Ultraslow isomerization in photoexcited gas-phase carbon cluster $${{\rm C}}_{10}^ -$$

Saha, Koushik; Chandrasekaran, Vijayanand; Heber, O.; Iron, Mark A.; Rappaport, Michael; Zajfman, D.

doi:10.1038/s41467-018-03197-w

Cited by 10 publications

(5 citation statements)

References 68 publications

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“…In addition to radiative spontaneous emission and C 2 thermodissociation, other processes can occur, such as delayed thermoionization and isomerization. Isomerization has been recently experimentally evidenced on the small C − 10 cluster ion (Saha et al 2018) and should be relevant at temperatures higher than 4000 K (Kim & Tománek 1994;Bonnin et al 2019).…”

Section: Dissociation and Radiative Emission Processesmentioning

confidence: 96%

Laboratory investigation of shock-induced dissociation of buckminsterfullerene and astrophysical insights

Chakraborty,

Yurchenko,

Georges

et al. 2024

A&A

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Fullerene C60 is one of the most iconic forms of carbon found in the interstellar medium (ISM). The interstellar chemistry of carbon-rich components, including fullerenes, is driven by a variety of energetic processes including UV and X-ray irradiation, cosmic-ray (CR) bombardment, electron impact, and shock waves. These violent events strongly alter the particle phase and lead to the release of new molecular species in the gas phase. Only a few experimental studies on the shock processing of cosmic analogs have been conducted so far. We explored in the laboratory the destruction of buckminsterfullerene C60 using a pressure-driven shock tube coupled with optical diagnostics. Our efforts were first devoted to probing in situ the shock-induced processing of C60 at high temperatures (≤ 4500 K) by optical emission spectroscopy. The analysis of the spectra points to the massive production of C2 units. A broad underlying continuum was observed as well and was attributed to the collective visible emission of carbon clusters, generated similarly in large amounts. This proposed assignment was performed with the help of calculated emission spectra of various carbon clusters. The competition between dissociation and radiative relaxation, determined by statistical analysis, alludes to a predominance of clusters with less than 40 carbon atoms. Our laboratory experiments, supported by molecular dynamics simulations performed in the canonical ensemble, suggest that C60 is very stable, and that high-energy input is required to process it under interstellar low-density conditions and to produce C2 units and an abundance of intermediate-sized carbon clusters. These results provide some insights into the life cycle of carbon in space. Our findings hint that only J-type shocks with velocities above ~100 km s−1 or C-type shocks with velocities above 9 km s−1 can lead to the destruction of fullerenes. Observational tracers of this process remain elusive, however. Our work confirms the potential of shock tubes for laboratory astrophysics.

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Section: Dissociation and Radiative Emission Processesmentioning

confidence: 96%

Laboratory investigation of shock-induced dissociation of buckminsterfullerene and astrophysical insights

Chakraborty,

Yurchenko,

Georges

et al. 2024

A&A

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“…Another relaxation mode is that of isomerization, which could be recently experimentally evidenced on the small C − 10 cluster ion. 85 Accounting for isomerization processes on the same footing as electronic or vibrational relaxation for each individual isomer is in principle possible but would require, at least, the independent identification of transition states between connected isomers together with the evaluation of isomerization rate constants, e.g. from harmonic transition state theory.…”

Section: B Approximate Analytical Expressions For the Rate Constantsmentioning

confidence: 99%

Radiative relaxation in isolated large carbon clusters: Vibrational emission versus recurrent fluorescence

Lacinbala

Calvo

Dubosq

et al. 2022

The Journal of Chemical Physics

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Recurrent fluorescence (RF) from isolated carbon clusters containing between 24 and 60 atoms is theoretically investigated as a function of internal energy, cluster size, and structural features. The vibrational relaxation kinetics and the associated IR emission spectra are determined by means of a Monte Carlo approach with vibrational density of states computed in the harmonic approximation. RF is generally found to be highly competitive with vibrational emission. The behaviors predicted for clusters of various sizes and archetypal structures indicate that the IR emission spectra are strongly influenced by RF, an energy gap law being obtained for the evolution of the RF rate constant depending on the electronic excitation state. The present results are relevant to the photophysics of the interstellar medium and could contribute to elucidating the carriers of the extended red emission bands and the continuum emission lying below the aromatic infrared bands believed to originate from mixed aromatic–aliphatic compounds.

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“…Statistical dissociation has been used as a tool for studying statistical properties of ions, for example, for radiative cooling measurements [218], for calorimetry [219]. In a recent work, it was shown that one can describe simultaneously the isomerization, the delayed electron emission and internal cooling for C − 10 molecules [220]. Even though statistical dissociation has been known for over 30 years, the proper methodology for modeling it is still an ongoing research topic and currently depends on the simultaneous deduction of many molecular parameters such as the ions activation energy, IED, polarizability, etc.…”

Section: Challenges and New Directionsmentioning

confidence: 99%

Roadmap on dynamics of molecules and clusters in the gas phase

et al. 2021

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This roadmap article highlights recent advances, challenges and future prospects in studies of the dynamics of molecules and clusters in the gas phase. It comprises nineteen contributions by scientists with leading expertise in complementary experimental and theoretical techniques to probe the dynamics on timescales spanning twenty order of magnitudes, from attoseconds to minutes and beyond, and for systems ranging in complexity from the smallest (diatomic) molecules to clusters and nanoparticles. Combining some of these techniques opens up new avenues to unravel hitherto unexplored reaction pathways and mechanisms, and to establish their significance in, e.g. radiotherapy and radiation damage on the nanoscale, astrophysics, astrochemistry and atmospheric science. Graphic abstract

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Ultraslow isomerization in photoexcited gas-phase carbon cluster $${{\rm C}}_{10}^ -$$

Cited by 10 publications

References 68 publications

Laboratory investigation of shock-induced dissociation of buckminsterfullerene and astrophysical insights

Laboratory investigation of shock-induced dissociation of buckminsterfullerene and astrophysical insights

Radiative relaxation in isolated large carbon clusters: Vibrational emission versus recurrent fluorescence

Roadmap on dynamics of molecules and clusters in the gas phase

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