Two-Step Model for Ultrafast Interfacial Electron Transfer: Limitations of Fermi's Golden Rule Revealed by Quantum Dynamics Simulations

Abstract

Interfacial electron transfer (IET) is one of the crucial steps in the light-harvesting process that occurs in various assemblies for solar energy conversion, such as dye-sensitized solar cells or dye-sensitized photoelectrosynthesis cells. Computational studies of IET in dyesemiconductor assemblies employ a variety of approaches, ranging from phenomenological models such as Fermis golden rule to more complex methods relying on explicit solutions of the time-dependent Schrodinger equation. This work investigates IET in a model pyridineTiO2 assembly, with the goals of assessing the validity of Fermis golden rule for calculation of the IET rates, understanding the importance of conformational sampling in modeling the IET process, and establishing an approach to rapid computational screening of dyesensitizers that undergo fast IET into the semiconductor.

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Document Details

Document Type
Technical Report
Publication Date
Jun 27, 2017
Accession Number
AD1070436

Entities

People

  • Chang Liu
  • Elena Jakubikova

Organizations

  • North Carolina State University

Tags

Communities of Interest

  • Advanced Electronics
  • Materials and Manufacturing Processes

DTIC Thesaurus Topics

  • Carboxylic Acids
  • Cells
  • Charge Carriers
  • Chemistry
  • Conduction Bands
  • Dihedral Angle
  • Dye-Sensitized Solar Cells
  • Electron Density
  • Electron Transfer
  • Electrons
  • Energy Levels
  • Molecular Dynamics
  • Regression Analysis
  • Semiconductors
  • Simulations
  • Solar Cells
  • Solar Energy

Readers

  • Geospatial Intelligence and Artificial Intelligence Analytics
  • Nanocomposite Materials Science
  • Quantum spin resonance or Electron Paramagnetic Resonance spectroscopy.

Technology Areas

  • Microelectronics
  • Quantum Computing