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Gary E. Douberly and Roger E. Miller

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1 Gary E. Douberly and Roger E. Miller
The HCN-Ca and HCN-Sr Complexes Formed on the Surface of Helium Nanodroplets: Spectroscopic Probes of Solvation Dynamics Gary E. Douberly and Roger E. Miller Department of Chemistry University of North Carolina at Chapel Hill NSF-Chemistry AFOSR

2 different; in particular, the dimple has to be much more pronounced…”
“…the binding to the helium environment, if compared to the alkalis, is quite different; in particular, the dimple has to be much more pronounced…” F. Stienkemeier, F. Meier, and H. O. Lutz J. Chem. Phys. 107 (24) 1997 Ancilotto Parameter 2-1/6-1re Solvated >1.9 Surface Bound <1.9 F. Ancilotto, et al. J. Low Temp. Phys. 101 (1995) 1123 HCN ~20 Na 0.7 Mg 2.62 Ca 2.08 Sr 1.95 C. C. Lovallo and M. Klobukowski Chem. Phys. Lett. 373 (2003) 439

3 Ancilotto Parameter 2-1/6-1re Solvated >1.9
HCN-Ca HCN-Mg I=255 amu-Å2 I=4x104 amu-Å2 HCN-Na Lambda is a measure of the relative stability of surface and solvated states Ancilotto Parameter 2-1/6-1re Solvated >1.9 Surface Bound <1.9 F. Ancilotto, et al. J. Low Temp. Phys. 101 (1995) 1123 HCN ~20 Na 0.7 Mg 2.62 Ca 2.08 Sr 1.95 C. C. Lovallo and M. Klobukowski Chem. Phys. Lett. 373 (2003) 439

4 Same dipole moment =6.9 Debye Increasing Field

5 Solvated Surface Increasing Droplet Size

6 Intensity Ratio Independent of Pick-up Order

7 HCN-Sr One Band Surface Bound
Reminiscent of HCN-Alkali

8 HCN-(Sr)3 (Solvated) HCN-Sr (Surface Bound)

9 How does vibrational excitation affect the downstream populations?
Solvated Surface Increasing Droplet Size

10 Pump Detune Pump

11 To Surface Bound Species
Pump Solvated N=17000 Increasing Droplet Size N=1000 Population Transfer To Surface Bound Species

12 Population Transfer To Solvated Species
Pump Surface Bound N=17000 Increasing Droplet Size N=1000 Population Transfer To Solvated Species

13 Increasing Droplet Size

14 Barrier height decreases with increasing
HCN-X (X=Ca, Sr) complexes form on the surface of helium droplets Droplet size dependent Barrier to solvation HCN-Ca Condensation Energy (~600 cm-1) larger than Barrier for N < 5000 HCN-Sr Condensation Energy less than barrier for N < 17000 However, barrier is less than photon energy (3000 cm-1) for N < 8000 Surface Bound Solvated Barrier height decreases with increasing droplet size

15 Acknowledgements Roger Miller The Miller Group Kevin Lehmann Roman Schmied

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