Chemical trends of the bulk and surface termination-dependent electronic structure of metal-intercalated transition metal dichalcogenides

DOI: 10.1021/acs.chemmater.4c00824

Authors: Brendan Edwards (University of St Andrews) , Darius-A. Deaconu (University of Manchester) , Philip A. E. Murgatroyd (University of St Andrews) , Sebastian Buchberger (University of St Andrews; Max Planck Institute for Chemical Physics of Solids) , Tommaso Antonelli (University of St Andrews) , Daniel Halliday (University of St Andrews; Diamond Light Source) , Gesa-R. Siemann (University of St Andrews) , Andela Zivanovic (University of St Andrews; Max Planck Institute for Chemical Physics of Solids,) , Liam Trzaska (University of St Andrews) , Akhil Rajan (University of St Andrews) , Edgar Abarca Morales (University of St Andrews; Max Planck Institute for Chemical Physics of Solid) , Daniel A. Mayoh (University of Warwick) , Amelia E. Hall (University of Warwick) , Rodion V. Belosludov (Tohoku University) , Matthew D. Watson (Diamond Light Source) , Timur K. Kim (Diamond Light Source) , Deepnarayan Biswas (Diamond Light Source) , Tien-Lin Lee (Diamond Light Source) , Craig M. Polley (MAX IV Laboratory, Lund University) , Dina Carbone (MAX IV Laboratory, Lund University) , Mats Leandersson (MAX IV Laboratory, Lund University) , Geetha Balakrishnan (University of Warwick) , Mohammad Saeed Bahramy (University of Manchester) , Phil D. C. King (University of St Andrews)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Chemistry Of Materials , VOL 8

State: Published (Approved)
Published: July 2024
Diamond Proposal Number(s): 32937 , 30125 , 31465

Abstract: The addition of metal intercalants into the van der Waals gaps of transition metal dichalcogenides has shown great promise as a method for controlling their functional properties. For example, chiral helimagnetic states, current-induced magnetization switching, and a giant valley-Zeeman effect have all been demonstrated, generating significant renewed interest in this materials family. Here, we present a combined photoemission and density-functional theory study of three such compounds: V1/3NbS2 , Cr1/3NbS2 , and Fe1/3NbS2 , to investigate chemical trends of the intercalant species on their bulk and surface electronic structure. Our resonant photoemission measurements indicate increased hybridization with the itinerant NbS2-derived conduction states with increasing atomic number of the intercalant, leading to pronounced mixing of the nominally localized intercalant states at the Fermi level. Using spatially and angle-resolved photoemission spectroscopy, we show how this impacts surface-termination-dependent charge transfers and leads to the formation of new dispersive states of mixed intercalant-Nb character at the Fermi level for the intercalant-terminated surfaces. This provides an explanation for the origin of anomalous states previously reported in this family of compounds and paves the way for tuning the nature of the magnetic interactions in these systems via control of the hybridization of the magnetic ions with the itinerant states.

Journal Keywords: Binding Energy; Electronic Structure; Hybridization; Layers; Magnetic Properties

Subject Areas: Materials, Chemistry, Physics


Instruments: I05-ARPES , I09-Surface and Interface Structural Analysis

Other Facilities: Bloch at MAX IV

Added On: 24/07/2024 14:37

Documents:
edwards-et-al-2024-chemical-trends-of-the-bulk-and-surface-termination-dependent-electronic-structure-of-metal.pdf

Discipline Tags:

Surfaces Physics Physical Chemistry Hard condensed matter - structures Chemistry Magnetism Materials Science

Technical Tags:

Spectroscopy Angle Resolved Photoemission Spectroscopy (ARPES) X-ray Absorption Spectroscopy (XAS) X-ray Photoelectron Spectroscopy (XPS)