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Deutsche Physikalische Gessellschaft IOP Institute of Physics

Mode selectivity with polarization shaping in the mid-IR

Focus on Quantum Control

David B Strasfeld, Chris T Middleton and Martin T Zanni1

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Part of Focus on Quantum Control

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.


PACS

33.15.Kr Electric and magnetic moments (and derivatives), polarizability, and magnetic susceptibility

33.20.Ea Infrared spectra

33.20.Tp Vibrational analysis

33.15.Mt Rotation, vibration, and vibration-rotation constants

33.20.Kf Visible spectra

Subjects

Atomic and molecular physics

Dates

Issue 10 (October 2009)

Received 1 June 2009

Published 30 October 2009



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