Pump-Probe Spectroscopy, Photon Echoes and Vibrational Wavepackets

Niklas Christensson, Benjamin Dietzek, Arkady P. Yartsev +1 more

Niklas Christensson, Arkady P. Yartsev, Tõnu Pullerits

Yi Jing Yan, Shaul Mukamel

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.

P. R. Berman

Samansa Maneshi, Chao Zhuang, Christopher R. Paul +2 more

Motivated by our observation of fast echo decay and a surprising coherence freeze, we have developed a pump-probe spectroscopy technique for vibrational states of 85Rb atoms in an optical lattice to gain information about the memory dynamics of the system. We monitor the time-dependent changes of frequencies experienced by atoms and characterize the probability distribution of these frequency trajectories. We show that the inferred distribution, unlike a naive microscopic model of the lattice, correctly predicts the main features of the observed echo decay.