Coherent Two-dimensional Infrared Spectroscopy of Vibrational Excitons in Hydrogen-bonded Liquids PDF Download
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Languages : en
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PhD.
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PhD.
Author: Alexander Paarmann
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ISBN: 9780494676752
Category :
Languages : en
Pages : 0
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The structure and structural dynamics of hydrogen bonded liquids were studied experimentally and theoretically with coherent two-dimensional infrared (2DIR) spectroscopy. The resonant intermolecular interactions within the fully resonant hydrogen bond networks give access to spatial correlations in the dynamics of the liquid structures. New experimental and theoretical tools were developed that significantly reduced the technical challenges of these studies. A nanofluidic flow device was designed and manufactured providing sub-micron thin, actively stabilized liquid sample layers between similarly thin windows. A simulation protocol for nonlinear vibrational response calculations of disordered fluctuating vibrational excitons was developed that allowed for the first treatment of resonant intermolecular interactions in the 2DIR response of liquid water. The 2DIR spectrum of the O-H stretching vibration of pure liquid water was studied experimentally at different temperatures. At ambient conditions the loss of frequency correlations is extremely fast, and is attributed to very efficient modulations of the two-dimensional O-H stretching vibrational potential through librational motions in the hydrogen bond network. At temperatures near freezing, the librational motions are significantly reduced leading to a pronounced slowing down of spectral diffusion dynamics. Comparison with energy transfer time scales revealed the first direct proof of delocalization of the vibrational excitations. This work establishes a fundamentally new view of vibrations in liquid water by providing a spatial length scale of correlated hydrogen-bond motions. The linear and 2DIR response of the amide I mode in neat liquid formamide was found to be dominated by excitonic effects due to largely delocalized vibrational excitations. The spectral response and dynamics are very sensitive to the excitonic mode structure and infrared activity distributions, leading to a pronounced asymmetry of linear and 2DIR line shapes. This was attributed to structurally different species in the liquid characterized by their degree of medium range structural order. The response is dominated by energy transfer effects, sensitive to time-averaged medium range structural order, while being essentially insensitive to structural dynamics. This work is the first to recognize the importance of energy transfer contributions to the 2DIR response in a liquid, and provides additional proof of the well-structured character of liquid formamide.
Author: Michael D. Fayer
Publisher: CRC Press
ISBN: 1466510137
Category : Science
Languages : en
Pages : 491
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The advent of laser-based sources of ultrafast infrared pulses has extended the study of very fast molecular dynamics to the observation of processes manifested through their effects on the vibrations of molecules. In addition, non-linear infrared spectroscopic techniques make it possible to examine intra- and intermolecular interactions and how such interactions evolve on very fast time scales, but also in some instances on very slow time scales. Ultrafast Infrared Vibrational Spectroscopy is an advanced overview of the field of ultrafast infrared vibrational spectroscopy based on the scientific research of the leading figures in the field. The book discusses experimental and theoretical topics reflecting the latest accomplishments and understanding of ultrafast infrared vibrational spectroscopy. Each chapter provides background, details of methods, and explication of a topic of current research interest. Experimental and theoretical studies cover topics as diverse as the dynamics of water and the dynamics and structure of biological molecules. Methods covered include vibrational echo chemical exchange spectroscopy, IR-Raman spectroscopy, time resolved sum frequency generation, and 2D IR spectroscopy. Edited by a recognized leader in the field and with contributions from top researchers, including experimentalists and theoreticians, this book presents the latest research methods and results. It will serve as an excellent resource for those new to the field, experts in the field, and individuals who want to gain an understanding of particular methods and research topics.
Author: Bob D. Guenther
Publisher: Academic Press
ISBN: 0128149825
Category : Technology & Engineering
Languages : en
Pages : 2253
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The Encyclopedia of Modern Optics, Second Edition, Five Volume Set provides a wide-ranging overview of the field, comprising authoritative reference articles for undergraduate and postgraduate students and those researching outside their area of expertise. Topics covered include classical and quantum optics, lasers, optical fibers and optical fiber systems, optical materials and light-emitting diodes (LEDs). Articles cover all subfields of optical physics and engineering, such as electro-optical design of modulators and detectors. This update contains contributions from international experts who discuss topics such as nano-photonics and plasmonics, optical interconnects, photonic crystals and 2D materials, such as graphene or holy fibers. Other topics of note include solar energy, high efficiency LED’s and their use in illumination, orbital angular momentum, quantum optics and information, metamaterials and transformation optics, high power fiber and UV fiber lasers, random lasers and bio-imaging. Addresses recent developments in the field and integrates concepts from fundamental physics with applications for manufacturing and engineering/design Provides a broad and interdisciplinary coverage of specialist areas Ensures that the material is appropriate for new researchers and those working in a new sub-field, as well as those in industry Thematically arranged and alphabetically indexed, with cross-references added to facilitate ease-of-use
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Publisher: Academic Press
ISBN: 0080951015
Category : Science
Languages : en
Pages : 457
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This volume continues the tradition of the Advances series. It contains contributions from experts in the field of atomic, molecular, and optical (AMO) physics. The articles contain some review material, but are intended to provide a comprehensive picture of recent important developments in AMO physics. Both theoretical and experimental articles are included in the volume. - International experts - Comprehensive articles - New developments
Author: Amber T. Krummel
Publisher:
ISBN:
Category :
Languages : en
Pages : 286
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Author: Ana Maria de Carvalho Vicente da Cunha
Publisher:
ISBN: 9789036799683
Category :
Languages : en
Pages : 202
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Author: Bo Xiang
Publisher:
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Category :
Languages : en
Pages : 129
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In this dissertation, the application of advanced spectroscopy, such as two-dimensional infrared (2D IR) spectroscopy to vibrational-polaritons challenges and advances our understanding in both fields, as mentioned detailly in the introduction. In the fourth chapter, 2D IR uniquely resolves excitation of hybrid light-matter polaritons and unexpected dark states in a state-selective manner, revealing otherwise hidden interactions between them. Moreover, 2D IR signals highlight the impact of molecular anharmonicities which are applicable to virtually all molecular systems. Besides revealing the polariton-dark modes interactions, the spectroscopy tools has also been employed to study the optical nonlinearities of the molecular vibrational polaritons. In the fifth chapter, the control of vibrational polariton coherent nonlinearities has been fulfilled by manipulation of macroscopic parameters such as cavity longitudinal length or molecular concentration. In chapter six, we studied the long-lived dynamics of vibrational polaritons in various solvent environments. While the relaxation from upper polariton (UP) to dark modes is always fast (
Author: Peter Hamm
Publisher: Cambridge University Press
ISBN: 1139497073
Category : Science
Languages : en
Pages : 297
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2D infrared (IR) spectroscopy is a cutting-edge technique, with applications in subjects as diverse as the energy sciences, biophysics and physical chemistry. This book introduces the essential concepts of 2D IR spectroscopy step-by-step to build an intuitive and in-depth understanding of the method. This unique book introduces the mathematical formalism in a simple manner, examines the design considerations for implementing the methods in the laboratory, and contains working computer code to simulate 2D IR spectra and exercises to illustrate involved concepts. Readers will learn how to accurately interpret 2D IR spectra, design their own spectrometer and invent their own pulse sequences. It is an excellent starting point for graduate students and researchers new to this exciting field. Computer codes and answers to the exercises can be downloaded from the authors' website, available at www.cambridge.org/9781107000056.
Author: Munira Khalil
Publisher:
ISBN:
Category :
Languages : en
Pages : 346
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(Cont.) rephasing spectra. The data is modeled by using Redfield theory to account for coherence transfer, vibrational dephasing and population relaxation in a multilevel vibrational system. Building on the studies of the RDC model system, 2D IR spectroscopy is used to study the thermal denaturation of RNase A by characterizing the temperature-dependent Amide I band. A nonlinear IR probe is used to study the early events in the laser temperature-jump initiated denaturation of RNase A.
