Journal
PHYSICAL REVIEW LETTERS
Volume 109, Issue 23, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.109.233903
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Funding
- Swiss National Science Foundation [PP00P2_128274]
- ETH Zurich [ETH-33 10-3]
- Marie Curie COFUND program
- Swiss National Science Foundation (SNF) [PP00P2_128274] Funding Source: Swiss National Science Foundation (SNF)
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We study the emission of even and odd high-harmonic orders from oriented OCS molecules. We use an intense, nonresonant femtosecond laser pulse superimposed with its phase-controlled second harmonic field to impulsively align and orient a dense sample of molecules from which we subsequently generate high-order harmonics. The even harmonics appear around the full revivals of the rotational dynamics. We demonstrate perfect coherent control over their intensity through the subcycle delay of the two-color fields. The odd harmonics are insensitive to the degree of orientation, but modulate with the degree of axis alignment, in agreement with calculated photorecombination dipole moments. We further compare the shape of the even and odd harmonic spectra with our calculations and determine the degree of orientation. DOI: 10.1103/PhysRevLett.109.233903
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