Abstract. The impact of aerosols on cloud properties is one of the largest uncertainties in the anthropogenic radiative forcing of the climate. Significant progress has been made in constraining this forcing using observations, but uncertainty remains, particularly in the magnitude of cloud rapid adjustments to aerosol perturbations. Cloud liquid water path (LWP) is the leading control on liquid-cloud albedo, making it important to observationally constrain the aerosol impact on LWP. Previous modelling and observational studies have shown that multiple processes play a role in determining the LWP response to aerosol perturbations, but that the aerosol effect can be difficult to isolate. Following previous studies using mediating variables, this work investigates use of the relationship between cloud droplet number concentration (Nd) and LWP for constraining the role of aerosols. Using joint-probability histograms to account for the non-linear relationship, this work finds a relationship that is broadly consistent with previous studies. There is significant geographical variation in the relationship, partly due to role of meteorological factors (particularly relative humidity). The Nd–LWP relationship is negative in the majority of regions, suggesting that aerosol-induced LWP reductions could offset a significant fraction of the instantaneous radiative forcing from aerosol–cloud interactions (RFaci). However, variations in the Nd–LWP relationship in response to volcanic and shipping aerosol perturbations indicate that the Nd–LWP relationship overestimates the causal Nd impact on LWP due to the role of confounding factors. The weaker LWP reduction implied by these “natural experiments” means that this work provides an upper bound to the radiative forcing from aerosol-induced changes in the LWP.

We present results from sun/sky radiometer measurements of aerosol optical characteristics carried out in New Delhi during March–June, 2006, as part of the Indian Space Research Organization's Integrated Campaign for Aerosol Radiation Budget. For the first time at this site, derived are parameters such as aerosol optical depth (AOD), single scattering albedo (SSA), asymmetry parameter, Ångstrom exponent, and real and imaginary refractive indices in five spectral channels. During the campaign, a consistent increase in aerosol loading from March to June with monthly average AOD values at 0.5μm of 0.55, 0.75, 1.22 and 1.18, respectively, was observed. Ångstrom exponent gradually decreases from 1.28 (March) to 0.47 (June), indicating an increased abundance of coarse particles due to dust storms that transport desert dust from the Thar desert and adjoining regions. SSA at 0.5 μm is found to be in the range of 0.84 to 0.74 from March to June, indicating an increasing contribution from the mixture of anthropogenic and desert dust absorbing aerosols. Optical properties derived during the campaign are used in a radiative‐transfer model to estimate aerosol radiative forcing at the surface and at the top‐of‐the atmosphere. A consistent increase in surface cooling is evident, ranging from −39 W m−2 (March) to −99 W m−2 (June) and an increase in heating of the atmosphere from 27 W m−2 (March) to 123 W m−2 (June). Heating rates in the lower atmosphere (up to 5 km) are 0.6, 1.3, 2.1, and 2.5K/d from March, April, May, and June 2006, respectively. Higher aerosol induced heating in the premonsoon period has been shown to have an impact on the regional monsoon climate.

[1] In situ aircraft measurements of cloud microphysical properties and aerosol during the 1st phase of the Cloud Aerosol Interaction and Precipitation Enhancement EXperiment (CAIPEEX-I) over the Indian sub-continent provided initial opportunities to investigate the dispersion effect and its implications for estimating aerosol indirect effects in continental cumuli. In contrast to earlier studies on continental shallow cumuli, it is found that not only the cloud droplet number concentration but also the relative dispersion increases with the aerosol number concentration in continental cumuli. The first aerosol indirect effect estimated from the relative changes in droplet concentration and effective radius with aerosol number concentration are 0.13 and 0.07, respectively. In-depth analysis reveals that the dispersion effect could offset the cooling by enhanced droplet concentration by 39% in these continental cumuli. Adiabaticity analysis revealed aerosol indirect effect is lesser in subadiabatic clouds possibly due to inhomogeneous mixing processes. This study shows that adequate representation of the dispersion effect would help in accurately estimating the cloud albedo effect for continental cumuli and can reduce uncertainty in aerosol indirect effect estimates.

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[1] The effect of increased aerosol concentrations on the low-level, non-precipitating, ice-free stratus clouds is examined using a suite of surface-based remote sensing systems. Cloud droplet effective radius and liquid water path are retrieved using cloud radar and microwave radiometer. Collocated measurements of aerosol scattering coefficient, size distribution and cloud condensation nuclei (CCN) concentrations were used to examine the response of cloud droplet size and optical thickness to increased CCN proxies. During the episodic events of increase in aerosol accumulation-mode volume distribution, the decrease in droplet size and increase in cloud optical thickness is observed. The indirect effect estimates are made for both droplet effective radius and cloud optical thickness for different liquid water path ranges and they range 0.02 -0.18 and 0.005 -0.154, respectively. Data are also categorized into thin and thick clouds based on cloud geometric thickness (Dz) and estimates show IE values are relatively higher for thicker clouds.

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Abstract. Using the method of offline radiative transfer modeling within the partial radiative perturbation (PRP) approach, the effective radiative forcing by aerosol–cloud interactions (ERFaci) in the ECHAM–HAMMOZ aerosol climate model is decomposed into a radiative forcing by anthropogenic cloud droplet number change and adjustments of the liquid water path and cloud fraction. The simulated radiative forcing by anthropogenic cloud droplet number change and liquid water path adjustment are of approximately equal magnitude at −0.52 and −0.53 W m−2, respectively, while the cloud-fraction adjustment is somewhat weaker at −0.31 W m−2 (constituting 38 %, 39 %, and 23 % of the total ERFaci, respectively); geographically, all three ERFaci components in the simulation peak over China, the subtropical eastern ocean boundaries, the northern Atlantic and Pacific oceans, Europe, and eastern North America (in order of prominence). Spatial correlations indicate that the temporal-mean liquid water path adjustment is proportional to the temporal-mean radiative forcing, while the relationship between cloud-fraction adjustment and radiative forcing is less direct. While the estimate of warm-cloud ERFaci is relatively insensitive to the treatment of ice and mixed-phase cloud overlying warm cloud, there are indications that more restrictive treatments of ice in the column result in a low bias in the estimated magnitude of the liquid water path adjustment and a high bias in the estimated magnitude of the droplet number forcing. Since the present work is the first PRP decomposition of the aerosol effective radiative forcing into radiative forcing and rapid cloud adjustments, idealized experiments are conducted to provide evidence that the PRP results are accurate. The experiments show that using low-frequency (daily or monthly) time-averaged model output of the cloud property fields underestimates the ERF, but 3-hourly mean output is sufficiently frequent.