Journal ArticleDOI
Femtosecond Real-Time Probing of Reactions. 23. Studies of Temporal, Velocity, Angular, and State Dynamics from Transition States to Final Products by Femtosecond-Resolved Mass Spectrometry
Dongping Zhong,Ahmed H. Zewail +1 more
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TLDR
In this paper, the femtosecond, time-resolved mass spectrometry in molecular beams for the studies of the elementary steps of complex reactions and the application to different systems is described.Abstract:
In this contribution, we give a full account of the approach of femtosecond, time-resolved mass spectrometry in molecular beams for the studies of the elementary steps of complex reactions and the application to different systems. The level of complexity varies from diatomics to polyatomics, from direct-mode to complex-mode, from one-center, to two-center, to four-center, and from uni- to bimolecular reactions. The systems studied are iodine, cyanogen iodide, methyl iodide, iodobenzene, 1,2-diiodotetrafluoroethane, mercury iodide, benzene· iodine complexes, and methyl iodide dimers. By resolving the femtosecond dynamics and simultaneously observing the evolution of velocity, angular, and state distribution(s) of the reaction, we are able to study multiple reaction paths, the nature of transition-state geometry and dynamics, coherent wave-packet motion, evolution of energy disposal, and the nonconcerted motion in multicenter reactions. These phenomena and concepts are elucidated in dissociation, elimination, and charge-transfer reactions and in the inelastic and reactive pathways of bimolecular reactions. Theoretical phenomenology, using frontier orbitals and molecular dynamics, are invoked to provide a relationship between the observed dynamics and molecular structures.read more
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Journal ArticleDOI
Ultrafast dynamics in isolated molecules and molecular clusters
Ingolf V. Hertel,W. Radloff +1 more
TL;DR: In this paper, a review summarizes the present knowledge on ultrafast dynamics in isolated molecules and molecular clusters evolving after excitation with femtosecond pulses as studied by pump-probe analysis in real time.
Journal ArticleDOI
Photochemistry of aryl halides: Photodissociation dynamics
Ke-Li Han,Guo-Zhong He +1 more
TL;DR: In this paper, a review on the photochemistry of aryl halides is presented, with emphasis on the recent progress in photodissociation dynamics at 266 nm by using photofragment translational spectroscopy.
Journal ArticleDOI
Chemical reaction dynamics with molecular beams
TL;DR: In this paper, a review describes advances which have occurred during the past decade in chemical reaction dynamics using crossed molecular beams, and a selection of case studies are considered in some detail, to exemplify recent improvements in our understanding of gas-phase neutral reaction dynamics.
Journal ArticleDOI
Electrons in Finite-Sized Water Cavities: Hydration Dynamics Observed in Real Time
TL;DR: By resolving the binding energy of the excess electron in real time with femtosecond resolution, this work captured the ultrafast dynamics of the electron in the presolvated (“wet”) and hydrated states and obtained, as a function of cluster size, the subsequent relaxation times.
Journal ArticleDOI
Imaging an Aligned Polyatomic Molecule with Laser-Induced Electron Diffraction
M. G. Pullen,Benjamin Wolter,Anh-Thu Le,Matthias Baudisch,Michael Hemmer,Arne Senftleben,Claus Dieter Schröter,Joachim Ullrich,Robert Moshammer,Chi Lin,Jens Biegert +10 more
TL;DR: In this article, the authors demonstrate the retrieval of multiple bond lengths from a polyatomic molecule by simultaneously measuring the C-C and C-H bond lengths in aligned acetylene, based on the combination of a 160 kHz mid-infrared few-cycle laser source with full three-dimensional electron-ion coincidence detection.
References
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Journal ArticleDOI
A Spectrophotometric Investigation of the Interaction of Iodine with Aromatic Hydrocarbons
H. A. Benesi,Joel H. Hildebrand +1 more
TL;DR: In this paper, it was shown that the position of the absorption bands of iodine solutions in the visible region moved gradually from violet to brown, the shift being only small in the case of benzene in which the color of iodine is a red-violet.
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Clusters: Structure, Energetics, and Dynamics of Intermediate States of Matter
A. W. Castleman,Kit H. Bowen +1 more
TL;DR: The field of cluster research can trace its origins back to the mid-nineteenth century when early studies of colloids, aerosols, and nucleation phenomena were reported.
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Real-time femtosecond probing of "transition states" in chemical reactions
Journal ArticleDOI
Triatomic Photofragment Spectra. II. Angular Distributions from NO2 Photodissociation
George E. Busch,Kent R. Wilson +1 more
TL;DR: The angular distribution of recoil of O atoms from the photodissociation of NO2 at 28 810 cm−1 was analyzed to obtain information about the lifetime and symmetry of the excited dissociative state.
Journal ArticleDOI
Doppler line shape of atomic fluorescence excited by molecular photodissociation
TL;DR: In this article, a semiclassical treatment of the photodissociation of a diatomic molecule is developed, and it is shown that the angular distribution of products will often be peaked parallel or perpendicular to the direction of the incident light beam.