Ultrafast Photophysics And Photochemistry After Excited State Intramolecular Charge Transfer In The Liquid Phase
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| Author | : Hanna A. Ernst |
| Publisher | : |
| Total Pages | : 0 |
| Release | : 2015 |
| Genre | : Charge transfer |
| ISBN | : 9783832539849 |
The ultrafast excited state dynamics of the small donor-acceptor molecules ortho-, meta- and para-nitrophenol, their corresponding phenolates as well as selected type-I photoinitiators have been studied by means of steady state UV-Vis and femtosecond time-resolved transient absorption spectroscopy in the liquid phase. The investigated compounds are characterized by intramolecular charge transfer in the ultra violet. The experimental findings were assisted by ab initio calculations at the (TD)-DFT and the CASSCF level of theory.
| Author | : Darya S Budkina |
| Publisher | : |
| Total Pages | : 230 |
| Release | : 2019 |
| Genre | : Energy transfer |
| ISBN | : |
This work aims at deeper understanding of chemical reaction dynamics, ultrafast photochemical and photophysical relaxation pathways, and energy redistribution and dissipation in the liquid phase on a femto-to-picosecond timescale. Breaking and making of chemical bonds, structural reorganization, and energy flow are all the essence of chemistry, and all occur on the time scale of molecular vibrations (tens of femtoseconds). Important insights about the structure of evolving molecules, relaxation phenomena, and ultrafast photochemical and photophysical population dynamics can be obtained using sub-50-fs time-resolved transient absorption spectroscopy. As a result, highly viable and/or unique information about the mechanism of relaxation dynamics and the nature of short-lived intermediates can be gained. Furthermore, ultrashort laser pulses with duration of 100 fs or shorter can help set up and detect coherent motion in vibronic excited and ground states. Coherence observed in product states provides the knowledge about electronic and nuclear motion along the relaxation path. This yields the information about the potential energy surfaces involved in the photochemical or photophysical process that occurs. The knowledge acquired from such experiments can be used as an entry point for control of femtochemical processes in solution. The technical aspect of this work focuses on developing and optimizing the ultrafast transient absorption setup for studying ultra-rapid photochemical relaxation dynamics in the molecules of interest, namely, geminal dibromocycloalkanes and halogen-containing transition metal complexes. Excitation pulses from deep-UV to near-IR were temporally compressed using prisms compressors to generate sub-40 fs laser pulses. Also, stable white-light continuum pulses used for probing were generated in the wide spectral range of 280 - 760 nm. This thesis is divided into two main parts. The first part provides information about ultrafast dynamics (10-fs time resolution after deconvolution) of geminal dibromocycloalkanes. The second part covers ultrafast radiationless relaxation dynamics of halogen-containing transition metal complexes (IrBr62-, IrCl62-, etc.). A particular focus in this part is on excitation into several vibronic states of the different nature (ligand-to-metal charge-transfer (LMCT) and intraconfigurational), where the lowest-excited intraconfigurational state is accessed via direct femtosecond near-IR (2000 nm) excitation.
| Author | : Thomas Wolf |
| Publisher | : KIT Scientific Publishing |
| Total Pages | : 210 |
| Release | : 2013 |
| Genre | : Science |
| ISBN | : 3866449402 |
The photoinduced dynamics of radical precursors in solution were investigated by means of femtosecond transient absorption spectroscopy assisted by quantum chemical calculations. The investigated systems show a wide range of excited state lifetimes ranging from tens of femtoseconds to nanoseconds. Thus, in the first case, on the investigated time scale the dynamics of the generated radicals can be additionally investigated. In the latter case only the excited singlet lifetime is observable.
| Author | : Lauro Tatsuo Kubota |
| Publisher | : Springer Nature |
| Total Pages | : 559 |
| Release | : 2021-11-25 |
| Genre | : Science |
| ISBN | : 3030823814 |
This textbook covers the main tools and techniques used in bioanalysis, provides an overview of their principles, and offers several examples of their application and future trends in diagnosis. Chapters from expert contributors explore the role of bioanalysis in different areas such as biochemistry, physiology, forensics, and clinical diagnosis, including topics from sampling/sample preparation, chemometrics in bioanalysis to the latest techniques used in the field. Particular attention is given to the recent advances in the application of mass spectrometry, NMR, electrochemical methods and separation techniques in bioanalysis. Readers will also find more about the application of microchip-based devices and analytical microarrays. This textbook will appeal to graduate/advanced undergraduate students in Chemistry, Biology, Biochemistry, Pharmacy, and Chemical Engineering. It is also a useful resource for researchers and professionals working in the fields of biomedicine and veterinary sciences, with clear explanations and examples of how the different bioanalytical devices are applied for clinical diagnosis.
| Author | : |
| Publisher | : Elsevier |
| Total Pages | : 330 |
| Release | : 2024-06 |
| Genre | : Science |
| ISBN | : 0443237468 |
Photochemistry and Photophysics of Earth-Abundant Transition Metal Complexes, Volume 83 in the Advances in Inorganic Chemistry series, highlights new advances in the field, with this new volume presenting interesting chapters on topics such as Radioluminescence of Copper(I) Clusters, Photophysics and Photochemistry of Chromium(III) Complexes (Molecular Rubies), Chromic behaviors of luminescent copper(I) complexes, Long-lived photoluminescence in group 4 metal complexes enabled by ligand-to-metal charge transfer, Photoactive MOFs for CO2 Activation utilizing Earth Abundant Metals, and more. Other sections cover Earth Abundant Metal Complexes for Optoelectronic Applications, Photoactive metal to ligand charge transfer excited states in 3d6 and 3d8 complexes, Ligand-to-metal charge-transfer excited states in d0 transition-metal complexes: Investigations into the photochemistry and photophysics of emissive titanocenes, Ultrafast dynamics in photoactive copper complexes from optical and Xray methods, and Photophysical properties of Ni(II) complexes and some copper(I) and zinc(II) complexes.
| Author | : Ke-Li Han |
| Publisher | : John Wiley & Sons |
| Total Pages | : 1229 |
| Release | : 2011-03-16 |
| Genre | : Science |
| ISBN | : 1119972922 |
This book gives an extensive description of the state-of-the-art in research on excited-state hydrogen bonding and hydrogen transfer in recent years. Initial chapters present both the experimental and theoretical investigations on the excited-state hydrogen bonding structures and dynamics of many organic and biological chromophores. Following this, several chapters describe the influences of the excited-state hydrogen bonding on various photophysical processes and photochemical reactions, for example: hydrogen bonding effects on fluorescence emission behaviors and photoisomerization; the role of hydrogen bonding in photosynthetic water splitting; photoinduced electron transfer and solvation dynamics in room temperature ionic liquids; and hydrogen bonding barrier crossing dynamics at bio-mimicking surfaces. Finally, the book examines experimental and theoretical studies on the nature and control of excited-state hydrogen transfer in various systems. Hydrogen Bonding and Transfer in the Excited State is an essential overview of this increasingly important field of study, surveying the entire field over 2 volumes, 40 chapters and 1200 pages. It will find a place on the bookshelves of researchers in photochemistry, photobiology, photophysics, physical chemistry and chemical physics.
| Author | : Sergey M. Matveev |
| Publisher | : |
| Total Pages | : 132 |
| Release | : 2016 |
| Genre | : Photochemistry |
| ISBN | : |
The present work is the detailed study of photophysical and photochemical processes in molecules by means of femtosecond (fs) time-resolved transient absorption spectroscopy both in the gas and solution phases. This knowledge is important for an understanding of many light-driven mechanisms in photosensitive systems -- building blocks of light-triggered molecular devices. Many light-driven reactions occur on a time scale comparable to that of vibration motion, and therefore, can only be "seen" by using advanced methods such as the fs transient absorption. This method provides ultrahigh temporal resolution on a vibrational period timescale, which is superior to other time-resolved methods and, importantly, can be utilized to study the dynamics of molecular systems. Specifically, ultrafast transient absorption spectroscopy was used to investigate radiationless relaxation dynamics of two paradigm transition metal complexes in octahedral (IrBr62 ) and tetrahedral (CuCl42-) environment. Following excitation at 2000-nm, both systems undergo internal conversion to the ground electronic state with significant difference in lifetimes (55-fs and 360 -ps for CuCl42- and IrBr62-, respectively). The difference was explained by the presence of conical intersection between the excited and ground electronic states in the Cu2+ system due to strong Jahn Teller effect and the strong spin-orbit coupling in the Ir4+ complex. Upon visible irradiation, IrBr62- was found to undergo cascade-like relaxation through the long-lived (360 ps) metal-centered 2Ug'(T2g) excited state. Transient absorption studies upon 330 nm excitation evidence ultrafast intersystem crossing in the initially-excited state to form an excited state in quartet multiplicity. This state decays via a series of internal conversion steps into the lowest-energy quartet excited state. We found that the electron transfer within the t2g metal orbital is found to be the rate-limited step for non-radiative relaxation of IrBr62-. For the first time, the photochemical reaction pathway was documented in the UV photochemistry of CH2I2 molecule. It was shown that CH2I2 excited into the S1 state undergoes direct ~50-fs isomerization through a conical intersection forming the isomeric species with the iodine-iodine bond. Methodologically, this work demonstrated the synergy between fs transient absorption spectroscopy and surface hopping dynamics simulations in revealing the evolution of complicated ultrafast photochemical reactions in small polyatomic molecules.
| Author | : Ramprasad Misra |
| Publisher | : John Wiley & Sons |
| Total Pages | : 257 |
| Release | : 2018-02-27 |
| Genre | : Science |
| ISBN | : 3527801944 |
Bridging the gap between the multitude of advanced research articles and the knowledge newcomers to the field are looking for, this is a timely and comprehensive monograph covering the interdisciplinary topic of intramolecular charge transfer (ICT). The book not only covers the fundamentals and physico-chemical background of the ICT process, but also places a special emphasis on the latest experimental and theoretical studies that have been undertaken to understand this process and discusses key technological applications. After outlining the discovery of ICT molecules, the authors go on to discuss several important substance classes. They present the latest techniques for studying the underlying processes and show the interplay between charge transfer and the surrounding medium. Examples taken from nonlinear optics, viscosity and polarity sensors, and organic electronics testify to the vast range of applications. The result is a unique information source for experimentalists as well as theoreticians, from postgraduate students to researchers.
| Author | : |
| Publisher | : |
| Total Pages | : 892 |
| Release | : 1994 |
| Genre | : Aeronautics |
| ISBN | : |
| Author | : Evgeniia Butaeva |
| Publisher | : |
| Total Pages | : 198 |
| Release | : 2015 |
| Genre | : Laser pulses, Ultrashort |
| ISBN | : |
A molecular level understanding of photodynamics in condensed media is one of the recent challenges to chemical physics. This is because of the intrinsic complexity of liquid-phase photophysical and photochemical singularities arising from competing intra- and intermolecular processes. Such processes often take place on a timescale of a few femtoseconds (10-15 s) to several tens of picoseconds (10-12 s). In this work, the model photochemical processes used to investigate ultrafast photo-induced reaction dynamics in solution. The model compounds are non-metal/metal polyhalogenated small molecules. The gas-phase photochemistry of these small molecules is thoroughly examined, which also enables to establish the connection between liquid and gas phase dynamics. Furthermore, contrary to the scrupulously investigated di- and triatomic molecular systems, more vibrational degrees of freedom are accessible both for the model parent molecules, nascent polyatomic radical species, and isomer photoproducts. Therefore, a detailed mapping of the photochemical reaction paths of these molecular systems can possibly reveal different couplings between the reactive modes and other dark states in a far-from-equilibrium situation. The complexity of the encountered ultrafast events requires the utilization of several experimental and computational approaches. Results of femtosecond transient absorption, picosecond transient resonance Raman, excited state ab initio calculations are discussed in this context.
