Radiatively-driven processes in forest fire and desert dust plumes

The absorption of solar radiation by atmospheric aerosol particles is important for the climate effects of aerosols. Absorption by aerosol particles heats atmospheric layers, even though the net effect for the entire atmospheric column may still be a cooling. Most experimental studies on absorbing aerosols so far focussed mainly on the aerosol properties and did not consider the influence of the aerosols on the thermodynamic structure of the atmosphere. In this study, data from two international aircraft field experiments, the Intercontinental Transport of Ozone and Precursors study (ITOP) 2004 and the Saharan Mineral Dust Experiment (SAMUM) 2006 are investigated. The ITOP data were collected before the work on this thesis started, while the logistics and the instrument preparation of the SAMUM campaign, the weather forecast during SAMUM and the in-situ aerosol measurements during SAMUM were done within this thesis. The experimental data are used to explore the impact of layers containing absorbing forest fire and desert dust aerosol particles on the atmospheric stability and the implications of a changed stability on the development of the aerosol microphysical and optical properties during long-range transport. For the first time, vertical profiles of the Richardson number Ri are used to assess the stability and mixing in forest fire and desert dust plumes. Also for the first time, the conclusions drawn from the observations of forest fire and desert dust aerosol, at first glance apparently quite different aerosol types, are discussed from a common perspective. Two mechanisms, the self-stabilising and the sealed ageing effect, acting in both forest fire and desert dust aerosol layers, are proposed to explain the characteristic temperature structure as well as the aerosol properties observed in lofted forest fire and desert dust plumes. The proposed effects impact on the ageing of particles within the plumes and reduce the plume dilution, therefore extending the plume lifetime. This study combines experimental data, modelling of optical parameters and calculated heating rates to assess the role of forest fire and desert dust plumes. The microphysical, optical and chemical properties of forest fire and desert dust aerosol, and their vertical distribution, were measured with multiple instruments on the DLR Falcon 20-E5 research aircraft during ITOP and SAMUM. Aerosol size information and absorption data were analysed with respect to the aerosol mixing state, effective diameter and parameterisation of forest fire and dust size distributions. Altogether, about 90 size distributions for particles from different sources were extracted from multiple instruments and parameterised with multi-modal log-normal distributions. Subsequently, the optical properties were calculated for the different aerosol layers and compared with other independent measurements of the optical properties like the extinction coefficient determined with a High Spectral Resolution Lidar. The aerosol optical properties serve as the basis for the radiative transfer calculations with libRadtran (library for radiative transfer). Finally, the aerosol microphysical and optical properties, the meteorological data and the heating rates are examined to investigate the proposed self-stabilising and sealed ageing effects. The investigation of numerous forest fire and desert dust plumes in this study revealed characteristic aerosol properties: the aged (age: 4-13 days) forest fire aerosol is characterised by the absence of a nucleation mode, a depleted Aitken mode and an enhanced accumulation mode. In addition, more than 80% of the particles in the Aitken mode and nearly all particles in the accumulation mode of the forest fire plumes are internally mixed with a solid core. The desert dust aerosol exhibits two size regimes of different mixing states: below 0.5 µm, particles have a non-volatile core and a volatile coating; larger particles above 0.5 µm consist of non-volatile components and contain absorbing material. After regional-scale transport from the Sahara to South-western Europe, the volatile fraction in the dust plume did not significantly increase. The lofted forest fire plumes were found during ITOP at altitudes between 3 and 9 km above sea level (ASL), while the lofted desert dust plumes were found during SAMUM between 1 and 6 km ASL. The transition of the aerosol plumes to the free tropospheric background above and below the plumes was remarkably sharp and characterised by strong inversions. Within a height range of 200-300 m, the particle concentrations decreased by more than one order of magnitude. The results of plume dilution were evident only in the upper part of the lofted forest fire and desert dust plumes. The daily mean heating rates in the forest fire and desert dust plumes showed maximum values of ~0.2 K day-1 and ~0.24 K day-1, respectively. Vertical profiles of the heating rate suggest that the processes caused by the interaction between the aerosol particles and the solar radiation stabilise the plume itself and decelerate plume dilution. Apparently, the aerosol in such plumes ages in an almost “closed” system, where suppressed entrainment of condensable gases from the surface inhibits particle nucleation and the formation of coated particles inside the plume. The processes described tend to extend the lifetime of the layer allowing the transport over long distances.