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Title: Ab Initio Simulation of Charge Transfer at the Semiconductor Quantum Dot/TiO 2 Interface in Quantum Dot-Sensitized Solar Cells

Abstract

Quantum dot-sensitized solar cells (QDSSCs) have emerged as a promising solar architecture for next-generation solar cells. The QDSSCs exhibit a remarkably fast electron transfer from the quantum dot (QD) donor to the TiO2 acceptor with size quantization properties of QDs that allows for the modulation of band energies to control photoresponse and photoconversion efficiency of solar cells. In order to understand the mechanisms that underpin this rapid charge transfer, the electronic properties of CdSe and PbSe QDs with different sizes on the TiO2 substrate are simulated using a rigorous ab initio density functional method. Our method capitalizes on localized orbital basis set, which is computationally less intensive. Quite intriguingly, a remarkable set of electron bridging states between QDs and TiO2 occurring via the strong bonding between the conduction bands of QDs and TiO2 is revealed. Such bridging states account for the fast adiabatic charge transfer from the QD donor to the TiO2 acceptor, and may be a general feature for strongly coupled donor/acceptor systems. All the QDs/TiO2 systems exhibit type II band alignments, with conduction band offsets that increase with the decrease in QD size. This facilitates the charge transfer from QDs donors to TiO2 acceptors and explains the dependencemore » of the increased charge transfer rate with the decreased QD size.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States)
  2. Iowa State Univ., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Lab., Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1226915
Report Number(s):
IS-J 8567
Journal ID: ISSN 0934-0866
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Particle & Particle Systems Characterization
Additional Journal Information:
Journal Volume: 32; Journal Issue: 1; Journal ID: ISSN 0934-0866
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 25 ENERGY STORAGE; quantum dot-sensitized solar cells; CdSe and PbSe quantum dots; ab initio simulation; charge transfer; bridging state

Citation Formats

Xin, Xukai, Li, Bo, Jung, Jaehan, Yoon, Young Jun, Biswas, Rana, and Lin, Zhiqun. Ab Initio Simulation of Charge Transfer at the Semiconductor Quantum Dot/TiO 2 Interface in Quantum Dot-Sensitized Solar Cells. United States: N. p., 2014. Web. doi:10.1002/ppsc.201400111.
Xin, Xukai, Li, Bo, Jung, Jaehan, Yoon, Young Jun, Biswas, Rana, & Lin, Zhiqun. Ab Initio Simulation of Charge Transfer at the Semiconductor Quantum Dot/TiO 2 Interface in Quantum Dot-Sensitized Solar Cells. United States. https://doi.org/10.1002/ppsc.201400111
Xin, Xukai, Li, Bo, Jung, Jaehan, Yoon, Young Jun, Biswas, Rana, and Lin, Zhiqun. 2014. "Ab Initio Simulation of Charge Transfer at the Semiconductor Quantum Dot/TiO 2 Interface in Quantum Dot-Sensitized Solar Cells". United States. https://doi.org/10.1002/ppsc.201400111. https://www.osti.gov/servlets/purl/1226915.
@article{osti_1226915,
title = {Ab Initio Simulation of Charge Transfer at the Semiconductor Quantum Dot/TiO 2 Interface in Quantum Dot-Sensitized Solar Cells},
author = {Xin, Xukai and Li, Bo and Jung, Jaehan and Yoon, Young Jun and Biswas, Rana and Lin, Zhiqun},
abstractNote = {Quantum dot-sensitized solar cells (QDSSCs) have emerged as a promising solar architecture for next-generation solar cells. The QDSSCs exhibit a remarkably fast electron transfer from the quantum dot (QD) donor to the TiO2 acceptor with size quantization properties of QDs that allows for the modulation of band energies to control photoresponse and photoconversion efficiency of solar cells. In order to understand the mechanisms that underpin this rapid charge transfer, the electronic properties of CdSe and PbSe QDs with different sizes on the TiO2 substrate are simulated using a rigorous ab initio density functional method. Our method capitalizes on localized orbital basis set, which is computationally less intensive. Quite intriguingly, a remarkable set of electron bridging states between QDs and TiO2 occurring via the strong bonding between the conduction bands of QDs and TiO2 is revealed. Such bridging states account for the fast adiabatic charge transfer from the QD donor to the TiO2 acceptor, and may be a general feature for strongly coupled donor/acceptor systems. All the QDs/TiO2 systems exhibit type II band alignments, with conduction band offsets that increase with the decrease in QD size. This facilitates the charge transfer from QDs donors to TiO2 acceptors and explains the dependence of the increased charge transfer rate with the decreased QD size.},
doi = {10.1002/ppsc.201400111},
url = {https://www.osti.gov/biblio/1226915}, journal = {Particle & Particle Systems Characterization},
issn = {0934-0866},
number = 1,
volume = 32,
place = {United States},
year = {Thu Jul 24 00:00:00 EDT 2014},
month = {Thu Jul 24 00:00:00 EDT 2014}
}

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Cited by: 29 works
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Works referencing / citing this record:

Rational Design of Metal Oxide-Based Cathodes for Efficient Dye-Sensitized Solar Cells
journal, July 2018


A review of one-dimensional TiO 2 nanostructured materials for environmental and energy applications
journal, January 2016


Quantum dot sensitized solar cells with efficiency over 12% based on tetraethyl orthosilicate additive in polysulfide electrolyte
journal, January 2017


Computational study of the absorption spectrum of defected ZnS nanoparticles
journal, April 2018