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Manipulation of Stacking Order in Td-WTe2 by Ultrafast Optical Excitation
KTH, School of Engineering Sciences (SCI), Applied Physics, Materials and Nanophysics.
Uppsala Univ, Dept Phys & Astron, Div Mat Theory, SE-75120 Uppsala, Sweden..
KTH, School of Engineering Sciences (SCI), Applied Physics, Materials and Nanophysics.ORCID iD: 0000-0003-1631-4293
2021 (English)In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 15, no 5, p. 8826-8835Article in journal (Refereed) Published
Abstract [en]

Subtle changes in stacking order of layered transition metal dichalcogenides may have profound influence on the electronic and optical properties. The intriguing electronic properties of Td-WTe2 can be traced to the break of inversion symmetry resulting from the ground-state stacking sequence. Strategies for perturbation of the stacking order are actively pursued for intentional tuning of material properties, where optical excitation is of specific interest since it holds the potential for integration of ultrafast switches in future device designs. Here we investigate the structural response in Td-WTe2 following ultrafast photoexcitation by time-resolved electron diffraction. A 0.23 THz shear phonon, involving layer displacement along the b axis, was excited by a 515 nm laser pulse. Pump fluences in excess of a threshold of similar to 1 mJ/cm(2) result in formation, with an similar to 5 ps time constant, of a new stacking order by layer displacement along the b axis in the direction toward the centrosymmetric 1T* phase. The shear displacement of the layers increases with pump fluence until saturation at similar to 8 pm. We demonstrate that the excitation of the shear phonon and the stabilization of the metastable phase are decoupled when using an optical pump as evidenced by observation of a transition also in samples with a pinned shear phonon. The results are compared to dynamic first-principles simulations and the transition is interpreted in terms of a mechanism where transient local disorder is prominent before settling at the atomic positions of the metastable phase. This interpretation is corroborated by results from diffuse scattering. The correlation between excitation of intralayer vibrations and interlayer interaction demonstrates the importance of including both short- and long-range interactions in an accurate description of how optical fields can be employed to manipulate the stacking order in 2-dimensional transition metal dichalcogenides.

Place, publisher, year, edition, pages
American Chemical Society (ACS) , 2021. Vol. 15, no 5, p. 8826-8835
Keywords [en]
Td-WTe2, stacking order, photoinduced metastable phase, shear phonon, ultrafast electron diffraction
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:kth:diva-298152DOI: 10.1021/acsnano.1c01301ISI: 000656994100080PubMedID: 33913693Scopus ID: 2-s2.0-85106499632OAI: oai:DiVA.org:kth-298152DiVA, id: diva2:1574963
Note

QC 20210629

Available from: 2021-06-29 Created: 2021-06-29 Last updated: 2022-06-25Bibliographically approved

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Ji, ShaozhengWeissenrieder, Jonas

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