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• W2892092479 startingPage "5759" @default.
• W2892092479 abstract "We use the Boltzmann transport equation (BE) to study time evolution of a photoexcited state, including phonon-mediated exciton relaxation, multiple exciton generation (MEG), and energy-transfer processes. BE collision integrals are derived using Kadanoff-Baym-Keldysh many-body perturbation theory (MBPT) based on density functional theory (DFT) simulations, including exciton effects. We apply the method to a nanostructured p- n junction composed of a 1 nm hydrogen-terminated Si quantum dot (QD) doped with two phosphorus atoms (Si36P2H42) adjacent to the (6, 2) single-wall carbon nanotube (CNT) with two chlorine atoms per two unit cells adsorbed to the surface. We find that an initial excitation localized on either the QD or CNT evolves into a transient charge-transfer (CT) state where either electron or hole transfer has taken place. The CT state lifetime is about 40 fs. Also, we study MEG in this system by computing internal quantum efficiency (QE), which is the number of excitons generated from an absorbed photon during relaxation. We predict efficient MEG starting at 3 Eg ≃ 1.5 eV and with QE reaching QE = 1.65 at about 5 Eg, where Eg ≃ 0.5 eV is the lowest exciton energy, i.e., the gap. However, we find that including energy transfer and MEG effects suppresses CT state generation." @default.
• W2892092479 created "2018-09-27" @default.
• W2892092479 creator A5007977342 @default.
• W2892092479 creator A5014118913 @default.
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• W2892092479 date "2018-09-10" @default.
• W2892092479 modified "2023-09-25" @default.
• W2892092479 title "Dynamics of Charge Transfer and Multiple Exciton Generation in the Doped Silicon Quantum Dot–Carbon Nanotube System: Density Functional Theory-Based Computation" @default.
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• W2892092479 doi "https://doi.org/10.1021/acs.jpclett.8b02288" @default.
• W2892092479 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/30199263" @default.
• W2892092479 hasPublicationYear "2018" @default.
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