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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

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 TiO 2 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 TiO 2 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 TiO 2 occurring via the strong bonding between the conduction bands of QDs and TiO 2 is revealed. Such bridging states account for the fast adiabatic charge transfer from the QD donor to the TiO 2 acceptor, and may be a general feature for strongly coupled donor/acceptor systems. All the QDs/TiO 2 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 tomore » TiO 2 acceptors and explains the dependence of the increased charge transfer rate with the decreased QD size.« less
 [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:
Report Number(s):
IS-J 8567
Journal ID: ISSN 0934-0866
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Particle & Particle Systems Characterization
Additional Journal Information:
Journal Volume: 32; Journal Issue: 1; Journal ID: ISSN 0934-0866
Research Org:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org:
Country of Publication:
United States
14 SOLAR ENERGY; 25 ENERGY STORAGE; quantum dot-sensitized solar cells; CdSe and PbSe quantum dots; ab initio simulation; charge transfer; bridging state
OSTI Identifier: