Ground-State Orbital Analysis Predicts S₁ Charge Transfer in Donor-Acceptor Materials

Area of Science:

• Materials Science
• Computational Chemistry
• Optoelectronics

Background:

• Donor-acceptor (D-A) materials possess unique photophysical properties crucial for advanced optoelectronics.
• Predicting D-A material properties often involves complex excited-state electronic structure calculations.
• The degree of charge transfer (DCT) in the S₁ state is a key parameter influencing D-A material characteristics.

Purpose of the Study:

• To introduce a novel metric for predicting S₁ DCT in D-A dimers.
• To establish a simplified prediction method that avoids computationally expensive excited-state calculations.
• To explore the correlation between ground-state orbital similarity and S₁ DCT.

Main Methods:

• Developed a novel metric based on the similarity of orbitals between D-A dimer complexes and their monomer components.
• Utilized ground-state orbital analysis for DCT prediction.
• Calculated S₁ DCT for a dataset of 31 D-A dimers using established quantum chemistry methods.

Main Results:

• A linear relationship was identified between the novel orbital similarity metric and the calculated S₁ DCT.
• The proposed metric effectively predicts S₁ DCT using only ground-state properties.
• This finding offers a more efficient approach to characterizing D-A materials.

Conclusions:

• The novel orbital similarity metric provides an accurate and computationally efficient way to predict S₁ DCT in D-A materials.
• This method facilitates the high-throughput screening of D-A materials for optoelectronic applications.
• The established orbital structure-function relationship advances the design of next-generation electronic devices.