface RH represents the average RH below 1.5 km (radiosonde both at the surface and vertical using ground-based and satellite ob­
measurements) indicating that the surface RH may have an impact servations. Seasonal changes in the vertical distribution of aerosol
on the aerosols present up to the boundary layer in all the seasons. compositions are quite different, which alters the relationship between
This finding also clearly demonstrated that the effect of RH on AOD RH and AOD. High aerosol concentrations, which are more hygroscopic
varies with altitude and season. and have a greater optical response to changes in RH, are most likely the
4. The above mentioned aspects are true in all the regions over India, cause for the increase in AOD. To quantify the relative contributions of
except over the East Coast (EC), obtained using the CALIPSO and different mechanisms to this relationship, more in-depth modelling
IMD radiosonde measurements. Thus, regardless of region, an in­ work is required. The combination of observations and modelling will
crease in AOD with increasing RH in all the seasons is consistent. In improve our understanding of the mechanisms underlying RH responses
all the regions, this feature is more prominent at lower altitudes to different aerosol types and their interactions.
(0–1.5 km) during winter and higher altitudes (1.5-6 km) during
other seasons. At higher altitudes, only a few regions (Central India CRediT authorship contribution statement
(CI), Indo-Gangetic Plain (IGP), and West Coast (WC)) showed an
inverse relationship between AOD and RH during the monsoon and P. Prasad: Methodology, Visualization, Validation, Data curation,
post-monsoon seasons. Writing – original draft. Ghouse Basha: Methodology, Visualization,
5. A sufficient number of hygroscopic particles are found during the Writing – original draft. M. Venkat Ratnam: Conceptualization, Visu­
winter season, followed by the post-monsoon, monsoon, and pre- alization, Investigation, Supervision, Writing – review & editing.

11
P. Prasad et al. Atmospheric Research 281 (2023) 106468

Declaration of Competing Interest Hemanth Kumar, A., Ratnam, M.V., Sunilkumar, S.V., Parameswaran, K., Murthy, B.V.K.,
2015. Role of deep convection on the tropical tropopause characteristics at
subdailyscales over the South India monsoon region. Atmos. Res. 161–162, 14–24.
Authors declare no financial interest. https://doi.org/10.1016/j.atmosres.2015.03.012.
IPCC, 2022. Climate Change 2022: Impacts, Adaptation, and Vulnerability. In:
Data availability Contribution of Working Group II to the Sixth Assessment Report of the
Intergovernmental Panel on Climate Change. Cambridge University Press. In Press.
Jain, C.D., Madhavan, B.L., Ratnam, M.V., 2019. Source apportionment of rainwater
Data will be made available on request. chemical composition to investigate the transport of lower atmospheric pollutants to
the UTLS region. Environ. Pollut. 248, 166–174. https://doi.org/10.1016/j.
envpol.2019.02.007.
Acknowledgements Jin, et al., 2022. The different sensitivities of aerosol optical properties to particle
concentration, humidity, and hygroscopicity between the surface level and the upper
We are thankful to the NARL and Department of Space for providing boundary layer in Guangzhou, China. Sci. Total Environ. 803 (2022), 150010
https://doi.org/10.1016/j.scitotenv.2021.150010.
necessary facilities and financial support to carry out this study. We Jung, J., Lee, H., Kim, Y.J., Liu, X., Zhang, Y., Gu, J., Fan, S., 2009. Aerosol Chemistry
would also like to thank ARTG group members (Dr. V. Ravi Kiran, Dr. B. and the effect of Aerosol Water Content on Visibility Impairment and Radiative
L. Madhavan and A. Sai Krishnaveni) for their dedicated effort in Forcing in Guangzhou during the 2006 Pearl River Delta Campaign. J. Environ.
Manag. 90 (11), 3231–3244. https://doi.org/10.1016/j.jenvman.2009.04.021.
obtaining the long-term quality checked observations used in this study. Krishnan, P., Kunhikrishnan, P.K., 2004. Temporal variations of ventilation coefficient at
The data used in the study can be obtained on the request. The authors a tropical Indian station using UHF wind profiler. Curr. Sci. 86, 447–451.
are thankful to CALIOP and MODIS team for providing data used in the Kuang, Y., Zhao, C.S., Tao, J.C., Bian, Y.X., Ma, N.J.A.E., 2016. Impact of aerosol
hygroscopic growth on the direct aerosol radiative effect in summer on North China
present study through their respective sites. We also acknowledge the
plain. Atmos. Environ. 147, 224–233. https://doi.org/10.1016/j.
IGRA for providing meteorological profile data used in this study. atmosenv.2016.10.013.
Kumar, et al., 2019. Atmospheric Aerosols over Indo Gangetic Plain: Characteristics,
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Publishing, Atmospheric Pollution and their complications.
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Supplementary data to this article can be found online at https://doi. distribution of speciated aerosol absorption over South Asia using spaceborne LIDAR
org/10.1016/j.atmosres.2022.106468. and ground-based observations. Remote Sens. Environ. 253, 112164 https://doi.
org/10.1016/j.rse.2020.112164.
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