Abstract

ABSTRACT In spite of the considerable advances made by Cassini–Huygens in our understanding of Titan, many questions endure. In particular, the detailed processes that lead to the formation of haze aerosols in Titan’s atmosphere, found in high concentrations at low altitudes, are not well identified. Hydrocarbons, which are abundant constituents of Titan’s cold atmosphere originating from photochemical processes, may simultaneously condense on the surface of existing aerosols, nucleate and grow to generate new aerosol seeds. The relative importance of the various processes depends on several factors, including the saturation ratio. The dynamics of hydrocarbon condensation and nucleation in Titan’s atmosphere remains poorly known. Aiming to progress on these issues, we investigate here the kinetics of propane dimer formation at low temperature through state-of-the-art laboratory experiments combined with theoretical calculations. Our results provide an estimate of the rate coefficients, which are then employed to evaluate the abundance of propane dimers in the lower atmosphere of Titan. The mixing ratios of propane dimers inferred, with a maximum abundance of 10 cm−3 near 100 km, is found to be under the detection limit of the Composite Infrared Spectrometer of the Cassini spacecraft. Based on our results, homogeneous nucleation of the most abundant species appears not to be relevant for the growth of aerosols. Future studies should focus on homogeneous nucleation of polar molecules or alternatively on heterogeneous processes, which are usually more efficient.

Highlights

  • A large variety of van der Waals complexes, in which molecules are bound by intermolecular dispersion forces, is expected in planetary atmospheres

  • We provide below some elements on the the energetics and the dynamics of the processes involved

  • Rigid-rotor harmonic-oscillator (RRHO) approximations were used in the evaluation of the state density, but with one torsional mode treated as a free rotor

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Summary

INTRODUCTION

A large variety of van der Waals complexes, in which molecules are bound by intermolecular dispersion forces, is expected in planetary atmospheres. They notably allow the critical cluster size range for nucleation to be determined They require molecular-level simulations for more detailed and quantitative information to be extracted on the growth mechanisms, and do not provide any quantitative information on the rate coefficients of formation of dimers or larger clusters. As temperature decreases rapidly in Titan’s lower atmosphere, most of the formed photochemical products condense below ∼150 km, suggesting that larger clusters should readily form This homogeneous nucleation mechanism would have to compete with the typically faster heterogeneous nucleation on the surface of the haze particles (Lavvas et al 2011), and it is important to evaluate if cluster formation can provide a significant additional component to the haze population.

EXPERIMENTAL METHODS
IONIZATION AND DETECTION OF PROPANE CLUSTERS
Dynamical aspects and fragmentation pattern
Energy deposition in the dimer following ionization
Dissociation lifetime of the cationic dimer
Fragmentation pathways of the cationic dimer
DIMER FORMATION RATE COEFFICIENT
THEORETICAL EVALUATION OF ASSOCIATION AND DISSOCIATION RATES
PROPANE DIMER FORMATION IN TITAN’S LOWER ATMOSPHERE
Findings
CONCLUDING REMARKS
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