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Journal of Modern Optics

PHOTONIC MATERIALS AND DEVICES Progress in relating rare-earth ion 4f and 5d energy levels to host bands in optical materials for hole burning, quantum information and phosphors

Charles W. Thiel, Yazhou Sun, R. L. Cone

Published Nov 1, 2002• 67 citations
Publisher

Abstract

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.

DOI
10.1080/0950034021000011491

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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.
Research and development of nanoscale luminescent and laser materials are part of the rapidly advancing nanoscience and nanotechnology. Because of unique spectroscopic properties and luminescent dynamics of f-electron states, doping luminescent rare earth ions into nano-hosts has been demonstrated as an optimistic approach to developing highly efficient and stable nanophosphors for various applications. In this article, we review the most recent progress in spectroscopic measurements of rare earth ion-activated low-dimensional nanostructures including nanolayers, core-shells, nanowires, nanotubes, and nanodisks. Among a large volume of work reported in the literature on many members of the rare earth series including Ce3+, Pr3+, Nd3+, Eu3+, and Er3+, we focus on recent findings in the spectroscopic and luminescence properties of Eu3+ doped nanolayers, core-shells, and nanotubes, because Eu3+ ions have been extensively studied and widely used as an ideal probe for fundamental understanding of nano-phenomena. Specifically, the dependence of the optical properties of rare earth ions on nanostructures is discussed in detail.
Unique spectroscopic properties of isolated rare earth ions in solids offer optical linewidths rivaling those of trapped single atoms and enable a variety of recent applications. We design rare-earth-doped crystals, ceramics, and fibers with persistent or transient "spectral hole" recording properties for applications including high-bandwidth optical signal processing where light and our solids replace the high-bandwidth portion of the electronics; quantum cryptography and information science including the goal of storage and recall of single photons; and medical imaging technology for the 700-900 nm therapeutic window. Ease of optically manipulating rare-earth ions in solids enables capturing complex spectral information in 105 to 108 frequency bins. Combining spatial holography and spectral hole burning provides a capability for processing high-bandwidth RF and optical signals with sub-MHz spectral resolution and bandwidths of tens to hundreds of GHz for applications including range-Doppler radar and high bandwidth RF spectral analysis. Simply stated, one can think of these crystals as holographic recording media capable of distinguishing up to 108 different colors. Ultra-narrow spectral holes also serve as a vibration-insensitive sub-kHz frequency reference for laser frequency stabilization to a part in 1013 over tens of milliseconds. The unusual properties and applications of spectral hole burning of rare earth ions in optical materials are reviewed. Experimental results on the promising Tm3+:LiNbO3 material system are presented and discussed for medical imaging applications. Finally, a new application of these materials as dynamic optical filters for laser noise suppression is discussed along with experimental demonstrations and theoretical modeling of the process.
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.
Rare-earth ion doped crystals possess stable solid state physicochemical properties and long optical coherence time and spin coherence time, thus showing important development prospect in quantum information science and technology area. Investigations on macroscopic bulk rare-earth single crystals have obtained many promising results, especially in the field of optical quantum memory. With the rapid development of quantum information science, a variety of new functions or multifunctional integrations are found in rare earth crystal systems, such as on chip quantum storage, microwave to optical frequency conversion, scalable quantum single photon sources, and quantum logic gates. As a result, beyond the macroscopic bulk rare-earth single crystals, micro/nano-scale rare-earth crystals have received much attention in recent years and they are regarded as promising candidates in highly integrated hybrid quantum systems and miniaturized quantum devices. Moreover, wet chemical method synthesized micro/nano-scale rare-earth crystals have lower growth difficulty and more flexible manipulation in volume, shape and composition. Therefore, exploring high-performance micro/nano-scale rare-earth crystals and precisely manipulating their quantum states have become one of the important directions in today’s quantum information science and technology research. In this review, we first briefly introduce the basic concepts and high resolution spectroscopic techniques that are commonly used in rare earth ion doped crystals for quantum information science and technologies, such as hole burning technique and photon echo technique. Then we summarize comprehensively recent research status and development trends of rare earth ion doped polycrystalline nanoparticles, thin films, single crystal based micro systems, and some other micro/nano-scale rare earth platforms in terms of material fabrication, quantum coherence property, dephasing mechanisms, and also quantum device explorations. The latest research advances in quantum information applications such as quantum storage, quantum frequency conversion, quantum single photon sources and quantum logic gates are given. Finally, we discuss the possible optimization directions and strategies to improve the component design, material synthesis and quantum performance of micro/nano-scale rare earth crystals and their related quantum devices. This review highlights that the micro/nano-scale rare earth crystals may offer many new possibilities for designing quantum light-matter interfaces, thus are promising quantum systems to develop scalable and integrated quantum devices in the future.
We have investigated the possibility of realizing a 4-center energy transfer among trivalent rare Earth ions in suitable hosts. A 4-center energy transfer process was originally proposed in the context of photo-physics of dendrimer molecular systems using molecular quantum electrodynamics methods. Later, a similar theoretical construct was proposed for rare Earth ions in crystalline solids. Here, we search for rare Earth ions suitable for 4-center energy transfer based on observed energy levels of 4f n multiplet structures in suitable hosts. A search for this 4-center cooperative energy transfer process experimentally will open a novel area of research in luminescence.