It is demonstrated by theory and experiment that it is possible to excite coherence uniformly in three-level systems with a wide range of anharmonicities by using a composite pulse excitation method. The theory is based on a formal analogy between the anharmonic three-level case and the simpler system with equally spaced energy levels where composite pulse techniques are already well known to compensate for the effects of mismatch between photon energies and level separations. Computer simulations and solid-state NMR experiments on the three-level system of deuterium (spin 1) verify the uniformity of the excitation. The NMR powder spectrum of deuterated polymethylmethacrylate is faithfully reproduced even using a radio-frequency (rf) field strength weaker than the quadrupole interactions.
It is demonstrated by theory and experiment that it is possible to excite coherence uniformly in three-level systems with a wide range of anharmonicities by using a composite pulse excitation method. The theory is based on a formal analogy between the anharmonic three-level case and the simpler system with equally spaced energy levels where composite pulse techniques are already well known to compensate for the effects of mismatch between photon energies and level separations. Computer simulations and solid-state NMR experiments on the three-level system of deuterium (spin 1) verify the uniformity of the excitation. The NMR powder spectrum of deuterated polymethylmethacrylate is faithfully reproduced even using a radio-frequency (rf) field strength weaker than the quadrupole interactions.
Experimentally achievable conditions where only weak off-resonant fields are used to excite coherence in a two-level system are explored. A brief review of previous theoretical results useful in treating multifrequency irradiation sequences is provided. Using an approximation method based on the Floquet formalism we derive an expression for the effective field strength as a function of the phases and amplitudes of the applied irradiation fields. Some of these results are rederived and/or explained in a simplified manner. Under conditions of four-frequency irradiation, three-photon excitation of a two-level system in NMR is experimentally demonstrated on the spin-1/2 system of the 31P nucleus in phosphoric acid. The behavior of the three-photon resonance is explored as a function of all important experimental parameters. The results of these tests conform closely to the theoretical predictions. Possible uses of multifrequency irradiation schemes in NMR are suggested.
The increasing interest in the study of the interaction of several resonant fields with multilevel quantum systems is due to a wide range of possible applications of various effects observed in the multi-frequency excitation of quantum objects. Among them, we can note color echo holography, information compression in three-level environments, copying of quantum information, and multi-level quantum gates that perform logical operations. In addition, the recording and reproduction of echo holograms in multi-level systems leads to the possibility, along with logical operations, to perform a change in the real-time scale and the sequence of events in the echo-hologram response, the data on which were embedded into the temporal structure of the object laser pulse. The formation of optical transient processes in multilevel systems occurs when the short laser pulses separated in time and resonant of different frequency transitions at the substance have an effect on the system, so that their interaction with each other becomes possible only through the medium and only if the medium has a sufficiently long phase memory. In this situation, each laser pulse transmits information about its wave characteristics to the medium, and this information is retained here until the arrival of the next laser pulses. The formation of optical transient processes in a multilevel system in a solid depends essentially on the degree of correlation of the inhomogeneous broadening on different frequency transitions and different time intervals, in connection with the possible destruction of the reversible phase memory of the system due to a partial mutual fixation energies of transitions. The influence of external spatially inhomogeneous electric fields on the resonant medium can lead to an additional artificially created inhomogeneous broadening. In this case, it is possible to control the phase memory of the system by changing the parameters of external spatially inhomogeneous electric fields, and the most pronounced effect on phase memory is the case of laser excitation of narrow frequency regions of inhomogeneously broadened lines of the resonance transitions. Moreover, the artificially created inhomogeneous broadening by external spatially inhomogeneous electric fields due to the Stark effect can be comparable with the spread of frequencies due to a partial mutual fixation of the transition energies, which leads to a partial restoration of the coherence of the multilevel system. This effect can lead to an increase in the intensity of the response of the stimulated photon echo (SPE) in the three-level system, which is the opposite effect of photon echo locking.
In this series of papers we report on the generation and application of multiple pulse phase coherent sequences in optical spectroscopy.In this paper the effects of intense pulse trains on systems with only two resonant energy levels are analyzed, with particular attention to the effects of extreme inhomogeneous broadening and population depletion to nonresonant levels.It is shown that these effects, which are present in virtually all optical systems, make the simple gyroscopic model of optical coherent transients invalid.Exact calculations show, e.g., that a two-pulse photon echo is not maximized by a 1:2 length ratio for the pulses; that the maximum excited state population is not created by a 180" pulse; and that three equal pulses are almost as effective as a 1:2:1 ratio for producing three pulse echoes.The role of pulse phase is extensively analyzed.Pulse sequences are proposed and experimentally demonstrated which permit optical phase sensitive detection and measurement of ground state relaxation parameters.The experimental results are based on an extension of the acousto-optic modulation and fluoresence detection techniques of Zewail and Orlowski [Zewail et al., Chem.Phys.Lett.48, 256 (1977); Orlowski et al., ibid.54, 197 (1978)).The relative merits offluorescence and transverse polarization detection are discussed, and fluorescence detection is shown to be more generally useful for these new sequences.Finally, composite pulse trains are shown to be capable of substantially increasing the signal available from highly inhomogenously broadened transitions.In paper II we extend the treatment to multilevel systems with some emphasis on solid state applications.
In this series of papers we report on the generation and application of multiple pulse phase coherent sequences in optical spectroscopy. In this paper the effects of intense pulse trains on systems with only two resonant energy levels are analyzed, with particular attention to the effects of extreme inhomogeneous broadening and population depletion to nonresonant levels. It is shown that these effects, which are present in virtually all optical systems, make the simple gyroscopic model of optical coherent transients invalid. Exact calculations show, e.g., that a two-pulse photon echo is not maximized by a 1:2 length ratio for the pulses; that the maximum excited state population is not created by a 180° pulse; and that three equal pulses are almost as effective as a 1:2:1 ratio for producing three pulse echoes. The role of pulse phase is extensively analyzed. Pulse sequences are proposed and experimentally demonstrated which permit optical phase sensitive detection and measurement of ground state relaxation parameters. The experimental results are based on an extension of the acousto-optic modulation and fluoresence detection techniques of Zewail and Orlowski [Zewail et al., Chem. Phys. Lett. 48, 256 (1977); Orlowski et al., ibid. 54, 197 (1978)]. The relative merits of fluorescence and transverse polarization detection are discussed, and fluorescence detection is shown to be more generally useful for these new sequences. Finally, composite pulse trains are shown to be capable of substantially increasing the signal available from highly inhomogenously broadened transitions. In paper II we extend the treatment to multilevel systems with some emphasis on solid state applications.
Photon echoes, observed recently in ruby and in NH2D gas by two-pulse laser excitation, exhibit a modulation behavior as the pulse delay time is varied. The effect, which arises in a three-level quantum system, is due to the interference of two optically coupled transitions that share a common level. In this article, the three-level echo problem is treated exactly. Wave-function solutions are incorporated that are handled conveniently by a Laplace-transform technique. We, therefore, extend the earlier theory of echo modulation by Lambert et al., by removing their restriction of on-resonance pulse excitation. This procedure allows us to examine the effect of inhomogeneous broadening on echo amplitude explicitly, and we treat the problem by numerical and also by analytical means for the case of a Doppler-broadened gas. Analytic expressions are derived either for a high or a low laser power regime corresponding to excitation of either a large or a small fraction of the Doppler linewidth. The former case is analogous to pulsed nuclear magnetic resonance and is well known, whereas the latter result is new and applies to current photon echo measurements.
Abstract When a two-level system is driven on resonance by a strong incident field, its emission spectrum is characterized by the well-known Mollow triplet. If the absorption from the excited state, in this continuously driven two-level system, to a third, higher energy level, is probed by a weak field, the resulting absorption spectrum features the Autler-Townes doublet with two peaks separated by the Rabi frequency of the strong driving field. It has been shown that when the two-level system is instead driven by a periodic pulse sequence, the emission spectrum obtained has similarities with the Mollow triplet even though the system is only driven during the short application time of the pulses and is allowed to evolve freely between pulses. Here, we evaluate the absorption spectrum of the three-level system in the ladder/cascade configuration when the bottom two levels are driven by a periodic pulse sequence while the transition between the middle and the highest level is probed by a weak field. The absorption spectrum displays similarities with the Autler-Townes doublet with frequency separation between the main peaks defined by the inter-pulse delay. In addition, this spectrum shows little dependence on the pulse carrier frequency. These results demonstrate the capacity to modulate the absorption spectrum of a three-level system with experimentally achievable pulse protocols.