Dynamics of Charge Transfer and Multiple Exciton Generation in the Doped Silicon Quantum Dot–Carbon Nanotube System: Density Functional Theory-Based Computation
Abstract
In this study, 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 3Eg ≃ 1.5 eV and with QE reaching QE = 1.65 at about 5Eg, where Eg ≃ 0.5 eV is the lowest exciton energy, i.e., the gap. However, we find that including energy transfer andmore »
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1543671
- Grant/Contract Number:
- AC02-05CH11231; SC00001717
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry Letters
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 19; Journal ID: ISSN 1948-7185
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
Citation Formats
Kryjevski, Andrei, Mihaylov, Deyan, and Kilin, Dmitri. Dynamics of Charge Transfer and Multiple Exciton Generation in the Doped Silicon Quantum Dot–Carbon Nanotube System: Density Functional Theory-Based Computation. United States: N. p., 2018.
Web. doi:10.1021/acs.jpclett.8b02288.
Kryjevski, Andrei, Mihaylov, Deyan, & Kilin, Dmitri. Dynamics of Charge Transfer and Multiple Exciton Generation in the Doped Silicon Quantum Dot–Carbon Nanotube System: Density Functional Theory-Based Computation. United States. https://doi.org/10.1021/acs.jpclett.8b02288
Kryjevski, Andrei, Mihaylov, Deyan, and Kilin, Dmitri. Mon .
"Dynamics of Charge Transfer and Multiple Exciton Generation in the Doped Silicon Quantum Dot–Carbon Nanotube System: Density Functional Theory-Based Computation". United States. https://doi.org/10.1021/acs.jpclett.8b02288. https://www.osti.gov/servlets/purl/1543671.
@article{osti_1543671,
title = {Dynamics of Charge Transfer and Multiple Exciton Generation in the Doped Silicon Quantum Dot–Carbon Nanotube System: Density Functional Theory-Based Computation},
author = {Kryjevski, Andrei and Mihaylov, Deyan and Kilin, Dmitri},
abstractNote = {In this study, 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 3Eg ≃ 1.5 eV and with QE reaching QE = 1.65 at about 5Eg, 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.},
doi = {10.1021/acs.jpclett.8b02288},
journal = {Journal of Physical Chemistry Letters},
number = 19,
volume = 9,
place = {United States},
year = {Mon Sep 10 00:00:00 EDT 2018},
month = {Mon Sep 10 00:00:00 EDT 2018}
}
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