Abstract:The spontaneous and photo-induced neutralization of C₇⁻ produced in a laser ablation source was measured in an electrostatic storage ring. The measurements provide three independent determinations of the radiative cooling of the ions, based on the short time spontaneous decay and on the integrated amplitude and the shape of the photo-induced neutralization signal. The amplitude of the photo-induced signal was measured between 0.5 ms and 35 ms and found to depend on photon wavelength and ion storage time. All t… Show more
“…A prompt spike comprizes neutralization within ∼T /4 after illumination. Then, similar to earlier experiments [9,10], spikes delayed by τ = nT /2 (integer n) follow from anions performing n half-roundtrips before electron emission. The spikes of R(τ ) integrate delayed electron emission events that clusters undergo during τ ± T /4.…”
supporting
confidence: 83%
“…Recently, ion-trap experiments could access internal energy relaxation through studies of delayed electron emission from molecular and cluster anions. Timeresolved measurements indirectly demonstrated Stefan-Boltzmann-like relaxation [8] and sampled shifts of internal energy distributions for up to ∼100 ms [9,10]. Yet, basic uncertainties remain: Without direct scanning of the internal energy distribution (IED) in a cluster ensemble it is unclear how closely the IEDs follow a canonical shape.…”
A method is presented to monitor the internal energy distribution of cluster anions via delayed electron detachment by pulsed photoexcitation and demonstrated on Co_{4}^{-} in an electrostatic ion beam trap. In a cryogenic operation, we calibrate the detachment delay to internal energy. By laser frequency scans, at room temperature, we reconstruct the time-dependent internal energy distribution of the clusters. The mean energies of ensembles from a cold and a hot ion source both approach thermal equilibrium. Our data yield a radiative emission law and the absorptivity of the cluster for thermal radiation.
“…A prompt spike comprizes neutralization within ∼T /4 after illumination. Then, similar to earlier experiments [9,10], spikes delayed by τ = nT /2 (integer n) follow from anions performing n half-roundtrips before electron emission. The spikes of R(τ ) integrate delayed electron emission events that clusters undergo during τ ± T /4.…”
supporting
confidence: 83%
“…Recently, ion-trap experiments could access internal energy relaxation through studies of delayed electron emission from molecular and cluster anions. Timeresolved measurements indirectly demonstrated Stefan-Boltzmann-like relaxation [8] and sampled shifts of internal energy distributions for up to ∼100 ms [9,10]. Yet, basic uncertainties remain: Without direct scanning of the internal energy distribution (IED) in a cluster ensemble it is unclear how closely the IEDs follow a canonical shape.…”
A method is presented to monitor the internal energy distribution of cluster anions via delayed electron detachment by pulsed photoexcitation and demonstrated on Co_{4}^{-} in an electrostatic ion beam trap. In a cryogenic operation, we calibrate the detachment delay to internal energy. By laser frequency scans, at room temperature, we reconstruct the time-dependent internal energy distribution of the clusters. The mean energies of ensembles from a cold and a hot ion source both approach thermal equilibrium. Our data yield a radiative emission law and the absorptivity of the cluster for thermal radiation.
“…The precise time dependence is determined by the energy of the emitted photons relative to an energy scale determined by the (microcanonical) temperature, the heat capacity, and the evaporative activation energy [9,23]. For the energy of the photons expected to describe the behavior observed here, a single rate constant, k p , gives the suppression directly (the continuous cooling approximation requires photon energies below 220 meV for n = 15; see [23]). The decay rate relevant here is then…”
Section: Fig 3 the Metastable Fraction Vs Ln(t 2 /T 1 ) For Aumentioning
Small positively charged gold clusters have been found to emit thermal radiation at a very high rate, with time constants ranging from one to 35 μs for Au n + (n = 6-13,15). For sizes n = 14,16-20 the radiation occurs on much longer time scales. Strong thermal suppression of the population of higher-lying states puts constraints on the possible energies of excited states that can contribute to the radiation. Taking that into account, an evaluation of the experimentally determined rate constants shows that the strong radiation originates from thermally excited low-lying electronic states hitherto not observed. The origin of these states is discussed and two possibilities are suggested: one is related to electron correlation and electron pairing, and the other results from thermal shape fluctuations.
“…Conversely, if the population of the anions with a specific rate constant is determined, the energy distribution is obtained from the function of k d ðEÞ. On the basis of this assumption, we have measured the radiative cooling rates of C À 5 and C À 7 [4,5]. Relevant experiments were conducted using an electrostatic ion storage ring at Tokyo Metropolitan University (TMU E-ring).…”
Section: Experimental Procedures To Derive the Internal Energymentioning
confidence: 99%
“…The fast cooling originates in the presence of low-lying electronically excited states. It is considered to be a common feature of the small even-numbered carbon cluster anions, whereas the cooling of odd-numbered clusters (C À 5 and C À 7 ) is as slow as polyyne anions [4,5].…”
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