Defect Engineering in Plasmonic Metal Oxide Nanocrystals

Runnerstrom, Evan L.; Bergerud, Amy; Agrawal, Ankit; Johns, Robert W.; Dahlman, Clayton J.; Singh, Ajay; Selbach, Sverre M.; Milliron, Delia J.

doi:10.1021/acs.nanolett.6b01171

Cited by 128 publications

(198 citation statements)

References 71 publications

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“…This phenomenon has also been observed in some metal oxides such as WO x 8 and Ce:In 2 O 3 . 9 The optical characteristics of plasmonic nanoparticles are tunable based on the size and the shape of the nanoparticle. 10 The energy accumulated in these oscillating surface plasmons can be used in several ways to accelerate the rates of chemical reactions.…”

Section: Introductionmentioning

confidence: 99%

Improving the rates of Pd-catalyzed reactions by exciting the surface plasmons of AuPd bimetallic nanotriangles

et al. 2017

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Gold nanoparticles exhibit unique optical properties due to surface plasmon oscillations when they interact with light. By utilizing their optical properties, the rates of many chemical reactions have been improved in the presence of visible light. The properties of plasmonic nanoparticles are highly tunable based on the size and shape of the nanoparticle. Here, we have used anisotropic AuPd bimetallic nanotriangles to improve the rates of Pd-catalyzed reactions in the presence of visible light. We synthesized AuPd core-shell bimetallic nanotriangles and performed Suzuki cross-coupling and hydrogenation reactions in light and dark conditions. Upon illuminating AuPd nanotriangles with an array of green LEDs (power $ 500 mW), enhanced catalytic activity of palladium was observed. In order to understand the relative contributions of individual plasmonic effects, such as plasmonic hot electron transfer and plasmonic heating effects, the reaction temperatures were monitored, and careful control experiments were run at different temperatures. Our results indicated that the enhancement in the rate of these Pd-catalyzed reactions is primarily due to the plasmonic heating effect.

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Section: Introductionmentioning

confidence: 99%

Improving the rates of Pd-catalyzed reactions by exciting the surface plasmons of AuPd bimetallic nanotriangles

et al. 2017

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“…Small variations are observed in the SPR peaks but it was hard to detect a regular increase or decrease concerning the nanocube sizes as reported in the literature. 51,52 In order to detect the photoluminescence (PL) features of the Pd decorated ZnO nanolayers, we measured the PL characteristics of all three Pd@ZnO@PAN-NFs and compare them with ZnO@PAN-NF, as shown in Fig. 7.…”

Section: Resultsmentioning

confidence: 99%

Pd nanocube decoration onto flexible nanofibrous mats of core–shell polymer–ZnO nanofibers for visible light photocatalysis

et al. 2017

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Plasmonic enhancement for electron-hole separation efficiency and visible light photocatalysis was achieved by Pd nanocube decoration on a ZnO nanolayer coated onto electrospun polymeric (polyacrylonitrile (PAN)) nanofibers. Since exciton formation and sustainable electron-hole separation have a vital importance for realizing better solar energy in photovoltaic and photocatalytic devices, we achieved visible light photocatalysis by Pd nanocube decoration onto well designed core-shell nanofibers of ZnO@PAN-NF. By controlling the cubic Pd nanoparticle size and the thickness of the crystalline ZnO nanolayer deposited onto electrospun PAN nanofibers via atomic layer deposition (ALD), defect mediated visible light photocatalysis efficiency can be increased. By utilizing nanofabrication techniques such as thermal decomposition, electrospinning and ALD, this fabricated template became an efficient, defect mediated, Pd nanocube plasmon enhanced photocatalytic system. Due to the enhanced contact features of the Pd nanocubes, an increase was observed for the visible light photocatalytic activity of the flexible and nanofibrous mat of Pd@ZnO@PAN-NF.

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“…For the electron mobility calculations, the effective carrier mass for Sn:In2O3 and Sn,Zr:In2O3 NCs was approximated as 0.39me whereas that for Zr:In2O3 NCs was 0.22me as suggested by Xu et al 28 Even if the same effective carrier mass is assumed, the electron mobilities in Zr:In2O3 NCs would be equivalent if not greater to that of Ce-doped In2O3 NCs. 26 We attribute this extraordinary electronic quality of Zr:In2O3 NCs to the optimized position of the Zr defect level in the electronic band structure of In2O3 coupled with surface segregated Zr doping, which ensures that the electrostatic potentials experienced by the electrons do not change significantly through the lattice of In2O3. These effects combine to produce a rare combination of high LSPR Q-factor, high dopant activation, and low levels of electron scattering implying high electron mobilities, all in one material.…”

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confidence: 99%

Dopant Selection Strategy for High Quality Factor LSPR from Doped Metal Oxide Nanocrystals

Tandon

Ghosh²,

Milliron³

2019

Preprint

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Thin films of degenerately doped metal oxides such as those of Sn-doped In2O3 (Sn:In2O3) are commercially significant for their broad utilization as transparent conducting electrodes in optoelectronic devices. Over the last decade, nanocrystals (NCs) of Sn:In2O3 and other doped metal oxides have also attracted interest for localized surface plasmon resonance (LSPR) that occurs in the near to mid-infrared region. The suitability of this LSPR for some applications depends on its capacity to concentrate light in small regions of space, known as near-field hot spots. This efficiency to create near-field hot spots can be judged through an LSPR figureof-merit such as Quality factor, defined as the ratio of LSPR peak energy to its linewidth. The free electron density determines the LSPR peak energy while the extent of electron scattering controls the LSPR linewidth and hence these factors together essentially dictate the value of the Quality factor. An unfortunate tradeoff arises when dopants are introduced since the aliovalent dopants generating the free electrons (increasing LSPR energy) also act as centers of scattering of electrons (increasing LSPR linewidth), thereby decreasing the LSPR Quality factor. Dopant selection is hence of paramount importance to achieve a high value of LSPR Quality factor. Here, we describe the properties of aliovalent cationic dopants that allow both high LSPR energy and low LSPR linewidth and, subsequently, high LSPR Quality factor. In this context, we identify Zr 4+ as a model aliovalent dopant for high LSPR Quality factor in the In2O3 lattice. The resulting Zr-doped In2O3 NCs exhibit one of the highest LSPR Quality factors reported in the mid-infrared region while also performing equivalently to the recognized materials for either high dopant activation (Sn:In2O3 NCs) or low LSPR linewidth (Ce-doped In2O3 NCs), simultaneously. The Zr donor level is positioned well into the conduction band of In2O3 and Zr doping is surface segregated, both minimizing electron scattering. The combination of this low electron scattering and high dopant activation of Zr 4+ ions is responsible for the high LSPR Quality factors. These strategies can be used to design a variety of doped metal oxide NC systems exhibiting high LSPR Quality factors.

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Defect Engineering in Plasmonic Metal Oxide Nanocrystals

Cited by 128 publications

References 71 publications

Improving the rates of Pd-catalyzed reactions by exciting the surface plasmons of AuPd bimetallic nanotriangles

Improving the rates of Pd-catalyzed reactions by exciting the surface plasmons of AuPd bimetallic nanotriangles

Pd nanocube decoration onto flexible nanofibrous mats of core–shell polymer–ZnO nanofibers for visible light photocatalysis

Dopant Selection Strategy for High Quality Factor LSPR from Doped Metal Oxide Nanocrystals

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