140 likes | 215 Views
Infrared Spectroscopy of Gas Phase Protonated CO 2 Clusters. Gary E. Douberly , Allen M. Ricks, Brian W. Ticknor, and Michael A. Duncan Department of Chemsitry University of Georgia http://www.arches.uga.edu/~maduncan. Funding: National Science Foundation. Motivation.
E N D
Infrared Spectroscopy of Gas Phase Protonated CO2 Clusters Gary E. Douberly, Allen M. Ricks, Brian W. Ticknor, and Michael A. Duncan Department of Chemsitry University of Georgia http://www.arches.uga.edu/~maduncan Funding: National Science Foundation
Motivation • Implementation of pulsed electric discharge source for protonated molecular clusters • Infrared Spectroscopy of Mass-Selected Clusters • Insight into proton environment with increasing cluster size. Structural Information
Experiment Pulsed Discharge Cluster Source
300 psi 1:10:100 CO2 : H2 : (70/30) Ne/He
300 psi 1:10:20:100 CO2 : H2 : Ar : (70/30) Ne/He n=3 n=2
900 V 750 ns Tunable mid-IR 2.3-5.0 m Tunable 4.2-10.1 m OPA OPO idler KTA diff. gen. + amp of idler beam KTP oscillator LiInS2 diff. gen. 532 nm signal (not used) 4 crystals angle tuned 1 crystal angle tuned 2 crystals angle tuned LaserVision (Dean Guyer) 1064 nm
(cm-1) e eeD0 1 242.8 11.8 1130 2 182.4 3.6 2210 Protonated CO2 Dopfer O, …, Maier J; Chem Phys Lett. (1998) 296, 585.
Protonated CO2 Dimer Monomer proton stretch
Protonated CO2 Trimer (cm-1) H+(CO2)3 H+(CO2)3-Ar De Local 2630 790 De Global 3080 960
Protonated CO2 Tetramer Microsolvation of n=3 motif
H+(CO2)7 Mode specific fragmentation dynamics
Summary • Demonstration of pulsed electric discharge cluster source for argon tagged H+(CO2)n • IR spectra from 950 to 2600 cm-1 reveals a rearrangement of Dimer structural motif for n=3 • Other protonated molecular clusters studied: H+(CO)n , H+(H2O)n , H+(C3H6O)n , H+(O2)n , H+(N2)n H+(C2H2)n , H+(C2H4)n, H3+(Ar)n, etc. RF06 Protonated Acetylene and Ethylene Clusters
Protonated Acetone Monomer and Dimer eg. Loss of Ar