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There is growing need to utilise Earth-abundant transition metal complexes in photovoltaic and photocatalytic applications, while reducing the current heavy reliance on rare, expensive and toxic heavy transition metal complex, such as Ru-based. Iron is the most abundant transition metal within the same group 8 as Ru while being very cheap and eco-friendly. But its photophysics suffers from the disadvantage of short excited-state lifetime of MLCT states due to low lying MC states. However ever since the introduction of NHC carbene-based ligands, the increased sigma donor strength has significantly improved the MLCT lifetimes and there has been a tremendous development in the last decade. This thesis delves into an extensive investigation of the photophysical and photochemical properties of diverse homoleptic and heteroleptic Fe-carbene complexes to unravel the influence of ligand architecture and design on excited-state dynamics. The primary objective of elucidating excited-state dynamics and deactivation pathways in relation to structure-property relationships. Expanding the scope of iron carbene complexes for functional applications is another key goal, achieved by introducing pH-sensitive functional ligands that hold immense significance for light-driven applications.
Advances in Inorganic Chemstry serial highlights new advances in the field with this new volume presenting interesting chapters. Each chapter is written by an international board of authors. Provides the authority and expertise of leading contributors from an international board of authors Presents the latest release in Advances in Inorganic Chemistry serials Updated release includes the latest information on Photochemistry and Photophysics of Earth-Abundant Transition Metal Complexes
Focusing on practical applications, the author provides a balanced introduction to the many possible technological uses of metal complexes. Coverage includes the transition metals, lanthanide and actinide complexes, metal porphyrins, and many other complexes. This volume meets the needs of students and scientists in inorganic chemistry, chemical physics, and solid-state physics.
Humanity's ever-growing energy demands require the implementation of more sustainable ways to harvest and store energy. At the same time, the reduction of greenhouse gas emission and thus global warming remains of paramount importance. To this end, solar energy harvesting presents an attractive route towards satisfying these requirements--be that by conversion to thermal energy, electricity or to chemical energy. Molecular systems based on iron could prove particularly interesting in this area, due to their advantageous properties such as appreciable visible light-absorption as well as the high availability and low cost of iron. As of yet, they have not been extensively studied though, which can be attributed to the inherently poor photophysical and -chemical properties associated with these systems. However, well thought-out structural design can be used to combat said issues. The ligand motif used in Fe-N-heterocyclic carbene (NHC) complexes aids in mitigating the formerly mentioned unfavourable properties, allowing for bimolecular quenching with electron donors and acceptors to occur, which is crucial for photocatalysis. In this thesis, the application of hexa-NHC complexes based on Earth-abundant iron as light-harvesters for solar-to-chemical energy conversion is demonstrated. The utility of Fe(III)-NHC complexes for sensitisation of artificial photosynthesis reactions as well as their performance as photoredox catalysts in organic transformations has been studied and the underlying mechanisms have been investigated, giving insight into the prospects and limitations associated with these systems. For the hydrogen evolution and aminomethylation reactions investigated here, conventional single-photon mechanisms were observed. Meanwhile, in the case of the atom transfer radical addition reactions, sequential photon absorption of two different oxidation states of the catalyst within the same catalytic turnover was shown to be operative. Furthermore, a study featuring the Fe(II)-congener of an Fe(III)-NHC complex with demonstrated photocatalytic activity revealed a less than favourable excited state lifetime compared to the Fe(III)-parent complex, showcasing that the preparation of Fe(II)-NHC complexes with synthetically useful photophysical and chemical properties is not necessarily facile. Early investigations of a photocatalytic reaction driven by heterogenisation of Fe(III)-NHC complexes are also shown. There the goal was to improve upon the sustainability of these catalysts by facilitating their recyclability. This thesis thus showcases the potential of Fe-NHC complexes for photocatalytic applications, whilst also revealing their shortcomings.
The scope of this paper is to recall fundamental notions of the molecular spectroscopy and dynamics, necessary for discussion of photophysical and photochemical processes in condensed phases. We will thus treat in a more detailed way the specific features which are important for molecular systems strongly interacting with their environment. Other aspects such as the time evolution of isolated molecules, single-level excitation and state-to-state chemistry, important for the gas-phase photophysics are omitted. We start (Sec.2) with a brief description of radiative processes (light absorption and emission) in molecules. In the quantum-mechanical treatment of this problem, the appropriate basis is that of so-called zero-order states, corresponding to the traditional scheme of electronic states (singlets, doublets, triplets etc.) and vibrational levels belonging to each state. The important point will be deduction of selection rules for most radiative transitions. At this stage all molecular states are considered as stationary states. In order to treat the breakdown of simple selection rules and non-radiative transitions between individual molecular states, it is necessary to take into account the mechanisms coupling the zero-order states (Sec.3). We will first focus on intramolecular coupling effects and then discuss the solvent effects on intramolecular relaxation processes. The problem of the non-radiative transfer of the electronic energy between different molecules - closely related to that of the energy dissipation within a single molecule will be treated in Sec.4.
Connects principles, processes, and experimental techniques with current research in the continuously expanding field of photochemistry and photophysics Photochemistry and Photophysics covers a wide spectrum of concepts in photochemistry and photophysics, introducing principles, processes, and experimental techniques, with a wealth of examples of current applications and research spanning natural photosynthesis, photomedicine, photochromism, luminescent sensors, energy conversion and storage, and sustainability issues. In this Second Edition, several chapters have been revised considerably and others have been almost entirely rewritten. A number of schemes and figures have been added, and the reference list at the end of each chapter has been extended and updated. Clearly structured, the first part of the text discusses the formation, properties, and reactivity of excited states of inorganic and organic molecules and supramolecular species, and the second part focuses on photochemical and photophysical processes in natural and artificial systems. Readers will learn how photochemical and photophysical processes can be exploited for novel, unusual, and unexpected applications. Written by world-renowned experts in the field, Photochemistry and Photophysics includes information on: Formation, electronic structure, properties, chemical reactivity, and radiative and nonradiative decay of electronically excited states Fundamental concepts and theoretical approaches concerning energy transfer and electron transfer Peculiar light absorption/emission spectra and the photochemical properties of the various families of organic molecules and metal complexes Equipment, techniques, procedures, and reference data concerning photochemical and photophysical experiments, including warnings to avoid mistakes and misinterpretations Relationships between photochemical, photophysical, and electrochemical properties of molecules that enable interconversion between light and chemical energy With an appropriate mix of introductory, intermediate, and advanced content, this is an ideal textbook resource for related undergraduate and postgraduate courses. The text is also valuable for scientists already active in photochemical and photophysical research who will find helpful suggestions to undertake novel scientific projects.
This book presents critical reviews of the current position and future trends in modern chemical research. It offers short and concise reports on chemistry, each written by world renowned experts.
Abstract: One of the advantages of using light as a reactant in a chemical reaction is the generation of an excited state that is able to overcome high activation barriers that are not accessible by heating. In addition, the light can be spatially controlled, by focusing the photons onto a given area; such control is not possible in conventional thermal reactions. The spatial control of light has been shown to be advantageous in a number of applications including cancer therapy, signaling, and data storage. The photophysical properties and photochemistry of various complexes that may be potentially useful in these three applications will be discussed in this dissertation. The work presented here focuses on the photochemical and photophysical properties of both bimetallic and mononuclear complexes. It is the goal of this dissertation to examine several of the processes possible once a complex is excited, including photochemical reactions, isomerizations, and differences in photophysical properties. There is a brief introduction at the beginning of each chapter that describes the possible photochemical applications related to the work presented and necessary background information in the specific area.
This dissertation, "Design, Synthesis, and Photophysics and Photochromic Study of Dithienylethene-containing Heterocyclic Derivatives and N-heterocyclic Carbene-ruthenium (II) Complexes" by Gongping, Duan, 段公平, was obtained from The University of Hong Kong (Pokfulam, Hong Kong) and is being sold pursuant to Creative Commons: Attribution 3.0 Hong Kong License. The content of this dissertation has not been altered in any way. We have altered the formatting in order to facilitate the ease of printing and reading of the dissertation. All rights not granted by the above license are retained by the author. DOI: 10.5353/th_b4424824 Subjects: Carbenes (Methylene compounds) - Synthesis Ruthenium compounds - Synthesis Complex compounds - Synthesis Photochromism Photochemistry