Abstract.Coherent controls over vibrational excitations in metal di-carbonyls were demonstrated by using phase-shaped mid-infrared pulses. The phase of the inter-state coherence between two different normal-modes was controlled by changing the phase step of the stepwise spectral phase profile. The quantum interference between multiple vibrational excitation paths in resonant two-step excitations was manipulated by the similar spectral phase control. The results experimentally confirmed that coherent control over multiple vibrational degrees of freedom works properly in condensed phases. There remains the possibility for increasing excitation efficiency by introducing group-delays and by optimizing polarization state of the excitation pulse.
Motivation and ObjectivesCoherent control is a technique that manipulates interference of wave functions by adjusting their amplitudes and phases. Recent developments in the pulse shaping technique in MIR [1] may open a way toward coherent control over molecular motions/reactions at the electronic ground states. Such control may serve for novel information processing and molecular reaction controls, including bond breakage, structural isomerization, hydrogen bond rearrangement, proton transfer, etc. [2][3][4]. So far the MIR pulse shaping was applied to the ladder climbing of a single vibrational mode [5].The broadband nature of the ultrashort MIR pulses, however, should also be able to excite multiple vibrational modes in a correlated manner to control nuclear motion in multi-dimensional coordinates and to create highly-excited vibrational states. The ability to handle multiple vibrational modes should increase the variety and efficiency of controllable reactions. For such coherent control applications, control over quantum interference as well as efficient ladder climbing is essential. In this paper, we show that the quantum interferences in IR vibrational excitations were successfully controlled for liquid-phase molecules by use of MIR phase-shaping.
MIR Pulse Shaping and Transient Absorption SpectroscopyMIR pulses of 100-fs duration and 5-J energy were generated by the OPA/DFG system. Major portion of the pulse energy was delivered to the pulse shaper, consisting of diffraction gratings, concave mirrors and the germanium AOM, developed by Zanni-group [1]. The shaped pulse was characterized by the electric-field cross correlation in the spectral interferometry with a reference EPJ Web of Conferences