Unimolecular Rate Constants and Cooling Mechanisms of Superhot<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mi mathvariant="normal">C</mml:mi></mml:mrow><mml:mrow><mml:mn>60</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math>Molecules

Kolodney, E.; Budrevich, A.; Tsipinyuk, B.

doi:10.1103/physrevlett.74.510

Cited by 74 publications

(54 citation statements)

References 14 publications

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“…Since neutral C 60 and C 70 molecules have larger HOMO-LUMO gaps than C 50 , the intensity of thermal radiation from these molecules should be very low in the temperature range of our measurements, at least an order of magnitude lower than observed for the anions. We therefore now believe that the apparent good agreement [8,11] between our results for C − 60 and the estimate in reference [4] of radiation from neutral C 60 molecules is fortuitous [26]. For the non-magic fullerenes with smaller HOMO-LUMO gaps, the single additional electron in the anions should be less important.…”

Section: Discussionmentioning

confidence: 66%

“…The key parameter in a statistical description is the energy barrier or activation energy for the decay. Most efforts have been devoted to studies of C 2 detachment, and there has been much controversy over the magnitude of the activation energy for this process [3][4][5]. Recently, it has been realised that radiative cooling of the hot fullerene molecules must be taken into account in the analysis of experiments, and attempts have been made to estimate the rate of this cooling from the experiments [4,[6][7][8][9].…”

Section: Introductionmentioning

confidence: 99%

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Radiative cooling of fullerene anions in a storage ring

Andersen

Gottrup

Hansen

et al. 2001

The European Physical Journal D

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Abstract. Thermionic emission from hot fullerene anions, C − N , has been measured in an electrostatic storage ring for even N values from 36 to 96. The decay is quenched by radiative cooling and hence the observations give information on the intensity of thermal radiation from fullerenes. The experiments are analysed by comparison with a simulation which includes the quantisation of photon energy and the statistics of emission. Experiments with heating of the molecules with a laser beam confirm the interpretation of the observations in terms of radiative cooling and give an independent estimate of the cooling rate for C − 60 . The measured cooling rates agree in general within a factor of two with the prediction from a classical dielectric model of a thermal radiation intensity of ∼ 300 eV/s for C60 at 1 400 K, scaling approximately with the 6th power of the temperature and with the number of atoms in the molecule. PACS

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Section: Discussionmentioning

confidence: 66%

Section: Introductionmentioning

confidence: 99%

Radiative cooling of fullerene anions in a storage ring

Andersen

Gottrup

Hansen

et al. 2001

The European Physical Journal D

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“…1. It consists of the Technion two stage effusive source for superhot C 60 [19][20][21][22][23][24] which is interfaced to the cluster molecular beam machine 18 at the research institute Rijnhuizen of the Stichting voor Fundamenteel Onderzoek der Materie ͑FOM͒. The beam of superhot C 60 can then be irradiated by the tunable IR radiation, emitted from FELIX.…”

Section: Methodsmentioning

confidence: 99%

“…[19][20][21][22][23][24] While the superhot thermal source method can not access the very high internal excitation range above 20 eV, it is presently the only method that can provide a controlled and well defined deposition of essentially pure vibrational thermal energy into C 60 molecules with a well defined canonical distribution. The combination of the thermally tunable superhot C 60 source with the ability of FELIX to resonantly heat thus provides a unique opportunity to study the behavior of an ensemble of extremely vibrationally excited C 60 molecules ͑Ē th = 50-100 eV͒ in a well controlled way.…”

Section: Introductionmentioning

confidence: 99%

Infrared multiphoton ionization of superhot C60: Experiment and model calculations

Bekkerman

Kolodney

Helden

et al. 2006

The Journal of Chemical Physics

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We address, both experimentally and theoretically, the issue of infrared ͑IR͒ resonance enhanced multiphoton ionization ͑IR-REMPI͒ and thermally induced redshifts of IR absorption lines in a very large and highly vibrationally excited molecular system. Isolated superhot C 60 molecules with well defined and variable average vibrational energy in the range of 9 -19 eV, effusing out of a constant flux thermal source, are excited and ionized after the absorption of multiple ͑500-800͒ infrared photons in the 450-1800 cm −1 spectral energy range. Recording the mass-selected ion signal as a function of IR wavelength gives well resolved IR-REMPI spectra, with zero off-resonance background signal. An enhancement of the ion signal of about a factor of 10 is observed when the temperature is increased from 1200 to 1800 K under otherwise identical conditions. A pronounced temperature dependent redshift of some of the IR absorption lines is observed. The observations are found to be in good agreement with a model which is based on the sequential absorption of single photons, always followed by instantaneous vibrational energy redistribution. The mass spectra ͑C 60 + fragmentation pattern͒ are found to be strongly excitation wavelength dependent. Extensive fragmentation down to C 32 + is observed following the absorption of 1350-1400 cm −1 as well as 1500-1530 cm −1 photons while negligible fragmentation is observed when exciting around 520 cm −1 .

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“…In highly excited C 60 energy release in the form of ionization (thermionic emission), fragmentation and radiative emission have been observed [3][4][5][6][7][8] . C 60 has also played an important role in the understanding of infrared (IR) multiple-photon excitation (IR-MPE) spectroscopy.…”

Section: Introductionmentioning

confidence: 99%