Research Goals and Approaches
- Extend photocarrier lifetimes (>10x radiative "limit") and control their dynamics during infrequent photon absorption events
- Enhance charge-separation yields (>50%) and redox selectivity (>90%), and therefore stability, under conditions of low-flux carrier transport (i.e. low current density)
- Program ensembles of artificial photosystems for large solar-to-hydrogen (STH) efficiencies (>10% STH)
To achieve these goals, EPN is developing powerful new and synergistic experimental and theoretical capabilities in nanomaterials synthesis, multiphysics modeling, and coupled correlative microscopies and spectroscopies. Results across a multitude of length and time scales teach physicochemical principles that dictate the behavior of ensembles of nanoreactors. This information serves as inputs to inverse design analyses, whose outputs guide optimization through a codesign feedback loop for bottom-up synthesis of multicomponent interphase coatings.
Thrusts
Thrust A
Electronic Charge Separation: (i) using operando correlative multimodal microscopies, reveal charge separation mechanisms; (ii) determine the influence of discrete photoinduced events on steady-state water splitting reactivity
Thrust B
Photochemical Charge Accumulation: (i) extend photogenerated charge-carrier lifetimes; (ii) control species accumulation at atomically precise reaction centers during infrequent photon absorption
Thrust C
Species-Selective Multicomponent Interphases: (i) understand in atomistic detail the function of encapsulated molecular reaction centers; (ii) codesign spatially distinct interphases for species-specific permeabilities and stabilities at low flux
Thrust D
Emergent Ensemble Behaviors: (i) experimentally validate interparticle interactions mediated by light and matter; (ii) guided by simulations bridging microenvironments, program desired physicochemical properties