Femtosecondspectroscopy of silver atoms in a xenon matrix

Abstract

The excitation of the s-p transition of single Ag atoms in a Xe matrix leads to a dynamical Jahn-Teller splitting which, in addition to the spin-orbit coupling removes the degeneracy of the excited p-orbital. The dynamics on these Jahn-Teller surfaces and the vibrational relaxation responsible for the strongly Stokes shifted emission bands are studied using pulses with 170 fs time resolution. The pulses with wavelengths around 660 nm and 330 nm and energies in the mJ-range are generated combining a commercial Titan-Sapphire laser system with a self-designed dye amplifier and are analyzed in a FROG setup. The wave packet dynamics is investigated by means of one-colour resonant pump-probe measurements that show an increase of the signal 1.3 ps after the excitation into the upper two states of the triplet. Simulations of the wave packet dynamics in the excited states support the interpretation of this increase in terms of a returning wave packet. Two-colour fluorescence depletion experiments are used to study the dynamics during the relaxation process toward the minima in the excited Jahn-Teller states. For Ag atoms in a Xe matrix the process is dominated by the absorption in energetically higher-lying states with a consequent reduction of the stimulated emission yield. An important result of these measurements is the determination of the energy of an Ag-ion state in the Xe at a value of 5.73 eV

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