Giant Enhancement in Low Energy Photoemission of Ar Confined in<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn>60</mml:mn></mml:msub></mml:math>

Madjet, Mohamed; Chakraborty, Himadri; Manson, Steven T.

doi:10.1103/physrevlett.99.243003

Cited by 71 publications

(107 citation statements)

References 21 publications

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“…The jellium model is employed for computing the relative delay [35]. This model enjoyed earlier successes in codiscovering with experimentalists a high-energy plasmon resonance [36], interpreting the energy-dependent oscillations in C 60 valence photo-intensities [37], and predicting giant enhancements in the confined atom's photoresponse from the coupling with C 60 plasmons [19]. Significant ground state hybridization of Ar 3p is found to occur with the C 60 3p orbital, resulting in 3p[Ar+C 60 ] and 3p[Ar-C 60 ] from, respectively, the symmetric and antisymmetric wavefunction mixing.…”

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“…1 which envisions the process. There are two compelling reasons for this choice: (i) such materials are highly stable, have lowcost sustenance at room temperature and are enjoying a rapid improvement in their synthesis techniques [18] and (ii) effects of correlations of the central atom with the cage electrons have been predicted to spectacularly influence the atomic valence photoionization [19]. In this Letter, by considering Ar@C 60 , we show that a confinementinduced correlation effect of C 60 at energies surrounding the Ar 3p Cooper minimum produces a faster and a slower emission of the Ar 3p electrons hybridized, respectively, in a symmetric and an antisymmetric mode with a near-degenerate C 60 orbital.…”

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Time Delay in the Recoiling Valence Photoemission of Ar Endohedrally Confined inC60

2013

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The effects of confinement and electron correlations on the relative time delay between the 3s and 3p photoemissions of Ar confined endohedrally in C60 are investigated using the time dependent local density approximation -a method that is also found to mostly agree with recent time delay measurements between the 3s and 3p subshells in atomic Ar. At energies in the neighborhood of 3p Cooper minimum, correlations with C60 electrons are found to induce opposite temporal effects in the emission of Ar 3p hybridized symmetrically versus that of Ar 3p hybridized antisymmetrically with C60. A recoil-type interaction model mediated by the confinement is found to best describe the phenomenon.PACS numbers: 32.80. Fb,With the tremendous advancement in technology for generating attosecond (as) isolated pulses as well as attosecond pulse trains, it becomes possible to study fundamental phenomena of light-matter interaction with unprecedented precision on an as timescale [1][2][3]. In particular, the relative time delay between the photoelectrons from different subshells on as timescale, a subject of intense recent activities, is expected to probe important aspects of electron correlations that predominantly influence the photoelectron. Pump-probe experiments have been performed to measure the relative delay in the photoemission processes, where extreme ultra-violet (XUV) pulses are used to remove an electron from a particular subshell and subsequently a weak infrared (IR) pulse accesses the temporal information of the emission event [4].Streaking measurements were carried out to probe photoemission from the valence and the conduction band in single-crystalline magnesium [5] and tungsten [6]. A streaking technique was also employed to measure the relative delay of approximately 21±5 as between the 2s and 2p subshells of atomic Ne at 106 eV photon energy [7]. Despite several theoretical attempts [8][9][10][11][12][13][14] to explain this measured delay in Ne, only about a half of the delay could be reproduced, keeping the time delay in Ne photoemissions still an open problem. Recently, the relative delay between the 3s and 3p subshells in Ar is measured at three photon energies by interferometric technique using attosecond pulses [15,16]. Theoretical methods (e.g. time-dependent nonperturbative method [8], diagrammatic many-body perturbation theory [13], Random phase approximation with exchange (RPAE) [14,16], and multi-configurational Hartree-Fock (MCHF) [17]) have been employed to investigate this relative delay in Ar, although agreements between theory and experiment is rather inconclusive. A ubiquitous understanding in all these studies is the dominant influence of electron correlations to determine the time behavior of outgoing electrons. Thus, it is fair to expect that the process near a Cooper minimum or a resonance will be particularly nuanced.It is therefore of spontaneous interest to extend the study to test the effect of correlations on the temporal photoresponse of atoms in material confinements. A brilliant natura...

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Time Delay in the Recoiling Valence Photoemission of Ar Endohedrally Confined inC60

2013

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“…There are two compelling reasons for this: (i) such materials are highly stable, have low-cost sustenance at the room temperature and are enjoying a rapid improvement in synthesis techniques [23]; and (ii) the effect of correlation of the central atom with the cage electrons have been predicted to spectacularly affect the atomic photoionization [24]. A first attempt to predict ICD in endofullerenes was made by calculating ICD rates for Ne@C 60 [25].…”

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“…In solving the Kohn-Sham equations to obtain the ground state wave function, a few essential optimizations were adopted [31]. The model has enjoyed earlier success in co-discovering with experimentalists a high energy plasmon resonance [32], interpreting the energy-dependent oscillations in C 60 valence photo-intensity data [33], and predicting giant enhancements in the confined atom's photoresponse from the coupling with C 60 plasmons [24]. Significant ground state hybridization of Ar 3p is found to occur with the C 60 3p orbital, resulting in two levels, (Ar+C 60 )3p and (Ar-C 60 )3p, from respectively, the symmetric and antisymmetric modes of mixing, the spherical analogs of bonding and antibonding states in molecules or dimers:…”

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Resonant Auger–intersite-Coulombic hybridized decay in the photoionization of endohedral fullerenes

Javani

Wise

et al. 2014

Phys. Rev. A

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Considering the photoionization of Ar@C 60 , we predict resonant femtosecond decays of both Ar and C 60 vacancies through the continua of atom-fullerene hybrid final states. The resulting resonances emerge from the interference between simultaneous autoionizing and intercoulombic decay (ICD) processes. For Ar 3s → np excitations, these resonances are far stronger than the Ar-to-C 60 resonant ICDs, while for C 60 excitations they are strikingly larger than the corresponding Auger features. The results indicate the power of hybridization to enhance decay rates, and modify lifetimes and line profiles. [4] research has gone into studying ICD processes in weakly bound atomic systems. These involve the observation of ICD in rare gas dimers [5], rare gas clusters [6], surfaces [7], and small water droplets [8,9]. ICD followed by resonant Auger decay has been identified in Ar dimers using momentum resolved electron-ion-ion coincidence spectroscopy [10,11]. Ultrafast ICDs of a dicationic monomer in a cluster to produce a cluster tricataion [12] Of particular interest is the resonant ICD (RICD) where the precursor excitation to form an inner-shell vacancy is accomplished by promoting an inner electron to an excited state by an external stimulant, generally electromagnetic radiation [17,18] or, more recently, chargeparticle impact [21]. A theoretical study of RICD followed by Ne 2s → np excitations in MgNe clusters suggested the leading contribution of RICD among other interatomic decay modes [22]. Photoelectron spectroscopy with Ne clusters for 2s → np excitations measured the signature of RICD processes [17]. Similar excitations in the double photoionization of Ne dimers were utilized to observe RICD by tracking the formation of energetic Ne + fragments [18]. Most recently, strong enhancement of the HeNe + yield, as He resonantly couples with the radiation, is detected [19], confirming an earlier prediction [20].Atoms confined in fullerene shells forming endofullerene compounds are particularly attractive natural laboratories to study RICD processes. There are two compelling reasons for this: (i) such materials are highly stable, have low-cost sustenance at the room temperature and are enjoying a rapid improvement in synthesis techniques [23]; and (ii) the effect of correlation of the central atom with the cage electrons have been predicted to spectacularly affect the atomic photoionization [24]. A first attempt to predict ICD in endofullerenes was made by calculating ICD rates for Ne@C 60 [25]. While some speculation on the role of Coulomb interaction mediated energy transfer from atom to fullerene to broaden Auger lines has been made [26,27], no studies, theoretical or experimental, of RICD resonances in the ionization cross section of endofullerenes have been performed. Furthermore, ICD of endofullerene molecules can uncover effects not yet known. This is because: (i) endofullerenes being spherical analogues of asymmetric dimers consisting of an atom and a cluster can also induce reverse RICD processes, the decay of...

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“…The cited paper has stimulated theoretical activity in the field. The dynamical screening was considered by using quantum mechanical approach [62,63], as well as by applying the model semi-classical approach [64,65] which turned out to be as accurate as much more sophisticated TDLDA-based calculations [66,67].…”

Section: Clusters and Fullerenes In External Fieldsmentioning

confidence: 99%

Atomic cluster collisions

Korol

Solov’yov

2013

Eur. Phys. J. D

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Abstract. Atomic cluster collisions are a field of rapidly emerging research interest by both experimentalists and theorists. The international symposium on atomic cluster collisions (ISSAC) is the premier forum to present cutting-edge research in this field. It was established in 2003 and the most recent conference was held in Berlin, Germany in July of 2011. This Topical Issue presents original research results from some of the participants, who attended this conference. This issues specifically focuses on two research areas, namely Clusters and Fullerenes in External Fields and Nanoscale Insights in Radiation Biodamage.

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Giant Enhancement in Low Energy Photoemission of Ar Confined inC60

Cited by 71 publications

References 21 publications

Time Delay in the Recoiling Valence Photoemission of Ar Endohedrally Confined inC60

Time Delay in the Recoiling Valence Photoemission of Ar Endohedrally Confined inC60

Resonant Auger–intersite-Coulombic hybridized decay in the photoionization of endohedral fullerenes

Atomic cluster collisions

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