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

T. J. Whitcher (), Angga Dito Fauzi, D. Caozheng, X. Chi, A. Syahroni, T. C. Asmara, M. B. H. Breese, A. H. Castro Neto, A. T. S. Wee, M. Aziz Majidi and A. Rusydi ()
Additional contact information
T. J. Whitcher: National University of Singapore
Angga Dito Fauzi: National University of Singapore
D. Caozheng: National University of Singapore
X. Chi: National University of Singapore
A. Syahroni: University of Indonesia
T. C. Asmara: National University of Singapore
M. B. H. Breese: National University of Singapore
A. H. Castro Neto: National University of Singapore
A. T. S. Wee: National University of Singapore
M. Aziz Majidi: University of Indonesia
A. Rusydi: National University of Singapore

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract 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.

Date: 2021
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DOI: 10.1038/s41467-021-27182-y

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