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Quantum Metamaterials

The main aim of QUANTUMMETALINK project, a research project supported by the European Reserch Council via an ERC Consolidator grant, is to develop an integrated theoretical and computational research program in an emerging area of metamaterials research, namely Quantum Metamaterials. The fundamental idea in this area of research is that remarkable physical properties beyond those available in naturally occurring materials can be achieved by designing the meta-constituents of the metamaterial and structuring it at a scale comparable or smaller than the optical wavelength. In this context, a new paradigm in metamaterials research emerges when the building blocks of metamaterials are quantum resonators, e.g., quantum dots, quantum dot molecules, graphene disks coupled to quantum dots, quantum nanowires, and quantum rings, case in which the macroscopic properties of quantum metamaterials are determined by the quantum properties of their basic constituents. We have organised our research in this field along three broad, synergistically integrated themes: the development of a general theory of the effective, macroscopic properties of quantum metamaterials, the development of a set of numerical methods and software tools for ab initio simulation of fundamental physical properties of quantum metamaterials, and the exploration of new science and potentially novel technological applications of quantum metamaterials.


Enhanced optical nonlinearity of 2D materials


Nonlinear optical gratings based on 2D materials


Quantum plasmons in graphene dots


Quantum plasmons based sensors



Publications
Giant Enhancement of Nonlinear Optical Interactions in 2D Materials
Remarkable optical and electrical properties of two-dimensional (2D) materials, such as graphene and transition-metal dichalcogenide (TMDC) monolayers, offer vast technological potential for novel and improved optoelectronic nanodevices, many of which rely on nonlinear optical effects in these 2D materials. Recently, we introduced a highly effective numerical method for efficient and accurate description of linear and nonlinear optical effects in nanostructured 2D materials embedded in periodic photonic structures containing regular three-dimensional (3D) optical materials, such as diffraction gratings and periodic metamaterials - see below a schematic of such an optical device. Our method builds upon the rigorous coupled-wave analysis and incorporates the nonlinear optical response of 2D materials by means of modified electromagnetic boundary conditions. This allows one to reduce the mathematical framework of the numerical method to an inhomogeneous scattering matrix formalism, which makes it more accurate and efficient than previously used approaches. To illustrate the versatility of our numerical method, we used it to investigate the linear and nonlinear multiresonant optical response of 2D-3D heteromaterials for enhanced and tunable second- and third-harmonic generation. In particular, by employing a TMDC monolayer optically coupled to a patterned slab waveguide, we demonstrate orders-of-magnitude enhancement of the intensity of generated second-harmonic.




Nonlinear Optical Diffraction Gratings Based on 2D Materials
Intriguing and unusual physical properties of graphene offer remarkable potential for advanced, photonics-related technological applications, particularly in the area of nonlinear optics at the deep-subwavelength scale. In this context, we have recently used an in-house developed numerical method to illustrate an efficient mechanism that can lead to orders-of-magnitude enhancement of the third-harmonic generation in graphene diffraction gratings. In particular, we demonstrate that by taking advantage of the geometry dependence of the resonance wavelength of localized surface-plasmon polaritons of graphene ribbons and discs one can engineer the spectral response of graphene gratings so that strong plasmonic resonances exist at both the fundamental frequency and third-harmonic. As a result of this double-resonant mechanism for optical near-field enhancement, the intensity of the TH can be increased by more than six orders of magnitude.




Quantum Plasmons in Single and Interacting Graphene Nanoflakes
In order to develop a computational framework to investigate and predict the optical properties of 2D quantum metamaterials, we started with the well-known single layer material – graphene and nanostructures made out of it. This choice has been motivated by the technical feasibility of synthetizing molecular-sized graphene nanoflakes, which could be the constituting bulding blocks of 2D quantum metamaterials. At the molecular scale the light-matter interaction is controlled by quantum mechanics, therefore it is expected that the quantum mechanical effects in graphene nanoflakes significantly influence the optical response of metamaterials based on such nanostructures. Hence the special name, quantum metamaterial can be given to this class of metamaterials. At the same time, it is also possible to produce large (but subwavelength size) graphene nanostructures using cutting techniques. If these nano-structures are used as metamaterial components the theoretical modelling can be performed based on classical electrodynamics. Therefore by using graphene one would have the practical means to investigate the transition between different physical regimes. To this end, we have studied the optical spectra for a variety of single and coupled graphene nanoflakes using time-dependent density functional theory within generalized gradient approximation as well as the dependence of these spectra on the shape and size of the graphene nanoflakes. Among other things, our analysis has shown that the physical properties of quantum plasmons of graphene nanoflakes are markedly distinct from those of their classical counterparts, e.g., their energy obeys a different power-law dependence on the nanoflake size.




Molecular Sensors based on Quantum Graphene Plasmons
The graphene nanoflakes discussed above and dimers formed from such graphene nanoflakes, can be viewed as very large molecular systems, characterized by specific optical absorption spectra. As a result, when a specific molecule is placed on top of a graphene nanoflake or in-between two graphene nanoflakes, as it is schematically illustrated in the figure below, one expects that the optical absorption spectrum of the combined physical system will be modified in a certain way, which is specific to the particular molecule added to the system and the shape and configuration of the graphene nanoflake and dimers made of graphene nanoflakes. Therefore, these changes of the optical spectra can be viewed as signatures of the specific molecules interacting with graphene nanoflakes and thus can be used to detect the molecules. A first step towards understanding how these quantum plasmon sensors work is to figure out the extent to which a molecular bridge linking two graphene nanoflakes affects the plasmon tunneling between the two graphene dots. In performing this analysis, as illustrated below, the optical spectra of the corresponding nanostructures prove to be powerful tools.