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تسجيل مستخدم جديدLaboratory formation and photo-chemistry of fullerene/anthracene cluster cations
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Besides buckminsterfullerene (C60), other fullerenes and their derivatives may also reside in space. In this work, we study the formation and photo-dissociation processes of astronomically relevant fullerene/anthracene (C14H10) cluster cations in the gas phase. Experiments are carried out using a quadrupole ion trap (QIT) in combination with time-of-flight (TOF) mass spectrometry. The results show that fullerene (C60, and C70)/anthracene (i.e., [(C14H10)nC60]+ and [(C14H10)nC70]+), fullerene (C56 and C58)/anthracene (i.e., [(C14H10)nC56]+ and [(C14H10)nC58]+) and fullerene (C66 and C68)/anthracene (i.e., [(C14H10)nC66]+ and [(C14H10)nC68]+) cluster cations, are formed in the gas phase through an ion-molecule reaction pathway. With irradiation, all the fullerene/anthracene cluster cations dissociate into mono$-$anthracene and fullerene species without dehydrogenation. The structure of newly formed fullerene/anthracene cluster cations and the bonding energy for these reaction pathways are investigated with quantum chemistry calculations. Our results provide a growth route towards large fullerene derivatives in a bottom-up process and insight in their photo-evolution behavior in the ISM, and clearly, when conditions are favorable, fullerene/PAH clusters can form efficiently. In addition, these clusters (from 80 to 154 atoms or ~ 2 nm in size) offer a good model for understanding the physical-chemical processes involved in the formation and evolution of carbon dust grains in space, and provide candidates of interest for the DIBs that could motivate spectroscopic studies.
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The formation and evolution mechanism of fullerenes in the planetary nebula or in the interstellar medium are still not understood. Here we present the study on the cluster formation and the relative reactivity of fullerene cations (from smaller to l
arger, C$_{44}$ to C$_{70}$) with anthracene molecule (C$_{14}$H$_{10}$). The experiment is performed in the apparatus that combines a quadrupole ion trap with a time-of-flight mass spectrometer. By using a 355 nm laser beam to irradiate the trapped fullerenes cations (C$_{60}$$^+$ or C$_{70}$$^+$), smaller fullerene cations C$_{(60-2n)}$$^+$, n=1-8 or C$_{(70-2m)}$$^+$, m=1-11 are generated, respectively. Then reacting with anthracene molecules, series of fullerene/anthracene cluster cations are newly formed (e.g., (C$_{14}$H$_{10}$)C$_{(60-2n)}$$^+$, n=1-8 and (C$_{14}$H$_{10}$)C$_{(70-2m)}$$^+$, m=1-11), and slight difference of the reactivity within the smaller fullerene cations are observed. Nevertheless, smaller fullerenes show obviously higher reactivity when comparing to fullerene C$_{60}$$^+$ and C$_{70}$$^+$. A successive loss of C$_2$ fragments mechanism is suggested to account for the formation of smaller fullerene cations, which then undergo addition reaction with anthracene molecules to form the fullerene-anthracene cluster cations. It is found that the higher laser energy and longer irradiation time are key factors that affect the formation of smaller fullerene cations. This may indicate that in the strong radiation field environment (such as photon-dominated regions) in space, fullerenes are expected to follow the top-down evolution route, and then form small grain dust (e.g., clusters) through collision reaction with co-existing molecules, here, smaller PAHs.
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