Unravelling strong electronic interlayer and intralayer correlations in a transition metal dichalcogenide

Electronic correlations play important roles in driving exotic phenomena in condensed matter physics. They determine low-energy properties through high-energy bands well-beyond optics. Great effort has been made to understand low-energy excitations such as low-energy excitons in transition metal dichalcogenides (TMDCs), however their high-energy bands and interlayer correlation remain mysteries. Herewith, by measuring temperature- and polarization-dependent complex dielectric and loss functions of bulk molybdenum disulphide from near-infrared to soft X-ray, supported with theoretical calculations, we discover unconventional soft X-ray correlated-plasmons with low-loss, and electronic transitions that reduce dimensionality and increase correlations, accompanied with significantly modified low-energy excitons. At room temperature, interlayer electronic correlations, together with the intralayer correlations in the c-axis, are surprisingly strong, yielding a three-dimensional-like system. Upon cooling, wide-range spectral-weight transfer occurs across a few tens of eV and in-plane p-d hybridizations become enhanced, revealing strong Coulomb correlations and electronic anisotropy, yielding a two-dimensional-like system. Our result shows the importance of strong electronic, interlayer and intralayer correlations in determining electronic structure and opens up applications of utilizing TMDCs on plasmonic nanolithrography. Electronic and interlayer correlations are expected to affect the electronic and optical properties of transition metal dichalcogenides. Here, by using spectroscopic ellipsometry in the broad energy range, the authors uncover new electronic transitions and correlated plasmons in bulk MoS2.

Automated summary

This study reveals unconventional soft X-ray correlated plasmons and electronic transitions in bulk MoS2 through measuring complex dielectric and loss functions. The electronic structure shows characteristics of both 3D and 2D systems as interlayer and intralayer correlations change with temperature.