Hybrid Organic–Inorganic Coordination Complexes as Tunable Optical Response Materials

Abstract

Novel lead and bismuth dipyrido complexes have been synthesized and characterized by single-crystal X-ray diffraction, which shows their structures to be directed by highly oriented π-stacking of planar fully conjugated organic ligands. Optical band gaps are influenced by the identity of both the organic and inorganic component. Density functional theory calculations show optical excitation leads to exciton separation between inorganic and organic components. Using UV-vis, photoluminescence, and X-ray photoemission spectroscopies, we have determined the materials' frontier energy levels and show their suitability for photovoltaic device fabrication by use of electron- and hole-transport materials such as TiO2 and spiro-OMeTAD respectively. Such organic/inorganic hybrid materials promise greater electronic tunability than the inflexible methylammonium lead iodide structure through variation of both the metal and organic components.

Narrow-band anisotropic electronic structure of ReS2

“…Geometry optimizations were performed using the PBEsol functional [28], a version of the Perdew, Burke, and Ernzerhof (PBE) functional [29] revised for solids. PBEsol has previously been shown to adequately account for weakly dispersive interactions, such as those seen in the layered structure of ReS 2 , without the need for an additional correction [30,31]. Optimizations were deemed converged when the sum of all forces on each atom totaled less than 10 meVÅ −1 .…”

Electronic and defect properties of (CH3NH3)2Pb(SCN)2I2analogues for photovoltaic applications

“…57,58 This combination of HSE06 with SOC has been shown to provide an accurate description of the electronic structures for many bismuth and lead containing solar absorbers and was therefore used during density of states and band structure calculations. [59][60][61][62] The Brillouin zone for the Pnm2 1 space group, illustrating the relevant high symmetry points, is provided in Fig. S1 of the ESI.…”

Defect Engineering of Earth-Abundant Solar Absorbers BiSI and BiSeI

“… 8 Third-generation solar absorbers present an exciting alternative with increased efficiency, roll-to-roll printing, and the use of lightweight flexible substrates offering routes to reduced costs. 5 , 9 , 10 …”