Studies of Photoinduced Molecular Dynamics Using a Fast Imaging Sensor

Studies of Photoinduced Molecular Dynamics Using a Fast Imaging Sensor
Author: Craig S. Slater
Publisher: Springer
Total Pages: 194
Release: 2015-10-15
Genre: Science
ISBN: 3319245171

The work presented in this thesis involves a number of sophisticated experiments highlighting novel applications of the Pixel Imaging Mass Spectrometry (PImMS) camera in the field of photoinduced molecular dynamics. This approach represents the union of a new enabling technology (a multiple memory register, CMOS-based pixel detector) with several modern chemical physics approaches and represents a significant leap forward in capabilities. Applications demonstrated include three-dimensional imaging of photofragment Newton spheres, simultaneous electron-ion detection using a single sensor, and ion-ion velocity correlation measurements that open the door to novel covariance imaging experiments. When combined with Coulomb explosion imaging, such an approach is demonstrated to allow the measurement of molecular structure and motion on a femtosecond timescale. This is illustrated through the controlled photoexcitation of torsional motion in biphenyl molecules and the subsequent real-time measurement of the torsional angle.

Laser Spectroscopy and Laser Imaging

Laser Spectroscopy and Laser Imaging
Author: Helmut H. Telle
Publisher: CRC Press
Total Pages: 751
Release: 2018-04-17
Genre: Science
ISBN: 1466588233

"a very valuable book for graduate students and researchers in the field of Laser Spectroscopy, which I can fully recommend" —Wolfgang Demtröder, Kaiserslautern University of Technology How would it be possible to provide a coherent picture of this field given all the techniques available today? The authors have taken on this daunting task in this impressive, groundbreaking text. Readers will benefit from the broad overview of basic concepts, focusing on practical scientific and real-life applications of laser spectroscopic analysis and imaging. Chapters follow a consistent structure, beginning with a succinct summary of key principles and concepts, followed by an overview of applications, advantages and pitfalls, and finally a brief discussion of seminal advances and current developments. The examples used in this text span physics and chemistry to environmental science, biology, and medicine. Focuses on practical use in the laboratory and real-world applications Covers the basic concepts, common experimental setups Highlights advantages and caveats of the techniques Concludes each chapter with a snapshot of cutting-edge advances This book is appropriate for anyone in the physical sciences, biology, or medicine looking for an introduction to laser spectroscopic and imaging methodologies. Helmut H. Telle is a full professor at the Instituto Pluridisciplinar, Universidad Complutense de Madrid, Spain. Ángel González Ureña is head of the Department of Molecular Beams and Lasers, Instituto Pluridisciplinar, Universidad Complutense de Madrid, Spain.

Photoinduced Molecular Dynamics in Solution

Photoinduced Molecular Dynamics in Solution
Author: Gianluca Levi
Publisher: Springer Nature
Total Pages: 208
Release: 2019-09-03
Genre: Science
ISBN: 3030286118

This book explores novel computational strategies for simulating excess energy dissipation alongside transient structural changes in photoexcited molecules, and accompanying solvent rearrangements. It also demonstrates in detail the synergy between theoretical modelling and ultrafast experiments in unravelling various aspects of the reaction dynamics of solvated photocatalytic metal complexes. Transition metal complexes play an important role as photocatalysts in solar energy conversion, and the rational design of metal-based photocatalytic systems with improved efficiency hinges on the fundamental understanding of the mechanisms behind light-induced chemical reactions in solution. Theory and atomistic modelling hold the key to uncovering these ultrafast processes. Linking atomistic simulations and modern X-ray scattering experiments with femtosecond time resolution, the book highlights previously unexplored dynamical changes in molecules, and discusses the development of theoretical and computational frameworks capable of interpreting the underlying ultrafast phenomena.

Analysis and Control of Ultrafast Photoinduced Reactions

Analysis and Control of Ultrafast Photoinduced Reactions
Author: Oliver Kühn
Publisher: Springer Science & Business Media
Total Pages: 854
Release: 2007-07-05
Genre: Science
ISBN: 3540680381

This book summarizes several years of research carried out by a collaboration of many groups on ultrafast photochemical reactions. It emphasizes the analysis and characterization of the nuclear dynamics within molecular systems in various environments induced by optical excitations and the study of the resulting molecular dynamics by further interaction with an optical field.

Imaging Photo-induced Dynamics in Halomethane Molecules with Coincident Ion Momentum Spectroscopy

Imaging Photo-induced Dynamics in Halomethane Molecules with Coincident Ion Momentum Spectroscopy
Author: Balram Kaderiya
Publisher:
Total Pages: 0
Release: 2021
Genre:
ISBN:

Molecular transformations triggered by the absorption of light are of tremendous importance in our day-to-day life, science, and technology. Examples of such "photo-induced" reactions include, among many others, photosynthesis, solar energy conversion, and mechanisms behind human vision. Besides knowing the final outcome of such reactions, for many scientific and technological applications it is crucially important to understand how they evolve in time, and how the motion of individual atoms leads to a certain outcome. For decades, resolving these processes in time represented a severe experimental challenge since the atomic motion involved is extremely fast. The availability of ultrashort, femtosecond laser pulses in combination with novel molecular imaging techniques provides experimental tools needed to address this challenge. This thesis describes the application of coincident ion momentum imaging setup, sometimes called "a reaction microscope", for studies of photo-induced dynamics in halomethane molecules (CH2I2, CH2ICl, CH3I). The main objective of this work is to visualize light-induced breaking, rearrangement and formation of molecular bonds, and to determine relevant mechanisms and time scales. Halomethanes are often considered as model systems for studying such prototypical photochemical events because they are small enough to allow for reasonable electronic structure calculations and for coincidence detection of all molecular fragments, while being large enough to be of chemical relevance and to undergo some fundamental chemical transformations. The work described here covers three different regimes of light-molecule interaction: (1) ionization and fragmentation by an intense near-infrared (NIR) field, (2) excitation of a neutral molecule by a single ultraviolet (UV) photon; and (3) ionization and fragmentation by a single extreme ultraviolet (XUV) photon. We specifically focus on several aspects of halomethane photochemistry that are of general importance, have been actively discussed in literature, and yet are difficult to access using more established imaging or spectroscopic techniques. More specifically, we first characterize molecular response to a single intense femtosecond NIR pulse at 800 nm, identifying and disentangling different ionization and fragmentation channels, and their signatures in various coincident observables. Then we apply multiple ionization and rapid dissociation ("Coulomb explosion") by such a pulse as a tool to map molecular dynamics in pump-probe experiments. In this approach, the information on molecular geometry at the time when the probe pulse arrives is extracted from the coincident measurement of the 3D momentum vectors of the detected fragment ions. We start with the NIR pump / NIR probe experiments on CH2I2 and CH2ICl molecules, aimed at characterizing bound and dissociating wave packets induced by a strong NIR field. Here, we find that both, dissociation dynamics and molecular halogen elimination (I2 or ICl) are mainly governed by the large-scale bending vibrations of the molecule, even though (weak) signatures of stretching vibrations can be also observed in the spectra. Focusing on the I2 (or ICl) elimination channel, which requires breaking two carbon-halogen bonds and formation of a new bond between the two halogen atoms, we demonstrate how it can be disentangled from the other fragmentation channels, and find that it is dominated by a direct, "synchronous" pathway. Then we apply the same approach and the same NIR probe pulses to study the photoexcitation of diiodomethane (CH2I2) by a femtosecond UV pulse at 266 nm in a UV pump / NIR probe experiment. Here, in addition to two-body dissociation and I2 elimination channels, we also observe a significant contribution of three-body dissociation. This channel can be easily separated in our triple-coincidence measurements, but is notoriously difficult to identify with most of the other techniques. Besides that, we find signatures of transient CH2I-I isomer formation within the first 100 femtoseconds after the initial photoexcitation. While the picosecond-scale isomerization of CH2I2 was clearly demonstrated earlier in the liquid-phase experiments in solution, and was shown to occur due to the interaction with the solvent, the existence of a much faster, intra-molecular isomerization pathway for isolated molecules in a gas phase was debated in literature. In this work, we provide direct evidence of such ultrafast, sub-100 fs CH2I2 isomerization, and demonstrate that the decay of this short-lived isomer opens up an additional pathway for molecular iodine elimination. Finally, we have performed a complementary study on CH2ICl and CH3I molecules employing short extreme ultraviolet pulses (XUV) from FLASH II free-electron laser facility in Hamburg, Germany. Here, one femtosecond XUV pulse at ~ 53 nm central wavelength is used to initiate the dynamics, mainly by single-photon ionization, while the second identical pulse is used to probe the evolution of the created ionic-state wave packets. Employing the same ion momentum imaging setup, we map different dissociative ionization channels and observe signature of intramolecular electron transfer between different sites of a dissociating molecular ion. In contrast to the results of earlier FEL experiments on X-ray inner-shell photoionization of dissociating halomethanes, which could be readily explained using the classical over-the-barrier charge transfer model, our data for valence XUV ionization suggest a more subtle dependence of the charge transfer probability on the internuclear distance, likely determined by the delocalization of molecular orbitals. Overall, the work presented in this thesis advances our understanding of different pathways in strong-field and single-photon induced photochemistry of halomethanes, and demonstrates an efficient and visual approach for mapping transient reaction intermediates. The tools and methodology presented here can be applied to study a broad range of ultrafast photochemical reactions, and can be useful for many strong-field imaging and control applications.

Imaging in Molecular Dynamics

Imaging in Molecular Dynamics
Author: Benjamin J. Whitaker
Publisher: Cambridge University Press
Total Pages: 0
Release: 2007-07-26
Genre: Science
ISBN: 9780521038324

Written in a tutorial style by some of the key practitioners in the field, this book provides a comprehensive account of charged particle imaging and describes many of its recent applications. The technique has revolutionized experimental studies of photodissociation and bimolecular collisions over the past couple of decades. It is of primary interest to researchers and graduate students working in chemical and molecular physics requiring an overview of the subject as well as ideas for future experiments.

Handbook of Neurophotonics

Handbook of Neurophotonics
Author: Francesco S. Pavone
Publisher: CRC Press
Total Pages: 439
Release: 2020-05-10
Genre: Science
ISBN: 0429530900

The Handbook of Neurophotonics provides a dedicated overview of neurophotonics, covering the use of advanced optical technologies to record, stimulate, and control the activity of the brain, yielding new insight and advantages over conventional tools due to the adaptability and non-invasive nature of light. Including 32 colour figures, this book addresses functional studies of neurovascular signaling, metabolism, electrical excitation, and hemodynamics, as well as clinical applications for imaging and manipulating brain structure and function. The unifying theme throughout is not only to highlight the technology, but to show how these novel methods are becoming critical to breakthroughs that will lead to advances in our ability to manage and treat human diseases of the brain. Key Features: Provides the first dedicated book on state-of-the-art optical techniques for sensing and imaging across at the cellular, molecular, network, and whole brain levels. Highlights how the methods are used for measurement, control, and tracking of molecular events in live neuronal cells, both in basic research and clinical practice. Covers the entire spectrum of approaches, from optogenetics to functional methods, photostimulation, optical dissection, multiscale imaging, microscopy, and structural imaging. Includes chapters that show use of voltage-sensitive dye imaging, hemodynamic imaging, multiphoton imaging, temporal multiplexing, multiplane microscopy, optoacoustic imaging, near-infrared spectroscopy, and miniature neuroimaging devices to track cortical brain activity.