Coherent Control of Atomic Dynamics with Chirped and Shaped Pulses

Jabir Chathanathil, Svetlana Malinovskaya

Solvejg Jørgensen, Ronnie Kosloff

Liat Levin, Wojciech Skomorowski, Ronnie Kosloff +2 more

Abstract The first step in the coherent control of a photoinduced binary reaction is bond making or photoassociation. We have recently demonstrated coherent control of bond making in multi-photon femtosecond photoassociation of hot magnesium atoms, using linearly chirped pulses (Levin et al 2015 Phys. Rev. Lett. 114 233003 ). The detected yield of photoassociated magnesium dimers was enhanced by positively chirped pulses which is explained theoretically by a combination of purification and chirp-dependent Raman transitions. The yield could be further enhanced by pulse optimization resulting in pulses with an effective linear chirp and a sub-pulse structure, where the latter allows for exploiting vibrational coherences. Here, we systematically explore the efficiency of phase-shaped pulses for the coherent control of bond making, employing a parametrization of the spectral phases in the form of cosine functions. We find up to an order of magnitude enhancement of the yield compared to the unshaped transform-limited pulse. The highly performing pulses all display an overall temporally increasing instantaneous frequency and are composed of several overlapping sub-pulses. The time delay between the first two sub-pulses fits very well the vibrational frequency of the generated intermediate wavepacket. These findings are in agreement with chirp-dependent Raman transitions and exploitation of vibrational dynamics as underlying control mechanisms.

Liat Levin, Daniel M. Reich, Moran Geva +3 more

Quantum coherent control of ultrafast bond making and the subsequent molecular dynamics is crucial for the realization of a new photochemistry, where a shaped laser field is actively driving the chemical system in a coherent way from the thermal initial state of the reactants to the final state of the desired products. We demonstrate here coherent control over the relative yields of Mg2 molecules that are generated via photoassociation and subsequently photodriven into different groups of final states. The strong-field process involves non-resonant multiphoton femtosecond photoassociation of a pair of thermally hot magnesium atoms into a bound Mg2 molecule and subsequent molecular dynamics on electronically excited states. The branching-ratio control is achieved with linearly chirped laser pulses, utilizing the different chirp dependence that various groups of final molecular states display for their post-pulse population. Our joint experimental and theoretical study establishes the feasibility of high degree coherent control over quantum molecular dynamics that is initiated by femtosecond photoassociation of thermal atoms.

Gagik P. Djotyan, Jozsef S. Bakos, Zs. Sörlei +7 more

Parvendra Kumar