Publication date: 16th July 2025
Inorganic metal halide double perovskites (HDPs) have emerged as promising alternatives to lead-based perovskites, effectively mitigating issues related to toxicity and poor stability. Despite this progress, achieving optimal optical performance remains a significant challenge. While the core@shell heterostructure approach is widely recognized for tailoring optical properties in various nanomaterials, it remains largely unexplored for metal halide double perovskite nanocrystals (NCs). This is primarily due to the intrinsic softness and ionic character of the perovskite lattice, which complicates controlled shell growth. In this work, we report a simple colloidal strategy to grow a lead-free Cs₂NaInCl₆ shell over Cs₂AgBiCl₆ cubic NCs. This heterostructure design results in a tenfold immediate enhancement in photoluminescence quantum yield (PLQY), which continues to improve over time. Optical characterization indicates the emergence of new emissive states likely originating from interfacial alloying, with carrier dynamics further elucidated via time-resolved photoluminescence and transient absorption spectroscopy. This approach offers a compelling route to modulate and enhance the optical behavior of lead-free halide double perovskites through heterostructure engineering.
RS acknowledges CSIR, India, for the senior research fellowship [grant no. 09/086(1388)/2019-EMR-I]. AS is thankful to IIT Delhi, India, for the Early-Doc fellowship. NS acknowledges IIT Delhi for Junior research fellowship. GS is thankful for Inspire fellowship from Department of Science and Technology, Government of India. PKS acknowledges Central Research Facilty (CRF), CeNS, Bengaluru and TEM facility (TALOS F200SG2 operated at 200 kV). DGs acknowledges the IIT Delhi SEED Grant (PLN12/04MS), the Science and Engineering Research Board (SERB), Department of Science and Technology (DST), India for Start-up Research Grant SRG/2022/00l234, and CSIR-Human Resource Development Group (HRDG) for ExtraMural Research-II Grant 01/3136/23/EMR-II. SS acknowledges Central Research Facility (CRF), IIT Delhi for XPS, TEM, HRTEM, DST-FIST grant for ultrafast spectroscopy facilities, DST-SATHI for PL and SERB grant no. CRG/2019/000935 for partial financial assistance.
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