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

TL;DR

This study reveals significant charge transfer effects in naturally occurring van der Waals heterostructures, showing how layer thickness and temperature dramatically influence electronic properties and superconductivity, with implications for future device applications.

Contribution

The paper provides the first detailed experimental analysis of charge transfer effects in naturally occurring VDWHs, highlighting unexpected increases with layer reduction and temperature-dependent charge transfer.

Findings

Charge transfer increases by over 250% when TiSe2 layer thickness is halved.

Superconductivity is observed only in the thicker m=2 compound with strong electron-phonon interaction.

Charge transfer nearly halves when warming from below 10 K to room temperature.

Abstract

Van der Waals heterostructures (VDWHs) exhibit rich properties and thus has potential for applications, and charge transfer between different layers in a heterostructure often dominates its properties and device performance. It is thus critical to reveal and understand the charge transfer effects in VDWHs, for which electronic structure measurements have proven to be effective. Using angle-resolved photoemission spectroscopy, we studied the electronic structures of (PbSe)1.16(TiSe2)m(m=1, 2), which are naturally occurring VDWHs, and discovered several striking charge transfer effects. When the thickness of the TiSe2 layers is halved from m=2 to m=1, the amount of charge transferred increases unexpectedly by more than 250%. This is accompanied by a dramatic drop in the electron-phonon interaction strength far beyond the prediction by first-principles calculations and, consequently, superconductivity only exists in the m=2 compound with strong electron-phonon interaction, albeit with lower carrier density. Furthermore, we found that the amount of charge transferred in both compounds is nearly halved when warmed from below 10 K to room temperature, due to the different thermal expansion coefficients of the constituent layers of these misfit compounds. These unprecedentedly large charge transfer effects might widely exist in VDWHs composed of metal-semiconductor contacts; thus, our results provide important insights for further understanding and applications of VDWHs.