Approximation scheme for the three-particle propagator

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We analyze in detail the accessible relaxation pathways via electron emission of the Ne 2+ Ar states populated via the K-LL Auger decay of Ne + ͑1s −1 ͒Ar. In particular, we concentrate on the "direct" interatomic Coulombic decay ͑ICD͒ of the Ne 2+ ͑2s −1 2p −1 ͒Ar weakly bound doubly ionized states into the manifold of the Ne 2+ ͑2p −2 ͒ -Ar + ͑3p −1 ͒ repulsive triply ionized ones. To carry out the present study the potential energy curves of the NeAr ground state, the core ionized state Ne + ͑1s −1 ͒Ar, the relevant dicationic and tricationic states, and the corresponding ICD transition rates have been computed using accurate ab initio methods and basis sets. The total and partial ICD electron spectra are computed within the framework of the time-dependent theory of wave packet propagation. Thereby, the impact of nuclear dynamics accompanying the electronic decay on the computed ICD-electron spectra is investigated in detail.

Section: A Potential Energy Curvesmentioning

confidence: 99%

Interatomic Coulombic decay and its dynamics in NeAr following K-LL Auger transition in the Ne atom

Demekhin

Chiang

Stoychev

et al. 2009

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“…The three-particle Green's function in its general form is given by a time-ordered expectation value of three creation and three annihilation operators, 18 G ␣␤,␥␦ ϭϪi 3 ͗⌿ 0 N ͉T͓a ␣ ͑t ␣ ͒a ␤ ͑t ␤ ͒a ͑t ͒a ␥ † ͑t ␥ ͒…”

Section: A Three-particle Propagatormentioning

confidence: 99%

“…In this work we report on the use of the second-order algebraic diagrammatic construction ͑ADC͒ [15][16][17][18] approximation of this quantity for the study of the triple ionization of molecules. In Sec.…”

Section: Introductionmentioning

confidence: 99%

“…This includes the implementation of the second-order working equations given in Ref. 18 and the development of the atomic three-hole population analysis, which allows the investigation of space localization of electron vacancies and of the charge distribution in the dense manifold of trication states. Section III contains exemplary applications which demonstrate that the presented method is very suitable for the theoretical study of triply ionized molecular systems and is helpful in the interpretation of experimental findings.…”

Section: Introductionmentioning

confidence: 99%

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Theoretical investigations of molecular triple ionization spectra

Handke

Tarantelli

Sgamellotti

et al. 1996

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Articles you may be interested inPotential energy surface for and pure rotational spectra of isotopomeric Cl2-Ar van der Waals complexes Triple ionization of molecular systems is investigated theoretically by means of the three-particle propagator. This enables us to efficiently calculate the very dense triple ionization spectra. To be able to interpret these spectra an atomic three-hole population analysis is developed which provides information about the charge distribution in the molecular trication. In exemplary applications on CO and a series of fluorides the use of the approach is demonstrated. A large number of triply ionized electronic states are energetically accessible in the available particle impact ionization experiments and it is shown that many of these states contribute to the observations. Triply ionized states are also produced by Auger decay. In particular, shake-off satellite lines of molecular Auger spectra can be reproduced using the triple ionization energies from the propagator calculation and an estimate of the transition rates based on the three-hole population analysis. In general a dramatically growing complexity of the triple ionization spectra with increasing molecular size is demonstrated. In spite of this complexity the three-hole population analysis is of valuable help for the interpretation of the spectra and often a simple picture in terms of various hole-localization patterns arises.

“…The ab initio many-body Green's function ADC methods have been first introduced for calculation of excitation and ionization energies of closed shell species 1, 2 and since then generalized for the description of double 3 and triple 4 ionization energies. The ADC(n) schemes of various orders (n) are size consistent and compact relative to the corresponding truncated CI expansions.…”

Section: Introductionmentioning

confidence: 99%

B-spline algebraic diagrammatic construction: Application to photoionization cross-sections and high-order harmonic generation

Ruberti

Averbukh

Decleva

2014

High-order optical harmonic generation as a process of single atom interaction with sub-relativistic single-and multicolor laser fields AIP Conf. Proc. 1464, 265 (2012) We present the first implementation of the ab initio many-body Green's function method, algebraic diagrammatic construction (ADC), in the B-spline single-electron basis. B-spline versions of the first order [ADC(1)] and second order [ADC (2)] schemes for the polarization propagator are developed and applied to the ab initio calculation of static (photoionization cross-sections) and dynamic (highorder harmonic generation spectra) quantities. We show that the cross-section features that pose a challenge for the Gaussian basis calculations, such as Cooper minima and high-energy tails, are found to be reproduced by the B-spline ADC in a very good agreement with the experiment. We also present the first dynamic B-spline ADC results, showing that the effect of the Cooper minimum on the high-order harmonic generation spectrum of Ar is correctly predicted by the time-dependent ADC calculation in the B-spline basis. The present development paves the way for the application of the B-spline ADC to both energy-and time-resolved theoretical studies of many-electron phenomena in atoms, molecules, and clusters.