TY - JOUR A1 - Kühn, Danilo A1 - Müller, Moritz A1 - Sorgenfrei, Florian A1 - Giangrisostomi, Erika A1 - Jay, Raphael Martin A1 - Ovsyannikov, Ruslan A1 - Martensson, Nils A1 - Sanchez-Portal, Daniel A1 - Föhlisch, Alexander T1 - Directional sub-femtosecond charge transfer dynamics and the dimensionality of 1T-TaS2 JF - Scientific reports N2 - For the layered transition metal dichalcogenide 1T-TaS2, we establish through a unique experimental approach and density functional theory, how ultrafast charge transfer in 1T-TaS2 takes on isotropic three-dimensional character or anisotropic two-dimensional character, depending on the commensurability of the charge density wave phases of 1T-TaS2. 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-TaS2 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. Y1 - 2019 U6 - https://doi.org/10.1038/s41598-018-36637-0 SN - 2045-2322 VL - 9 IS - 488 PB - Nature Publ. Group CY - London ER -