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Manipulating Emission Enhancement and Piezochromism in Two-Dimensional Organic-Inorganic Halide Perovskite [(HO)(CH 2 ) 2 NH 3 )] 2 PbI 4 by High Pressure

2020; Chinese Chemical Society; Volume: 3; Issue: 8 Linguagem: Inglês

10.31635/ccschem.020.202000430

2096-5745

Yuanyuan Fang, Long Zhang, Yi-Shuai Yu, Xinyi Yang, Kai Wang, Bo Zou,

Covalent Organic Framework Applications

Open AccessCCS ChemistryCOMMUNICATION1 Aug 2021Manipulating Emission Enhancement and Piezochromism in Two-Dimensional Organic-Inorganic Halide Perovskite [(HO)(CH2)2NH3)]2PbI4 by High Pressure Yuanyuan Fang, Long Zhang, Yishuai Yu, Xinyi Yang, Kai Wang and Bo Zou Yuanyuan Fang State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun 130012 , Long Zhang State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun 130012 , Yishuai Yu State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun 130012 , Xinyi Yang State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun 130012 , Kai Wang *Corresponding authors: E-mail Address: [email protected] E-mail Address: [email protected] State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun 130012 and Bo Zou *Corresponding authors: E-mail Address: [email protected] E-mail Address: [email protected] State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun 130012 https://doi.org/10.31635/ccschem.020.202000430 SectionsSupplemental MaterialAboutAbstractPDF ToolsAdd to favoritesDownload CitationsTrack Citations ShareFacebookTwitterLinked InEmail Two-dimensional (2D) organic–inorganic halide perovskites present remarkable stability and diversity and are promising alternatives to their three-dimensional (3D) counterparts. The 2D halide perovskite [(HO)(CH2)2NH3]2PbI4 (ETA2PbI4) is regarded as a superior moisture-stabile "smooth" perovskite because of distinct hydrogen-bond networks that connect adjacent organic–inorganic layers. However, effectively engineering the optical properties of ETA2PbI4 for practical applications still represents considerable challenges. Herein, we studied the effect of pressure on the optical characteristics and crystalline structure of ETA2PbI4 through a diamond anvil cell. The emission was enhanced four times at 1.5 GPa and was accompanied by a photoluminescence (PL) peak that became more symmetric, which was attributed to pressure-suppression nonradiative recombination and an increase in exciton binding energy. Moreover, the red shift of the PL peak from 542 to 674 nm was continuous at a rate of 14.4 nm/GPa with pressure up to 9.2 GPa. Meanwhile, the optical micrographs showed visualized piezochromism. High-pressure in situ synchrotron X-ray diffraction (XRD), Raman measurements, and first-principles calculations indicated a distortion of the [PbI6]4− inorganic octahedron with a decrease of the Pb−I−Pb bond angle and the Pb−I bond length leading to this series of transformations. Our findings demonstrate that 2D halide ETA2PbI4 is a prospective candidate for pressure sensors. Download figure Download PowerPoint Introduction The reduced-dimensionality perovskites, especially the two-dimensional (2D) organic–inorganic halide perovskites, have become the "next big thing" in emerging hybrid halide perovskites owing to their excellent tunability and photophysical properties.1–6 In strictly 2D organic–inorganic perovskite (A)2BX4, where the large (A)+ cations divide the infinite inorganic layers, the most common B-site cations are Pb2+, and the X-site cations typically are Cl−, Br−, or I− anions.7,8 In this case, each of the active layers is an infinite 2D sheet of the corner-sharing PbX6 octahedra.9 Through their unique crystal structures, quantum confinement leads to strong excitonic effects, therefore, strong photoluminescence (PL) was observed at room temperature.10 The uniform and stable emission spectra perovskite is the ideal material for making perovskite light-emitting diodes (LEDs).11 Moreover, 2D perovskites possess significant light absorption in the visible region which makes them a likely light absorber for photovoltaic applications.12 ETA2PbI4 (ETA = [(HO)(CH2)2NH3]+) is a unique organic–inorganic hybrid perovskite because it consists of alcohol-based bifunctional ammonium ions.13 The strong Coulomb interactions within the ETA organic layer are attributed to the extremely smooth crystal surface of ETA2PbI4. Therefore, ETA2PbI4 is considered a "smooth" 2D halide perovskite, which is less sensitive to ambient moisture and exhibits a considerably low dark current.14 However, it is essential to adjust the band gap in a wide range to realize PL tunability in this 2D hybrid perovskite. Pressure is a powerful and convenient strategy to alter the crystalline structure and electronic properties of 2D perovskite materials that are sometimes inaccessible by chemical tuning.15–21 Depending on the applied pressure, the (BA)2(MA)n− 1PbnI3n + 1 homologous series shows typical structural transition, which is accompanied by noticeable transformation in the optical properties of these materials.22,23 The model (EDBE)CuCl4 undergoes an α-to-β phase transition, triggering a color change from yellow to orange when pressure increases from 0.3 to 4.9 GPa.24 These results provided us a basic understanding of the relationship between crystalline structure and optical properties.25–33 However, most of these materials are limited by a pressure-induced decrease in PL, which limits their potential applications in optical devices.34 Despite this, controlling pressure to effectively adjust the band gap and PL increase of ETA2PbI4 remains a particularly promising approach. In this work, we report the evolution of the optical properties of 2D organic–inorganic halide perovskite ETA2PbI4 upon high-pressure processing. High-pressure PL spectra, optical micrographs, and UV–Vis absorption indicated the distinct piezochromism of the ETA2PbI4 crystal, exhibiting a red shift at approximately 132 nm from the initial 542 to 674 nm at 9.2 GPa. Furthermore, pressure-induced emission was enhanced up to 1.5 GPa resulting from the pressure-suppression nonradiative recombination and the increase in exciton binding energy. The XRD data and Raman spectra of ETA2PbI4 upon compression were obtained to trace the high-pressure changes of the inorganic [PbI6]4− octahedra. The achieved narrow emission with high color purity is favorable for applications of perovskite, which may prove a powerful candidate for pressure sensors at extreme conditions. Results and Discussion The pressure-dependent PL spectra were recorded up to 10.3 GPa (Figure 1). Under ambient conditions, ETA2PbI4 shows a sharp and narrow green-free exciton emission centered at 542 nm with full width at half maximum of 24 nm ( Supporting Information Figure S1) due to remarkable quantum confinement effects. Meanwhile, the low-energy PL tail of the ETA2PbI4 PL spectrum was ascribed to the radiative recombination of trap states.21 Intriguingly, ETA2PbI4 PL intensity was enhanced by four times from 1 atm to 1.5 GPa (Figure 1a), which was accompanied by a more symmetrical PL emission peak ( Supporting Information Figure S2). Upon further compression, the PL intensity gradually decreased until it completely disappeared at 10.3 GPa (Figure 1a). Upon decompression, the PL spectra returned to its original shape and position, but the PL intensity was slightly weaker than its atmospheric pressure state ( Supporting Information Figure S4). The emission spectra showed a wide range of pressure-induced peak change throughout the compression process (Figure 1b). A series of optical photographs clearly reveal the varying trend of the ETA2PbI4, and the following sequence could be easily visualized by the naked eyes: green → yellow → orange → red (Figure 1b). The PL emission peak of the ETA2PbI4 crystal can be tuned at a rate of 14.4 nm/GPa upon compression (Figure 1c). Furthermore, the chromaticity coordinates of PL upon compression from 1 atm to 9.2 GPa are shown in Figure 1d. The emission at 1 atm belongs to the green component (0.34, 0.64). At 9.2 GPa, the emission moved toward the monochromatic red light (0.70, 0.29). Compression resulted in high color purity and colorful PL modulation, which are favorable conditions for the development of pressure sensors.25,35 Consequently, we also used pressure to tune the chromaticity of emission, which facilitates the use of ETA2PbI4 as a pressure sensor with ultrasensitivity to pressure in the low-pressure regime (<8 GPa). Figure 1 | (a) Pressure-dependent PL spectra of ETA2PbI4 under increasing pressure. (b) The microphotographs in the sample chamber at selected pressures measured by a 355 nm laser. (c) The PL location of ETA2PbI4 as a function of pressure (red square) and PL intensity as a function of pressure (green pentagon). (d) Pressure-dependent chromaticity coordinates of the emissions from 1 atm to 9.2 GPa. PL, photoluminescence. Download figure Download PowerPoint The evolution process of the ETA2PbI4 band gap was obtained by UV–Vis absorption spectroscopy. At ambient conditions, a steep absorption edge was observed at approximately 553 nm and showed remarkable red shifts when the pressure reached 8.0 GPa (Figure 2a). The extraordinary piezochromism transition of ETA2PbI4 is evident in optical micrographs (Figure 2b). The band gap of the material was estimated by extrapolating the linear portion of (αdhν)2 versus the hν curve, where α is the absorption coefficient, d is the sample thickness, and hν is the photon energy (Figure 2c). ETA2PbI4 exhibited a direct gap of 2.24 eV at ambient conditions consistent with a previous report.13 With increasing pressure, the band gap of ETA2PbI4 obviously narrowed by 0.39 eV at 8.0 GPa, suggesting that the band gap of the 2D organic–inorganic halide perovskite is significantly modified by high pressure. Figure 2 | (a) Absorption spectra of ETA2PbI4 upon compression below 8.0 GPa. (b) Photochromic transitions of ETA2PbI4 crystals in the DAC chamber. (c) Band gap of ETA2PbI4 as a function of pressure calculated from Tauc plots. The inset shows the Tauc plot of ETA2PbI4 under ambient conditions. Download figure Download PowerPoint We obtained the in situ high-pressure angle-dispersive X-ray diffraction (ADXRD) patterns of ETA2PbI4 to investigate the correlation between the optical properties and structural variations of ETA2PbI4 (Figure 3a). Rietveld refinement results of the XRD data at ambient conditions showed that ETA2PbI4 possessed a monoclinic system with the P21/c space group; the lattice parameters were a = 10.22(1) Å, b = 8.04(1) Å, and c = 8.93(2) Å, β = 100.27(3)° ( Supporting Information Figure S6).13 Figure 3b shows the layered crystalline structure of ETA2PbI4 along the crystallographic b axis. It was formed by alternating sheets of the corner-sharing PbI6 octahedra and the organic (ETA) cation layers. Two continuous inorganic octahedral layers move slightly along the a axis, and the interlayer I–I bond was very short approximately along the c axis. Within the [PbI6]4− cluster, Pb–I bonds could be divided into two groups: four long bridging Pb–I1 bonds with I atoms located along the shared face and two shorter terminal Pb–I2 bonds that are oriented perpendicular to the shared face (Figure 3c). This structure possesses strong van der Waals interaction between the adjacent (ETA) organic layers and the inorganic octahedral layer, which causes remarkable quantum confinement effects. Accordingly, a different pressure-induced emission enhancement mechanism in ETA2PbI4 can be expected compared with that of the self-trapping exciton emission perovskites of Cs4PbBr6, C4N2H14SnBr4, and (C4H9NH3)4AgBiBr8.36–38 When pressure was applied to ETA2PbI4, all Bragg diffraction peaks monotonically shifted toward a small d-spacing due to lattice compression. Simultaneously, no new peaks appeared, while some original weak peaks disappeared. XRD spectrum revealed the partial disappearance of Bragg diffraction peaks and only left a few broad bands above 10.0 GPa. These phenomena indicate the gradual structural distortion and onset of reduced crystallinity of ETA2PbI4 upon compression, which caused the emission peak to disappear. Finally, a significantly low crystallinity appeared at approximately 20.2 GPa, accompanied by only a few weak and broad bands in the XRD pattern. To investigate the high-pressure behavior of inorganic [PbI6]4− octahedra, we analyzed ETA2PbI4 crystal by Raman spectroscopy, which was consistent with the high-pressure ADXRD result ( Supporting Information Figure S8). Figure 3 | (a) Representative ADXRD of ETA2PbI4 upon compression up to 20.2 GPa. (b) Crystal structure of ETA2PbI4 at ambient conditions, viewed along the b axis. Gray, violet, brown, silver, red, and pink spheres represent Pb, I, C, N, O, and H atoms, respectively. (c) Distorted Pb–I inorganic framework layer at ambient condition, viewed along the a axis. ADXRD, angle-dispersive X-ray diffraction. Download figure Download PowerPoint We also investigated the evolution of the cell parameters and volume ( Supporting Information Figure S9) to further analyze the structural evolution of ETA2PbI4. Crystal lattice parameters and volumes of ETA2PbI4 were stably and continuously compressed before occurrence of the severely disordered crystallinity. It was found that the deformation Δa (∼1.13 Å) was bigger than Δb (∼0.75 Å) and Δc (∼0.87 Å) under quasihydrostatic pressure at 13.0 GPa. Moreover, the deformation percentage along the a axis (11.1%) was greater than the b axis (8.3%) and the c axis (9.7%), with an average 24% decrease. As such, clear anisotropic compression may correspond to the sandwich structure made up of alternately connected organic and inorganic layers. Moreover, the experimental pressure−volume (P−V) data ( Supporting Information Figure S9b) obtained from atmospheric conditions to 13.0 GPa were fitted by utilizing the third-order Birch-Murnaghan equation of state. The fitting bulk modulus (K0) of ETA2PbI4 was 22.3 GPa, comparable to that of other 2D halide perovskites.39 The compressibility of a material is inversely proportional to K0. The compressibility of ETA2PbI4 is obviously smaller than that of its analog 3D perovskites (13.6 GPa of MAPbI3).40 Therefore, 2D perovskite ETA2PbI4 is harder and more resistant to pressure than 3D perovskites. First-principles calculations were performed to investigate the variations of the electronic band structure upon compression, calculated electronic band structure is essential to fully understand the interaction between crystal structure and excitonic bands under high pressure. The results indicate that ETA2PbI4 possesses a direct band gap of 1.78 eV at ambient conditions, and the band gap shrinks continuously with increasing pressure up to 8.0 GPa (Figure 4c), which is consistent with the results of our experiments. The valence band maximum (VBM) is mainly comprised of Pb 6s states with contribution of I 5p states. Simultaneously, the conduction band minimum (CBM) is mainly formed by Pb 6p orbitals with contribution of I 5s states ( Supporting Information Figure S10). Upon compression, all the Pb–I1–Pb angles showed a slight compression (Figure 4a and Supporting Information Table S1) because of the tilting and rotation of [PbI6]4− inorganic octahedra relative to its adjacent octahedra along the a axis. Meanwhile, the bridging Pb–I1 bonds and terminal Pb–I2 bonds were gradually reduced (Figure 4b and Supporting Information Table S2). As such, an increasing electronic band dispersion accompanied rising VBM and falling CBM (Figures 4d and 4e).22,23 Therefore, the band gap exhibits a remarkable decrease under 8.0 GPa.41 Figure 4 | (a) Schematic illustrations of Pb−I1−Pb bond angle within inorganic octahedral framework upon compression. (b) Schematic illustrations of Pb−I bond length within PbI6 octahedral framework upon compression. (c) First-principles calculated band gap for ETA2PbI4 at different pressures. (d and e) Electronic band structure for ETA2PbI4 under ambient conditions and 8.0 GPa, respectively. Download figure Download PowerPoint Under lower pressure, the well thickness (L) showed obvious decrease ( Supporting Information Figure S11) caused by the increase of dielectric confinement due to the negative correlation between L and dielectric confinement.42,43 Given that the exciton binding energy is positively correlated with the dielectric confinement, the exciton binding energy increase led to the PL enhancement of ETA2PbI4 under mild pressure.10,44–46 In addition, the more symmetrical PL peak ascribed to pressure-suppressed carrier trapping caused the decrease of the nonradiative recombination, which also triggers the enhanced emission.47 As a result, there was a four times PL enhancement of ETA2PbI4 observed under 1.5 GPa. Above 1.5 GPa, although L still decreased, the pressure-induced suppression effect on the PL began to dominate the emission process, which was mainly caused by the structural disorder and which resulted in slow and nonlinear PL weakening.21,48 Conclusion The pressure-engineered crystalline structure and optical properties of ETA2PbI4 were systematically studied with a symmetric diamond anvil cell (DAC) apparatus. The perovskite crystal exhibited distinct enhancement of PL intensity and narrowing of band gap when pressure was applied. High-pressure PL micrographs and UV–Vis absorption micrographs indicated the distinct piezochromism of ETA2PbI4 crystal. Synthetic experiments containing in situ high-pressure ADXRD and Raman measurements indicated that ETA2PbI4 crystal experienced remarkable distortion of the [PbI6]4− octahedral. Our work provides supplementary information on the intrinsic characteristics of 2D organometal halide perovskites. 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Google Scholar Previous articleNext article FiguresReferencesRelatedDetails Issue AssignmentVolume 3Issue 8Page: 2203-2210Supporting Information Copyright & Permissions© 2020 Chinese Chemical SocietyKeywordsband gap red shiftpiezochromismtwo-dimensional perovskitehigh pressureemission enhancementAcknowledgmentsThis work is supported by the National Science Foundation of China (NSFC) (nos. 21725304 and 11774120) and the Chang Jiang Scholars Program of China (no. T2016051). Angle-dispersive XRD measurement was performed on the BL15U1 at the Shanghai Synchrotron Radiation Facility (SSRF). Downloaded 1,895 times PDF DownloadLoading ...