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Conformationally Controlled Chemistry
Third-party funded project |
Project title |
Conformationally Controlled Chemistry |
Principal Investigator(s) |
Willitsch, Stefan
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Project Members |
Deb, Nabanita Kilaj, Ardita Rivero Gonzalez, Uxia Constanza Stranak, Patrik Rösch, Daniel Gao, Hong Ploenes, Ludger Bachmann, Daniel
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Organisation / Research unit |
Departement Chemie / Chemische Physik (Willitsch) |
Project start |
01.09.2015 |
Probable end |
30.11.2020 |
Status |
Completed |
Abstract |
The relationship between structure and reactivity is one of the central tenets of chemistry. In particular, many molecules exhibit structural isomers that interconvert over low barriers through rotations about covalent bonds (conformers). Conformers are the dominant isomers of complex molecules, and the conformation of a molecule can have pronounced effects on its chemical reactivity. Despite the eminent importance of conformational isomers in chemistry, very few studies have been reported thus far charac- terising conformational effects in chemical reactions under single-collision conditions. Consequently, the role of molecular conformations in fundamental reactions is only poorly understood. This striking lack of data reflects the experimental challenges to isolate und control specific conformers.
In a recent proof-of-principle study [Science 342 (2013), 98], we have spatially separated specific con- formers in a molecular beam through electrostatic deflection and directed them at a spatially localized reaction target of cold ions in a trap. This approach allowed us to study conformation-specific effects in ion-molecule reactions under precisely controlled experimental conditions in the gas phase. Here, we pro- pose a wide-ranging research programme aiming at extending our method to neutral reactions and applying it to a range of chemically relevant problems in order to explore the relationship between structure and reactivity in unprecedented detail. These methodological advances will enable for the first time detailed and systematic studies of the reaction mechanisms and dynamics of isolated conformers. The fundamental mechanistic insights gained will benefit a wide range of fields as diverse as fundamental reaction dynamics, organic synthesis, catalysis, atmospheric chemistry and rational molecule design.
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Financed by |
Swiss National Science Foundation (SNSF)
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Published results () |
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ID |
Autor(en) |
Titel |
ISSN / ISBN |
Erschienen in |
Art der Publikation |
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3720344 |
Rösch, Daniel; Gao, Hong; Kilaj, Ardita; Willitsch, Stefan |
Design and characterization of a linear quadrupole ion trap for high-resolution Coulomb-crystal time-of-flight mass spectrometry |
2195-7045 |
EPJ Techniques and Instrumentation |
Publication: JournalArticle (Originalarbeit in einer wissenschaftlichen Zeitschrift) |
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3728516 |
Rösch, Daniel |
Reactive collisions with conformationally controlled molecules |
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Publication: Thesis (Dissertationen, Habilitationen) |
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3932205 |
Rivero, Uxia; Meuwly, Markus; Willitsch, Stefan |
A computational study of the Diels-Alder reactions between 2,3-dibromo-1,3-butadiene and maleic anhydride |
0009-2614 |
Chemical Physics Letters |
Publication: JournalArticle (Originalarbeit in einer wissenschaftlichen Zeitschrift) |
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4496519 |
Kilaj, Ardita; Gao, Hong; Rösch, Daniel; Rivero, Uxia; Küpper, Jochen; Willitsch, Stefan |
Observation of different reactivities of para and ortho-water towards trapped diazenylium ions |
2041-1723 |
Nature Communications |
Publication: JournalArticle (Originalarbeit in einer wissenschaftlichen Zeitschrift) |
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4526113 |
Rivero, Uxia; Unke, Oliver T.; Meuwly, Markus; Willitsch, Stefan |
Reactive atomistic simulations of Diels-Alder reactions: The importance of molecular rotations |
0021-9606 ; 1089-7690 |
Journal of Chemical Physics |
Publication: JournalArticle (Originalarbeit in einer wissenschaftlichen Zeitschrift) |
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4600042 |
Kilaj, Ardita; Gao, Hong; Tahchieva, Diana; Ramakrishnan, Raghunathan; Bachmann, Daniel; Gillingham, Dennis; von Lilienfeld, O. Anatole; Kuepper, Jochen; Willitsch, Stefan |
Quantum-chemistry-aided identification, synthesis and experimental validation of model systems for conformationally controlled reaction studies: separation of the conformers of 2,3-dibromobuta-1,3-diene in the gas phase |
1463-9076 ; 1463-9084 |
Physical Chemistry Chemical Physics |
Publication: JournalArticle (Originalarbeit in einer wissenschaftlichen Zeitschrift) |
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4601337 |
Kilaj, Ardita; Gao, Hong; Tahchieva, Diana; Ramakrishnan, Raghunathan; Bachmann, Daniel; Gillingham, Dennis; von Lilienfeld, O. Anatole; Kuepper, Jochen; Willitsch, Stefan |
Quantum-chemistry-aided identification, synthesis and experimental validation of model systems for conformationally controlled reaction studies: separation of the conformers of 2,3-dibromobuta-1,3-diene in the gas phase |
1463-9076 eISSN: 1463-9084 cc-by |
Physical chemistry chemical physics |
Publication: JournalArticle (Originalarbeit in einer wissenschaftlichen Zeitschrift) |
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4612906 |
Wang, Jia; Kilaj, Ardita; He, Lanhai; Dlugolecki, Karol; Willitsch, Stefan; Kuepper, Jochen |
Spatial Separation of the Conformers of Methyl Vinyl Ketone |
1089-5639 |
The journal of physical chemistry. A |
Publication: JournalArticle (Originalarbeit in einer wissenschaftlichen Zeitschrift) |
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4612910 |
Rivero, Uxia; Turan, Haydar Taylan; Meuwly, Markus; Willitsch, Stefan |
Reactive atomistic simulations of Diels-Alder-type reactions: conformational and dynamic effects in the polar cycloaddition of 2,3-dibromobutadiene radical ions with maleic anhydride |
0026-8976 ; 1362-3028 |
Molecular Physics |
Publication: JournalArticle (Originalarbeit in einer wissenschaftlichen Zeitschrift) |
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