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Many-Exciton Quantum Dynamics in a Ruddlesden-Popper Tin Iodide
Esteban Rojas-Gatjens1,2, Hao Li3, Alejandro Vega-Flick1
1School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia, 30332, United States.
Tin halide (PEA)2SnI4 exhibits significantly stronger exciton-exciton interactions and localization than its lead counterpart, impacting quantum dynamics. This difference is linked to lattice disorder in tin-based Ruddlesden-Popper metal halides.
Area of Science:
- Materials Science
- Quantum Optics
- Solid-State Physics
Background:
- Ruddlesden-Popper metal halides (RPMHs) are promising optoelectronic materials.
- Understanding exciton dynamics is crucial for their application.
- Previous studies highlighted differences between lead and tin-based RPMHs.
Purpose of the Study:
- To investigate many-body exciton interactions in (PEA)2SnI4.
- To compare exciton dynamics in tin-based vs. lead-based RPMHs.
- To elucidate the role of lattice disorder and exciton-exciton interactions.
Main Methods:
- Coherent two-dimensional electronic spectroscopy (2D ES).
- Analysis of optical dephasing times and excitation-induced dephasing (EID).
- Modeling lineshapes using stochastic scattering theory.
Main Results:
- Observed significantly higher EID rates in (PEA)2SnI4 compared to (PEA)2PbI4.
- Evidence of exciton localization due to a more disordered lattice in the tin halide.
- Detection of a low-binding-energy biexcitonic state in (PEA)2SnI4.
Conclusions:
- Tin-based RPMHs exhibit distinct exciton quantum dynamics from lead-based counterparts.
- Exciton-exciton interaction strength and static lattice disorder are key differentiating factors.
- Findings provide insights into the fundamental properties of tin-based RPMHs.
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