Ultrafast molecular photodissociation dynamics studied by femtosecond photoelectron-photoion coincidence spectroscopy Bernhard Thaler Graz University.

Slides:

Advertisements

Similar presentations

Drew Rotunno Mentor: Dr. Itzik Ben-Itzhak, Bethany Joachim Bethany Joachim.

Advertisements

Lecture 7 Photoionization and photoelectron spectroscopy

Influence of solvation on 1-aminonaphthalene photophysics: ultrafast relaxation in the isolated molecule, molecular clusters and solution by Raúl Montero,

O BSERVATION OF ULTRAFAST CHARGE MIGRATION IN AN AMINO ACID SDG, Durham, January 2013 L OUISE B ELSHAW Observation of Ultrafast.

Frequency and Time Domain Studies of Toluene Adrian M. Gardner, Alistair M. Green, Julia A. Davies, Katharine L. Reid and Timothy G. Wright.

Ultraviolet Photodissociation Dynamics of the Cyclohexyl Radical Michael Lucas, Yanlin Liu, Jingsong Zhang Department of Chemistry University of California,

Generation of short pulses

Adenine Ultrafast Dynamics of N-H and O-H Bond Dissociation in Biomolecules K. L. Wells, A. I. Janjuah and V. G. Stavros Department of Chemistry, University.

Strong-field physics revealed through time-domain spectroscopy Grad student: Li Fang Funding : NSF-AMO May 20, 2009 DAMOP Charlottesville, VA George N.

TOF Mass Spectrometer &

1 Femtosecond Time and Angle-Resolved Photoelectron Spectroscopy of Aqueous Solutions Toshinori Suzuki Kyoto University photoelectron.

Xinxin Cheng, Yao Zhang, Michael P. Minitti, Sanghamitra Deb, James Budarz, Peter M. Weber Chemistry Department Brown University 66 th OSU International.

Pump-Probe Photoionization & Mass Spectroscopy of Pentamethylcyclopentadiene Fedor Rudakov Peter Weber Molecular Spectroscopy June 21, 2007.

Fragmentation mechanisms for Methane induced by electron impact

Evidence of Radiational Transitions in the Triplet Manifold of Large Molecules Haifeng Xu, Philip Johnson Stony Brook University Trevor Sears Brookhaven.

Laboratory for Optical Physics and Engineering MOLECULAR SPECTROSCOPY OF RARE EARTH AND METAL-HALIDE MOLECULES International Symposium on Molecular Spectroscopy.

Vibrational Relaxation of CH 2 ClI in Cold Argon Amber Jain Sibert Group 1.

Ultraviolet Photodissociation Dynamics of the 3-Cyclohexenyl Radical Michael Lucas, Yanlin Liu, Jasmine Minor, Raquel Bryant, Jingsong Zhang Department.

The Ohio State UniversityDepartment of Chemistry Ultrafast Vibrational Cooling Dynamics in 9Methyladenine Observed with UV Pump/UV Probe Transient Absorption.

Ionization Energy Measurements and Spectroscopy of HfO and HfO+

Femtosecond Laser Spectroscopy of C 60 Nieuwegein, The Netherlands August 21, 2001 Eleanor Campbell, Göteborg University & Chalmers, Sweden R.D. Levine,

W I S S E N T E C H N I K L E I D E N S C H A F T  Januar 13 Name und OE, Eingabe über > Kopf- und Fußzeile.

Sanghamitra Deb, Michael P. Minitti, Peter M. Weber Department Of Chemistry Brown University 64 th OSU International Symposium on Molecular Spectroscopy.

1 Pengqian Wang Department of Physics Western Illinois University March 4, 2013.

Chan Ho Kwon, Hong Lae Kim, and Myung Soo Kim* National Creative Research Initiative Center for Control of Reaction Dynamics and School of Chemistry, Seoul.

Wave packet dynamics in atoms and molecules Eva Heesel Corinne Glendinning Helen Fielding Department of Chemistry University College London UCL Progress.

of Xenon Collision Dimers in the VUV Energy Region

Photoionization induced intermolecular proton transfer in the CH ●●● O hydrogen bonded cyclopentanone dimer in the gas phase Arup K. Ghosh, Piyali Chatterjee.

Gas phase spectroscopy at the CLS

PFI-ZEKE Spectroscopy of Aluminum-Imidazole and -Pyrimidine Complexes JUNG SUP LEE, XU WANG, SERGIY KRASNOKUTSKI, and DONG-SHENG YANG University of Kentucky.

Main Title Manori Perera 1 and Ricardo Metz University of Massachusetts Amherst 64 th International Symposium on Molecular Spectroscopy June 25th, 2009.

Laser Spectroscopy of the C 1 Σ + – X 1 Σ + Transition of ScI ZHENWU LIAO, MEI YANG, MAN-CHOR CHAN Department of Chemistry, The Chinese University of Hong.

Intramolecular Energy Redistribution in C 60 M. Boyle, Max Born Institute.

Production of vibrationally hot H 2 (v=10–14) from H 2 S photolysis Mingli Niu.

An Ongoing Study of Electronic Communication in Covalently v. Non-Covalently Bound Polyfluorene Systems 2015 International Symposium of Molecular Spectroscopy.

BORONYL MIMICS GOLD: A PHOTOELECTRON SPECTROSCOPY STUDY Tian Jian, Gary V. Lopez, Lai-Sheng Wang Department of Chemistry, Brown University International.

Resonance-enhanced Photoassociative Formation of Ground-state Rb 2 and Spectroscopy of Mixed-Character Excited States H.K. Pechkis, D. Wang, Y. Huang,

Ultrafast Excited State Raman Spectroscopy

Intense laser field interaction with molecular ions Daniel Strasser

Photoelectron Spectroscopy of Doped Helium Nanodroplets

Modeling Auger processes DUE to high Intensity, ultrafast x-ray pulses

Dissociation of Molecular Ions Studied by

Example: Fragmentation of argon tetramer after sudden ionisation

Photoelectron Velocity Map Imaging of Vibrationally Excited, Gas-phase Biomolecules and their Anions Daniël Bakker, Sjors Bakels, Rutger van der Made,

Department of Chemistry

Dynamic time-resolved chirped-pulse rotational spectroscopy in a room temperature flow reactor Daniel zaleski, lawrence Harding, stephen klippenstein,

University of Missouri – Kansas City

Curtin University, Perth, Australia

N2 Vibrational Temperature, Gas Temperature,

Optical Stark Spectroscopy and Hyperfine study of Gold Sulfide (AuS)

Electronic Spectrum of Cryogenic Ruthenium-Tris-Bipyridine Dications

CO Stark Shift to Probe the Ionic Liquid-Ag Interface

Metastable States Arising from the Ablation of Solid Copper

Gas Phase IR and UV Spectroscopy of Neutral Contact Ion Pairs

(Kobe Univ. ) Takumi Nakano, Ryo Yamamoto, Shunji Kasahara

71 st International Symposium on Molecular Spectroscopy

Electron Transfer in cluster Anions:

Femtosecond Dynamics in the Photoprotection in Thymine

Single molecule spectroscopy: towards precision measurements on CaH+

Tunneling splittings in PH3+ and AsH3+ studied by zero-kinetic energy (ZEKE) photoelectron spectroscopy Yuxiang Mo Department of Physics, Tsinghua University,

PUMP-PROBE DELAYED IONIZATION STUDY OF PHENYLACETYLENE

International Symposium on Molecular Spectroscopy

Electronic Relaxation Processes of Transition Metal Atoms in Helium Nanodroplets Andreas Kautsch, Institute of Experimental Physics ISMS, 06/09/2014.

Frauke Schroeder and Edward R. Grant Department of Chemistry

PROBING THE MOLECULAR DYNAMICS OF A Cu(CD3OD) CLUSTER WITH

Electron Transfer in cluster Anions:

Simulation of Time-Resolved Carrier Dynamics

Recent Physics and Future Developments

Department of Chemistry University of Kentucky

Time-Resolved Recombination Dynamics of Large IBr-(CO2)n (n=11-14) Clusters Joshua P. Martin, Joshua P. Darr, Jack Barbera, Matt A. Thompson, Robert.

Presentation transcript:

Ultrafast molecular photodissociation dynamics studied by femtosecond photoelectron-photoion coincidence spectroscopy Bernhard Thaler Graz University of Technology, Institute of Experimental Physics International Symposium on Molecular Spectroscopy 2017

Motivation: time-resolved coincidence measurements in the gas phase population transfer energy conversion => fragmentation photoionization => fragmentation in neutral or ion? relaxation always to lowest states (Kashas rule) => Energy conversion leads to fragmentation

Time Resolved PhotoElectron PhotoIon COincidence (PEPICO) Spectroscopy electron kinetic energy ion masses

Time Resolved PEPICO: Experiment Time-of-Flight SHG / THG SHG magnetic bottle HV

Toy molecule acetone: electronic structure D0 Sn Rydberg series : 3p acetone IC mention Acetone as the standard ketone, π- π* S0 Shastri, A. Singh, PJ., J. Quant. Spectr. Rad. Trans., V.273, 92-105, 2016 Diau, EW., Kotting C., Solling T., Zewail, AH.Chem. Phy. Chem. 3, 57-78, 2002

Activation energy for fragmentation D0 Sn : 3p ΔE π- π* S0 Energy conversion threshold: (0.79 ±0.03) eV Koch M., Heim P., Thaler B., Kitzler. M., Ernst, WE., J. Phys. B: At. Mol. Opt. Phys. 50, 125102, 2017

Population transfer τ1 = 320 fs τ1 τ2 τ2 = 80 – 130 fs D0 Sn : 3p π- π* τ2 τ2 = 80 – 130 fs S0 Koch M., Thaler B., Heim P., Ernst W.E., submitted, 2017

Population transfer τ1 = 230 fs τ2 τ2 = 80 – 130 fs D0 Sn : 3p π- π* Koch M., Thaler B., Heim P., Ernst W.E., submitted, 2017

Fragmentation in the ion AND the neutral Δt = 20 ps Sn ? Norrish Type 1 dissociation : 3p 3p, 3d,… Sn π- π* excited acetyl 3p S0 Maierhofer P., Bainschab M., Thaler B., Heim P., Ernst W.E., Koch M., J. Phys. Chem. A 120, 6418-23, 2016

Motivation and Outlook Sn : 3p directly observe population transfer to lower states: 3s and π- π* 3s π- π* work in progress: access states directly: OPA

Conclusions couplings of Rydberg series with valence states (π- π*) provide very efficient relaxation pathways we observe direct population transfer between Rydberg states the energy conversion causes fragmentation of the molecule PEPICO spectroscopy allows to distinguish fragmentation in the ion or in the neutral

Acknowledgements Femtosecond Dynamics group: Sascha Ranftl Stefan Cesnik Ass. Prof. Dr. Markus Koch Bernhard Thaler Pascal Heim Leonhard Treiber Institute of Experimental Physics Financial support:

Thank you for your attention!

Ultrafast photodissociation dynamics in gas phase acetone vary pulse length rise of electron band of lower Rydberg states for longer pulses => population transfer within pulse duration strong increase of acetyl signal for negatively chirped pulses => different relaxation channels are activated Koch M., Heim P., Thaler B. et. al., J. Phys. B: At. Mol. Opt. Phys. 50, 125102, 2017

Ultrafast photodissociation dynamics in gas phase acetone time resolved study population decrease in Sn plateau for the 3p/3d/… states => direct observation of population transfer Koch M., Heim P., Thaler B. et. al., J. Phys. B: At. Mol. Opt. Phys. 50, 125102, 2017