Solar Energy Conversion: Dynamics of Interfacial Electron and Excitation Transfer (RSC Energy and Environment, 8) - Hardcover

Hardcover

ISBN 10: 1849733872 ISBN 13: 9781849733878

Verlag: Royal Society of Chemistry, 2013

Inhaltsangabe

The importance of developing new, clean and renewable sources of energy will continue to grow in the foreseeable future and so will the need for the education of researchers in this field of research. The interest and challenges of the field continue to shift from simple homogeneous solutions to increasingly more complex heterogeneous systems and interfaces. Over the past decade there have been numerous theoretical and experimental breakthroughs many of which still exist only in the primary literature. The aim of this book is to gather in one volume the description of modern, sometimes exploratory, experimental and theoretical techniques applied to the dynamics of interfacial electron and electronic excitation transfer processes studied in the context of solar energy conversion. The intended treatment will be fundamental in nature and thus applicable to a broad range of hybrid photovoltaic and photocatalytic materials and interfaces. The book will focus on the dynamic aspects of the electron injection, exciton and carrier relaxation processes, as well as coherence effects, which continue to provide the impetus and the greatest challenge for the development of new methodologies.

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Über die Autorin bzw. den Autor

Piotr Piotrowiak is Professor of Physical Chemistry at Rutgers University-Newark. He graduated with a Magisterium in Chemical Physics from the University of Wroc¦aw, Poland, in 1982 and a Ph.D in Physical Chemistry from the University of Chicago in 1988. He held a Postdoctoral Associate position at Argonne National Laboratory in the Electron Transfer and Energy Conversion Group between 1988 to 1991 and was an Assistant Professor at the Univeristy of New Orleans from 1991 to 1996. He then went on to hold An Associate position in 1996. He has been a visiting fellow at Tokyo Metropolitan University and visiting scientist in the protein engineering department at Genentech Inc., in San Francisco. He has been an active member of many scientific committees and international conferences including the International Symposium of the U.S. Civilian Research and Development Foundation for the Independent States of the FSU, Kiev, Ukraine, in October 2003; the International Organizing Committee for the XX IUPAC Symposium on Photochemistry, Granada, Spain, July 2004; Session Chair, Physical Chemistry of Interfaces and Nanomaterials, International SPIE Optics and Photonics Symposium, San Diego, California, July 2006; Symposium co-Chair, Physical Chemistry of Interfaces and Nanomaterials, International SPIE Optics and Photonics Symposium, San Diego, California, August 2007; Session Chair, Gordon Conference on Electronic Structure and Dynamics, Waterville, Maine, July 2009; Member of the NSF-MRI ARRA review panel for undergraduate institutions, Arlington, Virginia, November 2009; Invited speaker at the Special Symposium on the 50th Anniversary of the Laser, 239th ACS National Meeting, San Francisco, California, March 2010. His main research interests are the development of ultrafast microscopy methods applied to electron and excitation transfer at interfaces and in inhomogeneous systems, time-resolved laser spectroscopy of reactive intermediates, interactions between host-guest systems and redox proteins.

Von der hinteren Coverseite

The importance of developing new, clean and renewable sources of energy will continue to grow in the foreseeable future and so will the need for the education of researchers in this field of science. The interest and challenges of the field continue to shift from simple homogeneous solutions to increasingly more complex heterogeneous systems and interfaces. Over the past decade there have been numerous theoretical and experimental breakthroughs many of which still can be found only in the primary literature. Solar Energy Conversion: Dynamics of Interfacial Electron and Excitation Transfer gathers together, in one volume, the description of modern, sometimes exploratory, experimental and theoretical techniques applied to the dynamics of interfacial electron and electronic excitation transfer processes studied in the context of solar energy conversion. The treatment is fundamental in nature and thus applicable to a broad range of hybrid photovoltaic and photocatalytic materials and interfaces. The book focuses on the dynamic aspects of the electron injection, exciton and carrier relaxation processes, as well as coherence effects in inhomogeneous systems, plasmon-assisted solar photochemistry and femtosecond microscopy, which continue to provide the impetus and the greatest challenge for the development of new methodologies. The goal of the editor and his international team of authors is to give the reader not only a sound reference, but also a starting point for the design of new challenging experiments and superior solar energy conversion materials.

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Solar Energy Conversion

Dynamics of Interfacial Electron and Excitation Transfer

By Piotr Piotrowiak

The Royal Society of Chemistry

Copyright © 2013 The Royal Society of Chemistry
All rights reserved.

ISBN: 978-1-84973-387-8

Contents

Chapter 1 Computational Modeling of Photocatalytic Cells Steven J. Konezny and Victor S. Batista, 1, 
Chapter 2 Charge and Exciton Dynamics in Semiconductor Quantum Dots: A Time Domain, ab Initio View Amanda J. Neukirch and Oleg V. Prezhdo, 37, 
Chapter 3 Multiscale Modelling of Interfacial Electron Transfer Petter Persson, 77, 
Chapter 4 Plasmon-enhanced Solar Chemistry: Electrodynamics and Quantum Mechanics Hanning Chen, George C. Schatz and Mark A. Ratner, 111, 
Chapter 5 Dynamics of Interfacial Electron Transfer in Solar Energy Conversion As Viewed By Ultrafast Spectroscopy Villy Sundström and Arkady Yartsev, 135, 
Chapter 6 Semiconductor Nanocrystals Studied by Two-Dimensional Photon Echo Spectroscopy Cathy Y. Wong, Shun S. Lo and Gregory D. Scholes, 161, 
Chapter 7 Ultrafast Optical Imaging and Microspectroscopy Piotr Piotrowiak, Libai Huang and Lars Gundlach, 203, 
Chapter 8 Ultrafast Multiphoton Photoemission Microscopy of Solid Surfaces in Real and Reciprocal Space A. Winkelmann, C. Tusche, A.A. Ünal, C.-T. Chiang, A. Kubo, L. Wang and H. Petek, 225, 
Chapter 9 Light at the Tip: Hybrid Scanning Tunneling/Optical Spectroscopy Microscopy Jao van de Lagemaat and Manuel J. Romero, 261, 
Chapter 10 Time Resolved Infrared Spectroscopy of Metal Oxides and Interfaces Akihiro Furube, 281, 
Chapter 11 Carrier Dynamics in Photovoltaic Structures and Materials Studied by Time-Resolved Terahertz Spectroscopy Enrique Cánovas, Joep Pijpers, Ronald Ulbricht and Mischa Bonn, 301, 
Chapter 12 X-ray Transient Absorption Spectroscopy for Solar Energy Research Lin X. Chen, 337, 
Subject Index, 371, 

CHAPTER 1

Computational Modeling of Photocatalytic Cells

STEVEN J. KONEZNY AND VICTOR S. BATISTA

Department of Chemistry, Yale University, P.O. Box 208107, New Haven, CT 065208107, USA

1.1 Introduction

Solar energy conversion into chemical fuels is one of the "holy grails" of the 21st century. Significant research efforts are currently underway toward understanding natural photosynthesis and artificial biomimetic systems. Photocatalytic cells absorb solar energy and use it to drive catalytic water oxidation at photoanodes:

2H2O -> 4H+ + 4e- + O2(g) (1.1)

effectively extracting reducing equivalents from water (i.e., protons and electrons) that can be used to generate fuel, for example H2(g) by proton reduction:

4H+ + 4e- -> 2H2(g) (1.2)

The water oxidation half-reaction, introduced by Equation (1.1), is the most challenging obstacle for solar hydrogen production, since it requires a four-electron transfer process coupled to the removal of four protons from water molecules to form the oxygen–oxygen bond. In Nature, this process is driven by solar light captured by chlorophyll pigments embedded in the protein antennas of photosystem II and the energy harvested is used to oxidize water in the oxygen-evolving complex. The development of photocatalytic solar cells made of earth-abundant materials that mimic these mechanisms and photocatalyze water oxidation has been a long-standing challenge in photoelectrochemistry research, dating back to before the discovery of ultraviolet water oxidation on n-TiO2 electrodes by Fujishima and Honda 40 years ago. However, progress in the field has been hindered by a lack of fundamental understanding of the underlying elementary processes and the lack of reliable theoretical methods to model the photoconversion mechanisms.

The landscape of research in solar photocatalysis has been rapidly changing in recent years, with a flurry of activity in the development and analysis of catalysts for water oxidation and fundamental studies of photocatalysis based on semiconductor surfaces. Significant effort is currently focused on the development of more efficient catalysts based on earth-abundant materials and various strategies for the design of molecular assemblies that efficiently couple multielectron photoanodic processes to fuel production. The outstanding challenge is to identify robust materials that could catalyze the necessary multielectron transformations at energies and rates consistent with solar irradiance.

A promising approach for photocatalytic water oxidation involves designing high potential photoanodes based on surface-bound molecular complexes and coupling the anodic multielectron reactions to fuel production at the cathode with long-range free energy gradients. Such a design problem requires fundamental understanding of the factors affecting photoabsorption, interfacial electron transfer to the photoanode, charge transport, storage of oxidizing equivalents for catalysis at low overpotentials and irreversible carrier collection by fuel-forming reactions at the cathode. The characterization of these processes by computational techniques clearly requires methods for modeling the complete photocatalytic mechanism as well as methods for understanding and characterizing the elementary steps at the detailed molecular level, including visible light sensitization of semiconductor surfaces by molecular adsorbates, charge transport and redox catalytic processes. This chapter reviews recent advances in the field, with emphasis on computational research focused on modeling photocatalytic cells and the elementary processes involved at the molecular level. The reviewed studies are part of an interdisciplinary research program including synthesis, electrochemistry and spectroscopy in a joint theoretical and experimental effort to advance our understanding of structure/function relations in high potential photoanodes based on functionalization of nanoporous TiO2 thin films with transition metal catalysts.

The chapter is organized as follows. Section 1.2 reviews recent computational efforts focused on modeling current–voltage characteristics of functional dye-sensitized solar cells (DSSCs) under operational conditions, with emphasis on the effect of the nature of the molecular adsorbates and redox couple on the overall efficiency of photoconversion. Section 1.3 reviews recent developments of methods for inverse design of molecular adsorbers with suitable solar-light photoabsorption. Section 1.4 reviews the development of theoretical models of charge transport in nanoporous metal oxide thin films, with emphasis on the fluctuation-induced tunneling conduction (FITC) model as applied to the description of the temperature dependence of dc and ac conductivities and direct comparisons to experimental data. Section 1.5 is focused on reliable methods for modeling the redox properties of molecular adsorbates, with emphasis on the reduction of systematic errors introduced by either the level of theory (i.e., the choice of density functional theory (DFT) functional, basis set and solvation model) or the electrochemical measurement conditions, including the nature of the solvent, electrolyte and working electrode. Section 1.6 presents a summary of the conclusions and outlook.

1.2 Photoelectrochemical Device Modeling

Modeling can provide a fundamental insight into the effects of individual system components on the overall device functionality. A parameter-space analysis by systematic variation in device composition can lead to the discovery of assemblies with optimum performance....

Details zur Ausgabe

• Verlag: Royal Society of Chemistry
• Erscheinungsdatum: 2013
• Sprache: Englisch
• ISBN 10: 1849733872
• ISBN 13: 9781849733878
• Einband: Gebundene Ausgabe
• Anzahl der Seiten: 379
• Herausgeber: Piotrowiak Piotr
• Kontakt zum Hersteller: Nicht verfügbar
• Verantwortliche Person: Nicht verfügbar