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Andrea Griesi

Publications and source records attributed to Andrea Griesi.

7 recordsLinked to original sources

Heterostructure Design in Two-Dimensional Perovskites by Sequential Recrystallization

Low-dimensional metal halide perovskites provide exciting opportunities to fabricate new semiconductor materials. Semiconductor technology relies on electronic heterojunctions, and cost-efficient and flexible approaches to realize functional heterostructures are of fundamental importance. Lateral heterostructures define the energy landscape in the plane of the semiconducting lattice in such 2D materials, representing an ideal platform to tailor energy barriers and to control charge carrier flow. Here, we demonstrate a versatile one-pot synthesis to fabricate a large variety of 2D perovskite heterostructures based on different halides and/or metal cations. Exploiting sequential crystallization of different 2D perovskites, and playing with the composition and injection events of the materials, enables the design of diverse heterostructure architectures including multiple heterojunctions. We obtain crystalline quality of the heterojunctions, multicolor emission, and optical coupling between the different heterostructure regions. We foresee that the design freedom of our method will stimulate the development of novel optoelectronic devices where electronic band engineering is crucial.

cond-mat.mtrl-sci

Synthesis, Growth Mechanism, and Photocatalytic Properties of Metallic-Bi/Bi13S18Br2 Nano-Bell Heterostructures

We report the synthesis of bell-shaped Bi/Bi13S18Br2 metal/semiconductor heterostructures as a photocatalyst based on non-toxic and Earth-abundant elements. Their unique morphology arises from a multi-step growth process, involving 1) the nucleation of Bi13S18Br2 nanorods, 2) the reduction of a metallic-Bi domain on their surface induced by N,N-didodecylmethylamine, and 3) the heterostructure accretion by a localized reaction at the Bi/Bi13S18Br2 interface promoted by Ostwald ripening. These heterostructures display remarkable stability in polar solvents, remaining almost unaffected by prolonged exposure to isopropanol and water, and exhibit high photocatalytic efficiency for the degradation of organic dyes (i.e., Rhodamine-B and Methylene Blue) under visible-light irradiation, with good recyclability. Additionally, preliminary tests demonstrate CO2 reduction capabilities, which make them promising for both the photocatalytic degradation of pollutants and photo-electro CO2 conversion. The straightforward synthesis process and the use of non-toxic and earth-abundant elements offers significant potential for sustainable energy conversion technologies.

cond-mat.mtrl-sci

Silver Alloyed Wide Bandgap (Ag,Cu)(In,Ga)S2 Thin Film Solar Cells With 15.5% Efficiency

Sulfide chalcopyrite Cu(In,Ga)S2 (CIGS) is a wide bandgap semiconductor suitable for the top cell of a tandem solar device. Here we demonstrate significant improvements in absorber quality by alloying with Ag to form (Ag,Cu)(In,Ga)S2 (ACIGS) absorbers. We report the Ag alloying effect on compositional, structural, and optoelectronic properties of absorbers. We demonstrate suppressed bulk recombination and improved carrier lifetime in ACIGS, as a result of improved grain size, porosity reduction and defect passivation. We also show that Ag alloying flattens the Ga gradient. Consideration of this impact of Ag will be necessary in future engineering of the Ga profile to maximize charge carrier collection and avoid interface recombination. Exploiting the beneficial effects of Ag alloying, we report a wide bandgap (1.58 eV) ACIGS solar cell with a high power conversion efficiency of 15.5% and a large open-circuit voltage (VOC) of 948 mV, improving on the reference pure CIGS solar cell, with an 11.2% efficiency and an 821 mV VOC. Ag alloying is a useful route to further increase the efficiency of CIGS solar cells and future tandem devices.

cond-mat.mtrl-sci

Copper-based disordered plasmonic system with dense nanoisland morphology

Dry synthesis is a highly versatile method for the fabrication of nanoporous metal films, since it enables easy and reproducible deposition of single or multi-layer(s) of nanostructured materials that can find intriguing applications in plasmonics, photochemistry and photocatalysis, to name a few. Here, we extend the use of this methodology to the preparation of copper nanoislands that represent an affordable and versatile example of disordered plasmonic substrate. We perform detailed characterizations of the system using several techniques such as spectroscopic ellipsometry, cathodoluminescence, electron energy loss spectroscopy, ultrafast pump-probe spectroscopy and second-harmonic generation with the aim to investigate the optical properties of these systems in an unprecedented systematic way. Our study represents the starting point for future applications of this new disordered plasmonic system ranging from sensing to photochemistry and photocatalysis.

physics.app-ph

Dry synthesis of bi-layer nanoporous metal films as plasmonic metamaterial

Nanoporous metals are a class of nanostructured materials finding extensive applications in multiple fields thanks to their unique properties attributed to their high surface area and interconnected nanoscale ligaments. They can be pre-pared following different strategies, but the deposition of an arbitrary pure porous metal is still challenging. Recently, a dry synthesis of nanoporous films based on the plasma treat-ment of metal thin layers deposited by physical vapour deposition has been demonstrated, as a general route to form pure nanoporous films from a large set of metals. An interest-ing aspect related to this approach is the possibility to apply the same methodology to deposit the porous films as a multilayer. In this way, it is possible to explore the properties of different porous metals in close contact. As demonstrated in this paper, interesting plasmonic properties emerge in a nanoporous Au-Ag bi-layer. The versatility of the method coupled with the possibility to include many different metals, provides an opportunity to tailor their optical resonances and to exploit the chemical and mechanical properties of compo-nents, which is of great interest to applications ranging from sensing, to photochemistry and photocatalysis.

physics.app-ph

Hybrid improper dipolar density wave in NaLaCoWO$_6$

Hybrid Improper Ferroelectricity (HIF) allows the generation of an electrical polarization in the AA'BB'O$_6$ double perovskite materials thanks to the combination of two non-polar octahedral distortions. Nevertheless, for selected combination of the A/A' cations a non-polar incommensurate phase is observed with average symmetry $C2/m$. Thanks to a detailed crystallographic description of the incommensurate phase, based on electron, neutron and x-ray diffraction data, we show that the incommensurate modulation is related to an abrupt change of the out-of-phase tilting along the a- and c-axis whereas the tilting along the b-axis remain constant across the structure. By using group theory and symmetry analysis we show that we observe an incommensurate analog of HIF which induces a hybrid improper dipolar density wave in NaLaCoWO$_6$. The dipolar ordering is due also in this case to a trilinear invariant involving the commensurate and incommensurate octahedra tilting's.

cond-mat.mtrl-sci

Covalent Organic Functionalization of Graphene Nanosheets and Reduced Graphene Oxide via 1,3-Dipolar Cycloaddition of Azomethine Ylide

Organic functionalization of graphene is successfully performed via 1,3-dipolar cycloaddition of azomethine ylide in the liquid phase. The comparison between 1-methyl-2-pyrrolidinone and N,N-dimethylformamide as dispersant solvents, and between sonication and homogenization as dispersion techniques, proves N,N-dimethylformamide and homogenization as the most effective choice. The functionalization of graphene nanosheets and reduced graphene oxide is confirmed using different techniques. Among them, energy-dispersive X-ray spectroscopy allows to map the pyrrolidine ring of the azomethine ylide on the surface of functionalized graphene, while micro-Raman spectroscopy detects new features arising from the functionalization, which are described in agreement with the power spectrum obtained from ab initio molecular dynamics simulation. Moreover, X-ray photoemission spectroscopy of functionalized graphene allows the quantitative elemental analysis and the estimation of the surface coverage, showing a higher degree of functionalization for reduced graphene oxide. This more reactive behavior originates from the localization of partial charges on its surface due to the presence of oxygen defects, as shown by the simulation of the electrostatic features. Functionalization of graphene using 1,3-dipolar cycloaddition is shown to be a significant step towards the controlled synthesis of graphene-based complex structures and devices at the nanoscale.

cond-mat.mtrl-sci