Kar Moumita, Ghosh Atish, Sarkar Ritabrata, Pal Sougata, Sarkar Pranab
Department of Chemistry, Visva-Bharati University, Santiniketan, India.
Department of Chemistry, University of Gour Banga, Malda, India.
J Comput Chem. 2021 Oct 15;42(27):1982-1990. doi: 10.1002/jcc.26731. Epub 2021 Aug 14.
Recently, two-dimensional organic-inorganic hybrid perovskites have attracted great attention for their outstanding performances in solar energy conversion devices. By using first principles calculations, we explored the structural, electronic and optical properties of recently synthesized (PEA) PbI and (PEA) SnI organic-inorganic hybrid perovskites to understand the photovoltaic performances of these systems. Our study reveals that both the perovskites are direct band gap semiconductors and possess desirable band gap for solar energy absorption. We have further extended our study to fluoro-, chloro-, and bromo-functionalized phenethylammonium (PEA) cations based [X(X = F, Cl, Br)PEA] A(A = Pb, Sn)I perovskite materials. The halogenated benzene moiety confers an ultrahydrophobic character and protects the perovskites from ambient moisture. The halogen functionalized perovskites remain direct band gap semiconductors and all the perovskites show very strong optical absorption (∼7 × 10 cm ) across UV-visible region. We have further calculated the photo-conversion efficiency (PCE) of both arene and functionalized arene based perovskites. The halogen-functionalized PEA-based perovskites also exhibit high PCE as like pristine ones and finally achieve high PCE of up to 24.30%, making them competitive with other previously reported perovskite-based photovoltaic devices.
最近，二维有机-无机杂化钙钛矿因其在太阳能转换器件中的出色性能而备受关注。通过第一性原理计算，我们研究了最近合成的(PEA)PbI和(PEA)SnI有机-无机杂化钙钛矿的结构、电子和光学性质，以了解这些体系的光伏性能。我们的研究表明，这两种钙钛矿都是直接带隙半导体，并且具有适合太阳能吸收的带隙。我们进一步将研究扩展到基于氟、氯和溴功能化苯乙铵(PEA)阳离子的[X(X = F、Cl、Br)PEA]A(A = Pb、Sn)I钙钛矿材料。卤代苯部分赋予超疏水特性，并保护钙钛矿免受环境湿气影响。卤化功能化钙钛矿仍然是直接带隙半导体，并且所有钙钛矿在紫外-可见光区域都表现出非常强的光吸收(∼7×10⁵ cm⁻¹)。我们还进一步计算了基于芳烃和功能化芳烃的钙钛矿的光转换效率(PCE)。卤化功能化的基于PEA的钙钛矿也像原始钙钛矿一样表现出高PCE，最终实现高达24.30%的高PCE，使其与其他先前报道的基于钙钛矿的光伏器件具有竞争力。
