Polariton Chemistry
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Polariton Chemistry
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Author : Joel Yuen-Zhou
language : en
Publisher:
Release Date : 2023-05-09
Polariton Chemistry written by Joel Yuen-Zhou and has been published by this book supported file pdf, txt, epub, kindle and other format this book has been release on 2023-05-09 with categories.
This book provides a pedagogical introduction to the emerging field of Polariton Chemistry, where optical cavities are utilized to control the physicochemical properties and dynamics of molecular systems. Given the early stages of this interdisciplinary research area, it is important to provide a common language and starting point for interested researchers across Chemistry, Physics, and Engineering This edited compendium fills a void given that there is currently no analogue in the current literature. Topics covered include Single-Molecule Strong Light-Matter Coupling; Collective Strong Light-Matter Coupling; and Ultrastrong Light-Matter Coupling
Studies On Molecular Polaritons
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Author : Sindhana Selvi Pannir Sivajothi
language : en
Publisher:
Release Date : 2023
Studies On Molecular Polaritons written by Sindhana Selvi Pannir Sivajothi and has been published by this book supported file pdf, txt, epub, kindle and other format this book has been release on 2023 with categories.
When optical transitions in materials couple strongly to photon modes, light and matter degrees of freedom can no longer be treated separately with the light-matter coupling taken as a perturbation. They form hybrid light-matter modes called polariton modes. Several experiments over the last decade have demonstrated a change in chemical reactivity under collective vibrational strong coupling, where vibrational modes in many molecules couple collectively to a photon mode, starting the field of polariton chemistry. However, from theoretical studies, there is no clear explanation for this phenomenon. Additionally, some recent experiments have shown no effect of collective strong light-matter coupling on reactivity. In this dissertation, we propose strategies to enhance polaritonic effects and we also seek out avenues outside of chemical reactivity where the effect of strong light-matter coupling could be significant. We demonstrate that the effect of polaritons on chemical reactivity under vibrational strong coupling can be enhanced by vibrational polariton condensation. The macroscopic occupation of the polariton mode through Bose-Einstein condensation amplifies its contribution to the reaction rate. To explain an experimentally observed reduction in the dehydration temperature in an open cavity system under vibrational strong coupling on resonance, we develop a theoretical model for heat flow based on kinetic equations. We hypothesized that the reduction in temperature is not due to an inherent change in the dehydration temperature of the material, but due to a reduction in the thermal contact resistance across the interface between the molecules and the plasmonic structure due to polaritons. We also show that the topological properties of a system under electronic strong coupling can be modified through optical pumping with circularly polarized light. Our work relies on selectively saturating electronic transitions with circularly polarized light, and, therefore, creating a population imbalance in the system and breaking time-reversal symmetry. In the last part of this dissertation, we propose a way to measure small differences in the equilibrium positions of the vibrational coordinate between different electronic states using higher-energy Fock states. This work does not require strong light-matter coupling. Higher-energy vibrational Fock states have a smaller length scale associated with them than the ground vibrational state which aids in inferring smaller displacements in the vibrational coordinate from the electronic absorption spectrum.
Polaritonic Chemistry
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Author : Javier Galego Pascual
language : en
Publisher: Springer Nature
Release Date : 2020-06-25
Polaritonic Chemistry written by Javier Galego Pascual and has been published by Springer Nature this book supported file pdf, txt, epub, kindle and other format this book has been release on 2020-06-25 with Science categories.
Polaritonic chemistry is an emergent interdisciplinary field in which the strong interaction of organic molecules with confined electromagnetic field modes is exploited in order to manipulate the chemical structure and reactions of the system. In the regime of strong light-matter coupling the interaction with the electromagnetic vacuum obliges us to redefine the concept of a molecule and consider the hybrid system as a whole. This thesis builds on the foundations of chemistry and quantum electrodynamics in order to provide a theoretical framework to describe these organic light-matter hybrids. By fully embracing the structural complexity of molecules, this theory allows us to employ long-established quantum chemistry methods to understand polaritonic chemistry. This leads to predictions of substantial structural changes in organic molecules and the possibility of significantly influencing chemical reactions both in the excited and ground states of the system.
Polaritons In Periodic And Quasiperiodic Structures
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Author : Eudenilson L. Albuquerque
language : en
Publisher: Elsevier
Release Date : 2004-12-09
Polaritons In Periodic And Quasiperiodic Structures written by Eudenilson L. Albuquerque and has been published by Elsevier this book supported file pdf, txt, epub, kindle and other format this book has been release on 2004-12-09 with Science categories.
In recent years there have been exciting developments in techniques for producing multilayered structures of different materials, often with thicknesses as small as only a few atomic layers. These artificial structures, known as superlattices, can either be grown with the layers stacked in an alternating fashion (the periodic case) or according to some other well-defined mathematical rule (the quasiperiodic case). This book describes research on the excitations (or wave-like behavior) of these materials, with emphasis on how the material properties are coupled to photons (the quanta of the light or the electromagnetic radiation) to produce “mixed waves called polaritons. · Clear and comprehensive account of polaritons in multilayered structures · Covers both periodic and quasiperiodic superlattices · Careful attention to theoretical developments and tools · Invaluable guide for researchers in this field · Shows developments from the basics to advanced topics
Impact Of Strong Coupling On Chemical Properties And Nonlinear Response Of Organic Semiconductors
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Author : Nina Krainova
language : en
Publisher:
Release Date : 2023
Impact Of Strong Coupling On Chemical Properties And Nonlinear Response Of Organic Semiconductors written by Nina Krainova and has been published by this book supported file pdf, txt, epub, kindle and other format this book has been release on 2023 with categories.
Polariton chemistry is an emerging and intriguing field that seeks to address a fundamental question: Can we modify and control molecular properties by shaping the optical environment? By hybridizing light and matter and creating quasi-states that possess the properties of both, known as polaritons, can molecules harness photonic characteristics? We focus on intermolecular interactions in a strong light-matter coupling regime. More specifically, our research centers on the investigation of charge transfer events, with photocurrent or photoluminescence serving as our observables. For our photocurrent study, we looked into the photoexcitation of charged molecules, which transform into polaron-polaritons in a strong coupling regime. Fascinatingly, we have discovered evidence of an accelerated charge-transfer process when charged molecules are strongly coupled to light, as opposed to when they are not. The key finding lies in the distinct bias dependence observed between weakly and strongly coupled charged molecules within the same photonic structure. Weaker bias dependence of strongly coupled molecules, according to Onsager theory, indicates that a photoexcited polaron hops further away from its counter anion compare to weakly coupled case. Thus, we conclude that strong coupling regime enhances the intermolecular charge transfer rate. We explain the effect by considering the delocalized nature of polaritons and their ability to simultaneously sample all strongly coupled molecules, benefiting from molecules with fast charge-transfer rates. In our photoluminescence study, we sought a means to harness a donor exciton in donor-acceptor blends that feature high donor concentrations through the application of strong light-matter coupling. Our motivation was to utilize the delocalized nature of photons to promote the transmission of excitation from a distant donor to a donor in close proximity to an acceptor, thereby facilitating the formation of a charge-transfer state. We investigated two distinct systems in which exciton-polaritons originate from the first and second excited states of singlet excitons. Regrettably, we did not observe any systematic trends in the emission spectrum between excitons in strong and weak coupling regimes. We argue that temperature plays a critical role, and only at cryo temperatures where the coherent lifetime is much longer can the effect be observed. Unfortunately, unlike our photocurrent study, our investigation of the photoluminescence was conducted at room temperature. In the latter part of our research, we attempt to understand the effect of strong coupling on the nonlinear optical response of molecules. Specifically, we study electroabsorption (EA) which is responsible for the imaginary part of chi3 nonlinearity. We predict that the molecule with a degenerate excited state will have both linear and quadratic field dependencies of its EA response. Remarkably, we observe that the functional dependence of the EA response on the bias for the lower polariton (LP) strongly varies along the LP dispersion curve. When lower polariton approaches the energy of the uncoupled transition, its bias dependence becomes more quadratic; alternatively, when the energy of LP father away from the transition, the bias dependence is more linear. Furthermore, for both the uncoupled transition and middle polariton we observe the same strongly quadratic bias dependence, distinctly different from that for the lower polariton. Lastly, we have established the groundwork for an exploration of chi2 nonlinearity in an anisotropic organic crystal. We have verified the strong coupling regime for a primal crystal axis by altering the energy of an optical mode. We do not observe a strong coupling signature for light with polarization perpendicular to the primal crystal axis. We witness the strongest second harmonic signal when the incident light (fundamental) has twice the wavelength of the lower polariton, however, at the same time similar magnitude enhancement of SHG occurs at DBR sidebands. This preliminary finding undermines the notion that an exciton-polariton possesses strong hyperpolarizability. Additional measurements are suggested in the last chapter to solidify our findings.
Polaritons
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Author : Elias Burstein
language : en
Publisher: Pergamon
Release Date : 1974
Polaritons written by Elias Burstein and has been published by Pergamon this book supported file pdf, txt, epub, kindle and other format this book has been release on 1974 with Science categories.
Polariton Physics
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Author : Arash Rahimi-Iman
language : en
Publisher: Springer Nature
Release Date : 2020-03-05
Polariton Physics written by Arash Rahimi-Iman and has been published by Springer Nature this book supported file pdf, txt, epub, kindle and other format this book has been release on 2020-03-05 with Science categories.
This book offers an overview of polariton Bose–Einstein condensation and the emerging field of polaritonics, providing insights into the necessary theoretical basics, technological aspects and experimental studies in this fascinating field of science. Following a summary of theoretical considerations, it guides readers through the rich physics of polariton systems, shedding light on the concept of the polariton laser, polariton microcavities, and the technical realization of optoelectronic devices with polaritonic emissions, before discussing the role of external fields used for the manipulation and control of exciton–polaritons. A glossary provides simplified summaries of the most frequently discussed topics, allowing readers to quickly familiarize themselves with the content. The book pursues an uncomplicated and intuitive approach to the topics covered, while also providing a brief outlook on current and future work. Its straightforward content will make it accessible to a broad readership, ranging from research fellows, lecturers and students to interested science and engineering professionals in the interdisciplinary domains of nanotechnology, photonics, materials sciences and quantum physics.
Infrared Ellipsometry On Semiconductor Layer Structures
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Author : Mathias Schubert
language : en
Publisher: Springer Science & Business Media
Release Date : 2004-11-26
Infrared Ellipsometry On Semiconductor Layer Structures written by Mathias Schubert and has been published by Springer Science & Business Media this book supported file pdf, txt, epub, kindle and other format this book has been release on 2004-11-26 with Science categories.
The study of semiconductor-layer structures using infrared ellipsometry is a rapidly growing field within optical spectroscopy. This book offers basic insights into the concepts of phonons, plasmons and polaritons, and the infrared dielectric function of semiconductors in layered structures. It describes how strain, composition, and the state of the atomic order within complex layer structures of multinary alloys can be determined from an infrared ellipsometry examination. Special emphasis is given to free-charge-carrier properties, and magneto-optical effects. A broad range of experimental examples are described, including multinary alloys of zincblende and wurtzite structure semiconductor materials, and future applications such as organic layer structures and highly correlated electron systems are proposed.
Controlling Chemical Reactivities Beyond Existing Paradigms
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Author : Xinyang Li
language : en
Publisher:
Release Date : 2022
Controlling Chemical Reactivities Beyond Existing Paradigms written by Xinyang Li and has been published by this book supported file pdf, txt, epub, kindle and other format this book has been release on 2022 with categories.
"Traditionally, there are two well-known ways to control chemical reactions, namely, thermodynamic control and kinetic control. However, recent experimental progress has demonstrated that there could be many other paradigms beyond these two textbook examples. For example, new experiments have demonstrated the quantum tunneling control for the reactivities, as well as the vibrational strong coupling (VSC) regime in polariton chemistry by coupling molecular vibrations with the quantized radiation mode inside an optical cavity. Nuclear quantum effects (NQEs), including quantum mechanical tunneling and the zero-point energy (ZPE), can play a vital role in certain chemical reactions. Although the quantum tunnel through a barrier has a well-known effect, the ability to use quantum tunneling to control the direction of a chemical reaction has only been recognized recently. A product that is neither favored kinetically nor thermodynamically can be formed through intrinsic quantum tunneling, without using any additional catalyst. This new strategy is referred to as tunneling control. Thus, it is essential to incorporate the NQEs in the study of tunneling-controlled chemical reactions. Polariton chemistry is an exciting emerging field on manipulating chemical reactivities using intrinsic quantum light-matter interactions. When an ensemble of molecules are put into an optical cavity (which is formed by having two reflecting mirrors), a set of new light-matter entangled states, so-called polaritons. The polariton states can be generated from the strong coupling between molecular vibrational excitations and photonic excitations, under the so-called VSC regime. It has been experimentally demonstrated that the cavity can modify the ground state reactivities under the VSC regime and change the selectivities among competing reaction pathways. This effect can potentially open up new possibilities for synthetic chemistry. However, a clear theoretical understanding of the fundamental mechanism remains elusive. To investigate the fundamental reactive mechanism behind these new paradigms, we use theoretical approaches and dynamics simulations to directly investigate these processes. The reaction rate constant can directly reflect the relative contribution of the quantum mechanical tunneling effects and capture dynamical effects that otherwise will not be included in the transition state theory (TST) rate constant. With the reaction rate theory, one can accurately calculate the chemical reaction rate constant through the molecular dynamics (MD) simulations and, therefore, provide new theoretical insights into tunneling controlled reactions and VSC polariton chemistry, both of which can potentially lead to new chemical reactivities. In this thesis, we have studied a tunneling-controlled reaction and the rate suppression originated from the light-matter interaction inside an optical cavity, through MD simulations and the Grote-Hynes (GH) theory. We have theoretically demonstrated that it is possible for tunneling to control the reaction directions and it is feasible as well to simulate tunneling-controlled reactions ab initio with NQEs included. For the VSC regime in polariton chemistry, we show that the resonant effects can arise from the non-Markovian nature of the cavity radiation mode, where the photons act like a solvent trapping the reactive molecules in the barrier region, hence slowing down the reaction rate"--Pages x-xi.
Theoretical And Computational Photochemistry
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Author : García Iriepa Cristina
language : en
Publisher: Elsevier
Release Date : 2023-04-21
Theoretical And Computational Photochemistry written by García Iriepa Cristina and has been published by Elsevier this book supported file pdf, txt, epub, kindle and other format this book has been release on 2023-04-21 with Business & Economics categories.
Theoretical and Computational Photochemistry: Fundamentals, Methods, Applications and Synergy with Experimental Approaches provides a comprehensive overview of photoactive systems and photochemical processes. After an introduction to photochemistry, the book discusses the key computational chemistry methods applied to the study of light-induced processes over the past decade, and further outlines recent research topics to which these methods have been applied. By discussing the synergy between experimental and computational data, the book highlights how theoretical studies could facilitate understanding experimental findings. This helpful guide is for both theoretical chemists and experimental photochemistry researchers interested in utilizing computational photochemistry methods for their own work. Reviews the fundamentals of photochemistry, helping those new to the field in understanding key concepts Provides detailed guidance and comparison of computational and theoretical methods, highlighting the suitability of each method for different case studies Outlines current applications to encourage discussion of the synergy between experimental and computational data, and inspiring further application of these methods to other photochemical processes