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Optics Express

Photoinduced Kerr rotation spectroscopy for microscopic spin systems using heterodyne detection

Yasuyoshi Mitsumori, Kentaro Uedaira, S. Shimomura, Keiichi Edamatsu

Published Mar 10, 2021• 1 citation
Publisher

Abstract

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.

DOI
10.1364/oe.417193

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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.
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.
Spin noise spectroscopy has become a widespread technique to extract information on spin dynamics in atomic and solid-state systems, in a potentially nonperturbative way. Here we experimentally demonstrate a new approach in spin noise spectroscopy, based on the detection of single photons. Because of the large spin-dependent polarization rotations provided by a deterministically coupled quantum dot-micropillar device, giant spin noise signals induced by a single-hole spin are extracted in the form of photon-photon cross-correlations. Ultimately, such a technique can be extended to an ultrafast regime probing mechanisms down to few tens of picoseconds.
Pump‐probe time‐resolved Kerr rotation technique has been used for experimental investigation of hole spin coherence in 15‐nm wide GaAs/AlGaAs quantum well structure in regime of diluted two‐dimensional hole gas. Due to the spectral width of 1.5 ps laser pulses which correspond to ∼1 meV, selective excitation of trion and exciton states has been performed. In the case of resonant excitation of exciton only the electron spin beats have been observed in the presence of magnetic field. In the case of resonant excitation of the positively charged exciton two component decay of time‐resolved Kerr rotation (TRKR) signal appeared. From the period of the quantum beat oscillation related to long decay component (up to 650 ps) of TRKR signal we obtained in‐plain hole g‐factor of ∼0.048±0.005.
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.
The noise tenaciously appearing in the optically heterodyne detected (OHD) transient optical Kerr effect (OKE) o f simple molecular liquids is investigated. We show that, for liquid samples of interest to us, coherent coupling does exist and appears as noise when not properly resolved. The strength of coherent coupling relative to the OKE depends critically on the sample position, with respect to the beam waist of the probe laser, as well as the angle subtended by the pump and probe beams. When the optics alignment is optimized for the OKE against coherent coupling the OHD-OKE signal is found to increase linearly with the local oscillator strength; the coherent coupling signal also appears to increase though the trend is not clear-cut. PACS. 42.50.Md- Optical transient phenomena: quantum beats, photon echo, freeinduction decay, dephasings and revivals, optical nutation, and self-induced transparency. PACS. 78.47.+p- Time-resolved optical spectroscopies and other ultrafast optical measurements in condensed matter. I.