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Observation And Control Of Intramolecular Dynamics Of Gas Phase Molecules By Ultrafast Laser Pulses
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Book Synopsis Observation and Control of Intramolecular Dynamics of Gas-phase Molecules by Ultrafast Laser Pulses by : Igor Pastirk
Download or read book Observation and Control of Intramolecular Dynamics of Gas-phase Molecules by Ultrafast Laser Pulses written by Igor Pastirk and published by . This book was released on 2002 with total page 372 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Analysis and Control of Ultrafast Photoinduced Reactions by : Oliver Kuhn
Download or read book Analysis and Control of Ultrafast Photoinduced Reactions written by Oliver Kuhn and published by Springer. This book was released on 2016-05-01 with total page 860 pages. Available in PDF, EPUB and Kindle. Book excerpt: Dynamical processes in molecules like bond shaking, breaking or making c- monlytakeplaceonatimescalefromthepico-downtothefemtosecondrange. Theadventofequallyfastlasersourcesandreal-timeobservationschemeslike pump-probe spectroscopy has facilitated the direct insight into such processes wheninitiatedbylight. Inparallelthedevelopmentofadvancedcomputational methods treating the dynamics of photoexcited molecular systems allowed a convergence between theoretical description and experimental observation of such ultrafast dynamical processes. Consequently, the idea emerged, not only to analyze, but also to control molecular dynamics in real time by adequately designed light ?elds. Stimulated by theoretical concepts for in'uencing the motion of molecular wave packets by means of simple few-parameter elect- magnetic ?eld sequences, experiments were driven toward a practical reali- tion of arbitrarily shaped laser pulses. This development culminated in the active feedback control of even complex systems. In addition this o'ers the unique possibility not only to determine the outcome of chemical reactions, butalsotoretrievespeci'cinformationaboutthechosendynamicalpathways, that is, to perform analysis by control. This book illustrates a vital research ?eld by covering a broad spectrum of molecular systems with growing complexity while demonstrating at the same time the convergence of experimental and theoretical approaches. After a g- eral introduction in Chapter 1, Chapter 2 starts with small isolated molecules in the unperturbed environment of the gas phase and Chapter 3 proceeds to more complex systems, but still in vacuum. A higher level of complexity is then reached in Chapter 4 where small molecules in a rare gas matrices are discussed serving as prototype examples for condensed phase dynamics.
Book Synopsis Laser-driven Rotational Dynamics of Gas-phase Molecules by : Xiaoming Ren
Download or read book Laser-driven Rotational Dynamics of Gas-phase Molecules written by Xiaoming Ren and published by . This book was released on 2013 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: In this thesis, our work on developing new techniques to measure and enhance field-free molecular alignment and orientation is described. Non-resonant femtosecond laser pulses are used to align and orient rotationally-cold gas-phase molecules. The time-dependent Schrodinger equation is solved to simulate the experimental results. A single-shot kHz velocity map imaging (VMI) spectrometer is developed for characterizing 1D and 3D alignment. Stimulated by a novel metric for 3D alignment proposed by Makhija et al. [Phys. Rev. A 85,033425 (2012)], a multi-pulse scheme to improve 3D alignment is demonstrated experimentally on difluoro-iodobenzene molecules and the best field-free 3D alignment is achieved. A degenerate four wave mixing probe is developed to overcome limitations in VMI measurement; experiments on different types of molecules show good agreement with computational results. Highly aligned linear molecules are used for high harmonic generation experiments. Due to the high degree of alignment, fractional revivals, variation of revival structure with harmonic order and the shape resonance and Cooper minimum in the photoionization cross section of molecular nitrogen are all observed directly in experiment for the first time. Enhanced orientation from rotationally cold heteronuclear molecules is also demonstrated. We follow the theory developed by Zhang et al. [Phys. Rev. A 83, 043410 (2011)] and demonstrate experimentally for the first time that for rotationally cold carbon monoxide an aligning laser pulse followed by a two-color laser pulse can increase field-free orientation level by almost a factor of three compared to using just the two-color pulse.
Book Synopsis Ultrafast Dynamics Driven by Intense Light Pulses by : Markus Kitzler
Download or read book Ultrafast Dynamics Driven by Intense Light Pulses written by Markus Kitzler and published by Springer. This book was released on 2015-07-24 with total page 385 pages. Available in PDF, EPUB and Kindle. Book excerpt: This book documents the recent vivid developments in the research field of ultrashort intense light pulses for probing and controlling ultrafast dynamics. The recent fascinating results in studying and controlling ultrafast dynamics in ever more complicated systems such as (bio-)molecules and structures of meso- to macroscopic sizes on ever shorter time-scales are presented. The book is written by some of the most eminent experimental and theoretical experts in the field. It covers the new groundbreaking research directions that were opened by the availability of new light sources such as fully controlled intense laser fields with durations down to a single oscillation cycle, short-wavelength laser-driven attosecond pulses and intense X-ray pulses from the upcoming free electron lasers. These light sources allowed the investigation of dynamics in atoms, molecules, clusters, on surfaces and very recently also in nanostructures and solids in new regimes of parameters which, in turn, led to the identification of completely new dynamics and methods for controlling it. Example topics covered by this book include the study of ultrafast processes in large molecules using attosecond pulses, control of ultrafast electron dynamics in solids with shaped femtosecond laser pulses, light-driven ultrafast plasmonic processes on surfaces and in nanostructures as well as research on atomic and molecular systems under intense X-ray radiation. This book is equally helpful for people who would like to step into this field (e.g. young researchers), for whom it provides a broad introduction, as well as for already experienced researchers who may enjoy the exhaustive discussion that covers the research on essentially all currently studied objects and with all available ultrafast pulse sources.
Book Synopsis Dissociation Dynamics of Molecular Ions in Ultrafast, Intense Laser Fields by : Bethany Jochim
Download or read book Dissociation Dynamics of Molecular Ions in Ultrafast, Intense Laser Fields written by Bethany Jochim and published by . This book was released on 2019 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: Out of the many tools for probing molecular dynamics, intense, ultrafast laser pulses are particularly well suited for this purpose. First, these pulses have temporal durations shorter than the typical rotational and vibrational periods of molecules and therefore allow the observation of molecular dynamics on their native timescales. Further, the broad bandwidth and high peak intensities of these laser pulses can result in the excitation of many transition pathways that may interfere and enable control of dynamics. The primary focus of this work is the ultrafast laser-induced dissociation of molecular ions. We generate these ions as "fast" beam targets and study their fragmentation using a coincidence three-dimensional (3D) momentum imaging technique, which allows the measurement of all nuclear fragments, including neutrals. This approach is employed to study laser-induced processes in a variety of molecules. The goal of these efforts is not to study specific molecules but rather to use them as testing grounds to deepen our knowledge of laser-induced molecular dynamics in general. For example, we find that permanent-dipole transitions, which are commonly overlooked in the interpretation of strong-field experiments, play a key role in laser-induced dissociation of metastable NO2+ ions. General consideration of these transitions in heteronuclear molecules is important in building our understanding towards more complex molecules. Speaking of more complex systems, we have also begun investigating the laser-induced dynamics of simple hydrocarbons. Our use of molecular ion beam targets gives us the unique ability to exercise control over the initial "configuration," i.e., geometry of these molecules. Utilizing C2H2^q ion beam targets (where q is the molecular ion charge state) prepared in various initial configurations, including acetylene (HCCH), vinylidene (H2CC), and cis/trans, we have determined that this property has an immense impact on the isomerization dynamics, a finding that we anticipate will lead to future work towards deeper understanding. More broadly, this approach of probing molecules in different initial configurations offers a unique perspective that could be complementary to mainstream methods-not just in the case of C2H2 but other chemical systems as well. We also describe some improvements to the 3D momentum imaging methods that facilitate the study of molecular dynamics. One of these developments is a method to distinguish and evaluate the momenta of neutral-neutral channels resulting from the fragmentation of negative ion beams. The second is a technique for imaging the breakup of long-lived metastable molecules decaying in flight to the detector and retrieving the lifetime(s) of the populated states. Our collaborative efforts in adaptive closed-loop control are also discussed. Here, an evolutionary learning algorithm supplied with experimental feedback obtains optimally-shaped ultrashort laser pulses for driving targeted molecular dynamics. While the complexity of the shaped pulses can make interpretation challenging, the combination of these efforts with basic experiments like those we perform using ion beams can help. In closing, the work presented in this thesis extends from diatomic to polyatomic molecules, following the natural progression of building from simpler to more complex systems. We believe that the results of these efforts aid in the advancement of understanding strong-field molecular dynamics and will stimulate future research endeavors along these directions.
Book Synopsis Ultrashort Laser Pulses by : Wolfgang Kaiser
Download or read book Ultrashort Laser Pulses written by Wolfgang Kaiser and published by Springer Science & Business Media. This book was released on 2006-11-14 with total page 500 pages. Available in PDF, EPUB and Kindle. Book excerpt: This second edition in paperback provides an up-to-date review of the state of the art in different generation processes for ultrashort laser pulses. Inaddition, extensive applications in a wide range of fields - in physics,engineering, chemistry, and biology - are discussed: Eight chapters dealwith the following topics: -the generation of picosecond and femtosecond laser pulses -nonlinear wave interactions - new investigations in solid-state physics - recent progress in optoelectronics - advances in coherent material excitations - ultrafast vibrational lifetimes and energy redistribution in liquids - new observations of chemical reactions in the liquid state - the primary processes of important biological systems The book is essential reading for scientists and engineers who want to know what is going on in this rapidly advancing field. It should also interest graduate students and others who seek an introduction to laserpulses.
Book Synopsis Molecular-frame Measurements of Light-induced Processes Using Rotational Coherences Driven by Ultrafast Laser Pulses by : Huynh Van Sa Lam
Download or read book Molecular-frame Measurements of Light-induced Processes Using Rotational Coherences Driven by Ultrafast Laser Pulses written by Huynh Van Sa Lam and published by . This book was released on 2021 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: One of the main goals of ultrafast atomic, molecular, and optical physics is to monitor and control chemical reactions in real time. Ultrashort laser pulses (time scales in picoseconds or shorter) provide sufficiently high spatio-temporal resolution to study the reaction dynamics. Together with the development of shorter pulses, studies of these reactions in three-dimensional (3D) space are also crucial since the 3D structures determine the physical and chemical properties of molecules. For example, stereoisomers, such as chiral molecules, have the same molecular formula but can behave very differently in reactions with other stereoisomers or optical pulses because of the different orientations of their atoms in space. However, in a gas-phase experiment, the orientation-dependent information is usually lost after averaging over a randomly distributed molecular sample. Many different methods have been investigated to solve this important problem. In 2014, Makhija et al. demonstrated that the angle-dependent strong-field ionization of ethylene (C2H4), an asymmetric top molecule, can be retrieved from a time-resolved measurement of the yield of the cation. In this pump-probe experiment, the pump aligns and the probe ionizes the molecules, and the ion yield is measured as a function of pump-probe delay. The angle dependence is retrieved from fitting to this delay-dependent ion yield. This time-domain approach, called Orientation Resolution through Rotational Coherence Spectroscopy (ORRCS), has many advantages that can be exploited in other applications. The main theme of this work is the further development of ORRCS for extracting orientation-resolved information of different processes from rotational wave packet dynamics. The first goal of this dissertation is to systematically investigate and develop the ORRCS retrieval algorithm, since the retrieval of the angle dependence is sensitive to many parameters. We perform a series of experiments and statistical analyses to evaluate different types of errors, determine the appropriate size of the model, and check the consistency of the retrieval. Specifically, we look at the angle-dependent strong-field ionization of carbon dioxide (CO2, a linear molecule) and sulfur dioxide (SO2, an asymmetric top molecule). Strong-field ionization of CO2 has been discussed extensively in the literature because there were significant discrepancies between different experiments and theories, while SO2 has been used extensively in other experiments. The second goal of this dissertation is to expand the time-domain approach to momentum measurements. With this new development, we present two applications of ORRCS to the dissociation and photoionization of molecules. In the dissociation of molecules, the axial recoil approximation is often used without validation. We show that this approximation can be tested by measuring the momentum distributions of the fragment ions as a function of pump-probe delay. In particular, we examine the dissociation of CO2 and N2 with 800 nm and 262 nm laser pulses, respectively. In each case, we determine how the likelihood of dissociation depends on the initial orientation of the molecule and the effect of the laser field on the momentum distribution of the fragment ions. With a similar framework but different interpretation, we show that substantial information about molecular-frame photoelectron angular distributions can be obtained using rotational wave packets. We retrieve the alignment dependence of photoelectron angular distributions from N2, CO2, and C2H4 in the few-photon ionization regime. We also compare few-photon ionization with single-photon ionization and strong-field ionization to enrich our knowledge in this regime, which is not very well understood. We believe that the time-domain approach discussed in this work is useful in many areas of ultrafast physics and chemistry. With the rapid development of high-repetition-rate light sources in recent years, we expect that many measurements, including those using x-ray free-electron lasers and ultrafast electron beams, will have the ability to apply our method and gain valuable insights into molecular structures and dynamics in the near future.
Book Synopsis Progress in Ultrafast Intense Laser Science II by : See Leang Chin
Download or read book Progress in Ultrafast Intense Laser Science II written by See Leang Chin and published by Springer Science & Business Media. This book was released on 2007-06-10 with total page 378 pages. Available in PDF, EPUB and Kindle. Book excerpt: This book series addresses a newly emerging interdisciplinary research field, Ultrafast Intense Laser Science, spanning atomic and molecular physics, molecular science, and optical science. Highlights of this second volume include Coulomb explosion and fragmentation of molecules, control of chemical dynamics, high-order harmonic generation, propagation and filamentation, and laser-plasma interaction. All chapters are authored by foremost experts in their fields.
Book Synopsis Progress in Ultrafast Intense Laser Science by : Antonio Giulietti
Download or read book Progress in Ultrafast Intense Laser Science written by Antonio Giulietti and published by Springer Science & Business Media. This book was released on 2010-05-21 with total page 223 pages. Available in PDF, EPUB and Kindle. Book excerpt: This volume covers a range of topics from this interdisciplinary field, focusing on coherent responses of gaseous and condensed matter to ultrashort intense laser pulses, propagation of intense laser pulses, and laser-plasma interaction and its applications.
Download or read book The Chemical Bond written by Ahmed Zewail and published by Elsevier. This book was released on 1992-05-14 with total page 333 pages. Available in PDF, EPUB and Kindle. Book excerpt: This inspired book by some of the most influential scientists of our time--including six Nobel laureates--chronicles our emerging understanding of the chemical bond through the last nine decades and into the future. From Pauling's early structural work using x-ray and electron diffraction to Zewail's femtosecond lasers that probe molecular dynamics in real time; from Crick's molecular biology to Rich's molecular recognition, this book explores a rich tradition of scientific heritage and accomplishment. The perspectives given by Pauling, Perutz, Rich, Crick, Porter, Polanyi, Herschbach, Zewail, and Bernstein celebrate major scientific achievements in chemistry and biology with the chemical bond playing a fundamental role. In a unique presentation that also provides some lively insights into the very nature of scientific thought and discovery, The Chemical Bond: Structure and Dynamics will be of general interest to scientists, science historians, and the scientifically inclined populous.
Book Synopsis Molecular Dynamics in Diatomic Molecules with One- and Two-color Ultrafast Laser Pulses by : Vincent Tagliamonti
Download or read book Molecular Dynamics in Diatomic Molecules with One- and Two-color Ultrafast Laser Pulses written by Vincent Tagliamonti and published by . This book was released on 2014 with total page 182 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Understanding Photo-initiated Dynamics Using Programmable Shaped Pulses by : Muath Nairat
Download or read book Understanding Photo-initiated Dynamics Using Programmable Shaped Pulses written by Muath Nairat and published by . This book was released on 2018 with total page 184 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Femtochemistry and Femtobiology by : Abderrazzak Douhal
Download or read book Femtochemistry and Femtobiology written by Abderrazzak Douhal and published by World Scientific. This book was released on 2002 with total page 854 pages. Available in PDF, EPUB and Kindle. Book excerpt: This book contains important contributions from top international scientists on the-state-of-the-art of femtochemistry and femtobiology at the beginning of the new millennium. It consists of reviews and papers on ultrafast dynamics in molecular science.The coverage of topics highlights several important features of molecular science from the viewpoint of structure (space domain) and dynamics (time domain). First of all, the book presents the latest developments, such as experimental techniques for understanding ultrafast processes in gas, condensed and complex systems, including biological molecules, surfaces and nanostructures. At the same time it stresses the different ways to control the rates and pathways of reactive events in chemistry and biology. Particular emphasis is given to biological processes as an area where femtodynamics is becoming very useful for resolving the structural dynamics from techniques such as electron diffraction, and X-ray and IR spectroscopy. Finally, the latest developments in quantum control (in both theory and experiment) and the experimental pulse-shaping techniques are described.
Book Synopsis Dissertation Abstracts International by :
Download or read book Dissertation Abstracts International written by and published by . This book was released on 2003 with total page 812 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Advances in Multi-photon Processes and Spectroscopy by : Y. Fujimura
Download or read book Advances in Multi-photon Processes and Spectroscopy written by Y. Fujimura and published by World Scientific. This book was released on 2001 with total page 356 pages. Available in PDF, EPUB and Kindle. Book excerpt: In view of the rapid growth in both experimental and theoretical studies of multi-photon processes and multi-photon spectroscopy of atoms, ions and molecules in chemistry, physics, biology, materials science, etc., it is desirable to publish an advanced series of volumes containing review papers that can be read not only by active researchers in these areas, but also by those who are not experts but who intend to enter the field. The present series aims to serve this purpose. Each review article is written in a self-contained manner by the expert(s) in the area, so that the reader can grasp the knowledge without too much preparation.
Book Synopsis Theory of Laser-Pulse-Induced Molecular Dynamics: Gas-Phase Molecular Collisions and Adbond Dynamics by : Hai-Woong Lee
Download or read book Theory of Laser-Pulse-Induced Molecular Dynamics: Gas-Phase Molecular Collisions and Adbond Dynamics written by Hai-Woong Lee and published by . This book was released on 1987 with total page 16 pages. Available in PDF, EPUB and Kindle. Book excerpt: A semiclassical study presented here indicates that a sufficiently short and intense pulse can be much more effective in inducing a collisional radiative transition than cw radiation or a long pulse, although the intensity must not be too high because the Rabi oscillation can bring down the probability. For the situation of a molecule physisorbed on a crystalline surface and irradiated by a laser, a master equation approach, used to describe the time evolution of the population of the vibrational adbond levels, shows that for high intensities laser-induced vibrational excitation is the same for pulsed and cw lasers. Keywords: Molecular dynamics, Laser induced, Short pulses, Molecular collisions, Electronic transitions, Desorption.
Book Synopsis Controlling and Probing Atoms and Molecules with Ultrafast Laser Pulses by : Corneliu Manescu
Download or read book Controlling and Probing Atoms and Molecules with Ultrafast Laser Pulses written by Corneliu Manescu and published by . This book was released on 2004 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: The oscillations observed in the downhill ionization spectra are explained in this model by the interference of two classical trajectories leading to the same final state. The dependence of the ionization process on the length of the pulse is investigated. For downhill states, the results obtained by full-quantum calculations are explained successfully based on a "two interfering paths" theory. Finally, we show that the 1D model is not applicable in the case of the uphill states due to intrinsic 2D dynamics in these states. Multiple ionization trajectories with random phases wash out the oscillatory interference pattern.
