Vibronic Exciton-Phonon States in Stack-Engineered van der Waals Heterojunction Photodiodes.

Barati, Fatemeh; Arp, Trevor B; Su, Shanshan; Lake, Roger K; Aji, Vivek; van Grondelle, Rienk; Rudner, Mark S; Song, Justin C W et al. · Nano Lett · 2022

basic_science · Level V

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Abstract

Stack engineering, an atomic-scale metamaterial strategy, enables the design of optical and electronic properties in van der Waals heterostructure devices. Here we reveal the optoelectronic effects of stacking-induced strong coupling between atomic motion and interlayer excitons in WSe<sub>2</sub>/MoSe<sub>2</sub> heterojunction photodiodes. To do so, we introduce the photocurrent spectroscopy of a stack-engineered photodiode as a sensitive technique for probing interlayer excitons, enabling access to vibronic states typically found only in molecule-like systems. The vibronic states in our stack are manifest as a palisade of pronounced periodic sidebands in the photocurrent spectrum in frequency windows close to the interlayer exciton resonances and can be shifted "on demand" through the application of a perpendicular electric field via a source-drain bias voltage. The observation of multiple well-resolved sidebands as well as their ability to be shifted by applied voltages vividly demonstrates the emergence of interlayer exciton vibronic structure in a stack-engineered optoelectronic device.