Dynamics of transition metal ion molecule reactions
We are interested in how chemical reactions proceed at the atomic level, that is how atoms rearrange during the reaction and how energy is partitioned in the product channels. To gain insight into these fundamental process we investigate the dynamics of reactive collisions. Our experiment uses a combination of crossed beams with 3D velocity map imaging by recording product ion velocity distributions. Due to our single collision conditions we can control the collision energy of our reactive collision of choice.
Our research investigates the activation of small molecules by transition metal ions. We aim at mechanistic insight, e.g. if the atomistic mechanisms are direct or indirect. Transitions metal ions are known for their state-selective chemistry and we are interested in the influences of electronic states on the dynamical signatures or that of the principle of two state reactivity. Our chosen neutral reactants are small molecules for which the initial bond activation presents the rate limiting step. Currently we focus on methane and carbon dioxide or small olefins.
In the experiment, we prepare a beam of atomic cations of the respective transition metal and cross it with a molecular beam of the neutral reactant. Product ions are mapped onto a position and time sensitive detector. The recorded experimental angle and energy product ion velocity distributions correspond to differential scattering cross sections. The DCS contains signatures which we can interpret in light of atomistic mechanisms.
Dynamics of CH-bond activation
- J. Meyer, V. Tatji, E. Carrascosa, T. Gyori, M. Stei, T. Michaelsen, B. Bastian, G. Czakó, R. Wester; Atomistic dynamics of elimination and substitution disentangled for the F- + CH3CH2Cl reaction, Nat. Chem.2020
- J. Meyer, E. Carrascosa, T. Michaelsen, B. Bastian, A. Li, H. Guo, R. Wester, Unexpected Indirect Dynamics in Base-Induced Elimination. J. Am. Chem. Soc. 2019, 141, 20300
- M. Stei, E. Carrascosa, A. Dörfler, J. Meyer, B. Olasz, G. Czakó, A. Li, H. Guo, R. Wester, Stretching vibration is a spectator in nucleophilic substitution. Sci. Adv. 2018, 4, eaas9544
- E. Carrascosa, J. Meyer, T. Michaelsen, M. Stei, R. Wester, Conservation of direct dynamics in sterically hindered SN2/E2 reactions. Chem. Sci.2018, 9, 693
- J. Meyer, R. Wester, Ion-Molecule Reaction Dynamics, Annu. Rev. Phys. Chem.2017, 68, 333,
- E. Carrascosa, J. Meyer, R. Wester, Chem. Soc. Rev.2017, 46, 7498
- E. Carrascosa, J. Meyer, J. Zhang, M. Stei, T. Michaelsen, W. L. Hase, L. Yang, R. Wester, Imaging dynamic fingerprints of competing E2 and SN2 reactions, Nature Comm.2017, 8, 25
- M. Stei, E. Carrascosa, M. A. Kainz, M. A.; A. H. Kelkar, J. Meyer, I. Szabó, G. Czakó, R. Wester, Influence of the leaving group on the dynamics of a gas-phase SN2 reaction, Nature Chem. 2016, 8, 151
- J. Meyer, M. Tombers, C. van Wüllen, G. Niedner-Schatteburg, S. Peredkov, W. Eberhardt, M. Neeb,S. Palutke, M. Martins, W. Wurth, The spin and orbital contributions to the total magnetic moments of free Fe, Co, and Ni clusters, J. Chem. Phys.2015, 143, 104302
- D. Dieleman, M. Tombers, L. Peters, J. Meyer, S. Peredkov, J. Jalink, M. Neeb, W. Eberhardt, T. Rasing, G. Niedner-Schatteburg, A. Kirilyuk, Orbit and spin resolved magnetic properties of size selected [ConRh]⁺ and [ConAu]⁺ nanoalloy clusters, Phys. Chem. Chem. Phys.2015, 17, 28372
- S. Peredkov, M. Neeb, W. Eberhardt, J. Meyer, M. Tombers, H. Kampschulte, G. Niedner-Schatteburg, Spin and Orbital Magnetic Moments of Free Nanoparticles, Phys. Rev. Lett.2011, 107, 23340