Giant Nonlinear Optical Response in Triple Cation Halide Mixed Perovskite Films

Abstract

exceptional properties including high photostability, extremely long charge diffusion length, and thermal stability. The perovskites have become emerging high-performance materials for various optoelectronic applications such as solar cells, [1][2][3] light emitting diodes, [4,5] photodetectors, [6,7] and lasers. [8,9] The halide perovskites also exhibit strong nonlinear optical (NLO) responses, thus opening up possibilities for optoelectronic device applications. [10][11][12][13][14] For instance, organic-inorganic hybrid perovskites with large two-and three-photon absorption (2PA, 3PA) properties [14][15][16] can be utilized in applications such as bioimaging, [17,18] optical limiting, [19] optical sensor protection, [20] and optical data storage. [21] Nonlinear absorption properties of single crystal, nanocrystal, and filmed perovskites have been intensively studied. [10][11][12][13][14][15][16][22][23][24] Recently, lead halide perovskites such as MAPbI 3 (MA = CH 3 NH 3 ) and MAPbBr 3 have shown higher multiphoton absorption (MPA) probability as the excitation wavelength increases in the IR region. [10][11][12][13][14][22][23][24] Johnson et al. [25] reported that the observation of third-order nonlinearities and decay kinetics in MAPbBr 3 and MAPbBr 2 I with different halogen composition. They showed that the third-order nonlinearities of these materials are larger than those of conventional semiconductors. The photoluminescence of MAPbBr 3 single crystal has also been observed in the green region (522-550 nm) with 1044 nm femtosecond laser excitation due to 2PA. [26] Similar nonlinear optical properties were reported in inorganic perovskites, including CsPbI 3 and CsPbBr 3 . [22,27,28] Another type of perovskite, formamidinium lead iodide (FAPbI 3 ), has a low bandgap (1.47 eV) and greater photostability and thermal stability [29,30] than MAPbI 3 . However, FAPbI 3 has a weak structural stability due to humidity, which prevents it from real-life applications. [31] Recently, it has been demonstrated that the mixture of Cs and MAPbI 3 , CsMAPbI 3 , can lead to a stable solar cell with power conversion efficiency of ≈8%. [32] In addition, the mixture of Cs in FAPbI 3 , such as FA 0.9 Cs 0.1 PbI 3 , showed an improved thermal stability and results in high power conversion efficiency of ≈16.5%. [33] By using this material, Yi et al. have demonstrated power conversion efficiency up to 18% with a halide mixer I/Br. [34] The malleable association The versatility of perovskites through chemical composition modification is critical for enhancing performance of a range of potential applications such as light emitters and integrated photovoltaics. However, a systematic study on the nonlinear optical (NLO) responses of these perovskites is still lacking. Here, for the first time, the NLO properties of triple cation mixed halide perovskite (TCMHP) films, (Cs 0.06 FA 0.79 MA 0.15 )Pb (I 0.85 Br 0.15 ) 3 , using Z-scan and time-resolved spectroscopy, are investigated. It is found that TCMHP film shows strong saturable abs...

Perovskites: Multiphoton Absorption and Applications

“…It has been reported by Syed et al, [73] but, not included in Table 3 and Figure 2c, that a phonon-assisted anti-Stokes process can make a giant enhancement to the 3PA in triple cation mixed halide perovskite (Cs 0.06 FA 0.79 MA 0.15 )Pb(I 0.85 Br 0.15 ) 3 . By performing Z-scan measurements with ns laser pulses, Syed and co-workers found an intensity-dependent NLO performance at 790 nm.…”

Advances of Nonlinear Photonics in Low‐Dimensional Halide Perovskites

“…To date, beneficial from the remarkable NLO, perovskite materials have suggested great potential in various fields, for example, up-conversion light emission, [30,72,73] powerlimiting, [95] photon detector, [26,96,98] all-optical modulation, [105] optical rectification, [24,28] laser pulse autocorrelation [18] and so on. This section illustrates a summary and discussion about the recent progress for the application based on the NLO of LDPs.…”

“…Nevertheless, it is worth noting that, in the past few years, the tunable bandgap and large optical oscillator strength have enabled halide perovskites to be promising materials for the applications of NLO devices. Strong multiphoton absorption (MPA) has been observed in bulk 3D perovskite single crystals, [18][19][20][21][22][23][24] polycrystalline films, [25][26][27][28][29] and micro-resonators. [30][31][32][33][34] The two-photon absorption (2PA) coefficient of MAPbBr 3 single crystal was determined up to 8 cm GW −1 , [18,24] which is on the same order of the conventional semiconductors such as CdS, CdSe, ZnO, and ZnS.…”

Toward stable lead halide perovskite solar cells: A knob on the A/X sites components

“…Syed et al. demonstrated the strong saturable absorption peak of 395 nm as well as the reverse saturable absorption peak of 790 nm (two-photo absorption) and 1200 nm (three-photo absorption) in the mixed triple cation halide perovskite ( Syed et al., 2020 ). Strong three-photo absorption near to the band gap reveals optical stabilization, great spatial confinement, and large penetration depth, which is rooted in phonon-assisted anti-Stokes processes( Minda et al., 2018 ).…”