ArticleACS nano2026
Probing Ultrafast Excitonic Coherences and Charge-Generation Pathways in Quantum-Dot Photocells via Photocurrent-Detected Two-Dimensional Electronic Spectroscopy.
Article in ACS nano, 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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Abstract
Understanding how coherent excitonic states influence charge generation is essential for optimizing quantum-dot (QD) optoelectronic devices. Here, we apply photocurrent-detected two-dimensional electronic spectroscopy (PC-2DES) to a functioning CdSe QD photocell to track excitonic interactions and charge-separation dynamics under operational conditions. Selective excitation of the |1S⟩ manifold reveals strong contributions from red-shifted, delocalized excitons that dominate the photocurrent but contribute only weakly in optically detected 2DES. Global analysis uncovers three dynamical components, including a sub-100 fs process associated with photocurrent growth at specific spectral coordinates, consistent with rapid population transfer through delocalized states and possible trion formation. Unlike optical detection, PC-2DES suppresses longitudinal optical phonon signatures, enabling clear observation of higher-frequency beatings attributed to interdot electronic coherences. These results demonstrate the utility of PC-2DES for probing coherent charge-generation pathways in QD solids and for guiding the design of coherence-enabled optoelectronic devices.
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