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International Conference on Ultrafast Phenomena

Coherent Control of Multidimensional Nonlinear Optical Signals with Shaped Laser Pulses

Dmitri V. Voronine, Darius Abramavičius, Shaul Mukamel

Published Jan 1, 2010• 0 citations
Publisher

Abstract

Multidimensional nonlinear optical signals with shaped laser pulses are simulated using closed-form expressions that contain pulse envelopes. Multiparameter coherent control using linear and higher-order chirp is applied to photosynthetic excitons to enhance weak cross peaks.
DOI
10.1364/up.2010.tue5

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Controlling stimulated emission is of importance because it competes with absorption and fluorescence under intense laser excitation. We performed resonant nonlinear optical spectroscopy measurements using femtosecond pulses shaped by π- or π/2-step phase functions and carried out calculations based on density matrix representation to elucidate the experimental results. In addition, we compared enhancements obtained when using other pulse shaping functions (chirp, third-order dispersion, and a time-delayed probe). The light transmitted through the high optical density solution was dominated by an intense stimulated emission feature that was 14 times greater for shaped pulses than for transform limited pulses. Coherent enhancement depending on the frequency, temporal, and phase characteristics of the shaped pulse is responsible for the experimental observations.
Abstract The first step in the coherent control of a photoinduced binary reaction is bond making or photoassociation. We have recently demonstrated coherent control of bond making in multi-photon femtosecond photoassociation of hot magnesium atoms, using linearly chirped pulses (Levin et al 2015 Phys. Rev. Lett. 114 233003 ). The detected yield of photoassociated magnesium dimers was enhanced by positively chirped pulses which is explained theoretically by a combination of purification and chirp-dependent Raman transitions. The yield could be further enhanced by pulse optimization resulting in pulses with an effective linear chirp and a sub-pulse structure, where the latter allows for exploiting vibrational coherences. Here, we systematically explore the efficiency of phase-shaped pulses for the coherent control of bond making, employing a parametrization of the spectral phases in the form of cosine functions. We find up to an order of magnitude enhancement of the yield compared to the unshaped transform-limited pulse. The highly performing pulses all display an overall temporally increasing instantaneous frequency and are composed of several overlapping sub-pulses. The time delay between the first two sub-pulses fits very well the vibrational frequency of the generated intermediate wavepacket. These findings are in agreement with chirp-dependent Raman transitions and exploitation of vibrational dynamics as underlying control mechanisms.
Recently, the advances in generation and characterization techniques of ultrashort laser pulses made it practical to prepare precisely defined laser pulses, these open up new possibilities for studying and controlling dynamical processes in femtosecond time scale. Hitherto, frequency-synthesized or chirped laser pulses have been widely applied to high-order harmonic generation (HHG) [3], population transfer [4], multiphoton transitions between Rydberg states [5], ect. Both the interference of two-color pulses and the nontrivial time dependence of chirped pulse laser field may lead to very interesting results. Moreover, recent studies have manifested that chirping can also have much impacts on the laser pulses as it propagates through different medium. For example, the propagation properties of chirped soliton pulses in optical nonlinear Kenmedia were investigated by Desaix et al. [6]. The result indicates that the properties of asymptotically emerging solitons depend not only on the magnitude, but also on the form of the initial chirp. In particular, the splitting of an initial pulse into separating soliton pulse pairs only occurs for certain classes of initial chirp functions. The influence of pulse shape and frequency chirp on stability of optical solitons was studied by Klaus and Shaw [7]. They found that destabilization occurs when eigenvalues of an associated Zakharov-Shabat system, which move along the positive imaginary axis with increasing chirp parameter, either are absorbed into the lower half plane or collide with a nother eigenvalue. Furthermore, the signal and group velocities for chirped pulses propagating through a GaAs cavity were measured by Centini et al. [8]. They showed that the chirp substantially modifies the group velocity of the pulse, but leaves the signal velocity unaltered.
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.
Summary form only given. Ultrafast coherent control of excitons in semiconductors have been reported using Michelson interferometer with precise control of the pulse interval in time domain. In order to improve the phase controllability and realize arbitrary manipulation, the pulse shaping technique is a more attractive candidate. In this paper, we report very fine phase control of coherent, excitons in GaAs/AlGaAs single quantum wells using phase-locked pulses prepared by pulse shaping technique.