Heidelberg 2015 – wissenschaftliches Programm
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MO: Fachverband Molekülphysik
MO 2: Quantum Control
MO 2.2: Vortrag
Montag, 23. März 2015, 12:00–12:15, PH/HS1
Combination of Chirped and Multipulse Excitation: Control of Population and Vibrational Coherence — •Elisabeth Brühl1, Iduabo John Afa2, Carles Serrat2, Tiago Buckup1, and Marcus Motzkus1 — 1Physikalisch-Chemisches Institut, Ruprecht-Karls-Universität Heidelberg, D-69120 Heidelberg, Germany — 2Universitat Politècnica de Catalunya, Department de Fisica i Enginyeria Nuclear, Colom 11, 08222 Terrassa, Spain
Tailoring molecular vibrations is a potential control knob to steer photochemical reactions. Electronic near-resonant excitation with multipulses has been shown to enhance vibrational coherence in the excited state [1]. Additionally, vibrational coherence of the ground state can be also manipulated by using chirped pump pulses via intrapulse impulsive Raman scattering [2]. These two methods of mode selective control with tailored pump beams are now combined to tailor vibrational coherence and population in the electronic excited as well as in the ground state. This is demonstrated by systematic phase shaping of the excitation pulse in transient absorption of dye molecules. A four-level density matrix model is developed to simulate the enhancement and suppression of population and vibrational coherence using such chirped multipulse excitation. The effect of overlap between the excitation and absorption spectra, the degree of chirped excitation and the role of the molecular mode frequency are discussed.
[1] Buckup et al., JPB 2008, 41, 074024.
[2] Wand et al., PCCP 2010, 12, 2149.