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Japanese Journal of Applied Physics

Micro-Pump–Probe Spectroscopy of an Exciton in a Single Semiconductor Quantum Dot Using a Heterodyne Technique

Yasuyoshi Mitsumori, Yuki Miyahara, Kentaro Uedaira, Hideo Kosaka, S. Shimomura, S. Hiyamizu, Keiichi Edamatsu

Published Sep 1, 2011• 4 citations
Publisher

Abstract

A heterodyne detection scheme was applied to micro-pump–probe spectroscopy to study the transient response of an exciton in a single semiconductor quantum dot. The elimination of the pump pulse in the frequency domain provided us a direct probing of the energy relaxation process of the quantum state excited by the pump pulse. The excitonic Rabi oscillations were also monitored by this technique, even in the presence of a strong pump pulse. This spectroscopic technique is suitable for the observation of the optical response and coherent manipulation of a semiconductor quantum dot.

DOI
10.1143/jjap.50.095004

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A heterodyne detection scheme was applied to micro-pump–probe spectroscopy to study the transient response of an exciton in a single semiconductor quantum dot. The elimination of the pump pulse in the frequency domain provided us a direct probing of the energy relaxation process of the quantum state excited by the pump pulse. The excitonic Rabi oscillations were also monitored by this technique, even in the presence of a strong pump pulse. This spectroscopic technique is suitable for the observation of the optical response and coherent manipulation of a semiconductor quantum dot.
In this thesis, the coherent interaction of single semiconductor quantum dots and ultrafast optical pulses is studied. Under certain conditions, localized exciton transitions in quantum dots can be seen as semi-isolated two-level systems. While this description is sufficient for the explanation of some observations in coherent experiments, it is sometimes necessary to explicitly consider coupling of the discreet quantum states confined to the dot with the environment. We start out from simple, classical examples of coherent spectroscopy and then turn towards experiments where the interaction with the vicinity of the dot becomes an important factor. First, a novel method for transient differential reflectivity spectroscopy of single quantum systems is introduced. It is a pure far-field optical technique which does not require any sophisticated sample preparation steps which makes it applicable to a broad range of structures. Pump pulses excite the sample structure and probe pulses read out the pump-induced changes in the system after a variable delay time. In the case of a single dipole, the signal is given in the form of the spectral inteferogram between the backscattered wave from the particle and the probe light which is reflected at the sample surface. This form of homodyne detection amplifies the weak scattered wave from the particle and thus makes this kind of spectroscopy for single quantum dots feasible. In the remainder of this thesis our spectroscopic method is applied to either characterize the coherent properties of single quantum dots, to prepare and read-out a desired quantum state or to deliberately manipulate them. Coherence times and oscillator strengths are determined for localized exciton transitions. Arbitrary population states can be written by driving coherent population oscillations using resonant pulses, while entangled superpositions of two exciton states in a single dot are investigated by quantum beats on transient differential spectra. We finally exploit the interaction between the dot and a nearby absorbing layer to switch the dot's absorption spectrum on ultrafast timescales via light-induced transient electric fields.
Summary form only given. The optical properties of semiconductor quantum dots have been studied intensively in the past few years. Recently the experiment has demonstrated not only the ability to probe a single QD but also how to coherently control the exciton in a single QD on a time scale that is short compared with the decoherence time. We had proposed a scheme to use the excitons in QD as qubits and to use strong ultra-fast laser pulses to manipulate the qubits via Rabi flopping. As a result a full understanding of the multi-exciton coherent nonlinear spectroscopy with strong pump field is needed. In this work we present a non-perturbative calculation of the nonlinear CW pump-probe spectra.
We develop a transient photoinduced Kerr rotation spectroscopy technique using a heterodyne detection scheme to study spin dynamics of microscopic quantum states in solids, such as single quantum dots and spin helixes. The use of the heterodyne beat note signal generated by the interference of the frequency-shifted probe and reference pulses realizes the Kerr rotation measurements in combination with micro-spectroscopy, even when the probe pulse propagates collinearly with the strong pump pulse, which resonantly excites the probing state. In addition, the interference gives an optical amplification of the Kerr signal, which provides a clear observation of the photoinduced spin dynamics by the weak probe intensity. Here, we present results of Kerr rotation measurements for a single quantum dot exciton, which shows a maximum rotation angle of few µrad.
While the advanced coherent control of qubits is now routinely carried out in low frequency (GHz) systems like single spins, it is far more challenging to achieve for two-level systems in the optical domain. This is because the latter evolve typically in the THz range, calling for tools of ultrafast, coherent, nonlinear optics. Using four-wave mixing micro-spectroscopy, we here measure the optically driven dynamics of a single exciton quantum state confined in a semiconductor quantum dot. In a combined experimental and theoretical approach, we reveal the intrinsic Rabi oscillation dynamics by monitoring both central exciton quantities, i.e., its occupation and the microscopic coherence, as resolved by the four-wave mixing technique. In the frequency domain this oscillation generates the Autler-Townes splitting of the light-exciton dressed states, directly seen in the four-wave mixing spectra. We further demonstrate that the coupling to acoustic phonons strongly influences the FWM dynamics on the picosecond timescale, because it leads to transitions between the dressed states.
We present measurements of the dephasing time and of optical Rabi oscillations in the excitonic ground-state transition of an InGaAs quantum dot ensemble at low temperature, using an heterodyne pump–probe technique. Dephasing times of several hundred picoseconds are measured, enabling coherent light–matter interaction with picosecond optical pulses. Optical Rabi oscillations which are damped versus pulse area and change period when changing pulse duration are observed. Comparison with calculations indicates that the observed damping is not intrinsic to a single dot. Dephasing processes and the biexciton resonance change the amplitude and the period of the oscillations, respectively, while the damping versus pulse area is due to a distribution of transition dipole moments in the ensemble.
The focus of the thesis is nonlinear transient optical properties and coherent control of single interface fluctuation quantum dots (QD's). When single exciton and biexciton resonances were driven by strong resonant laser pulses, Rabi oscillations of these transitions were observed in the differential transmission (DT) geometry. These results extend the concept of coherent control to the limit of single quantum confined systems in solids and have important implications for the feasibility of building quantum information processing devices using semiconductor QD's. Exciton Rabi oscillations are equivalent to arbitrary single-bit operations. The pulsed control of the exciton-biexciton transition is utilized as the optical operation for building a two-bit controlled rotational gates (CROT) in a single QD. A fidelity of 0.79 was obtained from numerical evaluation of the gate operation itself assuming typical decay parameters measured from these dots. Next, the nonradiative quantum coherence between two orthogonally polarized excitons confined in a single QD was studied. By using pulses with large enough bandwidth and the proper polarization, two exciton states are simultaneously excited. The quantum beats between the two exciton states were temporally resolved as the relative phase between the two dipole oscillations changed. It was found that the nonradiative coherence time is limited by the lifetimes of the excitons involved even in the strong field regime. In the basis of the pseudo-spin Bloch vectors of exciton transitions, the total wavefunction following the pulsed excitation is an entangled state, i.e. the wavefunction is non-factorizable. Finally, the quantum coherence between the biexciton, exciton, and the crystal ground states was studied in a novel quantum beat experiment, where the oscillations only existed when the pump and probe pulses overlapped in time. Laser pulses generated after a passive pulse shaper with just enough bandwidth to cover both the exciton and biexciton transitions were used in this experiment. The appearance of the beats is indicative of a reasonably long coherence time between the biexciton and other states even in the presence of strong pulsed excitations.