Protonic structure of CH<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mrow /><mml:mn>3</mml:mn></mml:msub></mml:math>OH described by electroprotonic wave functions

Katō, Takako; Yamanouchi, Kaoru

doi:10.1103/physreva.85.034504

Cited by 15 publications

(3 citation statements)

References 24 publications

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“…Most recently, it was demonstrated that the proton density in methanol obtained from an electronproton orbital computation (with fixed carbon and oxygen nuclei) can be matched with the spatial configuration obtained from a BO electron-structure calculation [84]. Furthermore, in addition to the electronic and nuclear densities, flux densities have also been considered in Refs.…”

Section: A Probabilistic Interpretation Of the Wave Functionmentioning

confidence: 99%

Pre-Born–Oppenheimer molecular structure theory

Mátyus

2018

Molecular Physics

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In pre-Born-Oppenheimer (pre-BO) theory a molecule is considered as a quantum system as a whole, including the electrons and the atomic nuclei on the same footing. This approach is fundamentally different from the traditional quantum chemistry treatment, which relies on the separation of the motion of the electrons and the atomic nuclei. A fully quantum mechanical treatment of molecules has a great promise for future developments and applications. Its most accurate versions may contribute to the definition of new schemes for metrology and testing fundamental physical theories; its approximate versions can provide an efficient theoretical description for molecule-positron interactions and, in general, it would circumvent the tedious computation and fitting of potential energy surfaces and non-adiabatic coupling vectors. To achieve these goals, the review points out important technical and fundamental open questions. Most interestingly, the reconciliation of pre-BO theory with the classical chemistry knowledge touches upon fundamental problems related to the measurement problem of quantum mechanics. I. QUANTUM CHEMISTRY VS. QUANTUM MECHANICS AND CHEMISTRY?We start with a historical overview of the chemical theory of molecular structure and the origins of quantum chemistry, which is followed by a review of methodological details and applications of pre-Born-Oppenheimer theory. A. Historical background: Chemical structure, physical structure from organic chemistry experiments [T]he dominating story in chemistry of the 1860s, 1870s, and 1880s was neither the periodic law, nor the search for new elements, nor the early stages of the study of atoms and molecules as physical entities. It was the maturation, and demonstration of extraordinary scientific and technological power, of the "theory of chemical structure" ... Alan J. Rocke Image and Reality: Kekulé, Kopp, and the Scientific Imagination (The University of Chicago Press, Chicago and London, 2010) During the second half of the 19th century, the pioneering organic chemists generation-represented by Williamson, Kekulé, Butlerov, Crum Brown, Frankland, Wurtz, etc.-had explored an increasing number of chemical transformation in their laboratory experiments and worked towards the establishment of a logical framework for their observations. The "first chemist' conference", held in Karlsruhe on 3 September 1860, resulted in an internationally recognized definition of the atomic masses. This agreement ensured that the same molecular formula was then used for the same substance in all laboratories around the world, and thereby opened the route to the successful development of the theory of chemical structure. The development of the chemical theory has been surrounded by heated debatesabout what is reality and what is mere speculation. We note that contemporary physics (gravitation, electromagnetism) was not able to provide any satisfactory description for molecules. To give a taste of this exciting period, we reproduce a few extracts from Alan J. Rocke's chemical history bo...

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Section: A Probabilistic Interpretation Of the Wave Functionmentioning

confidence: 99%

Pre-Born–Oppenheimer molecular structure theory

Mátyus

2018

Molecular Physics

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“…The ideas presented here can also be extended to other derived theories emanating from the MCTDH theory, such that for mixtures of identical particles [87,88], also see Refs. [89,90]. The separation of the coefficients, which define the reduced density matrices, from the orbitals [79] suggests that other representations for the time-dependent manybody wavepackets would be amenable to linear response in the spirit presented here.…”

Section: Summary and Concluding Remarksmentioning

confidence: 99%

Unified view on linear response of interacting identical and distinguishable particles from multiconfigurational time-dependent Hartree methods

Alon

Streltsov

Cederbaum

2014

The Journal of Chemical Physics

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A unified view on linear response of interacting systems utilizing multicongurational timedependent Hartree methods is presented. The cases of one-particle and two-particle response operators for identical particles and up to all-system response operators for distinguishable degrees-offreedom are considered. The working equations for systems of identical bosons (LR-MCTDHB) and identical fermions (LR-MCTDHF), as well for systems of distinguishable particles (LR-MCTDH) are explicitly derived. These linear-response theories provide numerically-exact excitation energies and system's properties, when numerical convergence is achieved in the calculations.

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“…The migration, exchange, and scrambling processes of protons occurring within a very short period of time (B40 fs) may be a general phenomenon when hydrocarbon molecules are exposed to an intense laser field, and this highly correlated dynamics of protons (deuterons) may require a representation of protons as multiple-centered wave functions like those introduced recently by our group. 18,19…”

Section: Comparison Between I and I A And Between Ii And Ii Amentioning

confidence: 99%

Ultrafast hydrogen scrambling in methylacetylene and methyl-d3-acetylene ions induced by intense laser fields

Okino

Watanabe

et al. 2012

Phys. Chem. Chem. Phys.

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Three-body Coulomb explosion processes of triply charged positive ions of methylacetylene (CH(3)-C≡C-H) and its isotopomer, methyl-d(3)-acetylene (CD(3)-C≡C-H), induced by an ultrashort intense laser field (790 nm, ∼40 fs, 5.0 × 10(13) W cm(-2)) are investigated by the coincidence momentum imaging method. Two types of three-body decomposition processes accompanying the ejection of a proton are identified for methylacetylene, and six types of three-body decomposition processes accompanying the ejection of a proton or a deuteron are identified for methyl-d(3)-acetylene. From the observed momentum vectors of all the three fragment ions for each decomposition pathway, the proton and deuteron distributions are constructed in the coordinate space, and the hydrogen migration processes are investigated. It was shown that the hydrogen migration proceeds more efficiently from the methyl group than from the methine group. In addition to the decomposition pathways accompanying the migration of one H (or D) atom, the decomposition pathways accompanying the migration of two light atoms (H/D exchange and 2D migration) are identified. Furthermore, the decomposition pathways ascribable to the migration of three light atoms (H/D exchange followed by D migration) are identified, showing the high intramolecular mobilities of H and D atoms within methylacetylene and methyl-d(3)-acetylene in an intense laser field, resulting in the H/D scrambling.

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Protonic structure of CH3OH described by electroprotonic wave functions

Cited by 15 publications

References 24 publications

Pre-Born–Oppenheimer molecular structure theory

Pre-Born–Oppenheimer molecular structure theory

Unified view on linear response of interacting identical and distinguishable particles from multiconfigurational time-dependent Hartree methods

Ultrafast hydrogen scrambling in methylacetylene and methyl-d3-acetylene ions induced by intense laser fields

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