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Coherent motion of low frequency vibrations in ultrafast excited state proton transfer

1999, Pfeiffer, M., Chudoba, C., Lau, A., Lenz, K., Elsaesser, T.

Photoexcitation of internal proton transfer in the tinuvin molecule causes the excitation of some low frequency vibrational modes which oscillate with high amplitudes in a coherent manner over 700 fs. Such effect is observed for the first time applying two color pump/probe measurement with 25 fs pulses. Based on resonance Raman spectra a normal coordinate analysis of the modes is performed. It is shown that the nuclear movement given by the normal vibration of one of the modes serves to open up a barrierfree proton transfer path.

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Molecular dynamics investigated by temporally two-dimensional coherent Raman spectroscopy

1999, Lau, A., Pfeiffer, M., Kozich, V., Kummrow, A.

A six-wave set-up is described to determine molecular dynamics in the condensed phase. Applying two independent time delays between excitation and probe pulses additional information on the dynamics should be obtainable. We show experimentally that such investigations can be carried out with noisy light having intensity fluctuations in the femtosecond region. As first result we found a fast relaxation time in neat nitrobenzene of 100 fs, becoming even faster in mixtures with low viscosity liquids. Switching on a Raman resonance yields a longer relaxation time, which could be explained by an additional contribution by that vibration.

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Coupling a single solid-state quantum emitter to an array of resonant plasmonic antennas

2018, Pfeiffer, M., Atkinson, P., Rastelli, A., Schmidt, O.G., Giessen, H., Lippitz, M., Lindfors, K.

Plasmon resonant arrays or meta-surfaces shape both the incoming optical field and the local density of states for emission processes. They provide large regions of enhanced emission from emitters and greater design flexibility than single nanoantennas. This makes them of great interest for engineering optical absorption and emission. Here we study the coupling of a single quantum emitter, a self-assembled semiconductor quantum dot, to a plasmonic meta-surface. We investigate the influence of the spectral properties of the nanoantennas and the position of the emitter in the unit cell of the structure. We observe a resonant enhancement due to emitter-array coupling in the far-field regime and find a clear difference from the interaction of an emitter with a single antenna.