Heat dissipation and electron–phonon interaction
hindering
the charge carrier mobility are serious constraints for the fabrication
of various integrated electronic and optoelectronic devices based
on two-dimensional (2D) materials. In this paper, we examine the quantum
confinement and phonon anharmonicity of different-layered MoS2, synthesized via the chemical vapor deposition technique.
We explore the contribution of spin–orbit and interlayer couplings
both theoretically (first-principles density functional theory) and
experimentally (Raman and photoluminescence spectroscopies). Further,
we demonstrate the thermally driven layer-dependent bandgap tunability
in (1L, 3L, and 5L) triangular MoS2 grown over the SiO2/Si substrate. We have also scrutinized their phonon confinement
behavior and thermal response in a low-temperature regime (80–300
K) using the optothermal Raman spectroscopy technique. A semiquantitative
model comprising the volume and temperature effect provides insights
into the nonlinear temperature-dependent phonon anharmonicity, revealing
that the contribution of higher order (three) phonon scattering reduces
with increasing layer numbers in MoS2. We further measure
the interfacial thermal conductance (g) and thermal
conductivity (k
s) of synthesized MoS2, and the obtained values of g (and k
s) are observed to increase (and decrease) with
increasing layer number. Our study will advance the understanding
of anharmonic behavior of phonons in different-layered MoS2 nanostructures for designing MoS2-based next-generation
devices for various applications.