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

Xin, Xukai; Li, Bo; Jung, Jaehan; Yoon, Young Jun; Biswas, Rana; Lin, Zhiqun

doi:10.1002/ppsc.201400111

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

Journal Article · Thu Jul 24 00:00:00 EDT 2014 · Particle & Particle Systems Characterization

DOI:https://doi.org/10.1002/ppsc.201400111· OSTI ID:1226915

Xin, Xukai ^[1]; Li, Bo ^[1]; Jung, Jaehan ^[1]; Yoon, Young Jun ^[1]; Biswas, Rana ^[2]; Lin, Zhiqun ^[1]

Georgia Inst. of Technology, Atlanta, GA (United States)
Iowa State Univ., Ames, IA (United States)

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.

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Research Organization:: Ames Lab., Ames, IA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1226915

Report Number(s):: IS-J 8567

Journal Information:: Particle & Particle Systems Characterization, Vol. 32, Issue 1; ISSN 0934-0866

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 29 works

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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