New approaches to quantifying aerosol influence on the cloud radiative effect.

The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol-cloud interactions at ever-increasing levels of detail, but these models lack the resolution to represent clouds and aerosol-cloud interactions adequately. There is a dearth of observational constraints on aerosol-cloud interactions. We develop a conceptual approach to systematically constrain the aerosol-cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surface-based shortwave radiation measurements. We heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol-cloud radiation system.

Detection of iodine monoxide in the tropical free troposphere.

Atmospheric iodine monoxide (IO) is a radical that catalytically destroys heat trapping ozone and reacts further to form aerosols. Here, we report the detection of IO in the tropical free troposphere (FT). We present vertical profiles from airborne measurements over the Pacific Ocean that show significant IO up to 9.5 km altitude and locate, on average, two-thirds of the total column above the marine boundary layer. IO was observed in both recent deep convective outflow and aged free tropospheric air, suggesting a widespread abundance in the FT over tropical oceans. Our vertical profile measurements imply that most of the IO signal detected by satellites over tropical oceans could originate in the FT, which has implications for our understanding of iodine sources. Surprisingly, the IO concentration remains elevated in a transition layer that is decoupled from the ocean surface. This elevated concentration aloft is difficult to reconcile with our current understanding of iodine lifetimes and may indicate heterogeneous recycling of iodine from aerosols back to the gas phase. Chemical model simulations reveal that the iodine-induced ozone loss occurs mostly above the marine boundary layer (34%), in the transition layer (40%) and FT (26%) and accounts for up to 20% of the overall tropospheric ozone loss rate in the upper FT. Our results suggest that the halogen-driven ozone loss in the FT is currently underestimated. More research is needed to quantify the widespread impact that iodine species of marine origin have on free tropospheric composition, chemistry, and climate.

Physical science research needed to evaluate the viability and risks of marine cloud brightening.

Marine cloud brightening (MCB) is the deliberate injection of aerosol particles into shallow marine clouds to increase their reflection of solar radiation and reduce the amount of energy absorbed by the climate system. From the physical science perspective, the consensus of a broad international group of scientists is that the viability of MCB will ultimately depend on whether observations and models can robustly assess the scale-up of local-to-global brightening in today's climate and identify strategies that will ensure an equitable geographical distribution of the benefits and risks associated with projected regional changes in temperature and precipitation. To address the physical science knowledge gaps required to assess the societal implications of MCB, we propose a substantial and targeted program of research-field and laboratory experiments, monitoring, and numerical modeling across a range of scales.

The spectral signature of cloud spatial structure in shortwave irradiance.

In this paper, we used cloud imagery from a NASA field experiment in conjunction with three-dimensional radiative transfer calculations to show that cloud spatial structure manifests itself as a spectral signature in shortwave irradiance fields - specifically in transmittance and net horizontal photon transport in the visible and near-ultraviolet wavelength range. We found a robust correlation between the magnitude of net horizontal photon transport (H) and its spectral dependence (slope), which is scale-invariant and holds for the entire pixel population of a domain. This was surprising at first given the large degree of spatial inhomogeneity. We prove that the underlying physical mechanism for this phenomenon is molecular scattering in conjunction with cloud spatial structure. On this basis, we developed a simple parameterization through a single parameter ε, which quantifies the characteristic spectral signature of spatial inhomogeneities. In the case we studied, neglecting net horizontal photon transport leads to a local transmittance bias of ±12-19 %, even at the relatively coarse spatial resolution of 20 km. Since three-dimensional effects depend on the spatial context of a given pixel in a nontrivial way, the spectral dimension of this problem may emerge as the starting point for future bias corrections.