Radiative cooling of cationic carbon clusters, CN+, N = 8, 10, 13–16

Chen, F.-Q.; Kono, Naoko; Suzuki, Ryuta; Furukawa, T.; Tanuma, H.; Ferrari, Piero; Azuma, T.; Matsumoto, Jun; Shiromaru, H.; Zhaunerchyk, Vitali; Hansen, Klavs

doi:10.1039/c8cp06368k

Cited by 8 publications

(15 citation statements)

References 60 publications

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“…As k p is the rate constant for an activated process, it is in principle energy dependent and can therefore not rigorously be taken constant. A calculation of the leading order correction caused by the energy dependence of k p corrects fitted values of k p to the slightly different value k p (1 − hν/E a ), where hν is the energy of the photon emitting state and E a the activation energy of the observed, competing decay channel [68].…”

Section: Radiative Quenching Of Unimolecular Decaymentioning

confidence: 91%

“…An oscillatory pattern then appears with RF cooling for C − 4 [69,70], VC for C − 5 [94], RF cooling for C − 6 [70,[96][97][98], and VC for C − 7 [95]. Experiments on positively charged C + N clusters, in contrast, indicate RF cooling for all the non-fullerene sizes measured, N = 8, 10, 13 − 16 [68], with rate constants scattered around 10 4 s −1 . The consistently higher rates for these clusters may be caused by the higher internal energies per degree of freedom of these species compared with the anions.…”

Section: Decays Of Carbon-based Clustersmentioning

confidence: 91%

“…Carbon dissociation energies are significantly higher than electron affinities, and these two activation energies determine the internal energies, or the effective temperatures, of the clusters. Although the tendency for carbon cations to radiate electronically is therefore not surprising, the numerical values of the radiative constants of the carbon cations in [68] are not well understood theoretically at the time of writing.…”

Section: Decays Of Carbon-based Clustersmentioning

confidence: 99%

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Radiative cooling of size-selected gas phase clusters

Ferrari

Janssens

Lievens

et al. 2019

International Reviews in Physical Chemistry

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Predicted almost forty years ago, the radiation from thermally populated excited electronic states has recently been recognized as an important cooling mechanism in free molecules and clusters. It has presently been observed from both inorganic clusters and carbon-based molecules in molecular beams and ion storage devices. Experiments have demonstrated that many of these systems radiate at rates approaching microsecond time scales, and often with a distinct dependence on the precise number of atoms in the system. The radiation acts as a strongly stabilizing factor against both unimolecular decay and thermal electron emission. In astrophysical context, radiative cooling provides a mechanism to dissipate internal energy in star-forming processes, and stabilizes molecules selectively in the circumstellar medium. The consequences of an active radiative cooling channel for nanoparticle production will likewise favor special sizes in nonequilibrium formation processes. In this review, the radiative cooling of clusters is presented and illustrated with examples of experiments performed on small carbon, metal, and semiconductor clusters, and on PAH molecules. The experimental and theoretical techniques used are discussed, together with the consequences of radiative cooling on size-to-size stability patterns of clusters.

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Section: Radiative Quenching Of Unimolecular Decaymentioning

confidence: 91%

Section: Decays Of Carbon-based Clustersmentioning

confidence: 91%

Section: Decays Of Carbon-based Clustersmentioning

confidence: 99%

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Radiative cooling of size-selected gas phase clusters

Ferrari

Janssens

Lievens

et al. 2019

International Reviews in Physical Chemistry

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“…The experiments reported here measured the radiative quenching time for a number of cationic carbon clusters of medium size. They extend the measurements of the limited size range reported in [16] to a number of cluster sizes not previously produced in sufficient intensities to make the experiments feasible. For clusters C + 11 and C + 19 the measurements of spontaneous unimolecular decay quenching was supplemented by measurements of the decay rates induced by one-photon absorption at varying storage times, providing a test of the assumption of a statistical decay and broad initial cluster energy distributions.…”

Section: Introductionmentioning

confidence: 87%

“…[10,[12][13][14][15] for PAH molecules and other carbon-containing ions. Studies of radiative cooling of cationic carbon clusters were reported in [16]. Also the direct detection of photons emitted from size selected clusters in such processes has been accomplished recently, with the observation of thermal, visible photons emitted from C − 6 and C − 4 [17,18] and of naphthalene ions [19].…”

Section: Introductionmentioning

confidence: 99%

Thermal radiative cooling of carbon cluster cations C$_N^+$, $N = 9, 11,12, 17-27$

Iida,

Hu,

Zhang

et al. 2021

Preprint

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The thermal radiative cooling rates of C + N clusters (N = 9, 11, 12, 17 − 27) have been measured in the ultrahigh vacuum of an electrostatic storage ring. The rates are measured as a competing channel to unimolecular decay, and the rate constants, which are on the order of 10 4 s −1 , pertain to the excitation energies where these two channels compete. Such high values can only be explained as photon emission from thermally excited electronic states. The high rates have a very strong stabilizing effect on the clusters and the underlying mechanism gives a high energy conversion efficiency, with the potential to reach high quantum efficiencies in the emission process. The competing decay of unimolecular fragmentation defines upper limits for photon energies that can be down-converted to lower energy photons. Including previously measured cluster sizes provides the limits for all clusters C + N , N = 8 − 27, and gives values that varies from 10 to 14.5 eV, with a general increase with size. Clusters absorbing photons of energies below these limits cool down rapidly by emission of photons via electronic transitions and remain unfragmented.

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