Experimental and numerical investigation of a phase-only control mechanism in the linear intensity regime

• Verfasst von: Brühl, Elisabeth [VerfasserIn]
• Verfasst von: Buckup, Tiago [VerfasserIn]
• Verfasst von: Motzkus, Marcus [VerfasserIn]
• Titel: Experimental and numerical investigation of a phase-only control mechanism in the linear intensity regime
• Verf.angabe: Elisabeth Brühl, Tiago Buckup, and Marcus Motzkus
• E-Jahr: 2018
• Jahr: 7 June 2018
• Umfang: 11 S.
• Fussnoten: Gesehen am 15.10.2019
• Titel Quelle: Enthalten in: The journal of chemical physics
• Ort Quelle: Melville, NY : American Institute of Physics, 1933
• Jahr Quelle: 2018
• Band/Heft Quelle: 148(2018,2) Artikel-Nummer 214310, 11 Seiten
• ISSN Quelle: 1089-7690
• DOI: doi:10.1063/1.5029805
• Datenträger: Online-Ressource
• Sprache: eng
• K10plus-PPN: 1678911518

Abstract

Mechanisms and optimal experimental conditions in coherent control still intensely stimulate debates. In this work, a phase-only control mechanism in an open quantum system is investigated experimentally and numerically. Several parameterizations for femtosecond pulse shaping (combination of chirp and multipulses) are exploited in transient absorption of a prototype organic molecule to control population and vibrational coherence in ground and excited states. Experimental results are further numerically simulated and corroborated with a four-level density-matrix model, which reveals a phase-only control mechanism based on the interaction between the tailored phase of the excitation pulse and the induced transient absorption. In spite of performing experiment and numerical simulations in the linear regime of excitation, the control effect amplitude depends non-linearly on the excitation energy and is explained as a pump-dump control mechanism. No evidence of single-photon control is observed with the model. Moreover, our results also show that the control effect on the population and vibrational coherence is highly dependent on the spectral detuning of the excitation spectrum. Contrary to the popular belief in coherent control experiments, spectrally resonant tailored excitation will lead to the control of the excited state only for very specific conditions.