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Quantum Information and Computation

Coherent optical control of electronic excitations in functionalized semiconductor nanostructures

Luís G. C. Rego, Sabas G. Abuabara, Víctor S. Batista

Published Jul 1, 2005• 12 citations
Publisher

Abstract

The feasibility of creating and manipulating coherent quantum states on surfaces of functionalized semiconductor nanostructures is computationally investigated. Quantum dynamics simulations of electron-hole transfer between catechol molecules adsorbed on TiO_2 -anatase nanostructures under cryogenic and vacuum conditions indicate that laser induced coherent excitations can be prepared and manipulated to exhibit controllable spatial Rabi oscillations. The presented computational methods and results are particularly relevant to explore the basic model components of quantum-information electro-optic devices based on inexpensive and readily available semiconductor materials.

DOI
10.26421/qic5.45-4

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The feasibility of creating and manipulating coherent quantum states on surfaces of functionalized semiconductor nanostructures is computationally investigated. Quantum dynamics simulations of electron-hole transfer between catechol molecules adsorbed on TiO_2 -anatase nanostructures under cryogenic and vacuum conditions indicate that laser induced coherent excitations can be prepared and manipulated to exhibit controllable spatial Rabi oscillations. The presented computational methods and results are particularly relevant to explore the basic model components of quantum-information electro-optic devices based on inexpensive and readily available semiconductor materials.
The feasibility of achieving coherent control of tunnelling dynamics, associated with electronic excitations in functionalized semiconductor nanostructures, is investigated. The coherent control scenario is based on the application of frequent stochastic unitary pulses, affecting the interference phenomena between electronic wave-packet components and consequently the overall electronic tunnelling dynamics without collapsing the coherent quantum evolution of the system. It is shown that tunnelling can be inhibited and eventually halted by sufficiently frequent pulse fields that exchange energy with the system but do not affect the potential energy tunnelling barriers. Further, the proposed stochastic quantum-control scenario is demonstrated more generally as applied to an archetype model, a particle tunnelling in a quartic double-well potential.
Light matter coherent interactions require that the coherent state induced in the matter be maintained for the duration of the observation. The only way to induce and observe such interactions in room temperature semiconductors, where the coherence time is of the order of a few hundred femtoseconds, is to use ultrashort pulse excitations and an ultrafast characterization technique. For media comprising an ensemble of nanostructure semiconductors such as self-assembled quantum dots, the gain broadening inhomogeneity also affects the interaction. Moreover, when gain media in the form of an active waveguide, such as optical amplifiers, are used, the interaction is distributed and includes nonresonant incoherent phenomena that occur simultaneously with the coherent effects. Such a complex system can exhibit, nevertheless, clear coherent interactions even at room temperature. Using InAs/InP quantum dot and wirelike quantum dash amplifiers, Rabi oscillations, self-induced transparency, coherent control using spectral pulse shaping, Ramsey interference, and photon echo have been demonstrated. The characterization employed cross frequency resolved optical gating, and the experiments were accompanied by a comprehensive finite difference time domain model that solves the Maxwell and Lindblad equations. This work has major implications on the understanding of the details of dynamical processes in active semiconductor devices, on short pulse generation from semiconductor lasers, and on various future quantum devices.
We present a microscopic and fully quantized model to investigate the interaction between semiconductor nanostructures and quantum light fields including the many-body Coloumb interaction between photoexcited electrons and holes. Our approach describes the coupled dynamics of the quantum light field and single and double electron-hole pairs, i.e., excitons and biexcitons, and exactly accounts for Coulomb many-body correlations and carrier band dispersions. Using a straightforward yet exact approach, we study a one-dimensional two-band system interacting with a single-mode, two-photon quantum state within a Tavis-Cummings framework. By employing an exact coherent factorization scheme, the computational complexity is reduced significantly enabling numerical simulations. We also derive a simplified model that includes only the bound 1s1s1s-exciton and biexciton states for comparison. Our simulations reveal distinct single- and two-photon Rabi oscillations, corresponding to photon-exciton and exciton-biexciton transitions. We demonstrate, in particular, that biexciton continuum states significantly modify the dynamics in a way that cannot be captured by simplified models that consider only bound states. Our findings emphasize the importance of a comprehensive microscopic modeling in order to accurately describe quantum optical phenomena of interacting electronic many-body systems.
Summary form only given. The developments with coherent control (CC) techniques in optical spectroscopy have recently demonstrated population control and coherence manipulations when the induced optical phase is explored with phase-locked laser pulses. These and other developments have been guiding the new research field of quantum control including the recent applications to semiconductors and nanostructures. We study the influence of inhomogeneous broadening in semiconductors on CC results. Photoluminescence (PL) and the coherent emission in four-wave mixing (FWM) is recorded after resonant excitation with phase-locked laser pulses. The sample is a narrow GaAs single quantum well.
In this paper, by applying generalized density-matrix equations, we explore the ultrafast dynamics of photo-generated electron–hole pairs in the system composed of electromagnetically coupled GaAs/AlGaAs quantum dots and reveal the physics mechanism behind laser-controlled nonlinear-optical response of electron–hole pairs. For the single-dot system, we present numerical results to show the transient dependence of carrier occupations and induced quantum coherence of electron–hole pairs in the presence of either a single or double laser pulses, as well as for a step turning-on of the laser field. For a dipole-radiation coupled double-dot system, we study numerically the time dependence of both intradot and interdot self-consistent depolarization fields within and between two dots, respectively. Meanwhile, we further demonstrate the significance of phase matching between induced depolarization fields and incident-laser pulse in order to maximize the stimulated transitions of electron–hole pairs and ensure non-quenched Rabi oscillations in each quantum dot. The employed theoretical model and the associated numerical analysis method are expected to facilitate designing and developing artificial quantum molecules composed of arbitrarily dielectric-embedded quantum dots with non-local quantum interactions and entanglement, as well as optically manipulating electron states of artificial quantum molecules.
Vacuum Rabi oscillation is a damped oscillation in which energy can transfer between an atomic excitation and a photon when an atom is strongly coupled to a photonic cavity. This process is challenging to be coherently controlled due to the fact that interaction between the atom and the electromagnetic resonator needs to be modulated in a quick manner compared to vacuum Rabi frequency. This control has been achieved at microwave frequencies, but has remained challenging to be implemented in the optical domain. Here we demonstrated coherent control of energy transfer in a semiconductor quantum dot strongly coupled to a photonic crystal molecule by manipulating the vacuum Rabi oscillation of the system. Instead of using a single photonic crystal cavity, we utilized a photonic crystal molecule consisting two coupled photonic crystal defect cavities to obtain both strong quantum dot-cavity coupling and cavityenhanced AC stark shift. In our system the AC stark shift modulates the coupling interaction between the quantum dot and the cavity by shifting the quantum dot resonance, on timescales (picosecond) shorter than the vacuum Rabi period. We demonstrated the ability to transfer excitation between a quantum dot and cavity, and performed coherent control of light-matter states. Our results provides an ultra-fast approach for probing and controlling light-matter interactions in an integrated nanophotonic device, and could pave the way for gigahertz rate synthesis of arbitrary quantum states of light at optical frequencies.