Chemical Trends of the Bulk and Surface Termination-Dependent Electronic Structure of Metal-Intercalated Transition Metal Dichalcogenides
(2024) In Chemistry of Materials 36(15). p.7117-7126- 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: Formula Presented, Formula Presented, and Formula Presented, to investigate chemical trends of the intercalant species on their bulk and surface electronic structure. Our resonant photoemission measurements indicate increased hybridization with the... (More)
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: Formula Presented, Formula Presented, and Formula Presented, 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.
(Less)
- author
- organization
- publishing date
- 2024-08
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Chemistry of Materials
- volume
- 36
- issue
- 15
- pages
- 10 pages
- publisher
- The American Chemical Society (ACS)
- external identifiers
-
- scopus:85199449380
- pmid:39156710
- ISSN
- 0897-4756
- DOI
- 10.1021/acs.chemmater.4c00824
- language
- English
- LU publication?
- yes
- id
- 4c60e29b-8ed5-4377-aac5-18c1b2b5a610
- date added to LUP
- 2024-09-09 15:06:16
- date last changed
- 2025-05-20 15:16:29
@article{4c60e29b-8ed5-4377-aac5-18c1b2b5a610,
abstract = {{<p>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: Formula Presented, Formula Presented, and Formula Presented, 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 NbS<sub>2</sub>-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.</p>}},
author = {{Edwards, Brendan and Deaconu, Darius A. and Murgatroyd, Philip A.E. and Buchberger, Sebastian and Antonelli, Tommaso and Halliday, Daniel and Siemann, Gesa R. and Zivanovic, Andela and Trzaska, Liam and Rajan, Akhil and Abarca Morales, Edgar and Mayoh, Daniel A. and Hall, Amelia E. and Belosludov, Rodion V. and Watson, Matthew D. and Kim, Timur K. and Biswas, Deepnarayan and Lee, Tien Lin and Polley, Craig M. and Carbone, Dina and Leandersson, Mats and Balakrishnan, Geetha and Bahramy, Mohammad Saeed and King, Phil D.C.}},
issn = {{0897-4756}},
language = {{eng}},
number = {{15}},
pages = {{7117--7126}},
publisher = {{The American Chemical Society (ACS)}},
series = {{Chemistry of Materials}},
title = {{Chemical Trends of the Bulk and Surface Termination-Dependent Electronic Structure of Metal-Intercalated Transition Metal Dichalcogenides}},
url = {{http://dx.doi.org/10.1021/acs.chemmater.4c00824}},
doi = {{10.1021/acs.chemmater.4c00824}},
volume = {{36}},
year = {{2024}},
}