Synthesis, Structure, and Tunability of Zero-Dimensional Organic–Inorganic Metal Halides Utilizing the m-Xylylenediammonium Cation: MXD2PbI6, MXDBiI5, and MXD3Bi2Br12·2H2O

Klee, Pia S.; Hirano, Yuri; Cordes, David B.; Slawin, Alexandra M. Z.; Payne, Julia L.

doi:10.1021/acs.cgd.2c00187

Cited by 9 publications

(6 citation statements)

References 48 publications

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“…We found that (MXD)BiI 5 constructed with MXD 2+ cation has a zerodimensional (0 D) structure and crystallized in a centrosymmetry space group (P-1) (Figure S1, Supporting Information). [27] This is different from previous reported HPs (x-AMPY)BiI 5 and (x-AMP)BiI 5 (AMPY is (aminomethyl)pyridinium, AMP is (aminomethyl)piperidinium), which are also constructed with aromatic and aliphatic diammoniums, but both have 1 D chainlike structure. [25] In our system, the spatial confinement effect of the inorganic skeleton on organic ammonium cations in (MXD)BiI 5 is not as strong as in (1,3-BMACH)BiI 5 .…”

Section: Crystal Structure Characterizationcontrasting

confidence: 65%

Confinement‐Driven Bulk Photovoltaic in Lead‐Free Hybrid Perovskite for Self‐Powered X‐Ray Detection

Fu,

Ma,

Chen

et al. 2024

Advanced Optical Materials

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Lead‐free hybrid perovskites (HPs) are considered as environmentally friendly photodetection materials. However, there are few studies on self‐powered photodetection in lead‐free HPs, and most of them are achieved through the introduction of chiral ammonium cations induced bulk photovoltaic effect (BPVE). Notably, enantiomeric pure chiral ammonium cations are difficult to synthesize, the quantity is small and the price is high. Therefore, choosing achiral ammonium cations to induce BPVE in lead‐free HPs is crucial. Herein, achiral cations 1,3‐bis(aminomethyl)cyclohexane (1,3‐BMACH) is exploited to induce bulk photovoltaic through confinement effect in (1,3‐BMACH)BiI5, then self‐powered X‐ray detection is successfully realized. Due to the large space in zero‐dimensional (0 D) (MXD)BiI5 (MXD is meta‐xylylenediammonium), the confinement effect is not obvious, resulting in the disorderly arrangement of MXD2+ cations and a centrosymmetry structure of (MXD)BiI5. Benefiting from the large photovoltage (1.0 V) of (1,3‐BMACH)BiI5 under X‐ray, its single crystal devices exhibit ultra‐high sensitivity of 170 µC Gy−1 cm−2 and extremely low detection limit of 49 nGy s−1 under self‐powered mode, which almost surpassing most low‐dimensional single‐phase lead‐free HPs at 0 V bias. This work has promoted the application of lead‐free HPs in the field of self‐powered X‐ray detection.

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Section: Crystal Structure Characterizationcontrasting

confidence: 65%

Confinement‐Driven Bulk Photovoltaic in Lead‐Free Hybrid Perovskite for Self‐Powered X‐Ray Detection

Fu,

Ma,

Chen

et al. 2024

Advanced Optical Materials

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“…The lead-based HPs constructed with diammonium cation 1,3-xylylenediammonium did not form a 2D DJ structure but existed as a zerodimensional (0D) structure, and all crystallized in a centrosymmetric space group. 47 From the above analysis, it can be seen that the configuration of diammonium cations not only affects the dimension of the obtained HPs but also affects its structural symmetry.…”

Section: ■ Results and Discussionmentioning

confidence: 95%

Regulating the Stereoisomerism of Diammonium Cations to Construct Polar Dion-Jacobson Hybrid Perovskites for Self-Powered X-ray Detection

Fu,

Chen,

et al. 2024

Chem. Mater.

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Dion-Jacobson (DJ) hybrid perovskite (HP) singlecrystal photodetectors often require operation under external bias due to the centrosymmetric structure of the material, which is not conducive to the intelligence and lightweight of the devices. To solve this problem, the key issue is how to regulate the noncovalent interaction between interlayer diammonium cations and inorganic frameworks to successfully induce polarity. However, there is a lack of research on the relationship between the configuration of diammonium cations and the structure symmetry of DJ HPs. Herein, we successfully constructed a series of polar DJ HPs (1,3-BMACH)PbX 4 (X = Cl, Br, I; 1,3-BMACH is 1,3-bis(aminomethyl)cyclohexane) by changing the configuration of organic cations. It was found that the hydrogen bonding strength between 1,3-BMACH 2+ cations and the bilateral inorganic framework is different, and it causes the inorganic layer to be more twisted, resulting in a deviation of the positive and negative charge centers in (1,3-BMACH)PbX 4 (X = Cl, Br, I) and successfully inducing polarity. Subsequently, we achieved efficient self-powered X-ray detection in the single-crystal device of (1,3-BMACH)PbBr 4 through polarity-induced bulk photovoltaic effect, which owns outstanding sensitivity (157.3 μC Gy −1 cm −2 , 0 V bias) and stability under X-ray radiation. Studying the relationship between the configuration of diammonium cations and the crystal structure in DJ HPs can help us design more efficient self-powered optoelectronic devices.

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“…[ 15 ] This value close to those for some reported 0D binuclear BHPs, like ( R ‐1‐(4‐fluoro)‐phenylethylammonium) 4 Bi 2 I 10 (2.09 eV) [ 16 ] and (meta‐xylylenediammonium)BiI 5 (2.15 eV). [ 17 ] Considering the chiral‐polar structure of 1 R / 1 S , their chiroptical features were studied. As shown in Figure 2b, the obvious circular dichroism (CD) signals for 1 R and 1 S films (Figure S10, Supporting Information) were observed at the same wavelengths but with opposite values.…”

Section: Resultsmentioning

confidence: 99%

Inch‐Size Single Crystals of Lead‐Free Chiral Perovskites with Bulk Photovoltaic Effect for Stable Self‐Driven X‐Ray Detection

You

Zhu

Dai

et al. 2023

Adv Funct Materials

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Lead halide perovskites have made great advance in direct X‐ray detection, however the presence of toxic lead and the requirement of high working voltages severely limit their applicability and operational stability. Thus, exploring “green” lead‐free hybrid perovskites capable of detecting X‐rays at zero bias is crucial but remains toughly challenging. Here, utilizing chiral R/S‐1‐phenylpropylamine (R/S‐PPA) cations, a pair of 0D chiral‐polar perovskites, (R/S‐PPA)2BiI5 (1R/1S) are constructed. Their intrinsic spontaneous electric polarization induces a large bulk photovoltage of 0.63 V, which acts as a driving force to separate and transport photogenerated carriers, thus endowing them with the capability of self‐driven detection. Consequently, self‐driven X‐ray detectors with a low detection limit of 270 nGy s−1 are successfully constructed based on high‐quality, inch‐sized single crystals of 1R. Notably, they show suppressed baseline drift under the self‐driven mode, exhibiting superior operational stability. This study realizes self‐driven X‐ray detection in a single‐phase lead‐free hybrid perovskite by exploiting the intrinsic bulk photovoltaic effect, which sheds light on future explorations of lead‐free hybrid perovskites toward “green” self‐driven radiation detectors with high performance.

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Synthesis, Structure, and Tunability of Zero-Dimensional Organic–Inorganic Metal Halides Utilizing the m-Xylylenediammonium Cation: MXD₂PbI₆, MXDBiI₅, and MXD₃Bi₂Br₁₂·2H₂O

Cited by 9 publications

References 48 publications

Confinement‐Driven Bulk Photovoltaic in Lead‐Free Hybrid Perovskite for Self‐Powered X‐Ray Detection

Confinement‐Driven Bulk Photovoltaic in Lead‐Free Hybrid Perovskite for Self‐Powered X‐Ray Detection

Regulating the Stereoisomerism of Diammonium Cations to Construct Polar Dion-Jacobson Hybrid Perovskites for Self-Powered X-ray Detection

Inch‐Size Single Crystals of Lead‐Free Chiral Perovskites with Bulk Photovoltaic Effect for Stable Self‐Driven X‐Ray Detection

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