Pump–probe spectroscopy with phase-locked pulses in the condensed phase: decoherence and control of vibrational wavepackets

Abstract

Electronic and vibrational coherences of Cl2 embedded in solid Ar are investigated by exciting to the B state with a phase-locked pulse pair from an unbalanced Michelson interferometer, where the chirp difference matches the B state anharmonicity. Recording the A' --> X fluorescence after relaxation is compared to probing to charge transfer states by a third pulse. The three-pulse experiment delivers more details on the decoherence processes. The signal modulation due to phase tuning up to the third vibrational round-trip time indicates that the electronic coherence in the B <-- X transition is preserved for more than 660 fs in the solid Ar environment where many body electronic interactions take place. Vibrational coherence lasts longer than 3 ps according to the observed half revival of the wavepacket. Control of the coupling between wavepacket motion and lattice oscillation is demonstrated by tuning the relative phase between the phase-locked pulses, preparing wavepackets predominantly composed of either zero-phonon lines or phonon side bands.

Vibrational relaxation and dephasing of Rb2 attached to helium nanodroplets

“…More recently, dephasing times as well as relaxation rates have been studied extensively by the groups of Apkarian and Schwentner by means of femtosecond spectroscopy of the vibrational dynamics of halide molecules isolated in cryogenic rare-gas matrices [32][33][34][35][36][37]. Seminal work on time-resolved measurements of the dissipative fluid dynamics in bulk He-II has been performed using femtosecond pump-probe spectroscopy of triplet He * 2 excimers created inside He-II [38].…”

Quantum Interference Spectroscopy of Rubidium-Helium Exciplexes Formed on Helium Nanodroplets

“…Different variants of WP interferometry have also been applied to simple molecules [11][12][13][14][15] and even to molecular crystals [16]. Using pump-probe spectroscopy with phase-locked pulses the dynamics of electronic as well as vibrational coherence of Cl 2 molecules embedded in solid Ar has been investigated [15].…”

Development of ultrahigh-precision coherent control and its applications

“…Moreover, the closed-loop control of pulse shapes based on the genetic algorithm has been found to be effective in controlling the dynamics of large complex molecules. 12)–16) The concept of coherent control is cross-disciplinary now, and the range of its applications includes a variety of fields such as solid-state dynamics 17)–21) and information processing with quantum states of matter.…”