TY - JOUR
T1 - Unravelling strong electronic interlayer and intralayer correlations in a transition metal dichalcogenide
AU - Whitcher, T. J.
AU - Fauzi, Angga Dito
AU - Caozheng, D.
AU - Chi, X.
AU - Syahroni, A.
AU - Asmara, T. C.
AU - Breese, M. B.H.
AU - Neto, A. H.Castro
AU - Wee, A. T.S.
AU - Majidi, M. Aziz
AU - Rusydi, A.
N1 - Funding Information:
This work is supported by Singapore Ministry of Education (MOE) AcRF Tier-2 (MOE2017 T2-1-135, MOE2018-T2-2-117, and MOE2019-T2-1-163), MOE-AcRF Tier-1 (R-144-000-423-114, R-144-000-398-114, R-144-000-379-114 and R-144-000-368-112), the Singapore National Research Foundation under its Competitive Research Funding (No. R-398-000-087-281) and under its Medium Sized Centre Program (Centre for Advanced 2D Materials and Graphene Research Centre), NUS YIA, the 2015 PHC Merlion Project and NUS Core Support C-380-003-003-001. The authors would like to acknowledge the Singapore Synchrotron Light Source (SSLS) for providing the facility necessary for conducting the research. The SSLS is a National Research Infrastructure under the National Research Foundation Singapore.
Publisher Copyright:
© 2021, The Author(s).
PY - 2021/12
Y1 - 2021/12
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85120167326&partnerID=8YFLogxK
U2 - 10.1038/s41467-021-27182-y
DO - 10.1038/s41467-021-27182-y
M3 - Article
AN - SCOPUS:85120167326
SN - 2041-1723
VL - 12
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 6980
ER -