HCl - Water Clusters: Infrared Spectroscopy in He nanodroplets
HCl - Water Clusters: Infrared Spectroscopy in He Nanodroplets Steven Flynn, Alex Morrison, Tao Liang, and Gary Douberly University of Georgia Department of Chemistry 1001 Cedar St Athens GA 30602 Previous Studies of HCl H2O clusters Matrix Isolation FTIR Theoretical Studies -Florent Domine (ice films) -J.P. Devlin (ice nanocrystals) -V. Buch (ice nanocrystals) -R.B. Gerber -Many, many more Free-Jet FTIR -Martin Suhm Cavity Ringdown Microwave Spectroscopy
-Rich Saykally -Zbigniew Kisiel -R. Moszynski -J. Sadlej Other Helium Studies -Andrey Vilesov -Myong Yong Choi -Martina Havenith Instrumentation Lockheed-Martin Aculight Argos CW OPO 1MHz spectral resolution Range of 2570-4000cm-1 UGA He molecular beam instrument Average droplet size is 4000 He atoms Detection via Extrel CMS quadrupole Mass Spectrometer (Off Axis)
(HCl)m (H2O)n Survey Scan of H-Cl stretch region optimized for maximum 2:2 pickup 2774 / 2:1 2670 / 2:2 m:n 2715 / 1:1 2705 / 3:1 Bands are assigned With the aid of OSMS And PUC Pressure Dependence studies 2721 / 4:2 2650 2700 2750 -1
2800 Wavenumber (cm ) 2850 Cl---H-Cl Stretch Detected while monitoring all masses > 6 amu Detected at m/z = 19 amu (H3O+) By monitoring m/z 19 all (HCl)m clusters disappear! 2:1 Isotope Splitting Effects in the 2:1 HCl-H2O Clusters Natural Isotope Abundance 35 Cl:37Cl 3:1 Sum of simulations
Both Cls are 35 Cl(top)=37, Cl(bottom)=35 Cl(top)=35, Cl(bottom)=37 Both Cls are 37 2:1 I(field on) / I(field off) VTMA = 59.5 p= 2.39D mp2 6-311+g(3df,3pd) 1.10 1.05 Perpendicular 1.00 0.95 //
4.22D 36.6 0.4 0 Represents the structure previously assigned to the 2670 cm-1 band 10 20 30 40 Electric Field (kV/cm) 50 Simulations of Isotope Splitting 2
1 Data (m/z=19) Sum of B+C+D A) Both 1 & 2 are 35Cl B) C) D) 1=35Cl, 2=37Cl 1 & 2 =37Cl 1= 37Cl, 2= 35Cl Natural Isotope Abundance 35 Cl:37Cl 3:1 2667 2670 2673
-1 Wavenumber (cm ) Monitoring signal on mass 19 allows us to look at signal from all (HCl)2(H2O)2 isotopomers Limiting detection to mass 72 eliminates signal from clusters containing heavy Cl A) 19 u B) 72 u 2666 2668 2670 -1
2850 Acknowledgements Gary Douberly UGA Office of Vice President For Research THE GROUP Alex Morrison Tao Liang The Ohio State University University of Georgia Department of Chemistry Optically Selected Mass Spectrum OSMS Park Laser at 2670cm - Collect Mass Spectrum Peaks correspond to fragments
From ONLY those species that Are excited at the fixed laser wavelength 37 72 73 -1 m/z species 36 (HCl35)+ 37 H+(HCl35), H+(H2O)2 72 (HCl35)2+
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