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Modulation of Singlet-Triplet Gap in Atomically Precise Silver Cluster-Assembled Material.

Priyanka Chandrashekar¹, Gopa Sardar², Turbasu Sengupta³

¹School of Chemistry, Indian Institute of Science Education and Research Thiruvananthapuram, Kerala, 695551, India.

Angewandte Chemie (International Ed. in English)

|December 11, 2023

Summary

Researchers tuned silver cluster luminescence by controlling their molecular packing. Different ligands created distinct silver (Ag₁₂) cluster assemblies, influencing their photophysical properties and offering a new toolkit for optoelectronic materials.

Keywords:

Cluster Assembled Material Nanocluster Phosphorescence Silver Cluster Thermally Activated Fluorescence

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Area of Science:

Materials Science
Photochemistry
Nanotechnology

Background:

Silver clusters exhibit tunable luminescence, but controlling their aggregation and molecular interactions remains challenging.
Ligand design is crucial for stabilizing silver clusters and directing their assembly.
Understanding photophysical behavior linked to cluster packing is essential for advanced materials.

Purpose of the Study:

To modulate the packing pattern of silver (Ag₁₂) clusters by varying nitrogen-based ligands.
To investigate the photophysical properties of Ag₁₂ clusters as a function of their assembly.
To explore the relationship between cluster assembly, energy gaps, and luminescence behavior.

Main Methods:

Synthesized two distinct Ag₁₂ cluster assemblies (CAM-1 and NC-1) using different nitrogen-based ligands.
Characterized the assemblies' structures and coordination environments.
Analyzed temperature-dependent photoluminescence spectra to study emission properties.

Main Results:

Both assemblies displayed ligand-to-metal-metal charge transfer (LMMCT) based emission.
Temperature-dependent studies revealed blue shifts in emission at higher temperatures due to thermal reverse population.
The energy gap difference (ΔE_ST) varied between assemblies, impacting reverse intersystem crossing (RISC) temperatures.

Conclusions:

Assembly-defined photoluminescence properties were demonstrated for Ag₁₂ clusters.
Ligand-directed molecular packing offers a strategy to tune cluster optoelectronic behavior.
This work provides a toolkit for designing novel cluster assemblies with tailored properties.