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Van der Waals heterostructures (VDWHs) exhibit rich properties and thus haspotential for applications, and charge transfer between different layers in aheterostructure often dominates its properties and device performance. It isthus critical to reveal and understand the charge transfer effects in VDWHs,for which electronic structure measurements have proven to be effective. Usingangle-resolved photoemission spectroscopy, we studied the electronic structuresof (PbSe)1.16(TiSe2)m(m=1, 2), which are naturally occurring VDWHs, anddiscovered several striking charge transfer effects. When the thickness of theTiSe2 layers is halved from m=2 to m=1, the amount of charge transferredincreases unexpectedly by more than 250%. This is accompanied by a dramaticdrop in the electron-phonon interaction strength far beyond the prediction byfirst-principles calculations and, consequently, superconductivity only existsin the m=2 compound with strong electron-phonon interaction, albeit with lowercarrier density. Furthermore, we found that the amount of charge transferred inboth compounds is nearly halved when warmed from below 10 K to roomtemperature, due to the different thermal expansion coefficients of theconstituent layers of these misfit compounds. These unprecedentedly largecharge transfer effects might widely exist in VDWHs composed ofmetal-semiconductor contacts; thus, our results provide important insights forfurther understanding and applications of VDWHs.

Charge Transfer Effects in Naturally Occurring van der Waals Heterostructures (PbSe)1.16(TiSe2)m (m=1, 2)