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Modeling Generation and Characterization of Attosecond Pulses

Modeling Generation and Characterization of Attosecond Pulses
Author: Siddharth Bhardwaj
Publisher:
Total Pages: 142
Release: 2014
Genre:
ISBN:

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Generation of high-order harmonics has emerged as a powerful technique for the generation of broadband coherent radiation in the EUV regime. This has lead to the development of table-top EUV sources that can produce attosecond pulses. These pulses can serve as a probe to resolve atomic attosecond dynamics and image atomic orbitals and molecular motion. Due to high spatial and temporal coherence, high-order harmonic radiation can also be used to seed free electron lasers, which allow the generation of high-intensity X-ray radiation that can be used for imaging biomolecules. Since the first observation of high-order harmonics, effort has been made to accurately model both the generation and the characterization of attosecond pulses. Work on the modeling of high harmonic generation can be divided into two parts: (a) description of the interaction between the JR pulse and atoms that leads to emission of attosecond pulses (the single atom response) and (b) modeling of the propagation of attosecond pulses by accounting for macroscopic phase matching effects. In this work, we will focus on the single atom response which can be calculated either by numerically solving the time dependent Schrodinger equation (TDSE) or through the semi-classical three step model (TSM). In Chapter 2, the theory of light-atom interaction will be reviewed with the focus on the calculation of the dipole trasition matrix element (DTME) in the strong field formalism. It will be shown that the choice of the basis states - Volkov states and Coulomb Volkov states - to describe electrons in the continuum is crucial to the accuracy of DTME calculation. In Chapter 3, the TSM will be derived from the Schrodinger equation by using the saddle point approximation. Through this derivation, the quantum mechanical laser-atom interaction is reduced to a semi-classical model comprising of ionization, propagation and recombination . The numerical scheme for solving the TDSE will be discussed. It will then be used to demonstrate the generation of isolated attosecond pulses from non-sinusoidal sub-cycle pulses. The results of ADK and non-adiabatic ionization models will be compared with that from numerical TDSE, and then used to calculate the harmonic spectra in the tunneling and multi-photon ionization regimes. The recombination step of the TSM, which plays a crucial role in determining the qualitative shape of the high-order harmonic spectrum, will be investigated in Chapter 4. A commonly observed feature of Argon's high-order harmonic spectrum is the presence of a minimum at around 50 eV called the Cooper minimum. The minimum in the high-order harmonic spectrum has been attributed to the minimum in the recombination amplitude. The recombination amplitude will be calculated - in the strong field formalism - using length and acceleration form for two choices of continuum electron wavefunction description (Volkov and Coulomb-Volkov). Attosecond pulse characterization techniques, which are an extension of the subpicosecond pulse characterization technique like FROG and SPIDER, rely on the photoionization process to transfer the amplitude and phase information of the attosecond pulse to the photoelectron spectrum. For accurate pulse characterization, it is crucial to model the photoionization process accurately. Since photoionization and recombination are reverse processes, the improvements in the calculation of the recombination amplitude in Chapter 4, can be used to improve the model function of the pulse retrieval algorithm. It will be shown that the proposed improvements are crucial for accurate characterization of low energy EUV pulses.


Generation and Characterization of Sub-70 Isolated Attosecond Pulses

Generation and Characterization of Sub-70 Isolated Attosecond Pulses
Author: Qi Zhang
Publisher:
Total Pages: 115
Release: 2014
Genre:
ISBN:

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Dynamics occurring on microscopic scales, such as electronic motion inside atoms and molecules, are governed by quantum mechanics. However, the Schrödinger equation is usually too complicated to solve analytically for systems other than the hydrogen atom. Even for some simple atoms such as helium, it still takes months to do a full numerical analysis. Therefore, practical problems are often solved only after simplification. The results are then compared with the experimental outcome in both the spectral and temporal domain. For accurate experimental comparison, temporal resolution on the attosecond scale is required. This had not been achieved until the first demonstration of the single attosecond pulse in 2001. After this breakthrough, "attophysics" immediately became a hot field in the physics and optics community. While the attosecond pulse has served as an irreplaceable tool in many fundamental research studies of ultrafast dynamics, the pulse generation process itself is an interesting topic in the ultrafast field. When an intense femtosecond laser is tightly focused on a gaseous target, electrons inside the neutral atoms are ripped away through tunneling ionization. Under certain circumstances, the electrons are able to reunite with the parent ions and release photon bursts lasting only tens to hundreds of attoseconds. This process repeats itself every half cycle of the driving pulse, generating a train of single attosecond pulses which lasts longer than one femtosecond. To achieve true temporal resolution on the attosecond time scale, single isolated attosecond pulses are required, meaning only one attosecond pulse can be produced per driving pulse.


Attosecond and XUV Physics

Attosecond and XUV Physics
Author: Thomas Schultz
Publisher: John Wiley & Sons
Total Pages: 624
Release: 2013-11-13
Genre: Science
ISBN: 3527677658

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This book provides fundamental knowledge in the fields of attosecond science and free electron lasers, based on the insight that the further development of both disciplines can greatly benefit from mutual exposure and interaction between the two communities. With respect to the interaction of high intensity lasers with matter, it covers ultrafast lasers, high-harmonic generation, attosecond pulse generation and characterization. Other chapters review strong-field physics, free electron lasers and experimental instrumentation. Written in an easy accessible style, the book is aimed at graduate and postgraduate students so as to support the scientific training of early stage researchers in this emerging field. Special emphasis is placed on the practical approach of building experiments, allowing young researchers to develop a wide range of scientific skills in order to accelerate the development of spectroscopic techniques and their implementation in scientific experiments. The editors are managers of a research network devoted to the education of young scientists, and this book idea is based on a summer school organized by the ATTOFEL network.


Generation and Characterization of Attosecond Pulses

Generation and Characterization of Attosecond Pulses
Author:
Publisher:
Total Pages:
Release: 2006
Genre:
ISBN:

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The research undertaken in this project has been directed toward the area of attoscience, in particular the problem of attosecond metrology. That is, the accurate determination of the electric field of attosecond XUV radiation. This outstanding problem has been identified as a critical technology for further development of the field, and our research adds to the area by providing the first method for characterization using the harmonic radiation itself as a tool. The technical effectiveness of this approach is very high, since it is vastly easier to detect XUV radiation directly than via the spectrum of photoelectrons liberated from atoms by it. This means that the experimental data rate can be much higher in principle using all-optical detection that electron detection, which will greatly aid the utility of harmonic XUV sources in attoscience applications. There are as yet no direct public benefits from this area of scientific research, though access to material structural dynamics on unprecedented brief timescales are expected to yield significant benefits for the future.


Attosecond Pulse Generation and Characterization

Attosecond Pulse Generation and Characterization
Author: Razvan Cristian Chirla
Publisher:
Total Pages: 208
Release: 2011
Genre:
ISBN:

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Abstract: One of the research goals in the DiMauro group is the application of attosecond light pulses for understanding electronic processes and for molecular imaging. The objective of this dissertation work was the construction of an attosecond beamline at The Ohio State University, and the implementation of the so-called Rabbitt technique.


Attosecond and Strong-Field Physics

Attosecond and Strong-Field Physics
Author: C. D. Lin
Publisher: Cambridge University Press
Total Pages: 420
Release: 2018-05-10
Genre: Science
ISBN: 1108195660

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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.


Fundamentals of Attosecond Optics

Fundamentals of Attosecond Optics
Author: Zenghu Chang
Publisher: CRC Press
Total Pages: 0
Release: 2011-02-16
Genre: Technology & Engineering
ISBN: 9781420089370

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Attosecond optical pulse generation, along with the related process of high-order harmonic generation, is redefining ultrafast physics and chemistry. A practical understanding of attosecond optics requires significant background information and foundational theory to make full use of these cutting-edge lasers and advance the technology toward the next generation of ultrafast lasers. Fundamentals of Attosecond Optics provides the first focused introduction to the field. The author presents the underlying concepts and techniques required to enter the field, as well as recent research advances that are driving the field forward. A stand-alone textbook for courses on attosecond optics and the interaction of matter with ultrafast, high-power lasers, the book begins with basic theory and gradually advances to more complex ideas. Using both semi-classical models and quantum mechanics theories, the author explains foundational concepts and mechanisms including femtosecond lasers, high-order harmonic generation, and the technological leap that inspired attosecond pulse generation. The book introduces techniques for generating attosecond train using the basis of high-order harmonics, followed by an explanation of gating methods for extracting single isolated pulses. Chapters examine the connection between attosecond pulses and high harmonic generation, the use of driving lasers as key tools in attosecond generation, the mechanism of chirped pulse amplification, and the generation of few-cycle pulses. The book looks at carrier-envelope phase stabilization and the theoretical foundations for single atom and dipole phase response. It discusses propagation effects, introducing several approaches for improving phase matching; attosecond pulse generation and characterization, covering attosecond pulse train and single isolated pulses; and several examples of experimental applications for attosecond pulses.


Generation of Short and Intense Attosecond Pulses

Generation of Short and Intense Attosecond Pulses
Author: Sabih ud Din Khan
Publisher:
Total Pages:
Release: 2012
Genre:
ISBN:

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Extremely broad bandwidth attosecond pulses (which can support 16as pulses) have been demonstrated in our lab based on spectral measurements, however, compensation of intrinsic chirp and their characterization has been a major bottleneck. In this work, we developed an attosecond streak camera using a multi-layer Mo/Si mirror (bandwidth can support ~100as pulses) and position sensitive time-of-flight detector, and the shortest measured pulse was 107.5as using DOG, which is close to the mirror bandwidth. We also developed a PCGPA based FROG-CRAB algorithm to characterize such short pulses, however, it uses the central momentum approximation and cannot be used for ultra-broad bandwidth pulses. To facilitate the characterization of such pulses, we developed PROOF using Fourier filtering and an evolutionary algorithm. We have demonstrated the characterization of pulses with a bandwidth corresponding to ~20as using synthetic data. We also for the first time demonstrated single attosecond pulses (SAP) generated using GDOG with a narrow gate width from a multi-cycle driving laser without CE-phase lock, which opens the possibility of scaling attosecond photon flux by extending the technique to peta-watt class lasers. Further, we generated intense attosecond pulse trains (APT) from laser ablated carbon plasmas and demonstrated ~9.5 times more intense pulses as compared to those from argon gas and for the first time demonstrated a broad continuum from a carbon plasma using DOG. Additionally, we demonstrated ~100 times enhancement in APT from gases by switching to 400 nm (blue) driving pulses instead of 800 nm (red) pulses. We measured the ellipticity dependence of high harmonics from blue pulses in argon, neon and helium, and developed a simple theoretical model to numerically calculate the ellipticity dependence with good agreement with experiments. Based on the ellipticity dependence, we proposed a new scheme of blue GDOG which we predict can be employed to extract intense SAP from an APT driven by blue laser pulses. We also demonstrated compression of long blue pulses into>240 [mu]J broad-bandwidth pulses using neon filled hollow core fiber, which is the highest reported pulse energy of short blue pulses. However, compression of phase using chirp mirrors is still a technical challenge.


Generation and Application of Attosecond Pulses

Generation and Application of Attosecond Pulses
Author: Zsolt Diveki
Publisher:
Total Pages: 0
Release: 2011
Genre:
ISBN:

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To capture electronic rearrangements inside a molecule or during chemical reactions, attosecond (as, 1 as =10-18 s) time resolution is needed. To create a light pulse with this duration, the central frequency has to be in the XUV range and cover several tens of eVs. Moreover, the frequency components have to be synchronized. The so called High Harmonic Generation (HHG) in gases well suits this task. During this process a high intensity laser pulse is focused in a gas jet, where its electric field bends the potential barrier of an atom allowing an electron wave packet (EWP) to tunnel ionize. Following the electric field of the laser the EWP gets accelerated, gaining a large kinetic energy that may be released as a high energy (XUV) photon in the event of a re-collision with the ionic core. These recolliding EWP probe the structure and dynamics of the core in a self-probing scheme: the EWP, that is emitted by the molecule at a certain time, probes itself later. More precisely, this ”self-probing” scheme gives access to the complex valued recombination dipole moment (RDM) of the molecule which is determined by both the nuclear and electronic structure. The recombination encodes these characteristics into the spectral amplitude, phase and polarization state of the harmonic radiation emitted by the dipole. Due to the coherent nature of HHG it is possible to measure all these three parameters. Moreover, it is in principle possible through a tomographic procedure to reconstruct the radiating orbital.The objective of my thesis was two-fold. By implementing advanced characterization techniques of the harmonic amplitude, phase and polarization we studied i) the electronic structure of N2 and laser induced multi-channel tunnel ionization. We presented the reconstruction of molecular orbitals and revealed the ionization channel dependent ultrafast nuclear vibration. We also studied ii) the reflectivity and dispersion of recently designed chirped XUV mirrors that can shape the temporal profile of attosecond pulses. With these mirrors we could control the spectral phase over 20 eV and compensate the GDD of the harmonics or introduce a TOD. We also proposed a novel attosecond pulse shaper.


Study on Generation of Attosecond Pulse with Polarization Gating

Study on Generation of Attosecond Pulse with Polarization Gating
Author: Shambhu Ghimire
Publisher:
Total Pages: 135
Release: 2007
Genre:
ISBN: 9781109971347

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Finally, in order to temporarily characterize the attosecond pulses we designed and built an "Attosecond Streak Camera". Most of such cameras to date are limited to measuring a 1 dimensional energy spectrum and have only a few degrees of acceptance angle. Our camera is capable of measuring 2d momentum of the photoelectrons with large acceptance angle, for example ∼65° at the photoelectron of energy ∼15 eV. Recently, we observed the sidebands in addition to the main peaks in their laser assisted XUV photoelectron spectrum. The single attosecond pulses, after being characterized with this high speed camera, can be used to explore the dynamics of electrons at the attosecond scale.