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<p>Titanium dioxide (TiO<sub>2</sub>) photocatalysis is a promising route for air purification but remains fundamentally constrained by ultrafast charge-carrier recombination and a reliance on ultraviolet excitation. Here, we introduce a new mechanism the Stokes-Induced Stark Effect (SISE) in which molecular excited-state relaxation is repurposed to generate a transient interfacial electric field that actively suppresses recombination in real time. We develop a quantum–mechanical framework for quercetin-sensitized TiO<sub>2</sub> hybrids, showing that excited-state intramolecular proton transfer in chemisorbed quercetin drives an ultrafast dipole reorganization during its Stokes shift. This time-dependent dipole produces a picosecond-scale interfacial electric field on the order of 10⁶–10⁷ V m⁻<sup>1</sup>, sufficient to dynamically Stark-shift the TiO<sub>2</sub> conduction band by tens of millielectronvolts. Solutions of the time-dependent Schrödinger equation within a composite molecular–semiconductor Hilbert space reveal that the resulting field selectively lowers electron-injection barriers while exponentially suppressing back recombination through a Marcus–Levich–Jortner kinetic bottleneck. The model predicts order-of-magnitude enhancements in charge-separation efficiency under visible-light excitation, with quantum yields approaching technologically relevant levels under low-intensity illumination. These results establish a theoretical foundation for self-polarizing photocatalysts, in which molecular Stokes relaxation actively reshapes interfacial energetics rather than dissipating as heat. If experimentally validated, SISE offers a pathway toward energy-autonomous, visible-light-driven air purification and provides a general design principle for dynamically coupled hybrid optoelectronic materials.</p>

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Quantum modelling of the stokes-induced stark effect in quercetin–TiO2 hybrids for self-polarizing photocatalytic air purification

  • 期刊论文

  • 发表日期：

    2026年4月18日

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  • Moses G. Udoisoh,
  • Sozo T. Harry,
  • Ezekiel Oluwaseyi Ogungbemi,
  • Biame Clifford Ngah,
  • Okeshina Solomon Tosin

摘要

Titanium dioxide (TiO2) photocatalysis is a promising route for air purification but remains fundamentally constrained by ultrafast charge-carrier recombination and a reliance on ultraviolet excitation. Here, we introduce a new mechanism the Stokes-Induced Stark Effect (SISE) in which molecular excited-state relaxation is repurposed to generate a transient interfacial electric field that actively suppresses recombination in real time. We develop a quantum–mechanical framework for quercetin-sensitized TiO2 hybrids, showing that excited-state intramolecular proton transfer in chemisorbed quercetin drives an ultrafast dipole reorganization during its Stokes shift. This time-dependent dipole produces a picosecond-scale interfacial electric field on the order of 10⁶–10⁷ V m⁻1, sufficient to dynamically Stark-shift the TiO2 conduction band by tens of millielectronvolts. Solutions of the time-dependent Schrödinger equation within a composite molecular–semiconductor Hilbert space reveal that the resulting field selectively lowers electron-injection barriers while exponentially suppressing back recombination through a Marcus–Levich–Jortner kinetic bottleneck. The model predicts order-of-magnitude enhancements in charge-separation efficiency under visible-light excitation, with quantum yields approaching technologically relevant levels under low-intensity illumination. These results establish a theoretical foundation for self-polarizing photocatalysts, in which molecular Stokes relaxation actively reshapes interfacial energetics rather than dissipating as heat. If experimentally validated, SISE offers a pathway toward energy-autonomous, visible-light-driven air purification and provides a general design principle for dynamically coupled hybrid optoelectronic materials.