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Vibrational Spectroscopy

Electronic photon echo spectroscopy and vibrations

Niklas Christensson, Benjamin Dietzek, Arkady P. Yartsev, Tõnu Pullerits

Published Jan 25, 2010• 10 citations
Publisher
DOI
10.1016/j.vibspec.2010.01.009

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A theory of optical echo spectroscopies of large polyatomic molecules in condensed phases is developed. Using phase space correlation functions, we examine the interrelationships among the following optical measurements: ordinary photon echo, stimulated photon echo, accumulated photon echo, incoherent accumulated photon echo, and pump–probe absorption. Conditions for the elimination of inhomogeneous broadening in these experiments are specified. A multimode Brownian oscillator model is used to account for high frequency molecular vibrations, as well as solvent modes, and electronic dephasing processes. The effects of quantum beats, spectral diffusion, and homogeneous dephasing on the echo signals are studied and compared in detail with pump–probe and hole burning spectroscopy.
Semiconductor nanocrystals are a novel class of materials intermediate between the molecular and solid state forms of matter. Their homogenous linewidths and electronic structure are of considerable interest for the understanding of the physics of quantum confinement. In this work we study the electronic and vibrational dephasing dynamics in InP nanocrystals using femtosecond three pulse photon echo (3PPE) experiments1 complemented by nanosecond transient hole-burning (HB) spectroscopy.2 The echo decay is explained by taking into account the multi-level electronic structure as observed in the hole-burning experiment.