Interlayer coupling enables EPC-linked polarity inversion and enhanced heat dissipation in MoS₂/CrOCl heterostructures

Interlayer coupling is a central knob for engineering electronic reconstruction and energy dissipation in van der Waals heterostructures. However, a unified understanding that connects interlayer coupling to both electrical and thermal responses is still lacking. Electron–phonon coupling (EPC) could bridge this gap by linking interlayer coupling to both momentum and energy relaxation. Here we establish an electron–phonon-coupling-linked interpretation in MoS₂/CrOCl heterostructures, where interlayer coupling-driven interfacial charge transfer reshapes the MoS₂ electronic structure and, at the same time, renormalizes electron–phonon interactions that govern momentum relaxation and carrier–lattice energy relaxation. By using Raman and second-harmonic-generation (SHG) fingerprints, we identify 2L-MoS₂/CrOCl as the strongest coupling configuration. This is evidenced by the largest change in mode separation of 1.29 cm⁻¹ and a pronounced SHG suppression from 100% to 11.9% relative to pristine MoS₂. In this regime, interfacial charge redistribution downshifts the MoS₂ Fermi level and converts its native n-type character to p-type conduction. Along with electrical transport experiments, we also study the thermal transport and characterize the steady-state temperature rise through scanning thermal microscopy. The MoS₂/CrOCl heterostructure exhibits more efficient heat evacuation, reducing the temperature rise by 38.5% under identical thermal loading conditions compared with the situation for pristine MoS₂ on SiO₂/Si. According to the observed EPC-linked electron and phonon transport properties, interlayer coupling in MoS₂/CrOCl heterostructure has induced both carrier-polarity inversion and enhanced interfacial heat dissipation, providing a basis for codesigning electro-thermal multifunctional devices.