Higher excited states are attractive for driving high-energy photochemistry, but their ultrafast relaxation usually prevents direct utilization. Here we demonstrate, by pump-push-probe spectroscopy, ultrafast electron injection from higher excited states of perylene monoimide (PMI) coordinated to CdS and ZnS nanocrystals (NCs). Despite the weak electronic interaction between the lowest excited state of PMI and the NC surface, sequential excitation with 520 and 650 nm pulses generates long-lived charge-separated states through higher excited-state electron injection. A modified subtraction analysis disentangles the genuine higher excited-state dynamics from apparent population change of the lowest excited state, revealing sub-picosecond interfacial electron transfer and enhanced PMI radical anion formation in the ZnS system. This work establishes PMI-NC hybrids as a platform for harvesting short-lived high-energy excited states as long-lived reactive charges under visible light.
- Open Access
- Article
Ultrafast Electron Transfer from Higher Excited States in Perylene Monoimide—Nanocrystal Hybrids Revealed by Pump-Push-Probe Spectroscopy
Author Information
Received: 17 Apr 2026 | Revised: 20 May 2026 | Accepted: 05 Jun 2026 | Published: 07 Jun 2026
Abstract
Keywords
pump-push-probe spectroscopy | perylene monoimide | higher excited-state | nanocrystals | electron transfer
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