Mode selectivity with polarization shaping in the mid-IR

TitleMode selectivity with polarization shaping in the mid-IR
Publication TypeJournal Article
Year of Publication2009
AuthorsStrasfeld DB, Middleton CT, Zanni MT
Secondary TitleNew Journal of Physics
Date Published10/2009

We report that polarization-shaped mid-infrared (IR) pulses can be used to enhance the vibrational population of one mode over another in a coupled molecular system. A genetic algorithm and a new mid-IR polarization shaper were used to alter the relative vibrational excitation of the two carbonyl stretching modes in Mn(CO)5Br. One mode could be selectively enhanced over the other by 2–3 times. Control over the polarization leads to better optimization than phase-only control. Several possible mechanisms that indicate how polarization shaping leads to selective vibrational excitation are discussed using a formalism that separates polarization shaping effects on the signal strength from amplitude or phase shaping. The techniques introduced herein will have broad applications in quantum gating schemes, controlling ground state chemistry and enhancing the sensitivity of multidimensional IR and visible spectroscopies.

Short TitleNew J. Phys.