Strong Dopant-Dopant Electronic Coupling in Emissive Codoped Two Dimensional Metal Halide Hybrid

Area of Science:

• Materials Science
• Solid-State Chemistry
• Photophysics

Background:

• Multimetallic halide hybrids are crucial for studying exciton interactions.
• Synthesizing halide hybrids with multiple heterometal centers is challenging, hindering insights into electronic coupling.
• Understanding electronic coupling mechanisms in these materials is vital for advanced applications.

Purpose of the Study:

• To develop a synthetic strategy for emissive heterometallic halide hybrids.
• To investigate dopant-dopant interactions and electronic coupling in a codoped 2D halide hybrid.
• To gain physical insight into the energy transfer mechanisms between different dopant ions.

Main Methods:

• Codoping a 2D host (C6H22N4CdCl6) with manganese (Mn2+) and antimony (Sb3+) ions.
• Characterization of the resulting heterometallic halide hybrid (C6H22N4Sb0.003Mn0.128Cd0.868Cl6).
• Photoluminescence spectroscopy to analyze emission properties and energy transfer.
• Density Functional Theory (DFT) calculations to model electronic coupling.

Main Results:

• Successful synthesis of an emissive heterometallic halide hybrid through codoping.
• Observation of distinct green (Sb3+) and strong orange (Mn2+) emissions, indicating dopant-based luminescence.
• Evidence of efficient energy transfer from Sb3+ to Mn2+ dopants, signifying strong dopant-dopant interaction.
• DFT calculations confirmed electronic coupling mediated by the 2D host structure.

Conclusions:

• The codoping strategy enables the creation of multimetallic halide hybrids with significant dopant-dopant interactions.
• Efficient energy transfer between distant dopants highlights the importance of the host structure in mediating electronic coupling.
• This work provides fundamental physical insights into the coupling mechanisms of interacting excitons in complex halide hybrid materials.