Studies of Transient Neutral Molecules by Dissociative Photodetachment of Cooled Molecular Anions Christopher Johnson Continetti Research Lab University.

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Presentation transcript:

Studies of Transient Neutral Molecules by Dissociative Photodetachment of Cooled Molecular Anions Christopher Johnson Continetti Research Lab University of California, San Diego June 22, 2010

PPC Experiments Create precursor anion of interest Detach a single electron, collect it and resulting neutral fragments in coincidence (Dissociative Photodetachment) Full kinematic description of dissociation event DirectIndirect KE tot KE max KE tot KE max

Internal Excitation Effects Product Internal Excitation – Cold anions ABC - -> A + BC(v=0,1) + e - Gain internal energy, lose kinetic energy v=0 v=1 KE max ABC - A+BC

Internal Excitation Effects Anion Internal Excitation – Hot anions ABC - (v=0,1) -> A + BC(v=0) + e - Gain kinetic energy for given internal energy v=0 v=1 KE max ABC - A+BC

PPC Spectrometer with Trapping Electron and multiparticle neutral time and position detectors High duty cycle, trapping for many seconds at torr Ions Bunched, phase locked with external laser

HOCO Background Combustion intermediate Benchmark 4-atom complex forming system Complex PES QCT and Quantum Dynamics struggle with H + CO 2 Difficult to isolate HOCO - + hν ->HOCO* + e - OH + CO + e - H + CO 2 + e -

Channel-Resolved PE Spectra Black – “cold” data Gray – “hot” data Solid – trans- limit Dashed – cis-limit HOCO H + CO 2 OH + CO E hν = 3.20 eV (388 nm) Calculated Potential Energy Surface Photoelectron Spectra ZPE corrected Yu, Muckerman & Sears, 2001 Clements, Continetti & Francisco, 2002

OH + CO Channel eKE max Etot max Internal excitation! HotCold Hot anions => Significant enhancement of OH + CO channel!

H + CO 2 Channel eKE max Etot max eKE max -C 2v HotCold Possibly 0.2 – 0.5 eV in CO 2 product

Energy-Resolved Branching Ratios Processes occurring over > 6 orders of magnitude of time Possible to extract tunneling info using rate calculations? OH + CO H + CO 2 HOCO Transition regions

Conclusions Dynamical processes on HOCO PES revealed and well-separated Unambiguous dissociation below the calculated barriers to H + CO 2 Suggestion of a different route to H + CO 2 Need for better PES in the H + CO 2 region! See also: Johnson & Continetti, JPC Lett 1, 1895 (2010) Acknowledgements: D. Zajfman, M. Rappaport, Weizmann Inst. R. Thomas, R. Vane, M. Fogle Current and past members of the Continetti Lab US Department of Energy

Cold HOCO - Near-threshold photoelectron spectrum (hν = 1.60 eV) Calculated Adiabatic Electron Affinities (1) CCSD(T)/ G(3df,3pd) (1) Clements, Continetti and Francisco 2002

Linear Electrostatic Ion Beam Trap Beam Environment: ~ 20 K Background Pressure: < torr Beam Lifetimes: Many seconds Beam Energies: 4 – 16 keV Ion Frequency: 50 – 500 kHz Zajfman & co-workers 1998 GND + V - V Laser e-e-

Synchronization Clock source for experiment is laser fiber oscillator Phase lock function generator to laser fiber frequency Bunch ions with small RF voltage from generator Simple phase control

O 4 - Coincidence ms trapping time ms trapping time Dissociative Photodetachment Ionic Photodissociation