Switchable Photovoltaic Effect and Robust Nonlinear Optical Response in a High-Temperature Molecular Ferroelectric [C8N2H22][PbI4]

IF 4.3 2区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

Inorganic Chemistry Pub Date : 2024-10-20 DOI:10.1021/acs.inorgchem.4c03742

Zhibo Chen, Ganghua Zhang, Jinrong Wen, Zhanqiang Liu, Shu Chen, Jingshan Hou, Yongzheng Fang

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Abstract

Hybrid organic–inorganic molecular ferroelectrics (HOIMFs) have garnered significant attention for their potential applications in nonvolatile memory and spintronic devices. However, few efforts have been devoted to the photoelectric properties of lead halide molecular ferroelectrics, despite the fact that robust ferroelectricity and flexibility are desirable for thin-film photoelectric devices. Herein, we present a novel lead halide molecular ferroelectric [C₈N₂H₂₂][PbI₄] (1) synthesized hydrothermally. A polar monoclinic structure of 1 was solved by single-crystal X-ray diffraction and second-harmonic generation (SHG) tests. A direct band gap of 2.36 eV was confirmed by UV–vis spectrum and theoretical calculation. Hysteresis measurements demonstrated inherent room-temperature (RT) ferroelectricity in 1 with a spontaneous polarization (P_s) of 3.2 μC/cm². The 1-based photoelectric device shows a notable photovoltaic (PV) effect with V_oc ∼ 0.27 V, J_sc ∼ 38 nA/cm² under AM 1.5 G illumination, and a rapid response time of ∼1.5 ms. A considerable enhancement in PV performance has been achieved by adjusting the ferroelectric polarization, resulting in a maximum V_oc ∼ 0.75 V, J_sc ∼ 2.28 μA/cm². Notably, 1 exhibits a rather large SHG signal, which is approximately 2.61-fold higher than that of KH₂PO₄ (KDP) upon a 1064 nm laser radiation. This study offers a bright avenue for lead halide molecular ferroelectrics as promising optoelectronic devices and SHG materials.

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高温分子铁电[C8N2H22][PbI4]中的可切换光伏效应和稳健非线性光学响应

有机-无机混合分子铁电体（HOIMFs）因其在非易失性存储器和自旋电子器件中的潜在应用而备受关注。然而，卤化铅分子铁电体的光电特性却鲜有人问津，尽管薄膜光电器件所需的是稳健的铁电性和柔韧性。在此，我们介绍了一种水热合成的新型卤化铅分子铁电体 [C8N2H22][PbI4] (1)。通过单晶 X 射线衍射和二次谐波发生（SHG）测试，解决了 1 的极性单斜结构问题。紫外-可见光谱和理论计算证实了 2.36 eV 的直接带隙。磁滞测量表明，1 具有固有的室温（RT）铁电性，自发极化（Ps）为 3.2 μC/cm2。基于 1 的光电器件显示出显著的光伏（PV）效应，在 AM 1.5 G 光照下，Voc ∼ 0.27 V，Jsc ∼ 38 nA/cm2，快速响应时间 ∼ 1.5 ms。通过调整铁电极化，光伏性能有了显著提高，最大 Voc ∼ 0.75 V，Jsc ∼ 2.28 μA/cm2。值得注意的是，在 1064 纳米激光照射下，1 表现出相当大的 SHG 信号，比 KH2PO4（KDP）高出约 2.61 倍。这项研究为卤化铅分子铁电材料作为前景广阔的光电器件和 SHG 材料提供了一条光明大道。

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来源期刊

Inorganic Chemistry 化学-无机化学与核化学

CiteScore

7.60

自引率

13.00%

发文量

1960

审稿时长

1.9 months

期刊介绍： Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.