Lead-free halide double perovskite (HDP) Cs2AgBiBr6 has set a benchmark for research in HDP photoelectric applications due to its attractive optoelectronic properties. However, its narrow absorption range is a key limitation of this material. Herein, a novel dopant, palladium (Pd), is doped into Cs2AgBiBr6 and significantly extends the absorption to ≈1400 nm. Pd2+ ions are partially doped in the host lattice, most probably replacing Ag atoms and introducing a sub-bandgap state within the host bandgap, as indicated by the combination of spectroscopical measurements and theoretical calculations. Importantly, this sub-bandgap state extends the photoresponse of Cs2AgBiBr6 up to the NIR-II region of 1300 nm, setting a new record for HDPs. This work demonstrates a novel and efficient dopant for HDPs and highlights the effectiveness of employing a sub-bandgap to broaden the absorption of HDPs, shedding new light on tailoring large bandgap HDPs for NIR optoelectronic applications.

College of Engineering Huazhong Agricultural University Wuhan 430070 China

Department of Physics and Astronomy Uppsala University Uppsala SE 751 20 Sweden

Department of Physics Chemistry and Biology Linköping University Linköping SE 581 83 Sweden

Institute of Macromolecular Chemistry of the Czech Academy of Sciences Heyrovskeho nam 2 Prague 162 00 Czech Republic

School of Optical and Electronic Information and Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology Wuhan 430074 China

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