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Probing Side-Chain Engineering for Modulating Exciton Dynamics in Non‑fullerene Acceptors.

Sanyam Jain1,2, M Sridevi1,2, Tanushree Majhi1,2

  • 1Photovoltaic Metrology Section, Advanced Materials & Device Metrology Division, CSIR-National Physical Laboratory, Dr K. S. Krishnan Marg, New Delhi 110012, India.

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Summary
This summary is machine-generated.

Precise side-chain engineering of organic semiconductors allows tuning of energy levels in organic solar cells (OSCs). This method enables predictable control over electronic properties and charge behavior for improved photovoltaic performance.

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Area of Science:

  • Materials Science
  • Organic Electronics
  • Photovoltaics

Background:

  • Organic solar cells (OSCs) have advanced rapidly, requiring precise control over electronic properties of organic semiconductors.
  • Modulating frontier orbital energies (HOMO/LUMO) without affecting light absorption is key for optimizing OSC performance.

Purpose of the Study:

  • To develop a predictive side-chain engineering strategy for non-fullerene acceptors (NFAs).
  • To identify substituents that selectively tune HOMO/LUMO levels while maintaining the optical bandgap.
  • To understand how side-chain structure influences electronic properties and charge dynamics in NFAs.

Main Methods:

  • Utilized quantum-chemical calculations for substituent identification and electronic structure modeling.
  • Employed structural and excited-state simulations to guide the design of NFAs.
  • Applied ultrafast transient absorption spectroscopy (UTAS) to investigate exciton dynamics.

Main Results:

  • Designed two NFAs, PDIEH (flexible 2-ethylhexyl) and PDIIN (rigid indanyl), with similar optical gaps (~2.27 eV).
  • Flexible alkyl side chains induced inductive effects, stabilizing electronic structure and deepening LUMO levels.
  • Rigid aromatic side chains caused partial conjugative perturbations, leading to distinct energy level shifts and altered charge behavior.
  • PDIEH showed prolonged charge-separated lifetimes, while PDIIN exhibited faster recombination.

Conclusions:

  • Established a chemically intuitive framework for predictive side-chain engineering in organic photovoltaics.
  • Demonstrated that side-chain structure critically influences electronic properties and exciton dynamics.
  • Side-chain engineering offers a powerful tool for controlling charge behavior and optimizing NFA performance in OSCs.