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Register a new userTailoring a Molecules Optical Absorbance Using Surface Plasmonics
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The design of novel functional materials in silico is severely hampered by the lack of robust and computationally efficient methods for describing both molecular absorbance and screening on substrates. Here we employ our hybrid $G_0[W_0+Delta W]$-BSE implementation, which incorporates the substrate via its screening $Delta W$ at both the quasiparticle $G_0W_0$ level and when solving the Bethe-Salpeter equation (BSE). We show this method can be used to both efficiently and accurately describe the absorption spectra of physisorbed molecules on metal substrates and thereby tailor the molecules absorbance by altering the surface plasmons energy. Specifically, we investigate how the optical absorption spectra of three prototypical $pi$-conjugated molecules: benzene (C$_6$H$_6$), terrylene (C$_{30}$H$_{16}$) and fullerene (C$_{60}$), depends on the Wigner-Seitz radius $r_s$ of the metallic substrate. To gain further understanding of the light--molecule/substrate interaction, we also study the bright excitons electron and hole densities and their interactions with infrared active vibrational modes. Our results show that (1) benzenes bright $E_{1u}^1$ exciton at 7.0 eV, whose energy is insensitive to changes in $r_s$, could be relevant for photocatalytic dehydrogenation and polymerization reactions, (2) terrylenes bright $B_{3u}$ exciton at 2.3 eV hybridizes with the surface plasmon, allowing the tailoring of the excitonic energy and optical activation of a surface plasmon-like exciton, and (3) fullerenes $pi-pi^*$ bright and dark excitons at 6.4 and 6.8 eV hybridize with the surface plasmon, resulting in the tailoring of their excitonic energy and the activation of both a surface plasmon-like exciton and a dark quadrupolar mode via symmetry breaking by the substrate.
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Topological insulator films are promising materials for optoelectronics due to a strong optical absorption and a thickness dependent band gap of the topological surface states. They are superior candidates for photodetector applications in the THz-infrared spectrum, with a potential performance higher than graphene. Using a first-principles $kcdot p$ Hamiltonian, incorporating all symmetry-allowed terms to second order in the wave vector $k$, first order in the strain $epsilon$ and of order $epsilon k$, we demonstrate significantly improved optoelectronic performance due to strain. For Bi$_2$Se$_3$ films of variable thickness, the surface state band gap, and thereby the optical absorption, can be effectively tuned by application of uniaxial strain, $epsilon_{zz}$, leading to a divergent band edge absorbance for $epsilon_{zz}gtrsim 6%$. Shear strain breaks the crystal symmetry and leads to an absorbance varying significantly with polarization direction. Remarkably, the directional average of the absorbance always increases with strain, independent of material parameters.
Smooth interfaces of topological systems are known to host massive surface states along with the topologically protected chiral one. We show that in Weyl semimetals these massive states, along with the chiral Fermi arc, strongly alter the form of the Fermi-arc plasmon, Most saliently, they yield further collective plasmonic modes that are absent in a conventional interfaces. The plasmon modes are completely anisotropic as a consequence of the underlying anisotropy in the surface model and expected to have a clear-cut experimental signature, e.g. in electron-energy loss spectroscopy.
We investigate the band structure and topological phases of silicene embedded on halogenated Si(111) surface, by virtue of density functional theory and tight-binding calculations.Our results show that the Dirac character of low energy excitations in silicene is almost preserved in the presence of silicon substrate passivated by various halogens. Nevertheless, the combined effects of charge transfer into the substrate, stretching of bonds between silicon atoms, and symmetry breaking which originates from van der Waals interaction, result in a gap $E_{g1}$ in the spectrum of the embedded silicene. We further take the spin-orbit interaction into account and obtain its strength and the resulting enhancement in the gap $E_{g2}=2lambda$. Both $E_{g1}$ and $E_{g2}$ which contribute to the total gap, vary significantly when different halogen atoms are used for the passivation of the Si surface and for the case of iodine, they have very large values of $70$ and $23$ meV, respectively. To examine the topological properties, we calculate the projected band structure of silicene from which the tight binding parameters of the low-energy effective Hamiltonian are obtained by fitting. Our results based on Berry curvature and $mathbb{Z}_2$ invariant reveals that silicene on halogenated Si substrates has a topological insulating state which can survive even at room temperature for the substrate with iodine and bromine at the surface. Similar to the free standing silicene, by applying a perpendicular electric field and at a certain critical value which again depends on the type of halogens, the gap closes and silicene undergoes a transition to a trivial insulating state. As a key finding, we see that the presence of halogenated substrate except for the case of fluorine enhances the robustness of the topological phases against the vertical electric field and most probably other external perturbations.
The optical response of graphene micro-structures, such as micro-ribbons and disks, is dominated by the localized plasmon resonance in the far infrared (IR) spectral range. An ensemble of such structures is usually involved and the effect of the coupling between the individual structures is expected to play an important role. In this paper, the plasmonic coupling of graphene microstructures in different configurations is investigated. While a relatively weak coupling between graphene disks on the same plane is observed, the coupling between vertically stacked graphene disks is strong and a drastic increase of the resonance frequency is demonstrated. The plasmons in a more complex structure can be treated as the hybridization of plasmons from more elementary structures. As an example, the plasmon resonances of graphene micro-rings are presented, in conjunction with their response in a magnetic field. Finally, the coupling of the plasmon and the surface polar phonons of SiO2 substrate is demonstrated by the observation of a new hybrid resonance peak around 500cm-1.
Plasmonics has established itself as a branch of physics which promises to revolutionize data processing, improve photovoltaics, increase sensitivity of bio-detection. A widespread use of plasmonic devices is notably hindered (in addition to high losses) by the absence of stable and inexpensive metal films suitable for plasmonic applications. This may seem surprising given the number of metal compounds to choose from. Unfortunately, most of them either exhibit a strong damping of surface plasmons or easily oxidize and corrode. To this end, there has been continuous search for alternative plasmonic materials that are, unlike gold, the current metal of choice in plasmonics, compatible with complementary metal oxide semiconductor technology. Here we show that copper and silver protected by graphene are viable candidates. Copper films covered with one to a few graphene layers show excellent plasmonics characteristics surpassing those of gold films. They can be used to fabricate plasmonic devices and survive for at least a year, even in wet and corroding conditions. As a proof of concept, we use the graphene-protected copper to demonstrate dielectric loaded plasmonic waveguides and test sensitivity of surface plasmon resonances. Our results are likely to initiate a wide use of graphene-protected plasmonics.
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