Optical properties of Ag-Cu alloys : evidence for d-virtual bound states on Cu impurities

Rivory, J.; Thèye, M. L.

doi:10.1051/jphyslet:01975003605012900

“…The envelope is shaded blue for GLLB-SC, red for PBE, and gray for experimental data. Experimental data is from Peña-Rodríguez, for Au–Ag, from Koster and Stahl for Au–Cu, from Rivory and Theye for Ag–Cu, and from Myers et al for Pd–Au alloy. ε 1 plots can be found in Figure S6.…”

Section: Resultsmentioning

confidence: 99%

DFT-Based Approach Enables Deliberate Tuning of Alloy Nanostructure Plasmonic Properties

Bubaš

¹

,

Sancho‐Parramon

²

2021

View full text Add to dashboard Cite

Alloying of noble metals is lately being explored as a way to tune the optical and plasmonic properties of metal nanostructures. In order to rationally modulate properties by alloying, there is a need to fundamentally understand how the composition affects them. This work demonstrates that deep insights, useful for tailoring of noble alloy plasmonic and optical properties, can be gained by a low-cost approach based on density functional theory (DFT). We show in this work that the PBE functional, commonly used for calculation of alloy optical properties, can largely underestimate and in some cases even fail to predict a plasmonic response of an alloy. We propose the use of the GLLB-SC functional as a same-cost alternative and demonstrate it has an overall better performance than PBE for alloyed nanoparticles, thin films, and bulk alloys. The evolution of optical properties with composition range in the UV/Vis region is explained by connecting the alloy composition, band structure, and the resulting dielectric function. Additionally, an emergent property of alloying in the form of strong optical losses due to interband transitions in the IR region is identified and its origin is elucidated.

show abstract

“…The envelope is shaded blue for GLLB-SC, red for PBE and gray for experimental data. Experimental data is from [45], for Au-Ag, from [49] for Au-Cu, from [50] for Ag-Cu and from [51] for Pd-Au alloy. ε 1 plots can be found in Figure S6 with change of composition has qualitatively been reproduced by both GLLB-SC and PBE.…”

Section: Comparison For Pure Elementsmentioning

confidence: 99%

DFT-Based Approach Enables Deliberate Tuning of Alloy Nanostructures Plasmonic Properties

Bubaš

¹

,

Parramon²

2021

Preprint

0

View full text Add to dashboard Cite

<div>Using DFT we calculated band structures and dielectric functions of multiple binary alloy systems. The obtained data enabled us to elucidate the interconnection between alloy composition, fundamental properties such as band structure and their optical properties. The analysis provides the explanation for the smooth change of optical properties in the UV/VIS range and reveals the appearance of strong optical losses in the IR range due to interband transitions. Since they are present in all alloys but not in pure metals we identify such transitions as an emergent property of alloying. To predict plasmonic properties of different alloy nanostructures we performed electrodynamics simulations based on calculated and experimental dielectric functions. The results showed that that calculations based on the standardly used PBE functional in some cases drastically deviate from experiment-based results, and the calculations with an equally efficient GLLB-SC functional are superior. <br></div>

show abstract

“…A relatively smooth trend in optical properties variation The envelope is shaded blue for GLLB-SC, red for PBE and gray for experimental data. Experimental data is from [45], for Au-Ag, from [49] for Au-Cu, from [50] for Ag-Cu and from [51] for Pd-Au alloy. ε 1 plots can be found in Figure S6 with change of composition has qualitatively been reproduced by both GLLB-SC and PBE.…”

Section: Comparison Of Dielectric Functions For Alloysmentioning

confidence: 99%

“…The envelope is shaded blue for GLLB-SC, red for PBE and gray for experimental data. Experimental data is from[45], for Au-Ag, from[49] for Au-Cu, from[50] for Ag-Cu and from[51] for Pd-Au alloy. ε 1 plots can be found in FigureS6…”

mentioning

confidence: 99%

DFT-Based Approach Enables Deliberate Tuning of Alloy Nanostructures Plasmonic Properties

Bubaš

¹

,

Sancho‐Parramon²

2021

Preprint

0

View full text Add to dashboard Cite

<div>Using DFT we calculated band structures and dielectric functions of multiple binary alloy systems. The obtained data enabled us to elucidate the interconnection between alloy composition, fundamental properties such as band structure and their optical properties. The analysis provides the explanation for the smooth change of optical properties in the UV/VIS range and reveals the appearance of strong optical losses in the IR range due to interband transitions. Since they are present in all alloys but not in pure metals we identify such transitions as an emergent property of alloying. To predict plasmonic properties of different alloy nanostructures we performed electrodynamics simulations based on calculated and experimental dielectric functions. The results showed that that calculations based on the standardly used PBE functional in some cases drastically deviate from experiment-based results, and the calculations with an equally efficient GLLB-SC functional are superior. <br></div>

show abstract

Optical properties of Ag-Cu alloys : evidence for d-virtual bound states on Cu impurities

Abstract: The optical properties of metastable Ag-Cu solid solutions over the whole composition range have been determined and analyzed between 0.5 and 6 eV ; the results relative to Ag-rich alloys are interpreted in terms of the virtual bound state model

Cited by 12 publications

References 16 publications

DFT-Based Approach Enables Deliberate Tuning of Alloy Nanostructure Plasmonic Properties

DFT-Based Approach Enables Deliberate Tuning of Alloy Nanostructure Plasmonic Properties

DFT-Based Approach Enables Deliberate Tuning of Alloy Nanostructures Plasmonic Properties

DFT-Based Approach Enables Deliberate Tuning of Alloy Nanostructures Plasmonic Properties

Contact Info

Product

Resources

About