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Probing Polar Molecules with High Harmonic Spectroscopy

Eugene FrumkerJoint Attosecond Science Laboratory, University of Ottawa and National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada. [email protected]N. KajumbaJoint Attosecond Science Laboratory, University of Ottawa and National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, CanadaJ. B. BertrandJoint Attosecond Science Laboratory, University of Ottawa and National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, CanadaH. J. WörnerJoint Attosecond Science Laboratory, University of Ottawa and National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, CanadaChristoph T. HebeisenJoint Attosecond Science Laboratory, University of Ottawa and National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, CanadaPaul HockettSteacie Institute for Molecular Sciences, National Research Council of Canada, Ottawa, Ontario K1A 0R6, CanadaM. SpannerSteacie Institute for Molecular Sciences, National Research Council of Canada, Ottawa, Ontario K1A 0R6, CanadaS. PatchkovskiiSteacie Institute for Molecular Sciences, National Research Council of Canada, Ottawa, Ontario K1A 0R6, CanadaG. G. PaulusDepartment of Physics, Texas A&M University, College Station, Texas 77843, USAD. M. VilleneuveJoint Attosecond Science Laboratory, University of Ottawa and National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, CanadaA. NaumovJoint Attosecond Science Laboratory, University of Ottawa and National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, CanadaP. B. CorkumJoint Attosecond Science Laboratory, University of Ottawa and National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada

2012en

ABI

Annotatsiya

We bring the methodology of orienting polar molecules together with the phase sensitivity of high harmonic spectroscopy to experimentally compare the phase difference of attosecond bursts of radiation emitted upon electron recollision from different ends of a polar molecule. This phase difference has an impact on harmonics from aligned polar molecules, suppressing emission from the molecules parallel to the driving laser field while favoring the perpendicular ones. For oriented molecules, we measure the amplitude ratio of even to odd harmonics produced when intense light irradiates CO molecules and determine the degree of orientation and the phase difference of attosecond bursts using molecular frame ionization and recombination amplitudes. The sensitivity of the high harmonic spectrum to subtle phase differences in the emitted radiation makes it a detailed probe of polar molecules and will drive major advances in the theory of high harmonic generation.

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Identifikatorlar

DOI: 10.1103/physrevlett.109.233904

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