Multiorbital exciton formation in an organic semiconductor

Abstract

Harnessing the optoelectronic response of organic semiconductors requires a thorough understanding of the fundamental light-matter interaction that is dominated by the excitation of correlated electron-hole pairs, i.e. excitons. The nature of these excitons would be fully captured by knowing the quantum-mechanical wavefunction, which, however, is difficult to access both theoretically and experimentally. Here, we use femtosecond photoemission orbital tomography in combination with many-body perturbation theory to gain access to exciton wavefunctions in organic semiconductors. We find that the coherent sum of multiple electron-hole pair contributions that typically make up a single exciton can be experimentally evidenced by photoelectron spectroscopy. For the prototypical organic semiconductor buckminsterfullerene (C${}_{60}$), we show how to disentangle such multiorbital contributions and thereby access key properties of the exciton wavefunctions including localization, charge-transfer character, and ultrafast exciton formation and relaxation dynamics.

References in corpus (10)

• The Bethe-Salpeter Equation Formalism: From Physics to Chemistry
• Momentum-resolved observation of exciton formation dynamics in monolayer WS${}_2$
• Direct measurement of key exciton properties: energy, dynamics and spatial distribution of the wave function
• Orbital-resolved Observation of Singlet Fission
• Tracing orbital images on ultrafast time scales
• Correlated electron-hole mechanism for molecular doping in organic semiconductors
• Momentum-Resolved Exciton Coupling and Valley Polarization Dynamics in Monolayer WS${}_2$
• Signatures of an Atomic Crystal in the Band Structure of a Molecular Thin Film
• Multiorbital exciton formation in an organic semiconductor
• Photoemission orbital tomography for excitons in organic molecules

Cited by in corpus (8)

• Observation of Floquet states in graphene
• Multiorbital exciton formation in an organic semiconductor
• Revealing Hidden Spin Polarization in Centrosymmetric van der Waals Materials on Ultrafast Timescales
• Ultrafast nano-imaging of dark excitons
• Probing excitons with time-resolved momentum microscopy
• Hybrid Frenkel-Wannier excitons facilitate ultrafast energy transfer at a 2D-organic interface
• A minimalist approach to 3D photoemission orbital tomography: algorithms and data requirements
• Observing the spatial and temporal evolution of exciton wave functions