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Ultrafast Computational Screening of Molecules with Inverted Singlet–Triplet Energy Gaps Using the Pariser–Parr–Pople Semiempirical Quantum Chemistry Method

Kjell Jorner, Robert Pollice, Cyrille Lavigne, Alán Aspuru‐Guzik

2024The Journal of Physical Chemistry A42 citationsDOIOpen Access PDF

Abstract

Molecules with an inverted energy gap between their first singlet and triplet excited states have promising applications in the next generation of organic light-emitting diode (OLED) materials. Unfortunately, such molecules are rare, and only a handful of examples are currently known. High-throughput virtual screening could assist in finding novel classes of these molecules, but current efforts are hampered by the high computational cost of the required quantum chemical methods. We present a method based on the semiempirical Pariser-Parr-Pople theory augmented by perturbation theory and show that it reproduces inverted gaps at a fraction of the cost of currently employed excited-state calculations. Our study paves the way for ultrahigh-throughput virtual screening and inverse design to accelerate the discovery and development of this new generation of OLED materials.

Topics & Concepts

Excited stateOLEDSinglet stateMoleculeQuantumSinglet fissionQuantum chemistryChemistryUltrashort pulseDiodeComputational chemistryNanotechnologyMaterials scienceAtomic physicsPhysicsQuantum mechanicsOptoelectronicsSupramolecular chemistryLaserLayer (electronics)Organic Light-Emitting Diodes ResearchMolecular Junctions and NanostructuresOrganic Electronics and Photovoltaics
Ultrafast Computational Screening of Molecules with Inverted Singlet–Triplet Energy Gaps Using the Pariser–Parr–Pople Semiempirical Quantum Chemistry Method | Litcius