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Aggregation-Driven Thorough Cascaded Proton Transfer Process Targeting Ultralow-Threshold Near-Infrared Organic

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Summary

Researchers developed a new method using aggregation effects to improve near-infrared organic solid-state lasers (OSSLs). This approach enhances exciton utilization, leading to a record-low threshold for efficient lasing.

Keywords:
Excited‐state proton transferJ‐aggregatesMolecular crystalsNear‐infrared lasingOrganic semiconductors

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Area of Science:

  • Materials Science
  • Optoelectronics
  • Physical Chemistry

Background:

  • Near-infrared organic solid-state lasers (NIR OSSLs) are vital for lasing communication but face challenges with high thresholds and low optical gain due to inefficient exciton utilization.
  • Excited-state double proton transfer (ESDPT) in organic gain materials presents a promising pathway for NIR OSSLs, offering favorable six-electronic-level systems and significant red-shifted stimulated emission.

Purpose of the Study:

  • To investigate the modulation of ESDPT processes via aggregation effects to enhance exciton utilization and reduce lasing thresholds in NIR OSSLs.
  • To realize efficient NIR single-crystal lasing with a low threshold by optimizing the ESDPT mechanism.

Main Methods:

  • A novel strategy was employed to modulate the ESDPT process through aggregation, specifically utilizing crystallization-enhanced cascaded ESDPT.
  • The J-type coupling in DDMC single-crystal microwires was analyzed to understand its role in stabilizing excited states and facilitating ESDPT.
  • The efficiency of population inversion density (ΔN) was assessed in the context of a six-level energy system.

Main Results:

  • Crystallization-enhanced ESDPT significantly improved exciton utilization, enabling an ultralow lasing threshold.
  • Strong J-type coupling (4260 cm⁻¹) in DDMC single-crystal microwires effectively lowered excited-state energy, promoting a thorough ESDPT process.
  • A record-low lasing threshold of 486 nJ cm⁻² was achieved for NIR single-crystal lasing at approximately 870 nm, attributed to efficient population inversion.

Conclusions:

  • Aggregation effects can be strategically used to enhance ESDPT gain materials for low-threshold, high-gain NIR OSSLs.
  • The study elucidates the fundamental mechanisms of aggregation on ESDPT, providing a pathway for improved OSSL performance.
  • This work paves the way for future advancements, including electrically-pumped NIR OSSLs.