2016
DOI: 10.1103/physrevlett.117.133004
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Detection of Recurrent Fluorescence Photons

Abstract: We have detected visible photons emitted from the thermally populated electronic excited state, namely recurrent fluorescence (RF), of C_{6}^{-} stored in an electrostatic ion storage ring. Clear evidence is provided to distinguish RF from normal fluorescence, based on the temporal profile of detected photons synchronized with the revolution of C_{6}^{-} in the ring, for which the time scale is far longer than the lifetime of the intact photoexcited state. The relaxation (cooling) process via RF is likely to b… Show more

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Cited by 46 publications
(38 citation statements)
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“…The latter process can occur on a much more rapid timescale ( 2 × 10 −5 s ; Chandrasekaran et al 2014) than the slow emission of mid-infrared vibrational photons ( 3s), but it requires a highly vibrationally excited ground state and the presence of a low-lying electronic state with excitation energy E 2.3 eV above ground and a high transition probability to the ground state. The detection of red photons resulting from recurrent fluorescence in C − 6 ions was recently reported by Ebara et al (2016), confirming experimentally the viability of this process. More recently, recurrent fluorescence photons from C − 4 have also been demonstrated experimentally (Yoshida et al 2017).…”
Section: Introductionsupporting
confidence: 68%
“…The latter process can occur on a much more rapid timescale ( 2 × 10 −5 s ; Chandrasekaran et al 2014) than the slow emission of mid-infrared vibrational photons ( 3s), but it requires a highly vibrationally excited ground state and the presence of a low-lying electronic state with excitation energy E 2.3 eV above ground and a high transition probability to the ground state. The detection of red photons resulting from recurrent fluorescence in C − 6 ions was recently reported by Ebara et al (2016), confirming experimentally the viability of this process. More recently, recurrent fluorescence photons from C − 4 have also been demonstrated experimentally (Yoshida et al 2017).…”
Section: Introductionsupporting
confidence: 68%
“…Inverse internal conversion turns an initially large reservoir of vibrational energy into electronic excitation in systems where low-lying electronic states exist. Only recently has it been possible to experimentally confirm RF by measuring the critical rate coefficients in C − 6 (Chandrasekaran et al 2014;Martin et al 2013) and by observing the resulting red photons (Ebara et al 2016). It is an intrinsic characteristic of RF that its expected photon conversion efficiencies increases with a growing energy difference between that of the exciting photon and the resultant fluorescence photons, a behaviour totally opposite to that seen in classical fluorescence or photoluminescence.…”
Section: The Ere Emission Process and Ere Carrier Modelsmentioning
confidence: 99%
“…Moreover, the energy difference between exciting and emitted photons for optimum photon conversion efficiency, the Stokes shift, is typically of order 1 eV or less. On the other hand, recurrent fluorescence (Leger et al 1988;Duley 2009) in highly isolated molecules or molecular ions relies on inverse internal conversion of vibrational energy into excitation energy of low-lying electronic states (Nitzan & Jortner 1979;Martin et al 2013;Chandrasekaran et al 2014;Ebara et al 2016). This process results in the possible emission of more than one photon, following excitation by the absorption of a single photon of sufficiently high energy.…”
Section: Introductionmentioning
confidence: 99%
“…This type of radiation was proposed a long time ago [32,33] but was only recently detected for several excited carbon species [19,25,34,35] and very recently also confirmed by direct detection of emitted photons for C 6[36].…”
Section: Fig 4 Fits Of the Radiative Cooling Time Constant With Eqmentioning
confidence: 99%