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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Observation of persistent spectral hole–burning in semiconductor nanocrystals

Yasuaki Masumoto, Lev Zimin, Kazuhiko Naoe

Published Jan 1, 1994• 0 citations
Publisher

Abstract

So far, persistent spectral hole-burning (PSHB) phenomenon has been observed in a number of materials. They are molecules in glasses, crystals and polymers, color centers in alkali halide crystals, and rare earth and transition metal ions in glasses and crystals. They are molecular or ionic guests embedded in glass, crystal or polymer hosts. Basic requirements for the PSHB are summarized as follows: (1) The optical absorption of guests embedded in hosts must be broadened inhomogeneously. (2) There must exist more than one ground state configurations of the total system consisting of guests and hosts. (3) The relaxation among the ground states must be slower than the decay rate of any excited state. In fact, this set of requirements is satisfied in many kinds of molecular or ionic guests in hosts, such as glasses, crystals and polymers, at low temperatures. We can naturally understand that guests consisting of small number of atoms are greatly influenced by the surrounding hosts and that the energy levels of the guests are inhomogeneously broadened.

DOI
10.1364/shbs.1994.fb2

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So far, persistent spectral hole-burning (PSHB) phenomenon has been observed in a number of materials. They are molecules in glasses, crystals and polymers, color centers in alkali halide crystals, and rare earth and transition metal ions in glasses and crystals. They are molecular or ionic guests embedded in glass, crystal or polymer hosts. Basic requirements for the PSHB are summarized as follows: (1) The optical absorption of guests embedded in hosts must be broadened inhomogeneously. (2) There must exist more than one ground state configurations of the total system consisting of guests and hosts. (3) The relaxation among the ground states must be slower than the decay rate of any excited state. In fact, this set of requirements is satisfied in many kinds of molecular or ionic guests in hosts, such as glasses, crystals and polymers, at low temperatures. We can naturally understand that guests consisting of small number of atoms are greatly influenced by the surrounding hosts and that the energy levels of the guests are inhomogeneously broadened.
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 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
The persistent spectral hole-burning (PSHB) phenomenon has been known since 1974. It is still an important research area for the study of the intimacy of complex molecular systems in the solid state, revealing high-resolution spectra, photophysics, photochemistry, and dynamics of molecular doped amorphous media, organic as well as inorganic. From another point of view, PSHB allows the engraving of any spectral structures in the inhomogeneous absorption band profile of molecular doped amorphous hosts or ion doped crystals cooled down to liquid helium temperatures. Therefore, a PSHB material is programmable in the spectral domain and consequently it can be transformed in an optical processor capable of achieving user-defined optical functions. Some aspects of both fields are illustrated in the present paper. Concerning the search for efficient PSHB materials, the hole-burning performances and the photophysics of polymer and xerogel based systems are compared. The problem of high-temperature persistent spectral hole-burning materials and the search for new frequency selective photosensitive systems for fast optical pulse processing at 800nm are considered. Regarding the points treated, inorganic hosts based on silicate xerogels or porous glasses have shown the best results. Moreover, by combining inorganic and organic capabilities or by grafting organic species to the host, hybrid xerogels have not yet revealed all possibilities. Also, the interest of two-photon materials for engraving spectral features with near-infrared or infrared light is developed. As an introduction to possible applications of PSHB material, the basics of spectro-temporal holography are remembered and a demonstrative experiment using a naphthalocyanine-doped polymer film is described, proving that the temporal aberration free recompression of ultrashort light pulses is feasible, therefore opening a way for applications in ultrashort light pulse shaping. Aspects for a comparison between cw hole-burning and femtosecond spectro-temporal experiments are considered, and prospects for coherent control of light fields or photochemical processes are also evoked.
Summary form only given. Persistent spectral hole burning (PSHB) of rare-earth-doped inorganic materials has attracted much attention in view of application to high-density optical memories. In particular, it seems that the glass materials are advantageous for application in wavelength-selective optical devices, as well as the memory devices, because of their large inhomogeneous linewidth. The wavelength-selective devices are key components in the wavelength-division multiplexing system, which is important for the next-generation optical communication technology. The problem for practical application lies in the fact that PSHB of rare-earth ions in glasses is usually observed only at temperature below 20 K. However, room-temperature PSHB has been observed recently for Sm/sup 2+/-doped crystals and glasses.
Recently, the interests in optical memory based on persistent spectral hole burning (PSHB) are increased because of its possibility of the application to high density optical memory. PSHB was observed for an organic dye doped in polymer and rear earth or transition metal doped in inorganic crystal or glasses up to now. Since PSHB was observed by two Russian groups (Gorokhovskii et al. and Kharlamov et al.) for free base phthalocyanine in a n-octane Shpol'skii matrix1 and for perylene and 9-aminoacridine molecules in glassy ethanol matrix2, PSHB materials are studied primarily for the polymer doped with an organic dye. But such materials can make hole only at very low temperature. Room temperature PSHB phenomena were observed on Sm2+ doped fluoride crystals3-5 and glasses6 recently, however these materials' Гih(inhomogeneous line width)/Гh(homogeneous line width)'s which are the parameters of data multiplicity in PSHB optical memory are an order of unity. For the application of PSHB materials to optical memory, high operating temperature, high Гih/Гh, and rapid reaction rate are wanted. Glass has a superiority on the view point of optical memory application because of its broad inhomogeneous line width and productivity. Our group has discovered room temperature PSHB for Sm2+ in borate glass systems whose Гih/Гh is 24.7 PSHB for rear earth metal in glass matrix has not been studied seriously, yet. It is thought that the study of the relationship between the optical hole and glass structure is necessary.
For next generation high density optical storage, extensive studies on persistent spectral hole burning (PSHB) have been performed, because they have a large potential for a high density frequency-domain optical data storage. PSHB has been observed at room temperature in Sm-doped crystals and glasses. Among them, glasses are considered to be more favorable than single crystals, due to their wide inhomogeneous line width and easy process for mass production. In the study, we developed a new glass mixture which shows room temperature PSHB with a inhomogeneous line width broadened up to 70 cm/sup -1/. The PSHB was characterized by investigating the time decay pattern of fluorescence and the excitation spectra.