Diabatic and adiabatic processes in photochemistry

Förster, Th.

doi:10.1351/pac197024030443

Cited by 88 publications

(52 citation statements)

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“…Following the definition of Fçrster, in an adiabatic process deexcitation occurs either in the region of the reactant or of the product, whereas in the non-adiabatic case it occurs in between them. [215] Nowadays, one speaks about surface crossings mediated by CoIns to describe non-adiabatic photochemistry. It is also well-accepted that both adiabatic and nonadiabatic processes are ubiquitous in photochemistry.…”

Section: Nonadiabatic Photochemistrymentioning

confidence: 99%

Progress and Challenges in the Calculation of Electronic Excited States

2011

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A detailed understanding of the properties of electronic excited states and the reaction mechanisms that molecules undergo after light irradiation is a fundamental ingredient for following light-driven natural processes and for designing novel photonic materials. The aim of this review is to present an overview of the ab initio quantum chemical and time-dependent density functional theory methods that can be used to model spectroscopy and photochemistry in molecular systems. The applicability and limitations of the different methods as well as the main frontiers are discussed. To illustrate the progress achieved by excited-state chemistry in the recent years as well as the main challenges facing computational chemistry, three main applications that reflect the authors' experience are addressed: the UV/Vis spectroscopy of organic molecules, the assignment of absorption and emission bands of organometallic complexes, and finally, the obtainment of non-adiabatic photoinduced pathways mediated by conical intersections. In the latter case, special emphasis is put on the photochemistry of DNA. These applications show that the description of electronically excited states is a rewarding but challenging area of research.

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Section: Nonadiabatic Photochemistrymentioning

confidence: 99%

Progress and Challenges in the Calculation of Electronic Excited States

2011

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“…In some fluorophores, the electron redistribution in the photo-excited state leads to dramatic changes in the acidity or basicity of heteroatom substituents 78, 79. For example, the acidity of 2-naphthol increases from p K a = 9.5 in the ground state to p K a * = 2.8 in the lowest excited singlet state 79.…”

Section: Design Strategies For Cation-responsive Fluorescent Indicmentioning

confidence: 99%

Metal-Ion-Responsive Fluorescent Probes for Two-Photon Excitation Microscopy

2010

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Metal ion-responsive fluorescent probes are powerful tools for visualizing labile metal ion pools in live cells. To take full advantage of the benefits offered by two-photon excitation microscopy, including increased depth penetration, reduced phototoxicity, and intrinsic 3D capabilities, the photophysical properties of the probes must be optimized for nonlinear excitation. This review summarizes the challenges associated with the design of two-photon excitable fluorescent probes and labels and offers an overview on recent efforts in developing selective and sensitive reagents for the detection of metal ions in biological systems.

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“…In particular, mechanisms to switch molecules from a nonemissive to an emissive state under the influence of optical stimulations translate into the opportunity to photoactivate fluorescence. Interest in such photoactivatable fluorophores was sparked initially by the idea of monitoring the course of photochemical reactions with fluorescence measurements [4] and then by the possibility of using such compounds for photographic applications [5]. It became eventually apparent, however, that photoactivatable fluorophores can be a valuable complement to conventional ones The excitation of a fluorescent molecule from the ground state (S 0 ) to the second singlet excited state (S 2 ) is followed by internal conversion to the first singlet excited state (S 1 ).…”

Section: Introductionmentioning

confidence: 99%

Photoactivatable Fluorophores

Raymo

2012

ISRN Physical Chemistry

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Photoactivatable fluorophores switch from a nonemissive to an emissive state upon illumination at an activating wavelength and then emit after irradiation at an exciting wavelength. The interplay of such activation and excitation events can be exploited to switch fluorescence on in a defined region of space at a given interval of time. In turn, the spatiotemporal control of fluorescence translates into the opportunity to implement imaging and spectroscopic schemes that are not possible with conventional fluorophores. Specifically, photoactivatable fluorophores permit the monitoring of dynamic processes in real time as well as the reconstruction of images with subdiffraction resolution. These promising applications can have a significant impact on the characterization of the structures and functions of biomolecular systems. As a result, strategies to implement mechanisms for fluorescence photoactivation with synthetic fluorophores are particularly valuable. In fact, a number of versatile operating principles have already been identified to activate the fluorescence of numerous members of the main families of synthetic dyes. These methods are based on either the irreversible cleavage of covalent bonds or the reversible opening and closing of rings. This paper overviews the fundamental mechanisms that govern the behavior of these photoresponsive systems, illustrates structural designs for fluorescence photoactivation, and provides representative examples of photoactivatable fluorophores in actions.

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Diabatic and adiabatic processes in photochemistry

Abstract: Abstract

Cited by 88 publications

References 0 publications

Progress and Challenges in the Calculation of Electronic Excited States

Progress and Challenges in the Calculation of Electronic Excited States

Metal-Ion-Responsive Fluorescent Probes for Two-Photon Excitation Microscopy

Photoactivatable Fluorophores

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