Dynamics of Charge Transfer and Multiple Exciton Generation in the Doped Silicon Quantum Dot–Carbon Nanotube System: Density Functional Theory-Based Computation

Kryjevski, Andrei; Mihaylov, Deyan; Kilin, Dmitri

doi:10.1021/acs.jpclett.8b02288

Title: Dynamics of Charge Transfer and Multiple Exciton Generation in the Doped Silicon Quantum Dot–Carbon Nanotube System: Density Functional Theory-Based Computation

Journal Article · Mon Sep 10 00:00:00 EDT 2018 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.8b02288· OSTI ID:1543671

^[1]; Mihaylov, Deyan ^[1];

^[1]

North Dakota State Univ., Fargo, ND (United States)

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 3E_g ≃ 1.5 eV and with QE reaching QE = 1.65 at about 5E_g, where E_g ≃ 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.

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Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-05CH11231; SC00001717

OSTI ID:: 1543671

Journal Information:: Journal of Physical Chemistry Letters, Vol. 9, Issue 19; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 6 works

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References (41)

Detailed Balance Limit of Efficiency of p‐n Junction Solar Cells Shockley, William; Queisser, Hans J. Journal of Applied Physics, Vol. 32, Issue 3, p. 510-519 https://doi.org/10.1063/1.1736034	journal	March 1961
Highly Efficient Multiple Exciton Generation in Colloidal PbSe and PbS Quantum Dots Ellingson, Randy J.; Beard, Matthew C.; Johnson, Justin C. Nano Letters, Vol. 5, Issue 5, p. 865-871 https://doi.org/10.1021/nl0502672	journal	May 2005
Quantum dot solar cells Nozik, A. J. Physica E: Low-dimensional Systems and Nanostructures, Vol. 14, Issue 1-2, p. 115-120 https://doi.org/10.1016/S1386-9477(02)00374-0	journal	April 2002
Carrier Multiplication in Quantum Dots within the Framework of Two Competing Energy Relaxation Mechanisms Stewart, John T.; Padilha, Lazaro A.; Bae, Wan Ki The Journal of Physical Chemistry Letters, Vol. 4, Issue 12 https://doi.org/10.1021/jz4004334	journal	June 2013
Thresholds of impact ionization in semiconductors Bude, J.; Hess, K. Journal of Applied Physics, Vol. 72, Issue 8 https://doi.org/10.1063/1.351434	journal	October 1992
Impact ionization model for full band Monte Carlo simulation in GaAs Jung, H. K.; Taniguchi, K.; Hamaguchi, C. Journal of Applied Physics, Vol. 79, Issue 5 https://doi.org/10.1063/1.361176	journal	March 1996
Characteristics of impact ionization rates in direct and indirect gap semiconductors Harrison, D.; Abram, R. A.; Brand, S. Journal of Applied Physics, Vol. 85, Issue 12 https://doi.org/10.1063/1.370658	journal	June 1999
S PECTROSCOPY AND H OT E LECTRON R ELAXATION D YNAMICS IN S EMICONDUCTOR Q UANTUM W ELLS AND Q UANTUM D OTS Nozik, Arthur J. Annual Review of Physical Chemistry, Vol. 52, Issue 1 https://doi.org/10.1146/annurev.physchem.52.1.193	journal	October 2001
Apparent Versus True Carrier Multiplication Yields in Semiconductor Nanocrystals McGuire, John A.; Sykora, Milan; Joo, Jin Nano Letters, Vol. 10, Issue 6 https://doi.org/10.1021/nl100177c	journal	June 2010
Impact Excitation and Electron–Hole Multiplication in Graphene and Carbon Nanotubes Gabor, Nathaniel M. Accounts of Chemical Research, Vol. 46, Issue 6 https://doi.org/10.1021/ar300189j	journal	January 2013
Peak External Photocurrent Quantum Efficiency Exceeding 100% via MEG in a Quantum Dot Solar Cell Semonin, O. E.; Luther, J. M.; Choi, S. Science, Vol. 334, Issue 6062 https://doi.org/10.1126/science.1209845	journal	December 2011
Multiple Exciton Generation in Single-Walled Carbon Nanotubes Wang, Shujing; Khafizov, Marat; Tu, Xiaomin Nano Letters, Vol. 10, Issue 7 https://doi.org/10.1021/nl100343j	journal	July 2010
Lead Telluride Quantum Dot Solar Cells Displaying External Quantum Efficiencies Exceeding 120% Böhm, Marcus L.; Jellicoe, Tom C.; Tabachnyk, Maxim Nano Letters, Vol. 15, Issue 12 https://doi.org/10.1021/acs.nanolett.5b03161	journal	November 2015
Multiple-exciton generation in lead selenide nanorod solar cells with external quantum efficiencies exceeding 120% Davis, Nathaniel J. L. K.; Böhm, Marcus L.; Tabachnyk, Maxim Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9259	journal	September 2015
Carrier multiplication in germanium nanocrystals Saeed, Saba; de Weerd, Chris; Stallinga, Peter Light: Science & Applications, Vol. 4, Issue 2 https://doi.org/10.1038/lsa.2015.24	journal	February 2015
Direct generation of multiple excitons in adjacent silicon nanocrystals revealed by induced absorption Trinh, M. Tuan; Limpens, Rens; de Boer, Wieteke D. A. M. Nature Photonics, Vol. 6, Issue 5 https://doi.org/10.1038/nphoton.2012.36	journal	March 2012
Efficient Carrier Multiplication in Colloidal Silicon Nanorods Stolle, Carl Jackson; Lu, Xiaotang; Yu, Yixuan Nano Letters, Vol. 17, Issue 9 https://doi.org/10.1021/acs.nanolett.7b02386	journal	August 2017
Extremely Efficient Multiple Electron-Hole Pair Generation in Carbon Nanotube Photodiodes Gabor, N. M.; Zhong, Z.; Bosnick, K. Science, Vol. 325, Issue 5946 https://doi.org/10.1126/science.1176112	journal	September 2009
Impact of SWCNT processing on nanotube-silicon heterojunctions Harris, John M.; Headrick, Robert J.; Semler, Matthew R. Nanoscale, Vol. 8, Issue 15 https://doi.org/10.1039/C5NR08703A	journal	January 2016
Advances in Carbon Nanotube-Silicon Heterojunction Solar Cells Tune, Daniel D.; Flavel, Benjamin S. Advanced Energy Materials, Vol. 8, Issue 15 https://doi.org/10.1002/aenm.201703241	journal	February 2018
Numerical Study of Carrier Multiplication Pathways in Photoexcited Nanocrystal and Bulk Forms of PbSe Velizhanin, Kirill A.; Piryatinski, Andrei Physical Review Letters, Vol. 106, Issue 20 https://doi.org/10.1103/PhysRevLett.106.207401	journal	May 2011
Light-Driven and Phonon-Assisted Dynamics in Organic and Semiconductor Nanostructures Kilina, Svetlana; Kilin, Dmitri; Tretiak, Sergei Chemical Reviews, Vol. 115, Issue 12 https://doi.org/10.1021/acs.chemrev.5b00012	journal	May 2015
Multiple exciton generation in chiral carbon nanotubes: Density functional theory based computation Kryjevski, Andrei; Mihaylov, Deyan; Kilina, Svetlana The Journal of Chemical Physics, Vol. 147, Issue 15 https://doi.org/10.1063/1.4997048	journal	October 2017
Correlated electron dynamics in quantum-dot sensitized solar cell: Kadanoff-Baym versus Markovian approach Kolesov, Grigory; Dahnovsky, Yuri Physical Review B, Vol. 85, Issue 24 https://doi.org/10.1103/PhysRevB.85.241309	journal	June 2012
Unified theory of quantized electrons, phonons, and photons out of equilibrium: A simplified ab initio approach based on the generalized Baym-Kadanoff ansatz de Melo, Pedro Miguel M. C.; Marini, Andrea Physical Review B, Vol. 93, Issue 15 https://doi.org/10.1103/PhysRevB.93.155102	journal	April 2016
Theoretical predictions on efficiency of bi-exciton formation and dissociation in chiral carbon nanotubes Kryjevski, Andrei; Gifford, Brendan; Kilina, Svetlana The Journal of Chemical Physics, Vol. 145, Issue 15 https://doi.org/10.1063/1.4963735	journal	October 2016
Photoinduced Single- and Multiple-Electron Dynamics Processes Enhanced by Quantum Confinement in Lead Halide Perovskite Quantum Dots Vogel, Dayton J.; Kryjevski, Andrei; Inerbaev, Talgat The Journal of Physical Chemistry Letters, Vol. 8, Issue 13 https://doi.org/10.1021/acs.jpclett.6b03048	journal	June 2017
Singlet fission in chiral carbon nanotubes: Density functional theory based computation Kryjevski, Andrei; Mihaylov, Deyan; Gifford, Brendan The Journal of Chemical Physics, Vol. 147, Issue 3 https://doi.org/10.1063/1.4992785	journal	July 2017
Enhanced multiple exciton generation in amorphous silicon nanowires and films Kryjevski, Andrei; Kilin, Dmitri Molecular Physics https://doi.org/10.1080/00268976.2015.1076580	journal	September 2015
Electron-hole excitations and optical spectra from first principles Rohlfing, Michael; Louie, Steven G. Physical Review B, Vol. 62, Issue 8 https://doi.org/10.1103/PhysRevB.62.4927	journal	August 2000
Theoretical Studies of Photoinduced Electron Transfer in Dye-Sensitized TiO ₂ Duncan, Walter R.; Prezhdo, Oleg V. Annual Review of Physical Chemistry, Vol. 58, Issue 1 https://doi.org/10.1146/annurev.physchem.58.052306.144054	journal	May 2007
Trajectory Surface Hopping in the Time-Dependent Kohn-Sham Approach for Electron-Nuclear Dynamics Craig, Colleen F.; Duncan, Walter R.; Prezhdo, Oleg V. Physical Review Letters, Vol. 95, Issue 16 https://doi.org/10.1103/PhysRevLett.95.163001	journal	October 2005
Importance of short-range versus long-range Hartree-Fock exchange for the performance of hybrid density functionals Vydrov, Oleg A.; Heyd, Jochen; Krukau, Aliaksandr V. The Journal of Chemical Physics, Vol. 125, Issue 7 https://doi.org/10.1063/1.2244560	journal	August 2006
Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)] Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias The Journal of Chemical Physics, Vol. 124, Issue 21 https://doi.org/10.1063/1.2204597	journal	June 2006
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)] Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 78, Issue 7 https://doi.org/10.1103/PhysRevLett.78.1396	journal	February 1997
Ab initio study of the photocurrent at the Au/Si metal–semiconductor nanointerface Han, Yulun; Micha, David A.; Kilin, Dmitri S. Molecular Physics, Vol. 113, Issue 3-4 https://doi.org/10.1080/00268976.2014.944598	journal	August 2014
Photoinduced Charge Transfer at Interfaces of Carbon Nanotube and Lead Selenide Nanowire Erck, Adam; Sapp, Wendi; Kilina, Svetlana The Journal of Physical Chemistry C, Vol. 120, Issue 40 https://doi.org/10.1021/acs.jpcc.6b05571	journal	September 2016
Dynamics of charge transfer at Au/Si metal-semiconductor nano-interface Han, Yulun; Tretiak, Sergei; Kilin, Dmitri Molecular Physics, Vol. 112, Issue 3-4 https://doi.org/10.1080/00268976.2013.842007	journal	October 2013

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