A Unified Framework on Molecular Mass Growth Processes to Polycyclic Aromatic Hydrocarbons - From Deep Space to Combustion Systems and Nanomaterials

For decades, polycyclic aromatic hydrocarbons (PAHs) – organic molecules containing fused benzene rings - have been invoked in fundamental molecular mass growth processes leading eventually to carbonaceous nanostructures in the interstellar medium (grains) and in combustion processes (soot). However, the elementary steps involved in low- and high-temperature growth mecha­nisms of these aromatics have remained essentially elusive until recently. Extracted from gas phase molecular beam studies on the molecular level combined with isomer-selective photo­ionization mass spectrometry and electronic structure calculations, this talk presents a novel mecha­nistical framework on key elementary reaction mechanisms synthesizing aromatic mo­lecules in extreme environments. These versatile findings are translated from the interstellar medium to combustion systems and to two- and three-dimensional carbonaceous nanostructures such as graphenes, chiral heli­cenes, nano bowls, and fullerenes. Facile low-temperature ro­utes to complex aromatics signify a fundamental shift in the perception that PAHs can be only formed at high-tem­perature combustion and circum­stellar conditions on electronic ground state surfaces with novel mechanisms compri­sing excited state dynamics, submerged barriers, and uncon­ven­tional concer­ted reactions between aromatic radicals. An outlook is also presented on the synthesis of PAHs in low temperature, hydrocarbon-dominated solids upon inter­ac­tion with (non)-ionizing radiation driven predominantly by non-adiabatic dy­namics to PAHs as complex as coro­nene. Po­ten­tial future works involving condensed phase ultrafast spectroscopies and the exploration of gro­wth processes on surfaces of carbonaceous particles levitated in ultrasonic fields and radio­fre­quen­cy multipole traps are highlighted to ultimately shed light on the aromatic universe we live in.