Optical properties of two-dimensional perovskites

doi:10.1007/s11467-023-1256-8

Front. Phys.

2023, Vol. 18

Issue (3) : 33602 https://doi.org/10.1007/s11467-023-1256-8

TOPICAL REVIEW

Optical properties of two-dimensional perovskites

Junchao Hu¹, Xinglin Wen^1,²(

), Dehui Li^1,²(

)

¹. School of Optical and Electronic Information, Huazhong University of Science and Technology, Wuhan 430074, China
². Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074, China

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Abstract

The optical properties of two-dimensional (2D) perovskites recently receive numerous research focus thanks to the strong quantum and dielectric confinement effects. In addition to the strong excitonic effect at room temperature, 2D perovskites also have appealing features that their optical properties can be flexibly tuned by alternating organic or inorganic layers. Particularly, 2D chiral perovskites and 2D perovskites based heterostructures are emerging as new platforms to extend their functionalities. To optimize performance of 2D perovskites-based optoelectronic devices, it is critical to understand the fundamentals and explore the strategies to engineer their optical properties. This review begins with an introduction to the excitons and self-trapped excitons of 2D perovskites. Subsequently, inorganic/organic layer effects on optical properties and 2D perovskites based heterostructures are discussed. We also discussed the nonlinear optical properties of 2D perovskite. We are looking forward to that this review can stimulate more efforts to understand and optimize the optical properties of 2D perovskites.

Keywords optical properties two-dimensional perovskite heterostructures self-trapped excitons

Corresponding Author(s): Xinglin Wen,Dehui Li

Issue Date: 15 March 2023

Cite this article:

Junchao Hu,Xinglin Wen,Dehui Li. Optical properties of two-dimensional perovskites[J]. Front. Phys. , 2023, 18(3): 33602.

URL:

https://academic.hep.com.cn/fop/EN/10.1007/s11467-023-1256-8
https://academic.hep.com.cn/fop/EN/Y2023/V18/I3/33602

Fig.1 (a) Schematic of 3D and 2D perovskite structure. (b) Characteristic band-alignment in 2D perovskites.

Fig.2 (a) 2D plot of TA spectra of (BA)₂PbI₄ film [45]. (b) PL spectra of α-(DMEN)PbBr₄, (DMAPA)PbBr₄ and (DMABA)PbBr₄ [47]. (c) Absorption and PL of (NBT)₂PbI₄ and (EDBE)PbI₄ [43]. (d) Structure fragment of three-layered (EA)₄Pb₃Cl₁₀, (EA)₄Pb₃Br₁₀ and hydrogen bonding network in (EA)₄Pb₃Br₁₀. (e) Comparison of the distortion level of outer layer and inner layer of (EA)₄Pb₃Cl₁₀ and (EA)₄Pb₃Br₁₀. (f) PL of (EA)₄Pb₃Br_10−xCl_x (x = 0, 2, 4, 6, 8, 9.5 and 10). (d−f) Reproduced from Ref. [48].

Fig.3 (a) PL spectra of (BA)₄AgBiBr₈ under high pressure. (b) Pressure dependent PL. (c) Mechanism of pressure-induced emission associated with exciton self-trapping at ambient conditions and upon compression. Bi−Br−Ag bond angle is in bc plane of (BA)₄AgBiBr₈ under compression. Reproduced from Ref. [49].

Fig.4 (a) and (b) are energy level diagram of 2D RP perovskites (BA)₂(MA)_n−1Pb_nI_3n+1 and (BA)₂(MA)_n−1Ge_nI_3n+1 (n = 1−5 and n = ∞) [50]. (c) Crystalline structures of the 2D lead iodide perovskites (BA)₂(MA)_n−1Pb_nI_3n+1 (n = 1−4), the L-value denotes the thickness of the inorganic layer in each compound. (d) and (e) are optical absorption and PL of 2D perovskites with different thickness (n = 1−4 and n = ∞). (c−e) Reproduced from Ref. [49].

Fig.5 (a) UV-Vis absorption and (b) PL spectra of (PEA)₂PbX₄ nanosheets (X = Cl, Br, I) with different compositions [31]. (c) Electronic band structure of the polar configuration of (BA)₂(MA)_n−1Pb_nI_3n+1 (n = 1, 3, 4) [30]. (d) The computed electronic bandgaps of (BA)₂(MA)_n−1M_nI_3n+1 (M = Ge, Sn and Pb; n = 1−4 and n = ∞) based on the hybrid functional plus SOC schemes. The light-green horizontal bar denotes the optimal bandgap range (0.9 to 1.6 eV) for solar cells [33]. (e) Tauc plots of (PEA)₂Ge_1−xSn_xI₄ perovskite with different Sn content [52]. (f) PL spectra of bulk crystal of PEA₂PbI₄, PEA₂SnI₄ and PEA₂PbI₄:Sn (0.36%) at room temperature [54].

Fig.6 (a) Photoluminescence spectra in single crystal of (C_nH_2n+1NH₃)₂PbI₄ with n = 4, 8, 9, 10 and 12 at 1.6 K and optical density spectra in a cleaved thin crystal of (C₁₀H₂₁NH₃)₂PbI₄ at several temperatures [38]. (b) Absorption spectra at 300 K and 10 K for (C₁₀H₂₁NH₃)₂PbI₄, (PEA)₂PbI₄ and (PEA)₂(MA)Pb₂I₇ [57]. (c) 3-AMP and 4-AMP molecular structure and general crystal structure of the two series of DJ perovskite from n = 1 to 4. (d) The absorption band energy of n = 1 to 5. (e) Average equatorial Pb−I−Pb angles for 3-AMP and 4-AMP series from n = 1 to 4. (c−e) Reproduced from Ref. [58]. (f) Plot of absorbance peak positions verse A-site cation size of (HA)₂(A)Pb₂I₇ perovskite, and octahedral structure model of different A cation size [60].

Fig.7 (a) CD spectra and normalized extinction spectra of (S-MBA)₂PbI₄, (R-MBA)₂PbI₄ and (rac-MBA)₂PbI₄ film [71]. (b) CD spectra of pure S-MePEA, pure achiral (C4A) and mixed-cation perovskite film [72]. (c) Normalized extinction spectra and (d) CD spectra of (S-MBA)₂PbI_4(1−x)Br_4x and (R-MBA)₂PbI_4(1−x)Br_4x (x = 0, 0.1, 0.2, 0.3, 0.4 and 0.5) film [73].

Fig.8 Degree of polarization for (a) racemic-RDCP, (b) R-RDCP and (c) S-RDCP of low-dimensional perovskites with magnetic field varied from −7 T to 7 T [70]. Circularly polarized PL spectra of (d) (R-MBA)₂PbI₄ and (e) (S-MBA)₂PbI₄ excited by a 473 nm laser at 77 K [83]. (f) In-plane views of [PbBr₄]²⁻ layers in R-NPB, S-NPB and racemic-NPB. (g) Hydrogen bonding interactions between the equatorial Br atoms and NEA⁺ cations in R-NPB, S-NPB and racemic-NPB [92].

Fig.9 (a) Dependence of the circular dichroism (CD) signal on the concentration and temperature of the nanoplatelet (NP) solution [94]. (b) Ligand exchange on an OA-capped perovskite NC using pure enantiomers of DACH and CD spectra of low concentrations of DACH [89]. (c) Schematic representation of CD ligand ratio and CD strength of chiral perovskite nanoplates [90]. (d) Working principle of the circularly polarized light (CPL) system with the handedness superstructure stack [91].

Fig.10 (a) PL of (PEA)₂PbI₄/(PEA)₂(MA)Pb₂I₇ 2D perovskite heterostructures. (b) PL of the 532 nm (n = 1) and 576 nm (n = 2) peaks as a function of excitation power. The β indicates the slope of the relation. (a, b) Reproduced from Ref. [97]. (c) Schematic illustration of the synthesis of (BA)₂PbI₄/(BA)₂(MA)Pb₂I₇ heterostructures. (d) Normalized PL of (BA)₂PbI₄/(BA)₂(MA)Pb₂I₇ heterostructures with different mass ratios of BAI/MAI. (e) Normalized PL of (BA)₂PbI₄/(BA)₂(MA)Pb₂I₇ heterostructures with different maintaining times for a fixed MAI concentration. (c−e) Reproduced from Ref. [96]. (f) PL images of the vertical heterostructures (BA)₂PbBr₄-(BA)₂(MA)₂Pb₃I₁₀ under the heating treatment process. (g) Evolution of PL of the vertical heterostructures upon heating at 60 ℃. (f, g) Reproduced from Ref. [99]. (h) Schematic illustrations and proposed band alignments of (2T)₂PbI₄-(2T)₂PbBr₄ and (BA)₂PbI₄-(BA)₂PbBr₄ lateral heterostructures. (i) Optical and PL images of lateral heterostructures. (j) PL of the heterostructures before and after heating. (h−j) Reproduced from Ref. [98].

Fig.11 (a) Normalized PL of WSe₂/(iso-BA)₂PbI₄ (x = 1, 2, 3, 4) and 1L WSe₂/(iso-BA)₂(MA)Pb₂I₇ vdW heterostructure. (b) IXs emission energy as a function of the layer number x of the constituent materials and (c) band alignment of the vdW heterostructure formed by WSe₂ and (iso-BA)₂(MA)_n−1Pb_nI_3n+1 perovskites. (a−c) Reproduced from Ref. [105]. (d) Different electron transfer routes for excitons generated far from the WS₂/(PEA)₂PbI₄ interface. (e) PLE of a heterostructure at 110 K. (d, e) Reproduced from Ref. [104]. (f) IXs in the 2D perovskite/monolayer TMD heterostructure. (g) IXs emission of (iso-BA)₂PbI₄/WSe₂, (BA)₂PbI₄/WSe₂ and (S-MBA)₂PbI₄/WSe₂ under a 633 nm laser excitation. (f, g) Reproduced from Ref. [100]. (h) Manipulation of valley polarization in monolayer MoS₂ via chiral 2D perovskite/MoS₂ heterostructure [101].

Fig.12 (a) Schematics of the SHG measurements. λ/2 and λ/4 plates were used for linearly and circularly polarized experiments, respectively. (b) SHG of an (R-MPEA)_1.5PbBr_3.5(DMSO)_0.5 nanowire pumped at various wavelengths. (c) SHG intensity from the nanowire as function of the rotation angle of the λ/4 plate. (a−c) Reproduced from Ref. [120]. (d) SHG mapping of (R-ClPEA)₂PbI₄ microwire. (e) Wavelength-dependent SHG of (R-ClPEA)₂PbI₄ microwire arrays at the excitation wavelength varying from 720 to 880 nm. (f) Linear-polarization-dependent SHG of (R-ClPEA)₂PbI₄ microwire arrays. (d−f) Reproduced from Ref. [121]. (g) Conceptual illustration of SHG generation of as-prepared microwires. (h) Wavelength-dependent SHG intensity of (S-3AP)₄AgBiBr₁₂ microwire arrays at wavelengths varying from 760 to 920 nm. (i) Polarization-dependent SHG of (S-3AP)₄AgBiBr₁₂ microwire arrays. (g−i) Reproduced from Ref. [122].

Fig.13 (a) Fundamental wavelength dependence THG of (BA)₂Pb(I/Br)₄ and (BA)₂(MA)_n−1Pb_nI_3n+1 (n = 2, 3) perovskite crystals. (b) Thickness dependence THG with four different types of crystals excited at resonance. (a, b) Reproduced from Ref. [124]. (c) Comparison of THG of (BA)₂(MA)_n−1Pb_nI_3n+1 perovskite, n = 1 (purple), n = 2 (blue), n = 3 (green), n = 4 (red), n = ∞ and AgGaSe₂ (black). (d) Fine-scale THG scanned across the band edges of the 2D perovskites, overlaid with the measured absorption spectra (colored traces). (c, d) Reproduced from Ref. [125].

Fig.14 (a) Inverse transmission as a function of peak intensity for (PEA)₂PbI₄ flake, fitted by TPA saturation (red curve) and nonsaturation (blue dashed line) models. (b) Plot of TPA coefficient versus sample thickness for (PEA)₂PbI₄ flakes. (a, b) Reproduced from Ref. [127]. (c) PL of (BA)₂(FA)Pb₂Br₇ under the excitation at 800 nm [128]. (d) 2PPL spectra measured on the 316 nm thick (I_{n = 1}), 582 nm thick (I_{n = 2}), 154 nm thick (I_{n = 3}), 155 nm thick (I_{n = 4}) and 0.5 mm thick bulk CdS. The 2PPL peaks are normalized by their thickness. (e) Experimentally measured (colored dots) and theoretically calculated (colored curves) degenerate TPA spectra. (d, e) Reproduced from Ref. [129]. (f) Thickness-dependent TPA coefficient and TPA saturation intensity for n = 1/n = 2 heterostructures [130].

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