We study the dynamics of a two-electron system undergoing resonant excitation and inter-Coulombic decay (ICD) in a pair of quantum dots. The influence of the focus of the exciting laser on the ICD process is investigated for a -pulse with a close look on competing processes, i.e., direct ionization and multi-photon excitations. We scan through the field strength up to six Rabi cycles to show that ICD is still verifiable after several population inversions. With novel analyses, we determine for the first time populations of the different continuum states and thus conclude on the importance of several multi-photon excitation channels. Finally, we look into the influence of complex absorbing potentials on the dynamics.
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http://dx.doi.org/10.1063/1.5042208 | DOI Listing |
Molecules
December 2022
Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Hahn-Meitner-Platz 1, 14109 Berlin, Germany.
A detailed analysis of the electronic structure and decay dynamics in a symmetric system with three electrons in three linearly aligned binding sites representing quantum dots (QDs) is given. The two outer QDs are two-level potentials and can act as (virtual) photon emitters, whereas the central QD can be ionized from its one level into a continuum confined on the QD axis upon absorbing virtual photons in the inter-Coulombic decay (ICD) process. Two scenarios in such an ABA array are explored.
View Article and Find Full Text PDFJ Phys Condens Matter
February 2020
Facultad de Matemática, Astronomía y Física y Computación, Universidad Nacional de Córdoba and IFEG-CONICET, Ciudad Universitaria, X5000HUA Córdoba, Argentina.
The probability of the inter-Coulombic electron capture (ICEC) is studied for nanowire-embedded quantum-dot pairs where electron capture in one dot leads to electron emission from the other. Previous studies pointed to an interdependence of several ICEC pathways which can enhance the ICEC reaction probability. To identify favorable criteria for such synergies in a qualitative and quantitative manner, we conducted a considerable amount of simulations scanning multiple geometrical parameters.
View Article and Find Full Text PDFJ Chem Phys
June 2019
Department of Locally Sensitive and Time-Resolved Spectroscopy, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Hahn-Meitner-Platz 1, 14109 Berlin, Germany.
Ultrafast inter-Coulombic electron capture (ICEC) has been established as an important energy-transfer process in open paired-quantum-dot systems which can mediate between entrapment of free-moving electrons and release of trapped ones elsewhere by long-range electron-electron interaction within nanowires. Previous studies indicated ICEC enhancement through population and secondary decay of two-center resonance states, the latter known as inter-Coulombic decay (ICD). This study investigates the quantum-size effect of single- and double-electron states in an established model of a quasi-one-dimensional nanowire with two embedded confinement sites, represented by a pair of Gaussian wells.
View Article and Find Full Text PDFJ Chem Phys
October 2018
Institute of Methods for Material Development, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Str. 15, 12489 Berlin, Germany.
We study the dynamics of a two-electron system undergoing resonant excitation and inter-Coulombic decay (ICD) in a pair of quantum dots. The influence of the focus of the exciting laser on the ICD process is investigated for a -pulse with a close look on competing processes, i.e.
View Article and Find Full Text PDFPhys Rev Lett
November 2010
Department of Chemistry, University of California, Berkeley, California 94720, USA.
Inspired by recent photoelectron spectroscopy experiments on hydroxide solutions, we have examined the conditions necessary for enhanced (and, in the case of solutions, detectable) inter-Coulombic decay (ICD)--Auger emission from an atomic site other than that originally excited. We present general guidelines, based on energetic and spatial overlap of molecular orbitals, for this enhancement of inter-Coulombic decay-based energy transfer in solutions. These guidelines indicate that this decay process should be exhibited by broad classes of biomolecules and suggest a design criterion for targeted radiooncology protocols.
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