We calculate the photon echo decay for a strongly coupled electron–phonon system, without making unrealistic assumptions about excitation pulse durations. We find that asymptotically, the photon echo decay is exponential, and we provide a formal expression for the decay rate 1/T2 which is independent of pulse duration. In contrast to the usual results, our expression for 1/T2 is nonperturbative in the electron–phonon interaction. We calculate the dependences of the echo amplitude on pulse power and duration, finding that the strong electron–phonon coupling modifies the simple two level system result. We also focus on the relationship between the zero phonon line shape in the homogeneous optical absorption spectrum, and the photon echo decay rate. We find that the zero phonon line shape is Lorentzian, with width 1/πT2. We show that the usual optical Bloch equation approach to analyzing time-domain experiments, which normally is only applicable if the electron–phonon coupling is weak, can be extended to the case of strong coupling. These strong coupling Bloch equations are adequate for analyzing the time dependence, but not the pulse power and duration dependences, of time-domain experiments. Our results indicate that within the Condon approximation, electron–phonon coupling cannot explain the very low temperature anomaly of recent photon echo experiments on impurities in molecular crystals.
Multidimensional off resonant spectroscopy of crystals using a train of optical pulses can be effectively used to probe nuclear dynamics in solids. We predict a clear photon echo signal even in the absence of inhomogeneous broadening. This technique may be used for studying phonon dynamics in solids, in structurally frozen systems such as glasses, and in systems where the validity of the concept of phonons is not equally well established, such as liquids and gases. With this technique it is also possible to obtain information on the lifetime of phonons. We predict a long time tail of the nonlinear signal proportional to t−n/5, where n is the order of the response function studied.
An analytical study of the photon echoes associated with the three-level system interacting resonantly with optical pulses possessing two different frequencies is performed. It is predicted that photon echoes arise at anomalous times corresponding to the correlation between the inhomogeneous broadenings for the different spectral lines as well as at the normal time expected in a simple two-level system. This new effect is caused by the coupling of the two resonant transitions through the common energy level. Furthermore, if the particle does not have inversion symmetry, the echoes with the sum or difference frequency of the exciting optical pulses can be observed in such a system. The quantitative analysis is also given for intensities, direction of propagation and polarizations of the anomalous echoes which depend upon the exciting pulses with different frequency.
Fluorescence—line—narrowing, spectral hole—burning and single molecule spectroscopy are methods of selective spectroscopy using zero-phonon lines (ZPL) to make selection in molecular ensemble. However if electron-phonon coupling is strong or sample temperature is near to room temperature, ZPL are absent and the optical band consists of electron-phonon transitions which are called phonon-side-band (PSB). In these cases the above mentioned methods of selective spectroscopy do not work. Can we get an information concerning a homogeneous optical band from inhomogeneously broadened bands in these cases? The answer is yes if we use femtosecond photon echo.
Recent advances in laser technology have led to the production of ultrashort electromagnetic pulses of very high peak power. In this paper we develop a theory which describes the transient behavior of such pulses in a laser amplifier. The effects of atomic coherence and inhomogeneous broadening, necessary for a complete treatment of the problem, are included. In the present development, the degree of homogeneous and inhomogeneous broadening is variable. The two-level active atoms are characterized by a phase memory time
T2 and an inhomogeneous frequency distribution (which leads to a reversible decay time
T2∗). The field (Maxwell) and atomic (Schr\"odinger) equations are coupled in a self-consistent manner as in Lamb's theory of an optical maser. The resulting equations are solved analytically in certain limits, while the general case is integrated numerically. The emphasis is placed on the situation in which
T2∗ and the pulse width are much shorter than
T2. Thus our main effort is devoted to the physics of the inhomogeneously broadened system. The theory itself, however, contains the effects of both forms of broadening. The basic difference between inhomogeneous and homogeneous broadening is discussed. In the former case, the decay of radiation is caused by the dephasing of dipoles, and is reversible. The atomic memory is retained during the dephasing, and an internal reflection of the atomic coordinates, as is exemplified in the "photon echo" process, will cause the dipoles to rephase. The phonon interruptions or atomic collisions that bring about the homogeneous broadening are random processes which lead to an irreversible destruction of the atomic phase memory. The implications of the reversible versus irreversible decay processes are seen to have important consequences in the problem of pulse amplification.