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Japanese Journal of Applied Physics

Heterodyne-Detected Accumulated Photon-Echo Spectroscopy of CuCl Quantum Dots

Ryosuke Kuribayashi Tsekhomskii, Alexander V. Baranov

Published Jan 1, 1999• 3 citations
Publisher

Abstract

A heterodyne-detected accumulated photon-echo spectroscopy has been applied for the first time to the study of the excitonic dephasing dynamics in CuCl spherical quantum dots embedded in a glass matrix; this spectroscopy has the advantage that a hole-burning spectrum can be extracted from the Fourier-cosine transformation of the signal profile. Owing to this advantage, we reveal that an anomalously slow rise of the time-integrated echo signal at low temperatures, which was also observed in the previous ordinary photon-echo spectroscopy but the origin was left unknown, is caused by a spectral antihole. From the decay (single exponential one) part of the signal which is found to be not influenced by this anomaly, we have obtained rich unambiguous information about the dephasing time T 2 such as the temperature dependence, which is found to be essentially the same as the previous one that one might cast some doubt on.

DOI
10.1143/jjap.38.577

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A heterodyne-detected accumulated photon-echo spectroscopy has been applied for the first time to the study of the excitonic dephasing dynamics in CuCl spherical quantum dots embedded in a glass matrix; this spectroscopy has the advantage that a hole-burning spectrum can be extracted from the Fourier-cosine transformation of the signal profile. Owing to this advantage, we reveal that an anomalously slow rise of the time-integrated echo signal at low temperatures, which was also observed in the previous ordinary photon-echo spectroscopy but the origin was left unknown, is caused by a spectral antihole. From the decay (single exponential one) part of the signal which is found to be not influenced by this anomaly, we have obtained rich unambiguous information about the dephasing time T 2 such as the temperature dependence, which is found to be essentially the same as the previous one that one might cast some doubt on.
Persistent spectral-hole-burning (PSHB) phenomena have been observed in many kinds of semiconductor quantum dots (QDs). Luminescence hole burning and charged excitons have been observed in CuCl QDs in NaCl crystals. The observed PSHB phenomena are explained by the ionization of QDs. The energy of photoionized QDs is changed from the original energy and their new energies depend on the spatial arrangement of trapped carriers. Quantum confinement of carriers and the resulting strong Coulomb interaction between confined carriers and trapped carriers cause the energy change. PSHB has been widely applied to site-selective spectroscopy of QDs. Size-dependent excited exciton quantum states in CuCl quantum cubes, size-dependent excited electron-hole quantum states in CdTe QDs and renormalization of longitudinal optical phonons confined in CuCl QDs have been revealed by studying sideband holes. This also allowed the measurement of accumulated photon echo, which clarified the very sharp homogeneous spectral linewidth of QDs under weak excitation conditions.
Fourier-transform spectroscopy using the technique of femtosecond accumulated photon echo with incoherent light has been performed in dye-doped polymers. Several types of interference effect or quantum beat between the zero-phonon line and other spectral components including the phonon sideband, the vibronic lines, and the photoproduct state have been observed. Based on the density matrix incorporating the transition-frequency modulation, it is pointed out that the factorization approximation for the relaxation function holds rigorously in the accumulated photon echo. We also clarified that the Fourier cosine transform of the heterodyne-detected echo signal provides the hole-burning spectrum.
Temperature dependence of the homogeneous linewidth of CuBr quantum dots in glass and NaBr matrices and CdSe quantum dots in glass matrix has been investigated using heterodyne-detected accumulated photon echo. We can reproduce the observed nonlinear temperature dependence considering two characteristic mechanisms: the small energy excitation in two-level system and the two-phonon Raman process of confined acoustic phonons. The interaction with the two-level system is dominant below 15 K and 10 K for CuBr and CdSe quantum dots, respectively. Above these temperatures the interaction with confined phonons is dominant. These results are similar to those of a previous study of CuCl quantum dots in glass, showing the universal influence of confined phonons and surrounding matrices on the low-temperature dephasing process of very small semiconductor quantum dots.
Transient four-wave-mixing experiments reveal that the phase relaxation time T2{T}_{2}T2​ of an exciton in CuCl spherical quantum dots embedded in glass is very long at low temperatures, e.g., 130 ps ($\ensuremath{\approx}10\ensuremath{\mu}\mathrm{eV}$ in homogeneous spectral width) at 2 K. The measurement at very weak pumping power enables us to extract the intrinsic value of T2,{T}_{2},T2​, typically two orders of magnitude longer than the reported ones. The T2{T}_{2}T2​ value is substantially governed by the energy relaxation time T1{T}_{1}T1​ at 2 K and then becomes shorter with increasing temperature. The time-integrated signal behaves such that the temperature dependence is found to be analogous to that in a system of dye molecules in a polymer.
Ultranarrow homogeneous linewidth of a Z3{Z}_{3}Z3​ exciton in CuCl quantum dots was studied by using accumulated photon echo. CuCl quantum dots embedded in two kinds of matrices, namely, an alminoborosilicate glass and a NaCl crystal, were studied. The narrowest homogeneous linewidth at low temperature was 1 $\ensuremath{\mu}\mathrm{eV}.$ The temperature dependence of the homogeneous linewidth was similar, above 5 K for both kinds of samples, but in the lower-temperature region, a remarkable difference was observed between them. It indicates that the matrix definitely affects the dephasing process of a confined exciton in quantum dots at low temperatures. The observed temperature dependence was explained by the contribution of the confined phonon in quantum dots and the two-level system in the matrix.