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The low crystal symmetry of rhenium disulphide (ReS2) leads to the emergenceof dichroic optical and optoelectronic response, absent in other layeredtransition metal dichalcogenides, which could be exploited for deviceapplications requiring polarization resolution. To date, spectroscopy studieson the optical response of ReS2 have relied almost exclusively incharacterization techniques involving optical detection, such asphotoluminescence, absorbance, or reflectance spectroscopy. However, to realizethe full potential of this material, it is necessary to develop knowledge onits optoelectronic response with spectral resolution. In this work, we studythe polarization-dependent photocurrent spectra of few-layer ReS2photodetectors, both in room conditions and at cryogenic temperature. Ourspectral measurements reveal two main exciton lines at energies matching thosereported for optical spectroscopy measurements, as well as their excitedstates. Moreover, we also observe an additional exciton-like spectral featurewith a photoresponse intensity comparable to the two main exciton lines. Weattribute this feature, not observed in earlier photoluminescence measurements,to a non-radiative exciton transition. The intensities of the three mainexciton features, as well as their excited states, modulate with linearpolarization of light, each one acquiring maximal strength at a differentpolarization angle. We have performed first-principles exciton calculationsemploying the Bethe-Salpeter formalism, which corroborate our experimentalfindings. Our results bring new perspectives for the development of ReS2-basednanodevices.

Polarization-tuneable excitonic spectral features in the optoelectronic response of atomically thin ReS2