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Optics Letters

Photon-echo detection by six-wave mixing

Koos Duppen, Douwe A. Wiersma

Published Apr 1, 1988• 7 citations
Publisher

Abstract

Picosecond photon echoes have been generated and detected by using a resonant six-wave mixing effect. In this process, the induced echo polarization is used to drive a four-wave mixing process. The merits of this method compared with other techniques of photon-echo detection are discussed. Further examples of spectroscopically useful six-wave mixing effects are presented.

DOI
10.1364/ol.13.000318

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Phase relaxation of optical excitations in condensed matter can be studied by coherent four—wave—mixing experiments in the time domain without requiring assumptions on the spectral properties of the material. For inhomogeneously broadened transitions, three laser pulses at times t = 0, t = t21 and t = T with wave vectors k1, k2 and k3, respectively, generate a stimulated photon echo pulse, emitted time—delayed at t = T+t21 in the momentum—matching direction according to k3+k2−k1. As a function of t21 the echo amplitude decays due to scattering events, described by the dephasing time constant T2 [1].

International Conference on Ultrafast Phenomena•Jan 1, 1990•0 citations
Picosecond photon echoes have been generated and detected by using a resonant six-wave mixing effect. In this process, the induced echo polarization is used to drive a four-wave mixing process. The merits of this method compared with other techniques of photon-echo detection are discussed. Further examples of spectroscopically useful six-wave mixing effects are presented.
We demonstrate coherent control over interference between different Liouville-space pathways that describe the generation of the nonlinear optical polarization in a stimulated photon echo. This control was exercised by phase-locking of the excitation pulses and observed in the heterodyne detected echo signal. A theoretical analysis of the effect is presented and found to be in good agreement with the obtained results. The relation between this novel time-domain interference effect and the pressure-induced extra resonance in four-wave mixing spectroscopy is discussed.
The use of phase-locked pulses in various spectroscopic techniques related to the third-order polarization P(3) is analyzed. Using correlation function expressions for the nonlinear response function, we clarify the interrelationship among several photon echo, pump–probe, and spontaneous light emission techniques, without alluding to any specific model for the material system. By combining phase-locked pulses and heterodyne detection it becomes possible to probe separately the real and imaginary parts of the nonlinear response function. Combining two phase-locked pulse excitation with time-resolved detection of the spontaneous light emission allows direct separation of the Raman and fluorescence contributions.
A review of theoretical and experimental works on the polarization photon-echo spectroscopy (PPE spectroscopy) is carded out. The main attention is payed to the following advantages of the PPE spectroscopy. First, the PPE spectroscopy, free of the influence of the inhomogeneous spectral line broadening, allows to make the high precision measurements within the envelope of a inhomogeneously broadened spectral line. Second, the high resolution ability of the PPE spectroscopy, directly in the temporal field, unables to accomplish the investigations of the fast relaxation processes, when ultrashort nano- and picosecond exciting pulse are used. Third, in the PPE spectroscopy the investigated relaxation processes are not subjected to the perturbing action of the intensive laser radiation. Farther, it is necessary to note the flexibility of the PPE spectroscopy consisting in the existence of a great number of various methods used for receiving different spectroscopic information. Finally, as far as the signal intensifies of the photon echo and of its variants are proportional to the squared number of the resonant atoms (molecules), it secures the definite advantages for the PPE spectroscopy as compared to the spectroscopk methods based on the non-coherent phenomena (especially for low pressure a gas considered). The possibilities of new experiments on photon echo and its variants aimed for obtaining a detailed new spectroscopic information are discussed.
We report an experimental study of resonant six-wave mixing in coherently prepared Rb atoms. Electromagnetically induced transparency in a four-level atomic system suppresses the linear susceptibility and enhances the nonlinear susceptibilities, which leads to the resonantly enhanced, slow-photon six-wave mixing at low light intensities. The light emission in the six-wave mixing process can be viewed as resulting from diffraction of slow light off a resonant nonlinear grating induced in the four-level system by a standing-wave pump field.
Phase relaxation of optical excitations in condensed matter can be studied by coherent four—wave—mixing experiments in the time domain without requiring assumptions on the spectral properties of the material. For inhomogeneously broadened transitions, three laser pulses at times t = 0, t = t21 and t = T with wave vectors k1, k2 and k3, respectively, generate a stimulated photon echo pulse, emitted time—delayed at t = T+t21 in the momentum—matching direction according to k3+k2−k1. As a function of t21 the echo amplitude decays due to scattering events, described by the dephasing time constant T2 [1].