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Polarimetry of photon echo on charged and neutral excitons in CdTe/(Cd,Mg)Te quantum wells

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 Publication date 2018
  fields Physics
and research's language is English




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Coherent optical spectroscopy such as four-wave mixing and photon echo generation deliver detailed information on the energy levels involved in optical transitions through the analysis of polarization of the coherent response. In semiconductors, it can be applied to distinguish between different exciton complexes, which is a highly non-trivial problem in optical spectroscopy. We develop a simple approach based on photon echo polarimetry, in which polar plots of the photon echo amplitude are measured as function of the angle $varphi$ between the linear polarizations of the two exciting pulses. The rosette-like polar plots reveal a distinct difference between the neutral and charged exciton (trion) optical transitions in semiconductor nanostructures. We demonstrate this experimentally by photon echo polarimetry of a 20-nm-thick CdTe/(Cd,Mg)Te quantum well at temperature of 1.5~K. Applying narrow-band optical excitation we selectively excite different exciton complexes including the exciton, the trion, and the donor-bound exciton D$^0$X. We find that polarimetry of the photon echo on the trion and D$^0$X is substantially different from the exciton: The echoes of the trion and D$^0$X are linearly polarized at the angle $2varphi$ with respect to the first pulse polarization and their amplitudes are weakly dependent on $varphi$. While on the exciton the photon echo is co-polarized with the second exciting pulse and its amplitude scales as $cosvarphi$.



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We study the quantum beats in the polarization of the photon echo from donor-bound exciton ensembles in semiconductor quantum wells. To induce these quantum beats, a sequence composed of a circularly polarized and a linearly polarized picosecond laser pulse in combination with an external transverse magnetic field is used. This results in an oscillatory behavior of the photon echo amplitude, detected in the $sigma^+$ and $sigma^-$ circular polarizations, occurring with opposite phases relative to each other. The beating frequency is the sum of the Larmor frequencies of the resident electron and the heavy hole when the second pulse is polarized along the magnetic field. The beating frequency is, on the other hand, the difference of these Larmor frequencies when the second pulse is polarized orthogonal to the magnetic field. The measurement of both beating frequencies serves as a method to determine precisely the in-plane hole $g$ factor, including its sign. We apply this technique to observe the quantum beats in the polarization of the photon echo from the donor-bound excitons in a 20-nm-thick CdTe/Cd$_{0.76}$Mg$_{0.24}$Te quantum well. From these quantum beats we obtain the in-plane heavy hole $g$ factor $g_h=-0.143pm0.005$.
Spin-flip Raman scattering of electrons and heavy-holes is studied for resonant excitation of neutral and charged excitons in a CdTe/Cd$_{0.63}$Mg$_{0.37}$Te quantum well. The spin-flip scattering is characterized by its dependence on the incident and scattered light polarization as well as on the magnetic field strength and orientation. Model schemes of electric-dipole allowed spin-flip Raman processes in the exciton complexes are compared to the experimental observations, from which we find that lowering of the exciton symmetry, time of carrier spin relaxation, and mixing between electron states and, respectively, light- and heavy-hole states play an essential role in the scattering. At the exciton resonance, anisotropic exchange interaction induces heavy-hole spin-flip scattering, while acoustic phonon interaction is mainly responsible for the electron spin-flip. In resonance with the positively and negatively charged excitons, anisotropic electron-hole exchange as well as mixed electron states allow spin-flip scattering. Variations in the resonant excitation energy and lattice temperature demonstrate that localization of resident electrons and holes controls the Raman process probability and is also responsible for symmetry reduction. We show that the intensity of the electron spin-flip scattering is strongly affected by the lifetime of the exciton complex and in tilted magnetic fields by the angular dependence of the anisotropic electron-hole exchange interaction.
We use the two-pulse spin-dependent photon echo technique to study the in-plane hole spin anisotropy in a 20~nm-thick CdTe/Cd$_{0.76}$Mg$_{0.24}$Te single quantum well by exciting the donor-bound exciton resonance. We take advantage of the photon echo sensitivity to the relative phase of the electron and hole spin precession and study various interactions contributing to the hole in-plane spin properties. The main contribution is found to arise from the crystal cubic symmetry described by the Luttinger parameter $q=0.095$, which is substantially larger than the one theoretically expected for CdTe or found in other quantum well structures. Another contribution is induced by the strain within the quantum well. These two contributions manifest as different harmonics of the spin precession frequencies in the photon echo experiment, when strength and orientation of the Voigt magnetic field are varied. The magnitude of the effective in-plane hole $g$ factor is found to vary in the range $|tilde{g_h}|$=0.125--0.160 in the well plane.
We study optical pumping of resident electron spins under resonant excitation of trions in n-type CdTe/(Cd,Mg)Te quantum wells subject to a transverse magnetic field. In contrast to the comprehensively used time-resolved pump-probe techniques with polarimetric detection, we exploit here a single beam configuration in which the time-integrated intensity of the excitation laser light transmitted through the quantum wells is detected. The transmitted intensity reflects the bleaching of light absorption due to optical pumping of the resident electron spins and can be used to evaluate the Larmor precession frequency of the optically oriented carriers and their spin relaxation time. Application of the magnetic field leads to depolarization of the electron spin ensemble so that the Hanle effect is observed. Excitation with a periodic sequence of laser pulses leads to optical pumping in the rotating frame if the Larmor precession frequency is synchronized with the pulse repetition rate. This is manifested by the appearance of Hanle curves every 3.36 or 44.2 mT for pulse repetition rates of 75.8 or 999 MHz, respectively. From the experimental data we evaluate the g factor of |g|=1.61 and the spin relaxation time of 14 ns for the optically pumped resident electrons, in agreement with previous time-resolved pump-probe studies.
We study Rabi oscillations detected in the coherent optical response from various exciton complexes in a 20~nm-thick CdTe/(Cd,Mg)Te quantum well using time-resolved photon echoes. In order to evaluate the role of exciton localization and inhomogeneous broadening we use selective excitation with spectrally narrow ps-pulses. We demonstrate that the transient profile of the photon echo from the localized trion (X$^-$) and the donor-bound exciton (D$^0$X) transitions strongly depends on the strength of the first pulse. It acquires a non-Gaussian shape and experiences significant advancement for pulse areas larger than $pi$ due to non-negligible inhomogeneity-induced dephasing of the oscillators during the optical excitation. Next, we observe that an increase of the area of either the first (excitation) or the second (rephasing) pulse leads to a significant damping of the photon echo signal, which is strongest for the neutral excitons and less pronounced for the donor-bound exciton complex (D$^0$X). The measurements are analyzed using a theoretical model based on the optical Bloch equations which accounts for the inhomogeneity of optical transitions in order to reproduce the complex shape of the photon echo transients. In addition, the spreading of Rabi frequencies within the ensemble due to the spatial variation of the intensity of the focused Gaussian beams and excitation-induced dephasing are required to explain the fading and damping of Rabi oscillations. By analyzing the results of the simulation for the X$^-$ and the D$^0$X complexes we are able to establish a correlation between the degree of localization and the transition dipole moments determined as $mu($X$^-$)=73~D and $mu($D$^0$X)=58~D.
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