Attosecond Transient Absorption Spectroscopy of Atoms and Molecules

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ISBN 13 :
Total Pages : 150 pages
Book Rating : 4.:/5 (959 download)

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Book Synopsis Attosecond Transient Absorption Spectroscopy of Atoms and Molecules by : Yan Cheng

Download or read book Attosecond Transient Absorption Spectroscopy of Atoms and Molecules written by Yan Cheng and published by . This book was released on 2015 with total page 150 pages. Available in PDF, EPUB and Kindle. Book excerpt: One of the most fundamental goals of attosecond science is to observe and to control the dynamic evolutions of electrons in matter. The attosecond transient absorption spectroscopy is a powerful tool to utilize attosecond pulse to measure electron dynamics in quantum systems directly. In this work, isolated single attosecond pulses are used to probe electron dynamics in atoms and to study dynamics in hydrogen molecules using the attosecond transient absorption spectroscopy technique. The target atom/molecule is first pumped to excited states and then probed by a subsequent attosecond extreme ultraviolet (XUV) pulse or by a near infrared (NIR) laser pulse. By measuring the absorbed attosecond XUV pulse spectrum, the ultrafast electron correlation dynamics can be studied in real time. The quantum processes that can be studied using the attosecond transient absorption spectroscopy include the AC stark shift, multi-photon absorption, intermediate states of atoms, autoionizing states, and transitions of vibrational states in molecules. In all experiments, the absorption changes as a function of the time delay between the attosecond XUV probe pulse and the dressing NIR laser pulse, on a time scale of sub-cycle laser period, which reveals attosecond electron dynamics. These experiments demonstrate that the attosecond transient absorption spectroscopy can be performed to study and control electronic and nuclear dynamics in quantum systems with high temporal and spectral resolution, and it opens door for the study of electron dynamics in large molecules and other more complex systems.

Exploring Ultrafast Quantum Dynamics of Electrons by Attosecond Transient Absorption

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ISBN 13 :
Total Pages : pages
Book Rating : 4.:/5 (1 download)

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Book Synopsis Exploring Ultrafast Quantum Dynamics of Electrons by Attosecond Transient Absorption by : Chen-Ting Liao

Download or read book Exploring Ultrafast Quantum Dynamics of Electrons by Attosecond Transient Absorption written by Chen-Ting Liao and published by . This book was released on 2017 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: Quantum mechanical motion of electrons in atoms and molecules is at the heart of many photophysical and photochemical processes. As the natural timescale of electron dynamics is in the range of femtoseconds or shorter, ultrashort pulses are required to study such phenomena. The ultrashort pulse light-matter interaction at high intensity regime can however dramatically alter the atomic and molecular structures. Our current understanding of such transient electronic modification is far from complete, especially when complicated light-induced couplings are involved. In this dissertation, we investigated how a femtosecond strong-field pulse can control or modify the evolution of atomic or molecular polarization, representing electric dipole excitation in various systems. Extreme ultraviolet (XUV) attosecond pulse trains are used to coherently prepare superposition of excited states in various atomic and molecular systems. A subsequent phase-locked infrared (IR) femtosecond pulse is applied to perturb the dipoles, and transient changes in the transmitted XUV spectra are measured. This scheme is termed as XUV attosecond transient absorption spectroscopy. In the first study, we applied this technique to study the modification of Rydberg states in dilute helium gas. We observed several transient changes to the atomic structure, including the ac Stark shift, laser-induced quantum phase, laser-induced continuum structure, and quantum path interference. When the experiments were extended to the study of a dense helium gas sample, new spectral features in the absorption spectra emerged which cannot be explained by linear optical response models. We found that these absorption features arise from the interplay between the XUV resonant pulse propagation and the IR-imposed phase shift. A unified physical model was also developed to account for various scenarios. Extending our work to argon atoms, we studied how an external infrared field can be used to impulsively control different photo-excitation pathways and the transient absorption lineshape of an otherwise isolated autoionizing state. It is found that by controlling the field polarization of the IR pulse, we can modify the transient absorption line shape from Fano-like to Lorentzian-like profiles. Unlike atoms, in our study of autoionizing states of the oxygen molecule, we observed both positive and negative optical density changes for states with different electronic symmetries. The predictions of two distinct and simplified dipole perturbation models were compared against both the experimental results and a full theoretical calculation in order to understand the origin of the sign of absorption change. We relate this symmetry-dependent sign change to the Fano parameters of static photoabsorption. The same approach was applied to study molecular nitrogen, in which we observed the decay dynamics of IR perturbed doubly-excited Rydberg states with many vibrational progressions. In addition, we also conducted experiments to investigate Rydberg state dynamics of other molecular systems such as carbon dioxide. In summary, we experimentally explored the ephemeral light-induced phenomena associated with excited states of atoms and molecules. These studies provide real-time information on ultrafast electronic processes and provide strategies for direct time-domain control of the light-matter interaction.

Transient Absorption Spectroscopy with Isolated Attosecond Pulses

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ISBN 13 :
Total Pages : 230 pages
Book Rating : 4.:/5 (858 download)

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Book Synopsis Transient Absorption Spectroscopy with Isolated Attosecond Pulses by : Marie Justine Bell

Download or read book Transient Absorption Spectroscopy with Isolated Attosecond Pulses written by Marie Justine Bell and published by . This book was released on 2013 with total page 230 pages. Available in PDF, EPUB and Kindle. Book excerpt: Ultrashort pulses with durations less than one femtosecond advance understanding of chemistry and physics by facilitating time-resolved measurements on the timescale of electronic motion. A very pragmatic type of experiment incorporating isolated attosecond (10 & minus18 s) pulses is transient absorption measurements that utilize the broad bandwidth of attosecond pulses. In these measurements the dispersed spectrum of the isolated attosecond pulse is recorded after the attosecond pulse and a time-delayed optical pulse pass through an experimental target of interest. This thesis focuses on the development of an attosecond transient absorption spectrometer with the ultimate goal of using the spectrometer to measure atomic and molecular dynamics. Two experimental studies are presented: one focusing on the behavior of helium atoms bathed in a strong near-infrared optical field, and one focusing on measurement of the lifetimes of autoionizing states in xenon. Measurement of the absorption spectrum of atomic helium bathed in a near-infrared (780 nm) field exhibits new features when the attosecond pulse and the optical pulse are overlapped in the gas target. The features near the 1s2p transition at 21.21 eV are identified as intermediates in two-photon transitions to reach nearby s and d helium excited states that are inaccessible via one photon transitions from the 1s2 ground state of He. Initial measurements identified three intermediate states, and further experiments investigated the behavior of the states as the near infrared field intensity is increased. Attosecond time-resolved measurement of ultrashort lifetimes of autoionizing states is also investigated. The 5s5p66p and 5s5p67p autoionizing states of xenon are visible in the extreme-ultraviolet absorption spectrum of Xe as Fano resonances. The Fano resonances are suppressed by a time-delayed near-infrared pulse and recover with a time-constant that is related to the lifetime of the state. The studies here identified key parameters for time-resolved measurements of the autoionization lifetime, including spectral resolution of the attosecond transient absorption spectrometer.

Attosecond Transient Absorption Spectroscopy

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Publisher : CRC Press
ISBN 13 : 9781498736749
Total Pages : pages
Book Rating : 4.7/5 (367 download)

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Book Synopsis Attosecond Transient Absorption Spectroscopy by : Zenghu Chang

Download or read book Attosecond Transient Absorption Spectroscopy written by Zenghu Chang and published by CRC Press. This book was released on 2026-06-30 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: This book gives a complete picture of the science and application of attosecond transient absorption spectroscopy (ATAS). It explains how this all-optical technique allows substantial improvements in both the signal-to-noise ratio and the energy resolution when compared with photoelectron experiments. The authors explain why ATAS is so attractive for the study of electron dynamics in photochemical processes, dynamics in field-ionized atoms and bulk solids, as well as narrow-linewidth core-excited and doubly-excited states of atoms.

Attosecond Transient Absorption Spectroscopy in Atomic Species

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ISBN 13 :
Total Pages : pages
Book Rating : 4.:/5 (16 download)

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Book Synopsis Attosecond Transient Absorption Spectroscopy in Atomic Species by : Emma Simpson

Download or read book Attosecond Transient Absorption Spectroscopy in Atomic Species written by Emma Simpson and published by . This book was released on 2016 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt:

Molecular Spectroscopy and Quantum Dynamics

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Publisher : Elsevier
ISBN 13 : 0128172355
Total Pages : 376 pages
Book Rating : 4.1/5 (281 download)

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Book Synopsis Molecular Spectroscopy and Quantum Dynamics by : Roberto Marquardt

Download or read book Molecular Spectroscopy and Quantum Dynamics written by Roberto Marquardt and published by Elsevier. This book was released on 2020-09-18 with total page 376 pages. Available in PDF, EPUB and Kindle. Book excerpt: Molecular Spectroscopy and Quantum Dynamics, an exciting new work edited by Professors Martin Quack and Roberto Marquardt, contains comprehensive information on the current state-of-the-art experimental and theoretical methods and techniques used to unravel ultra-fast phenomena in atoms, molecules and condensed matter, along with future perspectives on the field. Contains new insights into the quantum dynamics and spectroscopy of electronic and nuclear motion Presents the most recent developments in the detection and interpretation of ultra-fast phenomena Includes a discussion of the importance of these phenomena for the understanding of chemical reaction dynamics and kinetics in relation to molecular spectra and structure

Attosecond Molecular Dynamics

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Publisher : Royal Society of Chemistry
ISBN 13 : 1782629955
Total Pages : 512 pages
Book Rating : 4.7/5 (826 download)

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Book Synopsis Attosecond Molecular Dynamics by : Marc J J Vrakking

Download or read book Attosecond Molecular Dynamics written by Marc J J Vrakking and published by Royal Society of Chemistry. This book was released on 2018-08-31 with total page 512 pages. Available in PDF, EPUB and Kindle. Book excerpt: Attosecond science is a new and rapidly developing research area in which molecular dynamics are studied at the timescale of a few attoseconds. Within the past decade, attosecond pump-probe spectroscopy has emerged as a powerful experimental technique that permits electron dynamics to be followed on their natural timescales. With the development of this technology, physical chemists have been able to observe and control molecular dynamics on attosecond timescales. From these observations it has been suggested that attosecond to few-femtosecond timescale charge migration may induce what has been called "post-Born-Oppenheimer dynamics", where the nuclei respond to rapidly time-dependent force fields resulting from transient localization of the electrons. These real-time observations have spurred exciting new advances in the theoretical work to both explain and predict these novel dynamics. This book presents an overview of current theoretical work relevant to attosecond science written by theoreticians who are presently at the forefront of its development. It is a valuable reference work for anyone working in the field of attosecond science as well as those studying the subject.

Advances in Atomic, Molecular, and Optical Physics

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Publisher : Academic Press
ISBN 13 : 012385508X
Total Pages : 562 pages
Book Rating : 4.1/5 (238 download)

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Book Synopsis Advances in Atomic, Molecular, and Optical Physics by : Paul R. Berman

Download or read book Advances in Atomic, Molecular, and Optical Physics written by Paul R. Berman and published by Academic Press. This book was released on 2011-10-03 with total page 562 pages. Available in PDF, EPUB and Kindle. Book excerpt: Advances in Atomic, Molecular, and Optical Physics publishes reviews of recent developments in a field which is in a state of rapid growth, as new experimental and theoretical techniques are used on many old and new problems. Topics covered include related applied areas, such as atmospheric science, astrophysics, surface physics and laser physics. Articles are written by distinguished experts, and contain both relevant review material and detailed descriptions of important recent developments. International experts Comprehensive articles New developments

Attosecond Transient Absorption of Solid-State and Phase-Change Materials

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ISBN 13 :
Total Pages : 109 pages
Book Rating : 4.:/5 (12 download)

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Book Synopsis Attosecond Transient Absorption of Solid-State and Phase-Change Materials by : Marieke Faye Jager

Download or read book Attosecond Transient Absorption of Solid-State and Phase-Change Materials written by Marieke Faye Jager and published by . This book was released on 2017 with total page 109 pages. Available in PDF, EPUB and Kindle. Book excerpt: Attosecond science, utilizing short bursts of extreme ultraviolet light, has opened up a fascinating new field of ultafast light-matter interactions, where dynamics in atomic, molecular, and solid state systems can now be followed on the timescale of electron motion. In this dissertation, applications of attosecond pulses toward performing transient absorption spectroscopy experiments on complex electron-correlation-driven processes in material systems are described. In the first chapter, a brief overview of ultrafast spectroscopy, attosecond pulse production, and light-matter interaction in the extreme ultraviolet is provided, which offers the necessary breadth and background for the detailed case study that follows, on the insulator-to-metal phase transition in vanadium dioxide. The origin of the bandgap in vanadium dioxide, which is not predicted to exist under conventional single-particle band theories, has been explained as the result of either electron correlation or structural distortion. The goal of the experiments presented herein is to use transient absorption spectroscopy with attosecond pulses to characterize the timescale of this process and gain a mechanistic understanding of how it occurs. Because vanadium dioxide is heat sensitive, an apparatus had to be specifically tailored to this type of experiments, and it is described in the second chapter. The results and analysis, including extreme ultraviolet static and time-resolved measurements on both the insulating and metallic phases, are described in the third chapter. The second half of this dissertation describes the design and construction of a new vacuum endstation to perform attosecond-pump attosecond-probe measurements, which was constructed and tested at Berkeley and installed at a high power attosecond beamline at the University of Central Florida. Ray tracing simulation and design considerations for the optical layout are described in the fourth chapter, and design of the vacuum endstation, diagnostics, and preliminary experiments and testing can be found in the fifth chapter.

Ultrafast Quantum Control of Atoms and Molecules : a Density Matrix Approach

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ISBN 13 :
Total Pages : 158 pages
Book Rating : 4.:/5 (112 download)

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Book Synopsis Ultrafast Quantum Control of Atoms and Molecules : a Density Matrix Approach by : Iduabo John Afa

Download or read book Ultrafast Quantum Control of Atoms and Molecules : a Density Matrix Approach written by Iduabo John Afa and published by . This book was released on 2018 with total page 158 pages. Available in PDF, EPUB and Kindle. Book excerpt: Control is important for transferring theoretical scientific knowledge into practical technology for applications in numerous fields. This is why coherent control study is significant on every timescale to have a complete understanding of dynamic processes that occur on the electron, atomic and molecular levels. As a result, numerous schemes have been proposed to carry out effective quantum control of diverse systems and study the dynamics of these systems based on their natural timescales from the picoseconds (10-12 s), femtosecond (10-15 s) to attosecond (10-18 s) regimes. The goals of these various studies depend on the desired application, for instance in Photochemistry a long standing objective is achieving selective population transfer from an initial state to a desired target state with little or no diminution in the energy transferred. In quantum computation, a central issue is the excitation of unoccupied Rydberg states with numerous proposals for its use in the design and implementation of robust fast quantum gates. Also, since the advent of the generation of attosecond XUV pulses, doors have been opened for achieving control of atomic-scale electron dynamics and observing them in real-time. This thesis explores the modelling of dynamical light-matter interaction processes, like effective population inversion and generation of vibrational coherences in atoms and molecules, on their fundamental timescales using the density matrix (DM) theory under and beyond the rotating wave approximation (RWA). The thesis begins by introducing the concept of coherent control of simple quantum systems based on the DM formalism and expands the application to a more complex Oxazine system. Multiphoton p-pulse scheme is demonstrated for the control of population transfer in multilevel systems, for example with a trichromatic p-pulse having a set of areas v3 p, 2p and v3 p, complete population transfer in a four level system can be achieved. The aforementioned scheme is used to achieve effective control of low-lying Rydberg states in rubidium atoms, demonstrating how the effective control can be crucially affected by numerous physical processes. One main advantage of the density matrix approach over other theoretical approaches is that it allows the possibility of easily computing relaxation terms and other physical parameters critical to successful coherent control. The DM formalism is shown to be successful in properly describing the enhancement effects in atoms and complex molecular systems. It is robust in coherent control and quantum control spectroscopy (QCS) schemes and is extendable to numerous systems and geometric configurations. In the last part of the thesis, experiments on laser dressing processes in attosecond transient absorption spectroscopy are compared to numerical simulations using the DM analysis beyond the RWA. The research in this thesis opens a pathway to numerous studies using the DM formalism for applications in diverse fields of femtochemistry, attophysics, high precision spectroscopy and quantum information processing.

Attosecond Optical Probe and Control of Atomic Autoionizing States

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ISBN 13 :
Total Pages : 0 pages
Book Rating : 4.:/5 (134 download)

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Book Synopsis Attosecond Optical Probe and Control of Atomic Autoionizing States by : Coleman Cariker

Download or read book Attosecond Optical Probe and Control of Atomic Autoionizing States written by Coleman Cariker and published by . This book was released on 2022 with total page 0 pages. Available in PDF, EPUB and Kindle. Book excerpt: The last two decades have witnessed the emergence of attosecond science, a new discipline that leverages light pulses with duration at the same characteristic time scale of electronic motion in atoms, molecules, and condensed matter. Attosecond spectroscopy has proven a particularly useful tool to monitor and control the evolution of transiently bound electronic states. These states, also known as autoionizing states, play a fundamental role in the ionization and charge transfer processes in matter. This thesis is a theoretical study on the role of such autoionizing states in the ionization of polyelectronic atoms by ultrashort pulses, which has been instrumental to four joint experimental and theoretical studies: i) with the group of Zenghu Chang, at UCF, concerning the core ionization of the argon atom at the L2,3 edge; ii) with the group of Arvinder Sandhu, at the University of Arizona, on the control of the lifetime of autionizing states in the argon atom, as well as iii) on the measurement of the lifetime of argon’s dark autoionizing states via non-colinear fourwave mixing; iv) with the group of Louis DiMauro, at the Ohio State University, on the verification of the Kramers-Krönig relations in the ionization of laser-dressed argon. We have adopted several complementary theoretical approaches. In solving the time-dependent Schroedinger equation, we introduced a novel "essential states" procedure, which drastically reduces the cost of ab initio calculations. We developed a model that shows how destructive interference between autoionization and radiative ionization channels can stabilize transient states, explaining experimental observations and providing the first evidence for a phenomenon first predicted four decades ago. We have devised the formalism needed to extrapolate, from the single-atom response, the off-axis dipolar emission from an extended sample, and implemented it to theoretically reproduce, for the first time and with semi-quantitative accuracy, four-wave mixing experimental spectra in argon. Lastly, we developed a model for propagating light through a laser-dressed sample, demonstrating its use by predicting the pressure dependence of transient absorption spectra in model systems.

Advances in Atomic, Molecular, and Optical Physics

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Publisher : Academic Press
ISBN 13 : 0123855098
Total Pages : 562 pages
Book Rating : 4.1/5 (238 download)

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Book Synopsis Advances in Atomic, Molecular, and Optical Physics by :

Download or read book Advances in Atomic, Molecular, and Optical Physics written by and published by Academic Press. This book was released on 2011-09-29 with total page 562 pages. Available in PDF, EPUB and Kindle. Book excerpt: Advances in Atomic, Molecular, and Optical Physics publishes reviews of recent developments in a field which is in a state of rapid growth, as new experimental and theoretical techniques are used on many old and new problems. Topics covered include related applied areas, such as atmospheric science, astrophysics, surface physics and laser physics. Articles are written by distinguished experts, and contain both relevant review material and detailed descriptions of important recent developments. International experts Comprehensive articles New developments

Advances in Atomic, Molecular, and Optical Physics

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Publisher : Academic Press
ISBN 13 : 0128209887
Total Pages : 316 pages
Book Rating : 4.1/5 (282 download)

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Book Synopsis Advances in Atomic, Molecular, and Optical Physics by : Susanne Yelin

Download or read book Advances in Atomic, Molecular, and Optical Physics written by Susanne Yelin and published by Academic Press. This book was released on 2020-06-17 with total page 316 pages. Available in PDF, EPUB and Kindle. Book excerpt: Advances in Atomic, Molecular, and Optical Physics, Volume 69, the latest release in this ongoing series, provides a comprehensive compilation of recent developments in a field that is in a state of rapid growth, as new experimental and theoretical techniques are used on many problems, both old and new. Topics covered in this new release include Strong-field ion spectroscopy, Configurable microscopic optical potentials, Polaritons, Rydberg excitation of trapped cold ions - a new platform for quantum technologies, High intensity QED, Recollision imaging, and more. Presents the work of international experts in the field Contains comprehensive articles that compile recent developments in a field that is experiencing rapid growth, with new experimental and theoretical techniques emerging Ideal for users interested in optics, excitons, plasmas and thermodynamics Covers atmospheric science, astrophysics, and surface and laser physics, amongst other topics

Attosecond Molecular Dynamics

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Publisher : Royal Society of Chemistry
ISBN 13 : 1788015134
Total Pages : 512 pages
Book Rating : 4.7/5 (88 download)

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Book Synopsis Attosecond Molecular Dynamics by : Marc J J Vrakking

Download or read book Attosecond Molecular Dynamics written by Marc J J Vrakking and published by Royal Society of Chemistry. This book was released on 2018-08-31 with total page 512 pages. Available in PDF, EPUB and Kindle. Book excerpt: Attosecond science is a new and rapidly developing research area in which molecular dynamics are studied at the timescale of a few attoseconds. Within the past decade, attosecond pump–probe spectroscopy has emerged as a powerful experimental technique that permits electron dynamics to be followed on their natural timescales. With the development of this technology, physical chemists have been able to observe and control molecular dynamics on attosecond timescales. From these observations it has been suggested that attosecond to few-femtosecond timescale charge migration may induce what has been called “post-Born-Oppenheimer dynamics”, where the nuclei respond to rapidly time-dependent force fields resulting from transient localization of the electrons. These real-time observations have spurred exciting new advances in the theoretical work to both explain and predict these novel dynamics. This book presents an overview of current theoretical work relevant to attosecond science written by theoreticians who are presently at the forefront of its development. It is a valuable reference work for anyone working in the field of attosecond science as well as those studying the subject.

Attosecond and Strong-Field Physics

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Publisher : Cambridge University Press
ISBN 13 : 1108187250
Total Pages : 419 pages
Book Rating : 4.1/5 (81 download)

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Book Synopsis Attosecond and Strong-Field Physics by : C. D. Lin

Download or read book Attosecond and Strong-Field Physics written by C. D. Lin and published by Cambridge University Press. This book was released on 2018-05-10 with total page 419 pages. Available in PDF, EPUB and Kindle. Book excerpt: Probing and controlling electrons and nuclei in matter at the attosecond timescale became possible with the generation of attosecond pulses by few-cycle intense lasers, and has revolutionized our understanding of atomic structure and molecular processes. This book provides an intuitive approach to this emerging field, utilizing simplified models to develop a clear understanding of how matter interacts with attosecond pulses of light. An introductory chapter outlines the structure of atoms and molecules and the properties of a focused laser beam. Detailed discussion of the fundamental theory of attosecond and strong-field physics follows, including the molecular tunnelling ionization model (MO-ADK theory), the quantitative rescattering (QRS) model, and the laser induced electronic diffraction (LIED) theory for probing the change of atomic configurations in a molecule. Highlighting the cutting-edge developments in attosecond and strong field physics, and identifying future opportunities and challenges, this self-contained text is invaluable for students and researchers in the field.

Attosecond Transient Absorption Spectroscopy

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Publisher :
ISBN 13 :
Total Pages : 0 pages
Book Rating : 4.:/5 (78 download)

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Book Synopsis Attosecond Transient Absorption Spectroscopy by : Adrian Wirth

Download or read book Attosecond Transient Absorption Spectroscopy written by Adrian Wirth and published by . This book was released on 2011 with total page 0 pages. Available in PDF, EPUB and Kindle. Book excerpt:

An Introduction to Atomic Absorption Spectroscopy

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Publisher :
ISBN 13 : 9780855017149
Total Pages : 138 pages
Book Rating : 4.0/5 (171 download)

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Book Synopsis An Introduction to Atomic Absorption Spectroscopy by : L. Ebdon

Download or read book An Introduction to Atomic Absorption Spectroscopy written by L. Ebdon and published by . This book was released on 1982 with total page 138 pages. Available in PDF, EPUB and Kindle. Book excerpt: