Intriguing electronic and optical prospects of FCC bimetallic two-dimensional heterostructures: epsilon near-zero behavior in UV-Vis range

• Published in: Physical chemistry chemical physics : PCCP Vol. 22; no. 28; pp. 16314 - 16324
• Main Authors: Maji, Tuhin Kumar, Vaibhav, Kumar, Hawaldar, Ranjit, Adarsh, K. V, Pal, Samir Kumar, Karmakar, Debjani
• Format: Journal Article
• Language: English
• Published: Cambridge Royal Society of Chemistry 22.07.2020
• Subjects: Bimetals; Charge density waves; Combinatorial analysis; Correlation; Critical temperature; Density functional theory; Dynamic response; Energy dissipation; First principles; Gold; Heterostructures; Mathematical analysis; Mathematical morphology; Nanostructure; Nesting; Palladium; Phonons; Platinum; Quantum transport; Response functions; Silver; Time dependence; Topology
• ISSN: 1463-9076; 1463-9084
• DOI: 10.1039/d0cp00951b

A higher superconducting critical temperature and large-area epsilon-near-zero systems are two long-standing goals of the scientific community, having an explicit relationship with the correlated electrons in localized orbitals. Motivated by the recent experimental findings of the strongly correlated phenomena in nanostructures of simple Drude metallic systems, we have theoretically investigated some potential bimetallic FCC combinations having close resemblance with the experimental systems. The explored systems include the large-area interface to the embedded and doped two-dimensional (2D) combinatorial nanostructures. Using different effective single-particle first-principles approaches encompassing density functional theory (DFT), time-dependent DFT (TDDFT), phonon and DFT-coupled quantum transport, we propose some interesting correlated prospects of potential bimetallic nanostructures like Au/Ag and Pt/Pd. For the 2D doped and embedded nanostructures of these systems, the DFT-calculated non-trivial band-structures indicate the interfacial morphology-induced band localization. The calculated Fermi-surface topology of the nanostructures and the corresponding nesting behavior may be emblematic to the presence of instabilities, such as charge density waves. The optical attributes extracted from the TDDFT calculations result in near-zero behavior of both real and imaginary parts of the dynamical dielectric response in the ultra-violet to visible (UV-Vis) optical range. In addition, low-energy intra-band plasmonic oscillations, as present for individual metallic surfaces, are completely suppressed for the embedded and doped nanostructures. The TDDFT-derived electron-energy loss spectra manifest the survival of only inter-band transitions. The presence of soft phonons and dynamic instabilities is observed from the phonon-dispersion of the nanostructured systems. Quantum transport calculations on the simplest possible device made out of these bimetallic systems reveal the generation of highly transmitting pockets over the cross-sectional area for some selected device geometry. We envisage that, if scrutinized experimentally, such systems may unveil many fascinating interdisciplinary aspects of orbital chemistry, physics and optics, promoting their relevant applications in many diverse fields. Nanostructures of noble metals, Au and Ag, indicate the localization-induced correlated phenomena and epsilon-near-zero behaviour from first-principles investigations.