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Directional sub-femtosecond charge transfer dynamics and the dimensionality of 1T-TaS(2)

For the layered transition metal dichalcogenide 1T-TaS(2), we establish through a unique experimental approach and density functional theory, how ultrafast charge transfer in 1T-TaS(2) takes on isotropic three-dimensional character or anisotropic two-dimensional character, depending on the commensur...

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Autores principales: Kühn, Danilo, Müller, Moritz, Sorgenfrei, Florian, Giangrisostomi, Erika, Jay, Raphael M., Ovsyannikov, Ruslan, Mårtensson, Nils, Sánchez-Portal, Daniel, Föhlisch, Alexander
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6346016/
https://www.ncbi.nlm.nih.gov/pubmed/30679501
http://dx.doi.org/10.1038/s41598-018-36637-0
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author Kühn, Danilo
Müller, Moritz
Sorgenfrei, Florian
Giangrisostomi, Erika
Jay, Raphael M.
Ovsyannikov, Ruslan
Mårtensson, Nils
Sánchez-Portal, Daniel
Föhlisch, Alexander
author_facet Kühn, Danilo
Müller, Moritz
Sorgenfrei, Florian
Giangrisostomi, Erika
Jay, Raphael M.
Ovsyannikov, Ruslan
Mårtensson, Nils
Sánchez-Portal, Daniel
Föhlisch, Alexander
author_sort Kühn, Danilo
collection PubMed
description For the layered transition metal dichalcogenide 1T-TaS(2), we establish through a unique experimental approach and density functional theory, how ultrafast charge transfer in 1T-TaS(2) takes on isotropic three-dimensional character or anisotropic two-dimensional character, depending on the commensurability of the charge density wave phases of 1T-TaS(2). The X-ray spectroscopic core-hole-clock method prepares selectively in- and out-of-plane polarized sulfur 3p orbital occupation with respect to the 1T-TaS(2) planes and monitors sub-femtosecond wave packet delocalization. Despite being a prototypical two-dimensional material, isotropic three-dimensional charge transfer is found in the commensurate charge density wave phase (CCDW), indicating strong coupling between layers. In contrast, anisotropic two-dimensional charge transfer occurs for the nearly commensurate phase (NCDW). In direct comparison, theory shows that interlayer interaction in the CCDW phase – not layer stacking variations – causes isotropic three-dimensional charge transfer. This is presumably a general mechanism for phase transitions and tailored properties of dichalcogenides with charge density waves.
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spelling pubmed-63460162019-01-29 Directional sub-femtosecond charge transfer dynamics and the dimensionality of 1T-TaS(2) Kühn, Danilo Müller, Moritz Sorgenfrei, Florian Giangrisostomi, Erika Jay, Raphael M. Ovsyannikov, Ruslan Mårtensson, Nils Sánchez-Portal, Daniel Föhlisch, Alexander Sci Rep Article For the layered transition metal dichalcogenide 1T-TaS(2), we establish through a unique experimental approach and density functional theory, how ultrafast charge transfer in 1T-TaS(2) takes on isotropic three-dimensional character or anisotropic two-dimensional character, depending on the commensurability of the charge density wave phases of 1T-TaS(2). The X-ray spectroscopic core-hole-clock method prepares selectively in- and out-of-plane polarized sulfur 3p orbital occupation with respect to the 1T-TaS(2) planes and monitors sub-femtosecond wave packet delocalization. Despite being a prototypical two-dimensional material, isotropic three-dimensional charge transfer is found in the commensurate charge density wave phase (CCDW), indicating strong coupling between layers. In contrast, anisotropic two-dimensional charge transfer occurs for the nearly commensurate phase (NCDW). In direct comparison, theory shows that interlayer interaction in the CCDW phase – not layer stacking variations – causes isotropic three-dimensional charge transfer. This is presumably a general mechanism for phase transitions and tailored properties of dichalcogenides with charge density waves. Nature Publishing Group UK 2019-01-24 /pmc/articles/PMC6346016/ /pubmed/30679501 http://dx.doi.org/10.1038/s41598-018-36637-0 Text en © The Author(s) 2019 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Kühn, Danilo
Müller, Moritz
Sorgenfrei, Florian
Giangrisostomi, Erika
Jay, Raphael M.
Ovsyannikov, Ruslan
Mårtensson, Nils
Sánchez-Portal, Daniel
Föhlisch, Alexander
Directional sub-femtosecond charge transfer dynamics and the dimensionality of 1T-TaS(2)
title Directional sub-femtosecond charge transfer dynamics and the dimensionality of 1T-TaS(2)
title_full Directional sub-femtosecond charge transfer dynamics and the dimensionality of 1T-TaS(2)
title_fullStr Directional sub-femtosecond charge transfer dynamics and the dimensionality of 1T-TaS(2)
title_full_unstemmed Directional sub-femtosecond charge transfer dynamics and the dimensionality of 1T-TaS(2)
title_short Directional sub-femtosecond charge transfer dynamics and the dimensionality of 1T-TaS(2)
title_sort directional sub-femtosecond charge transfer dynamics and the dimensionality of 1t-tas(2)
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6346016/
https://www.ncbi.nlm.nih.gov/pubmed/30679501
http://dx.doi.org/10.1038/s41598-018-36637-0
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