Ultrafast Dynamics at the Nanoscale: Biomolecules and Supramolecular Assemblies

✍ Scribed by Burghardt, Irene; Haacke, Stefan

• Publisher: Pan Stanford Publishing
• Year: 2017
• Tongue: English
• Leaves: 472
• Category: Library

✦ Synopsis

Ultrafast Dynamics at the Nanoscale provides a combined experimental and theoretical insight into the molecular-level investigation of light-induced quantum processes in biological systems and nanostructured (bio)assemblies. Topics include DNA photostability and repair, photoactive proteins, biological and artificial light-harvesting systems, plasmonic nanostructures, and organic photovoltaic materials, whose common denominator is the key importance of ultrafast quantum effects at the border between the molecular scale and the nanoscale. The functionality and control of these systems have been under intense investigation in recent years in view of developing a detailed understanding of ultrafast nanoscale energy and charge transfer, as well as fostering novel technologies based on sustainable energy resources.

Both experiment and theory have made big strides toward meeting the challenge of these truly complex systems. This book, thus, introduces the reader to cutting-edge developments in ultrafast nonlinear optical spectroscopies and the quantum dynamical simulation of the observed dynamics, including direct simulations of two-dimensional optical experiments. Taken together, these techniques attempt to elucidate whether the quantum coherent nature of ultrafast events enhances the efficiency of the relevant processes and where the quantum–classical boundary sets in, in these high-dimensional biological and material systems. The chapters contain well-illustrated accounts of the authors’ research work, including didactic introductory material, and address a multidisciplinary audience from chemistry, physics, biology, and materials sciences. The book is, therefore, a must-have for graduate- and postgraduate-level researchers who wish to learn about molecular nanoscience from a combined spectroscopic and theoretical viewpoint.

✦ Table of Contents

Content: Cover Page
Half Title
Title Page
Copyright Page
Contents
Preface
SECTION I EXPERIMENT
1 Excited States of Single-Stranded DNA Revealed by Femtosecond Transient Absorption Spectroscopy
1.1 Introduction
1.1.1 Origins
1.2 The TA Experiment
1.2.1 The TA Signal
1.2.2 Dispersive Pulse Broadening and Temporal Walk-off
1.3 Transient Absorption Signal Strength
1.3.1 Bleach Recovery Signals
1.3.2 DNA TA Experiments
1.4 Excited-State Dynamics of Single DNA Strands
1.4.1 Structure of (dA)n Single Strands
1.4.2 TA Signals from (dA)n Single Strands. 1.4.3 Estimating Quantum Yields from Bleach Signals1.4.4 Exciton Dynamics
1.5 Summary
2 Ultrafast Light-Induced Processes in DNA Photolyase and Its Substrate-Bound Complex
2.1 Introduction
2.2 Energy Transfer
2.3 Photoactivation
2.4 Photorepair
3 Dynamics and Mechanisms of Ultraviolet-Damaged DNA Repair by Photolyases
3.1 Introduction
3.2 Reaction Mechanism of CPD Repair by Photolyase
3.3 Reaction Mechanism of 6-4PP Repair by Photolyase
3.4 Electron-Tunneling Pathways in DNA Restoration
3.5 Concluding Remarks. 4 Photoactive Yellow Protein: Converting Light into a Metastable Structural Change4.1 Introduction
4.2 Ultrafast Experiments: How to ...?
4.3 Timescale and Mechanism of Isomerization
4.3.1 Timescales
4.3.2 Isomerization
4.3.2.1 Excited state
4.3.2.2 I0 state
4.3.2.3 I1 state
4.3.3 Mechanism
4.4 Role of Charges in the Protein Cavity
4.5 Role of Hydrogen Bonds to the Phenol Ring and the Carbonyl Group of the Chromophore
4.5.1 Hydrogen Bonds to the Phenol Ring
4.5.2 Hydrogen Bonds to the Carbonyl Group
4.6 Role of Water Molecules
4.7 Emerging Picture and Open Questions. 4.8 Applications of PYP: General Aspects4.9 Applications of PYP: Examples
5 Energy Transfer Mechanisms in Nanobiohybrid Structures Based on Quantum Dots and Photosensitive Membrane Proteins
5.1 Introduction
5.2 Possible Energy Transfer Mechanisms in Nanobiohybrid Structures Based on Photosensitive Biomolecules and Quantum Dots: Nonradiative and Radiative Energy Transfer
5.3 The Quantum Dot-Bacteriorhodopsin Nanobiohybrid Structure
5.3.1 Bacteriorhodopsin: Structure and Function
5.3.2 Energy Coupling between Quantum Dots and Bacteriorhodopsin in Aqueous Media. 5.3.3 Methods of Forming Heterostructures Containing Quantum Dot-Bacteriorhodopsin Complexes5.3.4 Quantum Dot-Bacteriorhodopsin Hybrids in Dried Films as Media for Sensing and Optical Applications
5.3.5 Enhancement of the Biological Functions of Bacteriorhodopsin by Means of Coupling with Quantum Dots
5.4 The Quantum Dot-Photosynthetic Reaction Center Nanobiohybrid Structure
5.4.1 Bacterial Photosynthetic Reaction Centers: Structure and Properties
5.4.2 Energy Transfer from Quantum Dots to Bacterial Reaction Centers
5.5 Conclusions and Perspectives.