The coupling of atomic vibrations to electronic excitations—traditionally understood to be a source of energy loss in semiconductors—has recently been explored in photosynthetic light harvesting as a means to circumvent dissipation by harnessing quantum vibronic coherence. Motivated by recent photocurrent measurements of vibronic sidebands in ${\mathrm{WSe}}_2/{\mathrm{MoSe}}_2$ optoelectronic devices [F. Barati et al., Nano Lett. 22, 5751 (2022)], we present a nonperturbative theoretical framework for phonon-assisted absorption in van der Waals heterostructures. Using a polaron transformation, a closed-form expression for the optical absorption spectrum at arbitrary temperatures is presented. Our model includes both intraband and interband electron–phonon coupling. Detailed analysis shows that the observed periodic sidebands originate from the strong coupling between interlayer excitons and nearly dispersionless optical phonon modes. By comparing two limiting cases, one involving only intraband couplings and the other incorporating coherent interband processes, we show that interband phonon-assisted transitions are needed to account for the observed data. Beyond enabling the direct estimation of vibronic coupling strengths from spectroscopic data, these findings have profound consequences for our understanding of optical and optoelectronic responses: coherent interband coupling of atomic vibrations to excitons is essential to quantifying photoresponse in transition metal dichalcogenide heterostructures.

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• Optical & microwave phenomena
• Heterostructures
• Green's function methods
• Hierarchical equations of motion