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Two distinct stacking orders in ReS2 are identified without ambiguity andtheir influence on vibrational, optical properties and carrier dynamics areinvestigated. With atomic resolution scanning transmission electron microscopy(STEM), two stacking orders are determined as AA stacking with negligibledisplacement across layers, and AB stacking with about a one-unit celldisplacement along the a axis. First-principle calculations confirm that thesetwo stacking orders correspond to two local energy minima. Raman spectra informa consistent difference of modes I & III, about 13 cm-1 for AA stacking, and 20cm-1 for AB stacking, making a simple tool for determining the stacking ordersin ReS2. Polarized photoluminescence (PL) reveals that AB stacking possessesblue-shifted PL peak positions, and broader peak widths, compared with AAstacking, indicating stronger interlayer interaction. Transient transmissionmeasured with femtosecond pump probe spectroscopy suggests exciton dynamicsbeing more anisotropic in AB stacking, where excited state absorption relatedto Exc. III mode disappears when probe polarization aligns perpendicular to baxis. Our findings underscore the stacking-order driven optical properties andcarrier dynamics of ReS2, mediate many seemingly contradictory results inliterature, and open up an opportunity to engineer electronic devices with newfunctionalities by manipulating the stacking order.

Stacking Order Driven Optical Properties and Carrier Dynamics in ReS2