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Physical Review Letters

Excitation mechanisms and optical properties of rare-earth ions in semiconductors

Stefan Schmitt-Rink, Chandra Mohan Varma, Anthony F. J. Levi

Published May 27, 1991• 75 citations
Publisher

Abstract

The optical activity of rare-earth ions in semiconductors is discussed taking into account the large 4f-level correlation energy. In addition to crystal-field effects, three many-body excitation mechanisms of 4f-4f transitions are identified; coherent or incoherent energy transfer via electron-hole pairs and nonequilibrium electron excitation. The first two give rise to novel nonlinear optical effects, while the last promises a simple means of achieving optical gain.

DOI
10.1103/physrevlett.66.2782

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The optical activity of rare-earth ions in semiconductors is discussed taking into account the large 4f-level correlation energy. In addition to crystal-field effects, three many-body excitation mechanisms of 4f-4f transitions are identified; coherent or incoherent energy transfer via electron-hole pairs and nonequilibrium electron excitation. The first two give rise to novel nonlinear optical effects, while the last promises a simple means of achieving optical gain.
Rare-earth ions play an important role in modern technology as optically active elements in solid-state luminescent materials. In many of these materials, interactions between the electronic band states of the host crystal and the rare-earth ion's localized 4f N and 4f N−1 5d states influence the material's optical properties. The importance of these interactions is discussed for material applications in photon-gated hole burning, quantum information and phosphors. Material dependent trends in the relative binding energies of the 4f N states and the host bands have been observed and are summarized. An empirical model for the ion dependence of the 4f electron binding energies is formulated in terms of atomic number and compared with previous models. These models are extended to describe the 4f N−1 5d states with one additional parameter. Improved estimates for the free-ion ionization potentials used in the model are also presented and discussed.
Participation of shallow states in the energy transfer processes between the rare-earth ions and a host semiconductor matrix is discussed. It is argued that shallow levels link the atomic-like states of the inner core of the rare-earth ion with the band structure of the host crystal. For the two most investigated systems InP:Yb and Si:Er the important role of these states at various stages of excitation and de-excitation mechanisms is shown. Models of the energy transfer process with a formation of a shallow intermediate state are discussed. It is shown that the formation of such a state is essential for the RE ion core activation. Experimental results supporting the involvement of shallow states are reviewed. Temperature dependencies of the photoluminescence activation and decay time constants are presented; these show an important role of shallow doping in the activation of Auger processes relevant to the mechanism of rare-earth ion photoluminescence. For the Si:Er system direct evidence for the two-stage excitation mechanism is discussed.
The absorption of a single photon by the simultaneous excitation of two rare-earth ions was first reported by Varsanyi and Dieke in 1961.1 D. L. Dexter explained this unusual observation by including the electron-electron interactions (that also give rise to energy transfer) between the rare earth ions with perturbation theory.2 In the 70's Dexter became interested in electronic-vibrational coupling. A theory of two-center optical transitions was developed for a rare-earth ion weakly coupled to a high energy, internal vibrational mode of a near-lying ion.3 Using theoretical techniques that had been developed for rare-earth ion pairs, intensities and selection rules could be determined.
The optical spectra of laser-excited semiconductors change with varying laser intensity. Close to exciton or biexciton resonances these optical nonlinearities are, e.g., large enough to obtain optical bistability. The cause for these large nonlinearities are many-body effects in the system of the electron-hole pair excitation. The use of nonequilibrium Green’s functions, or if a quasi-equilibrium exists of thermal Green’s functions, makes it possible to take radiative and Coulomb interactions consistently into account.
Summary form only given. Rare earth ions (RE) with optically activated 4f electrons present sharp spectral transitions in condensed matter due to the shielding of the 4f electrons by the outer 5s5p electrons. The quantum dot nature of RE makes them ideal for the study of condensed matter structures and dynamics. In this communication, we report on the fluorescence excitation spectra and the coherent femtosecond (fs) dynamics regarding the single ion and pair-transitions in Er:YAG at 77 K. We further apply fs interferometric techniques to control the single ion and ion-pairs emissions.