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Development of Coherent Two-dimensional Spectroscopy at Optical Frequencies and Application to Model Chromophores

Development of Coherent Two-dimensional Spectroscopy at Optical Frequencies and Application to Model Chromophores PDF Author: Hélène Seiler
Publisher:
ISBN:
Category :
Languages : en
Pages :

Book Description
"Ultrafast coherent multi-dimensional spectroscopies are a powerful set of techniques used to unravel complex processes. These processes range from electronic coherences in molecular chromophores to many-body interactions in quantum-confined materials. Yet these spectroscopies remain challenging to implement at the high frequencies of vibrational and electronic transitions, thereby limiting their widespread use. The work herein demonstrates three significant methodological improvements of two-dimensional spectroscopy at optical frequencies, followed by applications of the method on two different systems. First, we introduce a hollow-fibre setup for the production of broadband visible pulses. This source is comparatively simple to operate, and yields stable, 45 [mu]J pulses over the 520-700 nm region. Second, we demonstrate the feasibility of two-dimensional electronic spectroscopy in a single beam. By appropriately modulating the phases of the pulses within the beam,we show that it is possible to directly read out the relevant optical signals. This work shows that one needs neither complex beam geometries nor complex detection schemes in order to measure 2D spectra at optical frequencies. Finally, we introducea setup for complete and independent polarization control of each pulse in the sequence. Together, these methodological improvements represent important enabling steps towards the longstanding goal of achieving an "Optical NMR", and extendsthe realm of all-optical multi-dimensional spectroscopies to spatially heterogeneous samples. The methods are applied on two classes of systems. The model system Nile Blue is used to validate the performance of the instrument. The spectrometeris then used to reveal new processes in colloidal semiconductor CdSe nanocrystals, a system of contemporary interest." --

Development of Coherent Two-dimensional Spectroscopy at Optical Frequencies and Application to Model Chromophores

Development of Coherent Two-dimensional Spectroscopy at Optical Frequencies and Application to Model Chromophores PDF Author: Hélène Seiler
Publisher:
ISBN:
Category :
Languages : en
Pages :

Book Description
"Ultrafast coherent multi-dimensional spectroscopies are a powerful set of techniques used to unravel complex processes. These processes range from electronic coherences in molecular chromophores to many-body interactions in quantum-confined materials. Yet these spectroscopies remain challenging to implement at the high frequencies of vibrational and electronic transitions, thereby limiting their widespread use. The work herein demonstrates three significant methodological improvements of two-dimensional spectroscopy at optical frequencies, followed by applications of the method on two different systems. First, we introduce a hollow-fibre setup for the production of broadband visible pulses. This source is comparatively simple to operate, and yields stable, 45 [mu]J pulses over the 520-700 nm region. Second, we demonstrate the feasibility of two-dimensional electronic spectroscopy in a single beam. By appropriately modulating the phases of the pulses within the beam,we show that it is possible to directly read out the relevant optical signals. This work shows that one needs neither complex beam geometries nor complex detection schemes in order to measure 2D spectra at optical frequencies. Finally, we introducea setup for complete and independent polarization control of each pulse in the sequence. Together, these methodological improvements represent important enabling steps towards the longstanding goal of achieving an "Optical NMR", and extendsthe realm of all-optical multi-dimensional spectroscopies to spatially heterogeneous samples. The methods are applied on two classes of systems. The model system Nile Blue is used to validate the performance of the instrument. The spectrometeris then used to reveal new processes in colloidal semiconductor CdSe nanocrystals, a system of contemporary interest." --

Optical Multidimensional Coherent Spectroscopy

Optical Multidimensional Coherent Spectroscopy PDF Author: Associate Professor Hebin Li
Publisher: Oxford University Press
ISBN: 0192843869
Category : Science
Languages : en
Pages : 305

Book Description
This book provides an introduction to optical multidimensional coherent spectroscopy, a relatively new method of studying materials based on using ultrashort light pulses to perform spectroscopy. The technique has been developed and perfected over the last 25 years, resulting in multiple experimental approaches and applications to a broad array of systems ranging from atoms and molecules to solids and biological systems. Indeed, while this method is most often used by physical chemists, it is also relevant to materials of interest to physicists, which is the primary focus of this book. As well as an introduction to the method, the book also provides tutorials on the interpretation of the rather complex spectra that is broadly applicable across all subfields, and finishes with a survey of several emerging material systems and a discussion of future directions.

Two-Dimensional Correlation Spectroscopy

Two-Dimensional Correlation Spectroscopy PDF Author: Isao Noda
Publisher: John Wiley & Sons
ISBN: 0470012390
Category : Science
Languages : en
Pages : 310

Book Description
A valuable tool for individuals using correlation spectroscopy and those that want to start using this technique. Noda is known as the founder of this technique, and together with Ozaki, they are the two biggest names in the area First book on 2D vibrational and optical spectroscopy - single source of information, pulling together literature papers and reveiws Growing number of applications of this methodology - book now needed for people thinking of using this technique Limitations and benefits discussed and comparisons made with 2D NMR Discusses 20 optical and vibrational spectroscopy (IR, Raman, UV, Visible)

Coherent Multidimensional Spectroscopy

Coherent Multidimensional Spectroscopy PDF Author: Minhaeng Cho
Publisher: Springer
ISBN: 9789811397554
Category : Science
Languages : en
Pages : 394

Book Description
This book will fulfill the needs of time-domain spectroscopists who wish to deepen their understanding of both the theoretical and experimental features of this cutting-edge spectroscopy technique. Coherent Multidimensional Spectroscopy (CMDS) is a state-of-the-art technique with applications in a variety of subjects like chemistry, molecular physics, biochemistry, biophysics, and material science. Due to dramatic advancements of ultrafast laser technologies, diverse multidimensional spectroscopic methods utilizing combinations of THz, IR, visible, UV, and X-ray radiation sources have been developed and used to study real time dynamics of small molecules in solutions, proteins and nucleic acids in condensed phases and membranes, single and multiple excitons in functional materials like semiconductors, quantum dots, and solar cells, photo-excited states in light-harvesting complexes, ions in battery electrolytes, electronic and conformational changes in charge or proton transfer systems, and excess electrons and protons in water and biological systems.

Two-dimensional Optical Spectroscopy

Two-dimensional Optical Spectroscopy PDF Author: Minhaeng Cho
Publisher:
ISBN: 9780367577322
Category : Optical spectroscopy
Languages : en
Pages : 385

Book Description
Effectively introducing a newly developed research field, this book provides a detailed account of basic theory required for an understanding of two-dimensional vibrational and electronic spectroscopy. It also bridges the gap between the formal development of nonlinear optical spectroscopy and the application of the theory to explain experimenta

Coherent Two-dimensional Spectroscopy

Coherent Two-dimensional Spectroscopy PDF Author: Samuel Palato
Publisher:
ISBN:
Category :
Languages : en
Pages :

Book Description
"Spectra are usually interpreted in terms of transition energies and intensities. The lineshape is not discussed as often; yet it reveals fluctuations and disorder in the system. Nowhere is this analysis more powerful than in nonlinear spectroscopy, which enables resolution of lineshapes along multiple time-frequency axes. In some cases, the study of multidimensional lineshapes lays bare the origin of dephasing, such as coupling to coherent vibrational excitation. In the more common case, lineshapes and their dynamics provide important clues to the dynamics of materials.The interpretation of lineshapes requires solid theoretical foundations, which are introduced. The spectrometer allowing the observation of lineshape dynamics is then detailed.The bandwidth of the spectrometer is obtained by self-phase modulation in Argon. The response of Ar is instantaneous; this simple temporal response enables efficient modeling. The application of broadband two-dimensional spectroscopy to the analysis of coherent lineshape dynamics in CdSe nanocrystals (NCs) is reported. Two salient observations are made. First, modulations arising from the LO phonon are observed, and confirmed to be vibrational in nature by coherence mapping. Second, no electronic coherence are observed. This runs contrary to the predictions of continuum models of NCs. The lack of electronic coherence can be explained by the occurrence of intrinsic disorder present in a realistic NC. Finally, the general application of lineshape analysis is demonstrated by studying the time-resolved photoluminescence of dual-emitting NCs. The data suggests the existence of two surface states and electron transfer dynamics at the surface of the NCs, on a timescale of >10 ns, longer than previously thought." --

Development of Frequency Domain Multidimensional Spectroscopy with Applications in Semiconductor Photophysics

Development of Frequency Domain Multidimensional Spectroscopy with Applications in Semiconductor Photophysics PDF Author: Blaise Jonathan Thompson
Publisher:
ISBN:
Category :
Languages : en
Pages :

Book Description
Coherent multidimensional spectroscopy (CMDS) encompasses a family of experimental strategies involving the nonlinear interaction between electric fields and a material under investigation. This approach has several unique capabilities: (1) resolving congested states, (2) extracting spectra that would otherwise be selection-rule disallowed, (3) resolving fully coherent dynamics, (4) measuring coupling, and (5) resolving ultrafast dynamics. CMDS can be collected in the frequency or the time domain, and each approach has advantages and disadvantages. Frequency domain ``Multi-resonant'' CMDS (MR-CMDS) requires pulsed ultrafast light sources with tunable output frequencies. These pulses are directed into a material under investigation. The pulses interact with the material, and due to the specific interference between the multiple fields the material is driven to emit a new pulse: the MR-CMDS signal. This signal may have a different frequency and/or direction than the input pulses, depending on the exact experiment being performed. The MR-CMDS experiment involves tracking the intensity of this output signal as a function of different properties of the excitation pulses. These properties include (1) frequency. (2) relative arrival time and separation (delay), (3) fluence, and (4) polarization, among others. Thus MR-CMDS can be thought of as a multidimensional experimental space, where experiments typically involve explorations in one to four of the properties above. Because MR-CMDS is a family of related-but-separate experiments, each of them a multidimensional space, there are special challenges that must be addressed when designing a general-purpose MR-CMDS instrument. These issues require development of software, hardware, and theory. Part I: Background introduces relevant literature which informs on this development work. Part II: Development presents five strategies used to improve MR-CMDS: (1) processing software, (2) acquisition software (3), active artifact correction, (4) automated OPA calibration, and (5) finite pulse accountancy. Finally, Part III: Applications presents four examples where these instruments, with these improvements, have been used to address chemical questions in semiconductor systems.

Laser Optics of Condensed Matter

Laser Optics of Condensed Matter PDF Author: Elsa M. Garmire
Publisher: Springer Science & Business Media
ISBN:
Category : Science
Languages : en
Pages : 474

Book Description
Session 1 Elementary Excitations and Excitation Transport.- Picosecond Resolved Optically Driven Phonon Dynamics.- Relaxation and Propagation of High Frequency Phonons in Thin Crystalline Plates After Intense Laser Pumping.- Evolution in Real Time and Space of Short Polariton Pulses in Crystals.- Quasielastic Electronic Light Scattering in Semiconductors at Low Concentrations of Current Carriers.- Condensed Matter Science With Far Infra Red Free Electron Lasers (Abstract).- Nonequilibrium Terahertz Range Acoustic Phonons and Luminescence of Excitons in Semiconductors.- Session II Optical Properties of Surfaces and Interfaces.- Nonlinear Optical Studies of Molecular Adsorbates.- Enhancement of Exciton Transition Probabilities in Ultrathin Films of Cadmium Telluride.- Studies of Semiconductor Surfaces and Interfaces by Three Wave Mixing Spectroscopy (Abstract).- Time-Resolved Resonant Reflection of Light.- Femtosecond Photoemission Studies of Image Potential and Electron Dynamics in Metals.- High Intensity, Ultrashort Pulse Laser Heated Solids.- Session III Optical Studies of Growth, Instabilities and Pattern Formation.- Control of Transversal Interactions in Nonlinear Optics: New Spatio-Temporal Effects in Nonlinear Wave Dynamics (Abstract).- Synchronization of Atomic Quantum Transitions by Light Pulses.- Chaos in Nonlinear Optics.- Self-Organizaiton and Spatio-Temporal Chaos in Phase-Locked Semiconductor Laser Arrays (Abstract).- Competitive and Cooperative Dynamics in Optical Neural Networks (Abstract).- Transitions Between Ordered and Disordered Solid-Melt Patterns Formed on Silicon by Continuous Laser Beams: Competition Between Electrodynamics and Thermodynamics.- Session IV Elementary Excitations and Excitation Transport.- Light Scattering in Oxide Superconductors.- Raman Scattering in High-Tc Superconductors YBa2Cu3Ox With Different Oxygen Contents.- Raman Scattering from High Temperature Superconductors.- Decay of Exciton Gratings in Anthracene: Anisotropy of Lowest Exciton Bands and Coexistence of Longpath and Shortpath Waveguide Modes.- Excitation Transport in Polymeric Solids.- Vibron Lifetimes in Molecular Crystals.- Session V Optical Properties of Critical Phenomena Random Systems, and Coherent Phenomena.- Anomalies of the Elastic Light Scattering at Phase Transitions in Crystals with Point Defects.- Dynamical Fluctuations in a Dipolar Glass.- Localization of Light in Random Media (Abstract).- Quantum Optic and Transient Effects of Excitonic Polaritons, and Properties of Phonoritons.- Nonclassical Field Correlations in Quantum Optics (Abstract).- Phase-Conjugated Wave Enhanced by Weak Localization of Exciton-Polaritons.- Session VI Nonlinear Optical Properties of Semiconductors Organics and Fibers.- The Historical Relationship Between Nonlinear Optics and Condensed Matter (Abstract).- Optical Nonlinearities Enhanced by Carrier Transport.- Organic Nonlinear Optical Materials and Devices for Optoelectronics (Abstract).- Nonlinear Optical Susceptibilities of Surface Layers of Metals and Super- and Semiconductors Related to Electronic Structure and Crystal Symmetry.- Second Harmonic Generation in Optical Fibers.- Nonlinear Optical Probes of Glassy Polymers.- Session VII Quantum Wells.- Photoluminescence of Hot Electrons and Scattering Processes in Quantum-Well Structures.- High Resolution Nonlinear Laser Spectroscopy Measurements of Exciton Dynamics in GaAs Quantum Well Structures.- Optical Spectroscopy in the Regime of the Fractional Quantum Hall Effect.- Geminate Recombination in MQW Structures in a Magnetic Field.- Investigation of Two-Electron-Hole Pair Resonances in Semiconductor Quantum Dots.- Many Body Effects in Homogeneous Quasi 2D Electron-Hole Plasma in Undoped and Modulation Doped InGaAs Single Quantum Wells.- Session VIII Recent Significant Developments.- Pulsed Diffusing-Wave Spectroscopy in Dense Colloids.- Waves on Corrugated Surfaces: K-Gaps and Enhanced Backscattering.- Black Hole Radiation: Can Vir...

Coherent Multidimensional Spectroscopy

Coherent Multidimensional Spectroscopy PDF Author: Minhaeng Cho
Publisher: Springer
ISBN: 9811397538
Category : Science
Languages : en
Pages : 404

Book Description
This book will fulfill the needs of time-domain spectroscopists who wish to deepen their understanding of both the theoretical and experimental features of this cutting-edge spectroscopy technique. Coherent Multidimensional Spectroscopy (CMDS) is a state-of-the-art technique with applications in a variety of subjects like chemistry, molecular physics, biochemistry, biophysics, and material science. Due to dramatic advancements of ultrafast laser technologies, diverse multidimensional spectroscopic methods utilizing combinations of THz, IR, visible, UV, and X-ray radiation sources have been developed and used to study real time dynamics of small molecules in solutions, proteins and nucleic acids in condensed phases and membranes, single and multiple excitons in functional materials like semiconductors, quantum dots, and solar cells, photo-excited states in light-harvesting complexes, ions in battery electrolytes, electronic and conformational changes in charge or proton transfer systems, and excess electrons and protons in water and biological systems.

Trends and Perspectives in Modern Computational Science

Trends and Perspectives in Modern Computational Science PDF Author: George Maroulis
Publisher: CRC Press
ISBN: 9004155414
Category : Mathematics
Languages : en
Pages : 605

Book Description
This volume contains a collection of the lectures of the invited speakers and symposium organizers presented at the International Conference of Computational methods in Science and Engineering (ICCMSE 2006), held in Chania, Greece, October 2006. The content of the papers bears upon new developments of Computational Science pertinent to Physics, Chemistry, Biology, Medicine, Mathematics and Engineering. Molecular Science is a privileged ground for the application and evaluation of new mathematical tools and computational methods. In recent years, novelty and progress with greatest conceivable speed is common experience. This flavor of research findings carrying many consequences for distant fields is easily evidenced in the lectures collected in this volume.