Artikel
Lizenziert
Nicht lizenziert
Erfordert eine Authentifizierung
Exploring Pathways of Photoaddition Reactions by Artificial Force Induced Reaction Method: A Case Study on the Paternò–Büchi Reaction
-
Satoshi Maeda
Veröffentlicht/Copyright:
17. Juni 2013
Abstract
The present study demonstrates a priori prediction of the mechanism of Paternò–Büchi (PB) reaction by automated search for reaction pathways using the artificial force induced reaction (AFIR) method, for the simplest set of reactants, H2CO + C2H4. The search found all previously suggested pathways automatically without using any guess about the reaction mechanism. Even the reaction product was not assumed. In addition, a comprehensive view of the reaction path network obtained in the present extensive search gave new insights into the mechanism. Barriers on excited states explained the preference of the initial bonding sites. A seam of crossing between the lowest triplet and first singlet excited state is suggested to make a significant contribution to an intersystem crossing and the reaction mechanism of the present system.
Keywords: Automatic Search; Reaction Pathway; Artificial Force Induced Reaction Method; AFIR Method; Photoaddition Reaction; Paternò–Büchi Reaction
Received: 2013-2-8
Published Online: 2013-6-17
Published in Print: 2013-11-1
© 2013 by Walter de Gruyter Berlin Boston
Sie haben derzeit keinen Zugang zu diesem Inhalt.
Sie haben derzeit keinen Zugang zu diesem Inhalt.
Artikel in diesem Heft
- Masthead
- Masthead
- Editorial
- Milestones in Physical Chemistry (I) – A Special Issue Honoring the Seminal Work of Henry Eyring and Michael Polanyi
- International Collaborations are nothing new... and sometimes they are simply amazing
- Personal Perspective
- A Comment on Henry Eyring
- Comment
- Michael Polanyi, the Scientist
- Historical Paper
- On Simple Gas Reactions
- Feature Article
- Probing Quantum Dynamics of Elementary Chemical Reactions via Accurate Potential Energy Surfaces
- Elementary Gas Phase Reactions
- Experimental and Theoretical Studies of Roaming Dynamics in the Unimolecular Dissociation of CH3NO2 to CH3O + NO
- Simultaneous Measurement of Reactive and Inelastic Scattering: Differential Cross Section of the H + HD → HD(v′, j′) + H Reaction
- The Decomposition of Hydrazine in the Gas Phase and over an Iridium Catalyst
- A Theoretical Study of the X-Abstraction Reactions (X = H, Br, or I) from CH2IBr by OH Radicals: Implications for Atmospheric Chemistry
- Models for Intrinsic Non-RRKM Dynamics. Decomposition of the SN2 Intermediate Cl––CH3Br
- Chemical Reactions at Surfaces
- Electronic Excitations in the Course of the Reaction of H with Coinage and Noble Metal Surfaces: A Comparison
- 7D Quantum Dynamics of H2 Scattering from Cu(111): The Accuracy of the Phonon Sudden Approximationy
- Exploring Pathways of Photoaddition Reactions by Artificial Force Induced Reaction Method: A Case Study on the Paternò–Büchi Reaction
- Kinetic Prefactors of Reactions on Solid Surfaces
- Electron-Transfer-Induced Dissociation of H2 on Gold Nanoparticles: Excited-State Potential Energy Surfaces via Embedded Correlated Wavefunction Theory
- Toward Detection of Electron-Hole Pair Excitation in H-atom Collisions with Au(111): Adiabatic Molecular Dynamics with a Semi-Empirical Full-Dimensional Potential Energy Surface
- Initial Sticking Coefficient of H2 on the Pd–Cu(111) Surface Alloy at very Low Coverages
- Catalyzed Surface-Aligned Reaction, H(ad) + H2(ad) = H2(g) + H(ad) on Coinage Metals
- Nitrogen Scattering at Ru(0001) Surfaces
- Ready, Set and no Action: A Static Perspective on Potential Energy Surfaces commonly used in Gas-Surface Dynamics
- Reactions in Clusters
- Potential Energy Surfaces and Rates of Spin Transitions
- A Full-Dimensional Neural Network Potential-Energy Surface for Water Clusters up to the Hexamer
- Embedded Cluster Models for Reactivity of the Hydrated Electron
- Novel Experimenta Methods
- Stark Deceleration of NO Radicals
- A Forty-Segment Molecular Synchrotron
Schlagwörter für diesen Artikel
Automatic Search;
Reaction Pathway;
Artificial Force Induced Reaction Method;
AFIR Method;
Photoaddition Reaction;
Paternò–Büchi Reaction
Artikel in diesem Heft
- Masthead
- Masthead
- Editorial
- Milestones in Physical Chemistry (I) – A Special Issue Honoring the Seminal Work of Henry Eyring and Michael Polanyi
- International Collaborations are nothing new... and sometimes they are simply amazing
- Personal Perspective
- A Comment on Henry Eyring
- Comment
- Michael Polanyi, the Scientist
- Historical Paper
- On Simple Gas Reactions
- Feature Article
- Probing Quantum Dynamics of Elementary Chemical Reactions via Accurate Potential Energy Surfaces
- Elementary Gas Phase Reactions
- Experimental and Theoretical Studies of Roaming Dynamics in the Unimolecular Dissociation of CH3NO2 to CH3O + NO
- Simultaneous Measurement of Reactive and Inelastic Scattering: Differential Cross Section of the H + HD → HD(v′, j′) + H Reaction
- The Decomposition of Hydrazine in the Gas Phase and over an Iridium Catalyst
- A Theoretical Study of the X-Abstraction Reactions (X = H, Br, or I) from CH2IBr by OH Radicals: Implications for Atmospheric Chemistry
- Models for Intrinsic Non-RRKM Dynamics. Decomposition of the SN2 Intermediate Cl––CH3Br
- Chemical Reactions at Surfaces
- Electronic Excitations in the Course of the Reaction of H with Coinage and Noble Metal Surfaces: A Comparison
- 7D Quantum Dynamics of H2 Scattering from Cu(111): The Accuracy of the Phonon Sudden Approximationy
- Exploring Pathways of Photoaddition Reactions by Artificial Force Induced Reaction Method: A Case Study on the Paternò–Büchi Reaction
- Kinetic Prefactors of Reactions on Solid Surfaces
- Electron-Transfer-Induced Dissociation of H2 on Gold Nanoparticles: Excited-State Potential Energy Surfaces via Embedded Correlated Wavefunction Theory
- Toward Detection of Electron-Hole Pair Excitation in H-atom Collisions with Au(111): Adiabatic Molecular Dynamics with a Semi-Empirical Full-Dimensional Potential Energy Surface
- Initial Sticking Coefficient of H2 on the Pd–Cu(111) Surface Alloy at very Low Coverages
- Catalyzed Surface-Aligned Reaction, H(ad) + H2(ad) = H2(g) + H(ad) on Coinage Metals
- Nitrogen Scattering at Ru(0001) Surfaces
- Ready, Set and no Action: A Static Perspective on Potential Energy Surfaces commonly used in Gas-Surface Dynamics
- Reactions in Clusters
- Potential Energy Surfaces and Rates of Spin Transitions
- A Full-Dimensional Neural Network Potential-Energy Surface for Water Clusters up to the Hexamer
- Embedded Cluster Models for Reactivity of the Hydrated Electron
- Novel Experimenta Methods
- Stark Deceleration of NO Radicals
- A Forty-Segment Molecular Synchrotron
