Secondary through-space interactions facilitated single-molecule white-light emission from clusteroluminogens

Area of Science:

• Materials Science
• Photophysics
• Supramolecular Chemistry

Background:

• Clusteroluminogens are non-conjugated molecules exhibiting unique photophysical properties through aggregate formation and through-space interactions.
• Designing and controlling photophysical properties of clusteroluminogens remains challenging compared to conventional conjugated chromophores.

Purpose of the Study:

• To design and synthesize novel clusteroluminogens with tunable multiple emissions and single-molecule white-light emission.
• To investigate the role of halide substituents and secondary through-space interactions in controlling photophysical properties.

Main Methods:

• Synthesis of three non-conjugated donor-acceptor clusteroluminogens with varying halide substituents.
• Characterization of photophysical properties including multiple emissions and white-light emission in the crystalline state.
• Experimental and theoretical studies to elucidate the electronic origins of the observed emissions.

Main Results:

• The synthesized compounds exhibit multiple emission bands and single-molecule white-light emission in the crystalline state.
• The emission intensity ratio can be tuned by altering halide substituents and excitation wavelengths.
• Multiple emissions originate from through-space conjugation, secondary through-space interactions-based charge transfer, and room-temperature phosphorescence.

Conclusions:

• Secondary through-space interactions significantly enrich the photophysical properties of clusteroluminogens.
• This work establishes a foundation for novel aggregate photophysics in clusteroluminescence.
• The findings pave the way for designing advanced materials with tailored optical properties.