Enhanced Bulk Photovoltaics in Polar 2D Hybrid Perovskite via Pressure-Strengthened Organic-Inorganic Interactions

Year: 2026

Authors: Fang SY., Bu KJ., Ye H., Xu LJ., Wang D., Guo SH., Fu TH., Mao YH., Ye YC., Tang LW., Dalladay-Simpson P., Gorelli FA., Zhan YQ., Ding Y., Sun ZH., Luo JH., Lā€™ X.

Autors Affiliation: Ctr High Pressure Sci & Technol Adv Res, Shanghai, Peoples R China; Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou, Fujian, Peoples R China; Fudan Univ, Coll Future Informat Technol, Shanghai, Peoples R China; Shanghai Adv Res Phys Sci SHARPS, Shanghai, Peoples R China; Consiglio Nazl Ric CNR INO, Ist Nazl Ott, Sesto Fiorentino, Italy; European Lab Non Linear Spect LENS, Sesto Fiorentino, Italy.

Abstract: The development of bulk photovoltaic effect (BPVE) in polar two-dimensional (2D) organic-inorganic hybrid perovskites (OIHPs) is currently impeded by an insufficient understanding of the microscopic mechanisms linking organic-inorganic interactions to photovoltaic output. Here, we utilize pressure as an effective thermodynamic probe to decouple these interactions in BDA(EA)2Pb3Br10 (BDA is 1,4-butanediammonium, EA is ethylammonium), achieving the first pressure-engineered synergistic enhancement of short-circuit current (I SC) and open-circuit voltage (V OC). Comprehensive in situ characterizations reveal that pressure-strengthened N & horbar;H & centerdot;& centerdot;& centerdot;Br hydrogen bonding induces cooperative organic cation ordering and inorganic octahedral distortion. This structural synergy amplifies spontaneous polarization, resulting in a 530-fold increase in BPVE efficiency to 0.18% at 1.5 GPa, a value surpassing all previously reported OIHPs. Moreover, the enhanced organic-inorganic interaction stabilizes the ferroelectric state, elevating the Curie temperature to 433 K. These results elucidate the microscopic mechanism underlying BPVE enhancement in 2D OIHP ferroelectrics and establish pressure modulation as an effective strategy for mechanistic studies and photovoltaic optimization.

Journal/Review: ADVANCED MATERIALS

More Information: This work is supported by the National Natural Science Foundation of China (NSFC) (Grant Nos. 22275004, 22125110, 22505036, W2532012, and 22505008), Shanghai Science and Technology Committee (N o. 22JC1410300), Shanghai Key Laboratory of Novel Extreme Condition Materials (No. 22dz2260800), and National Key Research and Development Program of China (Grant No. 2022YFA1402301).
KeyWords: bulk photovoltaic effect; high pressure; organic-inorganic interactions; synergistic enhancement; two-dimensional hybrid perovskite
DOI: 10.1002/adma.75197