I05-ARPES
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Oliver J.
Clark
,
Anugrah
Azhar
,
Thi-Hai-Yen
Vu
,
Benjamin A.
Chambers
,
Federico
Mazzola
,
Sadhana
Sridhar
,
Geetha
Balakrishnan
,
Aaron
Bostwick
,
Chris
Jozwiak
,
Eli
Rotenberg
,
Sarah L.
Harmer
,
Mohammad Saeed
Bahramy
,
Michael S.
Fuhrer
,
Mark T.
Edmonds
Diamond Proposal Number(s):
[40610]
Open Access
Abstract: Discovering and engineering spin-polarized surface states in the electronic structures of condensed matter systems is a crucial first step in the development of spintronic devices, wherein spin-polarized bands crossing the Fermi level can facilitate information transfer. Here, through nanofocused angle-resolved photoemission spectroscopy (nano-ARPES) and density functional theory-based calculations, we show that the interface between monolayer WSe2 and metallic NbSe2 exhibits a negative Schottky barrier height of ∼ −30 meV: the K-point valleys of the semiconducting layer are shifted by ∼800 meV to produce a surface-localized Fermi surface populated only by spin-polarized charge carriers. By increasing the WSe2 thickness, the Fermi pockets can be moved from K to Γ, demonstrating tunability of novel semimetallic phases that exist atop a substrate additionally possessing charge density wave and superconducting phases. Together, this study provides a spectroscopic understanding into p-type, Schottky barrier-free interfaces, which are of urgent interest for bypassing the limitations of current-generation vertical field effect transistors, in addition to longer-term spintronics development.
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Feb 2026
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E02-JEM ARM 300CF
I05-ARPES
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Amy
Carl
,
Nicholas
Clark
,
David G.
Hopkinson
,
Matthew
Hamer
,
Matthew
Watson
,
Laxman
Nagireddy
,
James E.
Nunn
,
Alexei
Barinov
,
Yichao
Zou
,
William
Thornley
,
Casey
Cheung
,
Wendong
Wang
,
Sam
Sullivan-Allsop
,
Xiao
Li
,
Astrid
Weston
,
Eli G.
Castanon
,
Andrey V.
Kretinin
,
Cephise
Cacho
,
Neil R.
Wilson
,
Sarah J.
Haigh
,
Roman
Gorbachev
Diamond Proposal Number(s):
[21597, 21981, 24290, 24338]
Open Access
Abstract: Magnetic two-dimensional materials are a promising platform for novel nano-electronic device architectures. One such layered crystal is the ferromagnetic semiconductor chromium germanium telluride (Cr2Ge2Te6) which recently attracted interest due to its potential for spintronics and memory applications. Here we investigate its properties from the structural standpoint using atomic resolution Scanning Transmission Electron Microscopy (STEM) and present the first atomic resolution images down to its monolayer limit. We develop a novel technique that allows one to map the local tilt with unprecedented spatial resolution using only high-resolution images, enabling mapping of the topography and morphological variation of atomically thin crystals. Using it, we show that the Cr2Ge2Te6 monolayer has an unusually large out-of-plane rippling, with local tilt variation reaching 20° over few nm length scales. We hypothesize that such a strongly buckled structure originates from both point and extended lattice defects which are more prevalent in monolayer crystals. In addition, we correlate the structural observations with the band structure measurements using Angle-Resolved Photoemission Spectroscopy (ARPES). We believe that both the atomic scale insights we have gained on Cr2Ge2Te6 and our novel approach to nanoscale topography mapping will benefit the development of van der Waals heterostructures in both fundamental and applied research.
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Feb 2026
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I05-ARPES
|
Diamond Proposal Number(s):
[36633]
Open Access
Abstract: The 4Hb polytype of TaS2 is a natural heterostructure of H and T-type layers. Intriguing recent evidence points towards a possibly chiral superconducting ground state, unlike the superconductivity found in other polytypes where the T layers are absent, requiring understanding of the possible contributions of electrons from the T layers. Here we use micro-focused angle resolved photoemission spectroscopy to reveal that the T termination of the 4Hb structure is metallic, but a subsurface T layer - seen below an H termination and thus more representative of the bulk case - is gapped. The results imply a complete charge transfer of 1 electron per 13 Ta from the T to adjacent H layers in the bulk, but an incomplete charge transfer at the T termination, yielding a metallic Fermi surface with a planar-chiral character. A similar metallic state is found in an anomalous region with likely T-H-H’ stacking at the surface. Our results exclude cluster Mott localisation in either the bulk or surface of 4Hb-TaS2 and point to a scenario of superconductivity arising from Josephson-like tunneling between the H layers.
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Jan 2026
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I05-ARPES
|
Diamond Proposal Number(s):
[37658, 36215, 39549]
Open Access
Abstract: We report the electronic structure of monolayer CrSBr exfoliated onto mica template-stripped gold substrates. Angle-resolved photoemission spectroscopy reveals charge transfer from the substrate, populating the conduction band of monolayer CrSBr, accompanied by a pronounced reduction in the quasiparticle band gap. Furthermore, we observe two separate conduction bands that exhibit a splitting at the X point. This indicates a breaking of glide-mirror symmetry, which in the bulk or in a free-standing monolayer protects the band degeneracies at the Brillouin zone boundary. Our results demonstrate that ultraflat gold substrates do more than modify carrier densities and screening: they can lift symmetry-protected degeneracies and thus fundamentally reshape the band topology of 2D materials.
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Jan 2026
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I05-ARPES
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Diamond Proposal Number(s):
[34246]
Open Access
Abstract: Magnetic van der Waals materials are an important building block to realize spintronic functionalities in heterostructures of two-dimensional (2D) materials. However, establishing their magnetic and electronic properties and the interrelationship between the magnetic ground state and electronic structure is often challenging because only a limited number of techniques can probe magnetism and electronic structure on length scales of tens to hundreds of nanometers. Chromium chalcogenides are a class of 2D magnetic materials for which a rich interplay between structure and magnetism has been predicted. Here, we combine angle-resolved photoemission and quasiparticle interference imaging to establish the electronic structure of a monolayer of CrTe2 on graphite. From a comparison of model calculations with spectroscopic mapping using angle-resolved photoemission spectroscopy and scanning tunneling microscopy we establish the magnetic ground state and the low-energy electronic structure. We demonstrate that the band structure of monolayer CrTe2 is captured well by density functional theory (DFT) in a DFT+𝑈 framework when a Coulomb repulsion of 𝑈=2.5eV is accounted for.
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Dec 2025
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I05-ARPES
|
Hongyun
Zhang
,
Jinxi
Lu
,
Kai
Liu
,
Yijie
Wang
,
Size
Wu
,
Wanying
Chen
,
Xuanxi
Cai
,
Kenji
Watanabe
,
Takashi
Taniguchi
,
Jose
Avila
,
Pavel
Dudin
,
Matthew D.
Watson
,
Alex
Louat
,
Takafumi
Sato
,
Pu
Yu
,
Wenhui
Duan
,
Zhida
Song
,
Guorui
Chen
,
Shuyun
Zhou
Diamond Proposal Number(s):
[37939]
Abstract: The fractional quantum anomalous Hall effect (FQAHE) is a fascinating emergent quantum state characterized by fractionally charged excitations in the absence of a magnetic field. Recently, the FQAHE has been observed in aligned rhombohedral pentalayer graphene on BN (aligned R5G/BN)1 with moiré potential. Intriguingly, the FQAHE preferably emerges when carriers are displaced away from the moiré interface1,2,3, raising debates about the role of moiré potential4,5,6,7,8,9,10,11,12,13,14,15,16,17. Here, by performing nanospot angle-resolved photoemission spectroscopy, we directly visualize the topological flat band in both aligned and non-aligned R5G/BN. The moiré potential in the aligned sample generates moiré bands and enhances the topological flat band as compared to non-aligned sample. Combined with theoretical calculations, we propose that the moiré bands on the top surface arise through the interlayer Coulomb interaction with the moiré-modulated bottom layer. Our results provide direct experimental evidence for the role of moiré potential in aligned rhombohedral graphene, and establish a foundation for understanding its emergent quantum phenomena.
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Nov 2025
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I05-ARPES
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Diamond Proposal Number(s):
[34479, 33317, 35210]
Open Access
Abstract: Understanding the interface between metals and two-dimensional materials is critical for their application in electronics and for the development of metal-mediated exfoliation of large area monolayers. Studying the intricate interactions at the interface requires model systems that enable control of the roughness, purity, and crystallinity of the metal surface. Here, we use angle-resolved photoemission spectroscopy to investigate the layer-dependent electronic structure of WSe\textsubscript{2}~on template-stripped gold substrates fabricated using both silicon and mica templates, giving crystallographically disordered and Au(111) ordered surfaces, respectively, and contrast these findings with \textit{ab initio} predictions. We observe strong hybridization around the Brillouin zone centre at $\overline{\Gamma}$, indicating a covalent admixture in the gold-WSe\textsubscript{2}~interaction, and band shifts that suggest charge rearrangement at the Au(111) / WSe\textsubscript{2}~interface. Core-level spectroscopy shows a single chemical environment for the interfacial WSe\textsubscript{2}~layer on the template-stripped gold, distinct from the subsequent layers. These results reveal a mixture of van der Waals and covalent interactions, best described as a covalent-like quasi-bonding with intermediate interaction strength.
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Oct 2025
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I05-ARPES
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Diamond Proposal Number(s):
[28445]
Open Access
Abstract: The metallic delafossites host ultrahigh-mobility carriers in the bulk, while at their polar surfaces, intrinsic electronic reconstructions stabilize markedly distinct electronic phases, from charge-disproportionated insulators to Rashba-split heavy-hole gases and ferromagnetic metals. The understanding of these phases has been strongly informed by surface spectroscopic measurements, but previous studies have been complicated by the presence of spatially varying terminations of the material surface. Here, we demonstrate the potential of microscopic-area angle-resolved photoemission to overcome these challenges. Our measurements of the model compound PdCoO2 yield extremely high quality spectra of the electronic structure, which allows us to place stringent experimental constraints on the weak electron-phonon coupling in the bulk of PdCoO2, while revealing much stronger interactions at its surfaces. While the CoO2-terminated surface exhibits a conventional weak-coupling behavior, our measurements reveal surprising spectroscopic signatures of polaron formation at the Pd-terminated surface, despite its pronounced metallicity. Together, our findings reveal how mode- and symmetry-selective couplings can markedly tune the electron-phonon interactions in a single host material, here opening routes to stabilize surprisingly persistent polaronic quasiparticles.
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Aug 2025
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I05-ARPES
|
Diamond Proposal Number(s):
[32858]
Open Access
Abstract: Rare-earth tellurides present unique opportunities to explore the interplay between charge density waves (CDWs) and electronic structure in quasi-two-dimensional systems. Unlike their van der Waals counterparts, the rare-earth tritellurides, ditellurides such as LaTe2 feature distinct polar surfaces and Fermi-surface nesting properties. In this paper, we investigate the electronic band structure of LaTe2, distinguishing the surface states from the bulk bands, and enabling the study of the impact of band filling on CDW stability. We uncover the intricate dependence of CDW formation on the electronic environment and highlight the robustness of the CDW order against variations in band filling. The results provide insights into the complex relationship between electronic structure and CDW formation in this class of materials.
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Feb 2025
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I05-ARPES
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Chi Ming
Yim
,
Gesa-R.
Siemann
,
Srdjan
Stavrić
,
Seunghyun
Khim
,
Izidor
Benedičič
,
Philip A. E.
Murgatroyd
,
Tommaso
Antonelli
,
Matthew D.
Watson
,
Andrew P.
Mackenzie
,
Silvia
Picozzi
,
Phil D. C.
King
,
Peter
Wahl
Diamond Proposal Number(s):
[28445]
Open Access
Abstract: Doping of a Mott insulator gives rise to a wide variety of exotic emergent states, from high-temperature superconductivity to charge, spin, and orbital orders. The physics underpinning their evolution is, however, poorly understood. A major challenge is the chemical complexity associated with traditional routes to doping. Here, we study the Mott insulating CrO2 layer of the delafossite PdCrO2, where an intrinsic polar catastrophe provides a clean route to doping of the surface. From scanning tunnelling microscopy and angle-resolved photoemission, we find that the surface stays insulating accompanied by a short-range ordered state. From density functional theory, we demonstrate how the formation of charge disproportionation results in an insulating ground state of the surface that is disparate from the hidden Mott insulator in the bulk. We demonstrate that voltage pulses induce local modifications to this state which relax over tens of minutes, pointing to a glassy nature of the charge order.
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Sep 2024
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