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Applied Physics Letters

Enhancement of the optical nonlinearity in pseudoisocyanine J aggregates embedded in distributed feedback microcavities

Fumio Sasaki, Sora Kobayashi, Satoshi Haraichi

Published Jul 15, 2002• 9 citations
Publisher

Abstract

Coherent transients of pseudoisocyanine J aggregates in distributed feedback microcavities are reported. Under the resonant excitation of the cavity-mode observed at the low-energy side of the excitonic resonance, the response time is about 0.5 ps, approximately equal to the pump–pulse duration. We find the enhancement of the optical nonlinearity by one order of magnitude in the microcavity. The excitation of the dielectric-band mode is effective to enhance the nonlinearity with the ultrafast response.

DOI
10.1063/1.1493643

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Coherent transients of pseudoisocyanine J aggregates in distributed feedback microcavities are reported. Under the resonant excitation of the cavity-mode observed at the low-energy side of the excitonic resonance, the response time is about 0.5 ps, approximately equal to the pump–pulse duration. We find the enhancement of the optical nonlinearity by one order of magnitude in the microcavity. The excitation of the dielectric-band mode is effective to enhance the nonlinearity with the ultrafast response.
Results of coherent transients of pseudoisocyanine J aggregates in distributed feedback microcavities are reported. Under resonant excitation of the cavity-mode observed at the low energy side of the excitonic resonance, the response time is less than 1 ps, approximately equal to the pump pulse duration. We find an enhancement of the optical nonlinearity by one-order of magnitude in the microcavity. The excitation of the cavity-mode is effective in enhancing the nonlinearity with ultrafast response.
J-aggregates are the subject of great interest due to high values of optical susceptibilities of intensive excitonic resonance, originated from delocalization of electronic excitation in molecular aggregate. In [1,2] resonant enhancement of third-order susceptibiltity of J-aggregates of pseudoisocyanine (PIC) solutions was observed. The dephasing time of excitonic transition of PIC J-aggregate solutions was determined in [3] as 16 ps by low-temperature photon echo, and T2=0.17 ps at room temperature by measuring the dispersion of nonlinear susceptibility in the process of four-wave mixing [2].
We predict that an ensemble of organic dye molecules with permanent electric dipole moments embedded in a microcavity can lead to strong optical nonlinearities at the single-photon level. The strong long-range electrostatic interaction between chromophores due to their permanent dipoles introduces the desired nonlinearity of the light-matter coupling in the microcavity. We develop a semiclassical model to obtain the absorption spectra of a weak probe field under the influence of strong exciton-photon coupling with the cavity field. Using realistic parameters, we demonstrate that a cavity field with an average photon number near unity can significantly modify the absorptive and dispersive response of the medium to a weak probe field at a different frequency. Finally, we show that the system is in the regime of cavity-induced transparency with a broad transparency window for dye dimers. We illustrate our findings using pseudoisocyanine chloride (PIC) J-aggregates in currently available optical microcavities.
Summary form only given. The optical coherent control of quantum mechanical systems enables the direct manipulation of quantum states, and has been demonstrated on excitonic transitions in semiconductors. We have demonstrated the coherent control of the nonlinear optical response of quantum-well excitons in a resonant high-Q microcavity. There are two significant advantages to using excitons in microcavities instead of bare quantum wells: first, the multiple reflections which occur in the cavity strongly enhance the optical nonlinearity, enabling large-signal coherent control, and second, 2-color coherent control may be implemented, where a pump pulse tuned to one of the normal modes of the coupled exciton-microcavity system can control the response of a probe tuned to the other normal mode. The nonlinear response of the normal modes is due to the nonlinearity of the underlying exciton transition.
This dissertation presents investigations of fundamental optical nonlinearities in semi-conductor microstructures. Two distinct effects are studied. In the first part the excitonic optical Stark effect in InGaAs and GaAs multiple quantum-well structures is investigated by means of pump-probe spectroscopy. For nonresonant excitation below the excitonic transition the direction of the shift of the resonance depends on the polarization of the pump and probe pulses. In particular, for anti-circular polarization a surprising red-shift is observed. For resonant excitation, induced absorption energetically above and below the exciton transition and bleaching of the resonance is found. Experiments using both resonant and nonresonant excitation reveal the importance of bound and unbound two-exciton states in absorption changes of the 1s heavy-hole exciton resonance. It is found that higher-order Coulomb contributions determine the intensity as well as the time dependence of the differential excitonic absorption. In addition, the influence of light-hole excitons is analyzed. It is shown that the direction of the optical Stark shift for nonresonant excitation depends also sensitively on the heavy-hole to light-hole splitting and the detuning of the pump pulse. For very high pump intensities and nonresonant excitation the absorption is split when a circularly polarized pump and a linearly polarized probe beam are used. For co-circular excitation traces of hyper-Raman gain are observed. In the second part of this dissertation, the nonlinear optical response of semiconductor microcavities in the nonperturbative regime is studied in resonant single-beam transmission and pump-probe experiments. In both types of experiment, a pronounced third transmission peak lying spectrally between the two normal modes is observed. Its dependence on the probe intensity, pump intensity, pump-probe delay, exciton-cavity detuning and pump detuning is investigated. For single-beam transmission, the energy of the third peak parallels the position of the cavity resonance. It is more pronounced for circularly polarized excitation and lasts longer than the two normal modes. For pump-probe experiments, the third peak increases with decreasing probe intensity and increasing pump intensity. Its energy is close to the low-energy side of the pump spectrum and virtually unaffected by the cavity-exciton detuning. The appearance of the third peak requires temporal overlap of pump and probe pulses. The origin of this complex nonlinearity is the quantum nature of light, which induces intraband polarizations in the presence of a coherent driving field and a finite carrier density. It is found that the coupling of the intraband polarizations via guided modes to the polarization of the fundamental longitudinal mode is responsible for the third transmission peak. A fully quantized theory reproduces the experimental observations.
The effect of phonons on a nonlinear optical response of a quantum dot-cavity system in quantum strong coupling regime can be accounted for by a fully analytical treatment, provided that the exciton-phonon dynamics is much faster than the exciton-cavity dynamics. Modern experiments involving semiconductor quantum dots embedded in optical microcavities typically meet this criterion. We find that, for a relatively small exciton-cavity coupling, the effect of phonons is concentrated mainly in the polaron shift of the exciton frequency and reduction of exciton-cavity coupling by the Huang-Rhys factor. We have generalized this result to an arbitrary optical nonlinearity and demonstrated a good agreement with the exact solution in a wide range of temperatures. This generalization provides access to higher rungs of the Jaynes-Cummings ladder, where exact numerical approaches are impractical or even impossible. At larger coupling strengths and low temperatures, our approximation is also in good agreement with the exact solution, which makes it a very useful tool for addressing the phonon contribution to the coherent dynamics of a nonlinear optical system. We demonstrate our results for third-order optical polarization with varying observation time and delay time between excitation pulses in the form of two-dimensional spectra. These spectra provide useful information about the coherent coupling between the exciton and the cavity modes. The presented analytical approach is also compared with another useful approximation, having the form of a matrix product, which is a special case of the asymptotically exact solution in the limit of a short phonon memory time.