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Applied Physics Letters

Hole-filling of persistent spectral holes in the excitonic absorption band of CuBr quantum dots

Jan Valenta, J. Moniatte, P. Gilliot, R. Lévy, B. Hönerlage, A. I. Ekimov

Published Feb 10, 1997• 19 citations
Publisher

Abstract

Persistent spectral-holes (p-SH) are burned in the Z1,2 excitonic band of CuBr nanocrystals by a pulsed laser excitation. The annealing of p-SH is studied by three types of hole-filling (HF) experiments: (i) the spontaneous HF, (ii) thermally-induced HF, and (iii) the laser-induced HF. Results are compared to the well developed theory of the persistent spectral hole-burning (p-SHB) in the system of molecules in amorphous matrices. Both p-SHB and HF phenomena can be explained within the framework of a photochemical reaction like the photoionization of nanocrystals. The potential application of p-SHB to the frequency-domain optical data storage is discussed.

DOI
10.1063/1.118273

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Persistent spectral-holes (p-SH) are burned in the Z1,2 excitonic band of CuBr nanocrystals by a pulsed laser excitation. The annealing of p-SH is studied by three types of hole-filling (HF) experiments: (i) the spontaneous HF, (ii) thermally-induced HF, and (iii) the laser-induced HF. Results are compared to the well developed theory of the persistent spectral hole-burning (p-SHB) in the system of molecules in amorphous matrices. Both p-SHB and HF phenomena can be explained within the framework of a photochemical reaction like the photoionization of nanocrystals. The potential application of p-SHB to the frequency-domain optical data storage is discussed.
The persistent spectral hole-burning (PSHB) phenomenon was observed in semiconductor quantum dots, CdSe , CuCl , and CuBr , embedded in glass and crystal. In inhomogeneously broadened exciton absorption spectra of these dots, the narrow bleaching hole and its associated structure are made by the narrowband laser excitation and are conserved for more than several hours at 2 K after the laser irradiation. The observation of the PSHB phenomenon in these four kinds of samples shows the generality of the phenomenon in semiconductor quantum dots and requires the existence of more than one ground-state configurations of the total system consisting of quantum dots and surrounding matrix. It means that not only the size distribution but also these ground-state configurations give inhomoge-neous broadening to semiconductor quantum dots. Thermally annealing and light-induced hole-filling phenomena were observed. Hole-burning and hole-filling mechanisms are discussed. Quantum dots consisting of 103–104 atoms behave like molecules or ions in matrix to give the PSHB phenomenon.
We study CuBr nanocrystals embedded in a borosilicate matrix. The excitonic absorption line is strongly inhomogeneously broadened by the size dispersion of the quantum dots. We explore two ways in order to study the dephasing processes of the transition. The homogeneous absorption linewidth is first determined by spectral hole-burning (SHB) measurements, using a nanosecond dye laser excitation. We then perform degenerate four-wave-mixing experiments (FWM), using 100 fs pulses from a frequency-doubled Ti:sapphire laser. Due to the inhomogeneous broadening, we observe a so-called photon-echo signal and we measure its dynamics. From SHB experiments, we obtain homogeneous linewidths larger than 0.3 meV. From the FWM experiment, we obtain values smaller than 0.2 meV. These discrepancies between SHB and FWM measurements can be explained if we take into account the high excitation intensity necessary to induce absorption saturation in SHB experiments. Moreover, during the 20 ns pulses used, spectral diffusion may occur due to interactions between the nanocrystals and their matrix. Spectrally resolved four-wave-mixing experiments (SR-FWM) are also performed. The oscillations with a 250 fs period we observe at short time delays could be interpreted in terms of quantum beats between two-exciton and one-exciton states.
Persistent spectral hole-burning phenomenon in CuBr quantum dots embedded in glass was observed. The spectral hole and the sideband holes were made together with the redshift of the absorption spectrum in proportion to the logarithm of the laser fluence and were preserved for more than 8 h at 2 K. They were erasable by the temperature rise or by the light exposure. Electron trapping at the surface of the dots and hole tunneling into traps in the glass host is the most probable origin of the persistent spectral hole-burning phenomenon in CuBr quantum dots.
We have studied persistent spectral hole-burning (PSHB) phenomena of cuprous halide (CuCl) nanocrystals.In particular, we concentrate on two aspects: Fundamental physics and applications of the PSHB phenomena.Stark effects by trapped carriers or photoionization were proposed as the mechanisms of the PSHB phenomena.However, the further study is needed for the better understanding of the mechanism.In the course of the study to this direction, we found correlations between the PSHB phenomena and photoluminescence spectral-changes of excitons bound to Cu+-ion vacancies in CuCl nanocrystals and of Cu+ dimers in a NaCl crystal in CuCl nanocrystals embedded in a NaCl crystal.The spectral-changes can be triggered by Cu+-ion displacements in CuCl nanocrystals and in a NaCl crystal.On the other hand, in CuCl nanocrystals embedded in alumino borosilicate glass, the PSHB phenomena are considered to be caused by photophysical mechanisms, e. g., photoinduced structural-change at nanocrystal-glass interface and/or glass.PSHB phenomena can be applied to not only optical memory but also the precise, highresolution spectroscopy for the nanocrystals with a certain size.We report the nanocrystalsize dependent acoustic phonons confined in CuCl nanocrystals by using the PSHB phenomena.The size-dependent energy-intervals between zero-phonon lines and phonon sidebands in the hole-burning spectra almost coincide with the calculated energies of confined acoustic phonons in nanometer-size elastic spheres.We conclude that the phonon sidebands are due to confined acoustic phonons in CuCl nanocrystals.The observed confined acoustic
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.