Incorporating an Aromatic Diammonium To Assemble Bilayered Dion–Jacobson Perovskite Crystals for Weak Light Detection

Xiao

Advanced Optical Materials

et al. 2023

Perovskite hydrates have attracted extensive attention in diverse fields with intriguing optoelectronic properties, while their structural distortions usually cause large band gaps, which yield inferior light absorption and diminished optoelectronic device performance. Herein, modulating the structural distortion by steric hindrance effects is reported. Specifically, an N,N,N′,N′‐tetramethyl‐1,4‐phenylenediammonium (TMPD)2+ is adopted to template regular BiBr5 chains by interacting with bismuth bromide via weakening and reorienting H‐bonds, yielding a mixed 0D/1D (TMPD)2Bi2Br10.H2O with a narrow bandgap of 1.89 eV. The 0D/1D (TMPD)2Bi2Br10.H2O can be reversibly transformed into 0D (TMPD)2Bi2Br10 (Eg = 2.55 eV) with good cycling behavior. The (TMPD)2Bi2Br10.H2O turns out to be more stable than (TMPD)2Bi2Br10, and a mechanism involving vacancy‐assisted bromide ion migration is proposed for understanding the formation of BiBr5 chains. Density functional theory (DFT) calculations indicate that the (TMPD)2+ triggered hydration has a crucial impact on the downshift of the conduction band edge, thus decreasing the band gap. Moreover, the (TMPD)2Bi2Br10.H2O single crystal exhibits promising photoconductive behavior under a high moisture atmosphere, showing superiority over the conventional CH3NH3PbI3 perovskites that cannot survive moisture. This finding offers new insights into developing narrow band gap perovskite hydrates toward practical optoelectronic applications.

Section: Resultsmentioning

confidence: 99%

“…H 2 O single crystal as the active material with symmetrical Ag electrodes in a lateral contact, just as that of the recently reported (3AMPY)(MA)Pb 2 Br 7 [ 25 ] and (3AMPY)(EA)Pb 2 Br 7 devices. [ 26 ] Weak light is applied to monitor the simple photoconductivity of the devices under 10 V bias voltage (Figures S11 and S12, Supporting Information). Under the relatively high humidity (corresponding to the (TMPD) 2 Bi 2 Br 10 .…”

Section: Resultsmentioning

confidence: 99%

Narrow‐Bandgap Mixed 0D/1D Bismuth Bromide Perovskite Hydrate Enabled by Aromatic Ditertiary Ammonium Spacer

Xiao

Advanced Optical Materials

et al. 2023

“…For example, Priya’s group reported a series of quasi-2D RP-type halide perovskite single-crystal photodetectors based on (C 4 H 9 NH 3 ) n (CH 3 NH 3 ) n −1 Pb n I 3 n +1 ( n = 1, 2, 3, 4, and ∞), which show a higher on/off ratio of 10 4 . A single-crystal (C 6 H 5 C 2 H 4 NH 3 ) 2 PbI 4 device with a high detectivity ( D *) of 1.89 × 10 15 Jones and an (NH 3 C 4 H 8 NH 3 )PbI 4 device with a low X-ray detection limit of 430 nGy air s –1 have been reported by Liu’s group. , Our team has reported multiple cases of DJ-type HOIPs single-crystal photodetectors, such as (3AMPY)(EA)Pb 2 Br 7 (3AMPY = 3-(aminomethyl)pyridinium, EA = ethylammonium), (3AMPY)(FA)Pb 2 I 7 (FA = formamidinium), (3AMPY)(MA)Pb 2 Br 7 (MA = methylammonium), and so on (details on the performance are listed in Table S1). However, these photodetectors require an external bias to operate, which is a significant obstacle for practical applications.…”

Section: Introductionmentioning

confidence: 99%

Polar Bilayered Dion–Jacobson Hybrid Perovskite Single Crystal with Bulk Photovoltaic Effect for Self-Driven X-ray–Ultraviolet–Visible Photodetection

Fu,

Chen,

Chang

et al. 2023

Chem. Mater.

Self Cite

Polar two-dimensional (2D) multilayered hybrid perovskites (HPs) have emerged as an outstanding class of selfdriven photodetection materials. However, the current market for self-driven photodetection is almost dominated by Ruddlesden− Popper (RP) HPs. Up to now, most of the Dion−Jacobson (DJ) HPs reported have crystallized in the centrosymmetric space group, so the photodetection based on this needs to be driven by external circuits, which not only increases the cost of the device but also limits the flexibility and photostability of the device. Therefore, constructing a broadband self-driven photodetection system that integrates sensing and energy supply in DJ HPs is the development trend of the future. Herein, we constructed two new polar DJ HPs (1,3-BMACH)(MA)Pb 2 I 7 and (1,3-BMACH)(FA)Pb 2 I 7 (1,3-BMACH is 1,3-bis(aminomethyl)cyclohexane, MA is methylammonium, FA is formamidinium) using cyclic diammonium as the spacer and MA, FA as perovskitizers, respectively. Due to the larger size of FA than MA, the elongation of Pb−I bond length results in (1,3-BMACH)(FA)Pb 2 I 7 (λ cutoff = 630 nm) having a narrower light absorption range than (1,3-BMACH)(MA)Pb 2 I 7 (λ cutoff = 650 nm). The devices based on (1,3-BMACH)(MA)Pb 2 I 7 single crystals can achieve high-efficiency broadband self-driven photodetection from the X-ray and ultraviolet to visible-light region. The self-driven detection for X-ray has a high sensitivity (199 μC Gy air −1 cm −2 ) and a low detection limit (106 nGy air s −1 ). Especially, the detectivity and responsivity of the device can reach 4.82 × 10 10 Jones and 0.58 mA/W under zero bias at 405 nm laser illumination. Meanwhile, (1,3-BMACH)(MA)Pb 2 I 7 and (1,3-BMACH)(FA)Pb 2 I 7 also exhibit reversible thermochromic transformation from light red to dark red.

Spacer Conformation Induced Multiple Hydrogen Bonds in 2D Perovskite toward Highly Efficient Optoelectronic Devices

Dong,

Yang,

Yao

et al. 2024

Advanced Materials

Two‐dimensional (2D) Dion–Jacobson (DJ) perovskites typically outperform Ruddlesden–Popper analogs in terms of photodetection (PD). However, the mechanism behind this enhanced performance remains elusive. Theoretical calculations for elucidating interlayer spacer conformation‐induced multiple hydrogen bonds in 2D perovskite are presented, along with the synthesis of DPAPbBr4 (DPB) single crystals (SCs) and their PD properties under X‐ray/ultraviolet (UV) excitation. The high‐quality DPB single crystal enhances PD with exceptional photoresponse attributes, including a high on/off ratio (4.89×104), high responsivity (2.44 A/W), along with large dynamic linear range (154 dB) and low detection limit (7.1 nW/cm2), which are currently the best results among 2D perovskite single crystal detectors, respectively. Importantly, high‐resolution images are obtained under UV illumination with weak light levels. The SC X‐ray detector exhibits a high sensitivity of 663 μC Gyair–1 cm–2 at 10 V and a detection limit of 1.44 μGyair s–1. This study explores 2D DJ perovskites for efficient and innovative optoelectronic applications.This article is protected by copyright. All rights reserved