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Title: Synthesis-driven, structure-dependent optical behavior in phase-tunable NaYF 4:Yb,Er-based motifs and associated heterostructures

Understanding the key parameters necessary for generating uniform Er,Yb co-activated NaYF 4 possessing various selected phases (i.e. cubic or hexagonal) represents an important chemical strategy towards tailoring optical behavior in these systems. In this paper, we report on a straightforward hydrothermal synthesis in which the separate effects of reaction temperature, reaction time, and precursor stoichiometry in the absence of any surfactant were independently investigated. Interestingly, the presence and the concentration of NH 4OH appear to be the most critical determinants of the phase and morphology. For example, with NH 4OH as an additive, we have observed the formation of novel hierarchical nanowire bundles which possess overall lengths of ~5 μm and widths of ~1.5 μm but are composed of constituent component sub-units of long, ultrathin (~5 nm) nanowires. These motifs have yet to be reported as distinctive morphological manifestations of fluoride materials. The optical properties of as-generated structures have also been carefully analyzed. Specifically, we have observed tunable, structure-dependent energy transfer behavior associated with the formation of a unique class of NaYF 4–CdSe quantum dot (QD) heterostructures, incorporating zero-dimensional (0D), one-dimensional (1D), and three-dimensional (3D) NaYF 4 structures. Our results have demonstrated the key roles of the intrinsic morphology-specific physicalmore » surface area and porosity as factors in governing the resulting opto-electronic behavior. Finally and specifically, the trend in energy transfer efficiency correlates well with the corresponding QD loading within these heterostructures, thereby implying that the efficiency of FRET appears to be directly affected by the amount of QDs immobilized onto the external surfaces of the underlying fluoride host materials.« less
Authors:
 [1] ;  [2] ;  [1] ;  [1] ;  [3] ;  [4] ;  [5]
  1. Stony Brook Univ., NY (United States). Dept. of Chemistry
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter of Physics and Materials Sciences Division
  3. Stony Brook Univ., NY (United States). Materials Science and Engineering Dept.
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  5. Stony Brook Univ., NY (United States). Dept. of Chemistry; Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter of Physics and Materials Sciences Division
Publication Date:
Report Number(s):
BNL-113365-2016-JA
Journal ID: ISSN 1463-9076; R&D Project: PM037; KC0201030; TRN: US1701041
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 19; Journal Issue: 3; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; NaYF4 nanocrystals; phase control; quantum dots; upconversion; energy transfer
OSTI Identifier:
1341646