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• W2016325725 abstract "The energetics and ultrafast dynamics in the H atom transfer configuration of ammonia dimer and trimer clusters have been studied. The clusters are first excited to the electronic à state with a 208 nm femtosecond laser pump pulse. This state is allowed to relax for about 1 ps during which the H-transfer state is formed which is then electronically excited by a time-delayed infrared control pulse at 832 nm and finally ionized with a third femtosecond probe pulse at 416 nm. We have also performed complementary theoretical studies elucidating the experimental findings. For the dimer in the excited NH4(3p)⋯NH2(X̃) state the time-dependent ion signals reveal an isotope-independent short lifetime of about τ6=(130±60) fs which can be explained by a curve crossing with the repulsive NH4(3s)⋯NH2(Ã) state, whereas the trimer signal persists on a time scale being more than one order of magnitude longer and exhibits a very large isotope effect. This is interpreted as being due to internal conversion from the excited state NH3NH4(3p)⋯NH2(X̃) back to the NH3NH4(3s)⋯NH2(X̃) ground state. The analysis of the corresponding photoelectron spectra also confirms the transition energies between the electronic states involved, e.g., ΔE[NH4(3s→3p)⋯NH2]=1.5 eV and ΔE[NH3NH4(3s→3p)⋯NH2]=1.2 eV, as determined by our ab initio calculations." @default.
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• W2016325725 date "2002-01-22" @default.
• W2016325725 modified "2023-09-23" @default.
• W2016325725 title "Ultrafast photodissociation dynamics and energetics of the electronically excited H atom transfer state of the ammonia dimer and trimer" @default.
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• W2016325725 doi "https://doi.org/10.1063/1.1429952" @default.
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