The fabrication of reusable SERS substrates with sensitivity at the single‐molecule level remains challenging but promising. Herein, a composite surface‐enhanced Raman scattering (SERS) substrate is proposed that includes Ag nanoparticle (Ag NPs) /Graphene/BaTiO3 (Ag/G/BTO) from a chemical enhancement perspective. The pyroelectric field generated by BaTiO3 drives the charge transfer between the SERS substrate and molecules, achieving a significant improvement in the SERS performance and self‐cleaning properties. The SERS signals of rhodamine 6G (R6G) molecules are further amplified up to 70‐fold. Thus, the detection limit is reduced by three orders of magnitude in this study, reaching 10−14 m after applying a pyroelectric field. In addition, the substrate exhibits a higher degradation efficiency than previous self‐cleaning SERS substrates because of the outstanding catalytic properties of BaTiO3. Target molecules are degraded effectively after several temperature cycles. A detailed mechanism analysis of pyroelectric SERS is conducted based on theoretical simulations and experimental results. This study is considered to deepen the understanding of SERS mechanisms and boost the application of SERS technology.

中文翻译：

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热释电驱动电荷转移及其对 SERS 和自清洁性能的优势


制造具有单分子水平灵敏度的可重复使用的 SERS 底物仍然具有挑战性，但前景广阔。在此，从化学增强的角度来看，提出了一种复合表面增强拉曼散射 （SERS） 衬底，其中包括 Ag 纳米颗粒 （Ag NPs） /石墨烯/BaTiO3 （Ag/G/BTO）。BaTiO3 产生的热释电场驱动 SERS 衬底和分子之间的电荷转移，从而显著提高 SERS 性能和自清洁性能。罗丹明 6G （R6G） 分子的 SERS 信号被进一步放大高达 70 倍。因此，本研究中的检测限降低了三个数量级，在施加热释电场后达到 10-14m。此外，由于 BaTiO3 出色的催化性能，该底物表现出比以前的自清洁 SERS 底物更高的降解效率。目标分子在几个温度循环后被有效降解。基于理论仿真和实验结果，对热释电 SERS 进行了详细的机理分析。本研究被认为加深了对 SERS 机制的理解并促进了 SERS 技术的应用。