Excited-state dynamics and enhanced near-IR emission in Nd3+-structurally activated aluminophosphate glass containing silver and tinOptical Materials


José A. Jiménez, Sergiy Lysenko, Mariana Sendova, Chunqing Zhao
Electrical and Electronic Engineering / Computer Science (all) / Atomic and Molecular Physics, and Optics / Electronic, Optical and Magnetic Materials


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Received 14 February 2015

Received in revised form 25 March 2015

Accepted 4 April 2015

Available online xxxx aluminophosphate glass containing silver and tin have been investigated under pulsed-laser and of Ag nanoparticles on upconversion processes [3,13,16].

Neodymium-doped materials have widespread use in laser technology which has impacted today’s society tremendously, for instance, in information processing, communications, medicine, and scientific research in general [18,19]. In particular, Nd3+ solid-state lasers based on high-solubility phosphate glass s reducing agent ently, heat treatptical properties. nt is believed to cant diffe of stoichio amounts of SnO to Ag2O containing glass [23,29,30]. It ha observed that the absence of tin in glass containing 4 mol resulted in a decreased silver solubility, and as a consequence, in an increased susceptibility of the matrix to support the formation of silver species in various oxidation and aggregation states [30].

Hence, addition of SnO has been deemed necessary for the efficient dispersion of single Ag+ ions in the melt-quenched aluminphosphate glass [23]. An important role of SnO has been similarly recognized for the effective stabilization of Cu+ ions in the matrix ⇑ Corresponding author. Tel.: +1 904 620 1963; fax: +1 904 620 3535.

E-mail address: jose.jimenez@unf.edu (J.A. Jiménez).

Optical Materials xxx (2015) xxx–xxx

Contents lists availab

M .e lstransfer [5,7–12,14], or plasmon-enhanced processes (e.g. upconversion), have been reported [1,4,6,13,16]. Achieving enhanced optical properties is particularly attractive for photonic device applications and continues to be an active area of research [17].

Nevertheless, reports on the influence of silver species on Nd3+ ions in glasses are limited. They are mostly related to the influence [23,28]. Additional co-doping with tin(II) oxide a allows for Ag nanoparticles precipitation. Consequ ment produces a remarkable change in material o [14,23,26]. Moreover, tin as a metalophilic age increase glass matrix solubility. Indeed, signifi have been reported by our group upon additionhttp://dx.doi.org/10.1016/j.optmat.2015.04.007 0925-3467/ 2015 Elsevier B.V. All rights reserved.

Please cite this article in press as: J.A. Jiménez et al., Opt. Mater. (2015), http://dx.doi.org/10.1016/j.optmat.2015.04.007rences metric s been % Ag2OThe influence of silver species on the spectroscopic properties of rare-earth (RE) ions in glasses has been the subject of interest in optical materials research for several decades [1–16]. Silver ions, clusters, and nanoparticles have all been reported to affect the photoluminescence (PL) of RE ions in distinct ways. For example, emission enhancements or quenching in connection to energy [20,21]. This has led to the current initiative of exploring the potential of such for laser fusion power plants to generate electricity (concept of Laser Inertial Fusion Energy – LIFE) [22].

Aluminophosphate glass of the P2O5:Al2O3:MO (M = Ca, Sr, Ba) type is one of such matrices proposed for incorporating noble metals and RE ions [11,14,23–27]. The addition of Al2O3 is known to add chemical and thermo-mechanical stability to glass hostsKeywords:


Energy transfer


Rare-earths 1. Introductionsteady-state excitation at 266 nm. A comparative emission dynamics assessment was carried out concerning Ag and Sn dopants in the glass matrix with and without neodymium. The data indicates an effective non-radiative energy transfer from single Ag+ ions and Sn centers as donors to neodymium activator ions which ultimately populates the 4F3/2 emitting state in Nd3+. As a result, the near-IR (1.06 lm) emission from the 4F3/2 metastable state in Nd3+ is enhanced about an order of magnitude relative to a purely Nd-doped reference. In addition, the 4F3/2 excited state lifetime becomes significantly longer in the presence of silver and tin. A comparative 31P nuclear magnetic resonance spectroscopy study suggests glass depolymerization upon neodymium doping. It is proposed that a structural alteration might be linked to the established non-radiative energy transfer.  2015 Elsevier B.V. All rights reserved. matrices are much valued for high-power lasing applicationsArticle history: The excited state dynamics and near-infrared (IR) luminescent properties of Nd3+-doped melt-quenchedExcited-state dynamics and enhanced ne in Nd3+-structurally activated aluminoph containing silver and tin

José A. Jiménez a,⇑, Sergiy Lysenko b, Mariana Sendov aDepartment of Chemistry, University of North Florida, Jacksonville, FL 32224, USA bDepartment of Physics, University of Puerto Rico, Mayagüez, PR 00681, USA cOptical Spectroscopy & Nano-Materials Lab, New College of Florida, Sarasota, FL 34243 a r t i c l e i n f o a b s t r a c t

Optical journal homepage: www-IR emission phate glass , Chunqing Zhao a

A le at ScienceDirect aterials evier .com/locate /optmat transitions in @Sn [23–26]. On the other hand, the AgSnANd glass presents dips in correspondence with some Nd3+ transitions as observed by comparison with the absorption profile in (c) for the

Nd glass (main spectroscopic states [31] indicated). This is

Fig. 1. Optical absorption spectra of Nd and AgSnANd glasses. The inset shows the

Fig. 2. PL spectra obtained under ps laser excitation at 266 nm for (a) AgSn and (b)

AgSnANd glasses, together with (c) the absorption spectrum of the Nd glass; Nd3+

Materials xxx (2015) xxx–xxxShown in Fig. 1 are the optical absorption spectra for the Nd and

AgSnANd glasses where a redshift in the UV glass absorption edge is observed upon the Ag2O and SnO co-doping. Additional information on the effect of silver and tin on UV absorption is obtained from the difference absorption spectrum presented in the inset, obtained by scanning the AgSnANd glass together with the Nd glass as reference. A broad absorption band is observed which displays a peak at about 275 nm with a shoulder to the high energy wing around 255 nm. This type of absorption profile has been previously observed for Ag/Sn containing glasses and attributed to both isolated Ag+ ions and twofold-coordinated tin centers (referred to as @Sn, where @ represents the bonds with two oxygen atoms and  represents the two paired electrons) [8,25,26].