2D and 3D double perovskite with dimensionality-dependent optoelectronic properties: first-principle study on Cs₂AgBiBr₆ and Cs₄AgBiBr₈

Abstract

Recently, the effect of dimensional control on the optoelectronic performance of two-dimensional (2D)/three-dimensional (3D) single perovskites has been confirmed. However, how the dimensional change affects the photoelectric properties of 2D/3D all-inorganic double perovskites remains unclear. In this study, we present a detailed theoretical research on a comparison between the optoelectronic properties of 3D all-inorganic double perovskite Cs2AgBiBr6 and recently reported 2D all-inorganic double perovskite Cs4AgBiBr8 with Ruddlesden–Popper (RP) structure based on density functional theory calculations. The results demonstrate the charge carrier mobility and absorption coefficients in the visible spectrum of Cs4AgBiBr8 (2D) is poorer than Cs2AgBiBr6 (3D). Moreover, the value of exciton-binding energy for 2D RP all-inorganic double perovskite Cs4AgBiBr8 (720 meV) is 3 times larger than that of 3D all-inorganic double perovskite Cs2AgBiBr6 (240 meV). Our works indicate that Cs4AgBiBr8 (2D) is a promising material for luminescent device, while Cs2AgBiBr6 (3D) may be suitable for photovoltaic applications. This study provides a theoretical guidance for the understanding of 2D RP all-inorganic double perovskite with potential applications in photo-luminescent devices.

Preparation and Energy Storage Performance of Perovskite Luminescent Materials by an Electrochemiluminescence Method

“…Replacing conventional energy sources with fossil fuels, including lithium-ion batteries (LIB), solar cells (solar cells), supercapacitors (SC), nanogenerators (NG), biofuel cells (BFC), and photodetectors (PDs) [17], is therefore necessary to develop self-powered systems to meet the growing demand for long-term energy use in different environmental scenarios [18][19][20]. With the development of integrated power plant, small, light, high-density and high-reliability energy systems will be better combined [21][22][23]. For example, LIB and solar cell, if a new perovskite material with excellent photovoltaic effect is designed into an integrated dual-function device, it will have a broad development prospect in the future.…”

First-principles study on photoelectric properties of all-inorganic two-dimensional double perovskite Cs3AgBiBr7

“…Theoretically, Chen et al studied the photoelectric properties of 2D inorganic double perovskite Cs 4 AgBiBr 8 and confirmed that it is more suitable for luminescence application than 3D all-inorganic double perovskite. 15 Murgulv et al theoretically investigated the detection performance of X-ray, revealing that the double perovskite (BA) 2 CsAgBiBr 7 has great potential in the biomedical field. 16 Palummo et al theoretically revealed electronic and optical properties of a pair of Pb-free 2D layered hybrid perovskites, (BA) 4 AgBiBr 8 and (BA) 2 CsAgBiBr 7 , indicating that the 2D compounds can be used as polarization sensitive optical devices.…”

Bandgap Engineering of Two-Dimensional Double Perovskite Cs4AgBiBr8/WSe2 Heterostructure from Indirect Bandgap to Direct Bandgap by Introducing Se Vacancy

“…Recently, all-inorganic halide perovskites, especially the double perovskite, without molecules and lead-free perovskite showing excellent stability against moisture, heat, and light, have attracted extensive attention [ 1 , 2 , 3 ]. In general, since the 2D all-inorganic double perovskite Cs 4 AgBiBr 8 has a high exciton-binding energy, which is 3 times larger than that of the 3D all-inorganic double perovskite Cs 2 AgBiBr 6 , the charge carrier mobility and absorption coefficients of Cs 4 AgBiBr 8 (2D) in the visible spectrum are worse than those of Cs 2 AgBiBr 6 (3D) [ 4 ]. However, in 2021, Wang et al reported the upconversion photovoltaic effect of WS 2 monolayer/(C 6 H 5 C 2 H 4 NH 3 ) 2 PbI 4 2D perovskite heterostructures by below-bandgap two-photon absorption via a virtual intermediate state, which enables heterojunction devices with good photoresponsivity and excellent current on/off ratio [ 5 ].…”