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Electronic Structure Manipulation of Topological Materials Probed by Angle-Resolved Photoemission
KTH, School of Engineering Sciences (SCI), Applied Physics.
2026 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Topological quantum materials host electronic states protected by topology and symmetry, giving rise to robust surface or edge states and unconventional electronic properties. Understanding how their electronic band structures respond to external perturbations is essential for both fundamental physics and potential applications. This thesis investigates the electronic structure of topological materials and its evolution under controlled perturbations by combining static angle-resolved photoemission spectroscopy (ARPES) and time-resolved ARPES (tr-ARPES).

First, chemical doping is an effective method for manipulating the electronic structure of materials. Cl-doped Bi2Se3 is systematically studied here. Chlorine incorporation acts as an effective electron donor, shifting the Fermi level while preserving the topological band structure and reinforcing the intrinsic n-type character through heterovalent substitution at Se sites. The time evolution of the band structure reveals a strongly reduced energy shift under prolonged extreme ultraviolet radiation (XUV) exposure compared to pristine Bi2Se3, indicating suppressed adsorption-induced band bending and a modified near-surface defect landscape. Together, these results demonstrate that chemical doping can simultaneously tune the bulk carrier density and stabilize the surface electronic environment, providing a controlled strategy to engineer the electronic structure of topological insulators without compromising their topological character.

Second, optical excitation with femtosecond laser pulses is employed as a route to investigate topological phases in the topological crystalline insulator (TCI) Pb1-xSnxSe. By combining time-resolved ARPES and static X-ray diffraction, we demonstrate that the lattice constant serves as the fundamental control parameter of the normal-insulator-to-topological-crystalline-insulator transition. tr-ARPES measurements reveal that optical excitation, generating electronic temperatures far above the topological-to-normal transition temperature Tc, unexpectedly drives the system deeper into the TCI phase. Analysis of the transient electronic structure shows that the excitation induces an ultrafast lattice contraction on a sub-picosecond timescale. This contraction originates from an electronically induced strengthening of bonds in the inverted band-gap regime. These results show that the TCI phase is robust against optical excitation.

Finally, a spatially structured optical pump, realized using a transient optical grating geometry, is combined with tr-ARPES to investigate ultrafast dynamics in quasi-free-standing bilayer graphene. Although this approach enables spatially and temporally modulated excitation, efficient strain-wave generation requires high pump fluence, leading to enhanced space-charge and surface photovoltage effects. These effects distort photoelectron trajectories and shift measured energies, thereby limiting the sensitivity to subtle band-structure changes. This highlights important experimental constraints in high-fluence ultrafast photoemission measurements.

From a methodological perspective, we optimized the spot sizes of both the pump and probe beams in the tr-ARPES setup, thereby improving the spatial resolution and reducing the influence of sample inhomogeneity. A smaller spot size also increases the achievable upper limit of the pulse fluence for a given laser power, providing greater flexibility for different experimental conditions. In parallel, we employ ultrafast laser-assisted scribing to guide the cleavage process along a desired crystallographic plane, which enhances the reliability and reproducibility of sample preparation. In addition, comprehensive data processing and electron-optics-assisted conversion of raw data from a time-of-flight photoelectron analyzer are implemented to reconstruct the electronic structure in energy–momentum space.

Overall, this thesis demonstrates how static and time-resolved ARPES can be used to probe the electronic structure of topological materials and their evolution under controlled perturbations, highlighting general strategies for tuning electronic states as well as key experimental challenges in exploring the dynamic properties of quantum materials.

Abstract [sv]

Topologiska kvantmaterial hyser elektroniska tillstånd som skyddas av topologi och symmetri, vilket ger upphov till robusta yt- eller kanttillstånd och okonventionella elektroniska egenskaper. Att förstå hur deras elektroniska bandstruktur svarar på externa störningar är avgörande för både grundläggande fysik och potentiella tillämpningar. Denna avhandling undersöker den elektroniska strukturen hos topologiska material och dess utveckling under kontrollerade störningar genom att kombinera statisk vinkelupplöst fotoelektronspektroskopi (ARPES) och tidsupplöst ARPES (tr-ARPES).

För det första är kemisk dopning en effektiv metod för att manipulera materials elektroniska struktur. Cl-dopad Bi₂Se₃ studeras här systematiskt. Inkorporering av klor fungerar som en effektiv elektrondonator, vilket skiftar Ferminivån samtidigt som den topologiska bandstrukturen bevaras och den inneboende n-typ-karaktären förstärks genom heterovalent substitution vid Se-platser. Tidsutvecklingen av bandstrukturen påvisar ett kraftigt reducerat energiskift under långvarig exponering för extrem ultraviolett strålning (XUV) jämfört med ursprunglig Bi₂Se₃, vilket indikerar undertryckt adsorptionsinducerad bandböjning och ett modifierat landskap av defekter nära ytan. Sammantaget visar dessa resultat att kemisk dopning samtidigt kan justera laddningsbärartätheten i bulken och stabilisera den yt-elektroniska miljön, vilket ger en kontrollerad strategi för att manipulera den elektroniska strukturen hos topologiska isolatorer utan att kompromissa med deras topologiska karaktär.

För det andra används optisk excitation med femtosekundslaserpulser som en väg för att undersöka topologiska faser i den topologiska kristallina isolatorn (TCI) Pb₁₋ₓSnₓSe. Genom att kombinera tidsupplöst ARPES och statisk röntgendiffraktion visar vi att gitterkonstanten fungerar som den grundläggande kontrollparametern för övergången från normal isolator till topologisk kristallin isolator. tr-ARPES-mätningar avslöjar att optisk excitation, som genererar elektroniska temperaturer långt över den topologiska-till-normala övergångstemperaturen Tc, oväntat driver systemet djupare in i TCI-fasen. Analys av den transienta elektroniska strukturen visar att excitationen inducerar en ultrasnabb gitterkontraktion på en sub-pikosekund-tidsskala. Denna kontraktion härrör från en elektroniskt inducerad förstärkning av bindningar i regimen med inverterat bandgap. Dessa resultat visar att TCI-fasen är robust mot optisk excitation.

Slutligen kombineras en spatialt strukturerad optisk pump, realiserad genom en transient optisk gittergeometri, med tr-ARPES för att undersöka ultrasnabb dynamik i kvasi-fristående grafendubbelskikt. Även om detta tillvägagångssätt möjliggör spatialt och temporalt modulerad excitation, kräver effektiv generering av töjningsvågor hög pumpfluens, vilket leder till förstärkta rymdladdnings- och yt-fotospänningseffekter. Dessa effekter förvränger fotoelektronernas banor och skiftar de uppmätta energierna, vilket begränsar känsligheten för subtila förändringar i bandstrukturen. Detta belyser viktiga experimentella begränsningar vid ultrasnabba fotoemissionsmätningar med hög fluens.

Ur ett metodologiskt perspektiv optimerade vi punktstorlekarna för både pump- och probstrålarna i tr-ARPES-uppställningen, vilket förbättrade den spatiala upplösningen och minskade inverkan av provinhomogenitet. En mindre punktstorlek ökar också den uppnåeliga övre gränsen för pulsfluensen för en given lasereffekt, vilket ger större flexibilitet för olika experimentella förhållanden. Parallellt använder vi ultrasnabb laserassisterad ritsning för att styra klyvningsprocessen längs ett önskat kristallografiskt plan, vilket förbättrar tillförlitligheten och reproducerbarheten vid provpreparering. Dessutom implementeras omfattande databehandling och elektronoptik-assisterad konvertering av rådata från en time-of-flight-foto-elektronanalysator för att rekonstruera den elektroniska strukturen i energi--rörelsemängdsrymden.

Sammantaget visar denna avhandling hur statisk och tidsupplöst ARPES kan användas för att undersöka den elektroniska strukturen hos topologiska material och deras utveckling under kontrollerade störningar, vilket belyser generella strategier för att justera elektroniska tillstånd såväl som viktiga experimentella utmaningar vid utforskandet av kvantmaterials dynamiska egenskaper.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2026. , p. 91
Series
TRITA-SCI-FOU ; 2026:11
Keywords [en]
Topological quantum materials, angle-resolved photoemission spectroscopy, femtosecond laser, electron dynamics
Keywords [sv]
Topologiska kvantmaterial, vinkelupplöst fotoelektronspektroskopi, femtosekundslaser, elektrondynamik
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:kth:diva-381342ISBN: 978-91-8106-618-0 (print)OAI: oai:DiVA.org:kth-381342DiVA, id: diva2:2060041
Public defence
2026-06-05, 4204, Hus 3, Hannes Alfvéns väg 12, Stockholm, 14:00 (English)
Opponent
Supervisors
Note

QC 2026-05-13

Available from: 2026-05-13 Created: 2026-05-13 Last updated: 2026-06-01Bibliographically approved
List of papers
1. Fermi Level Tuning and Surface Electronic Structure Evolution in Cl-Doped Bi2Se3
Open this publication in new window or tab >>Fermi Level Tuning and Surface Electronic Structure Evolution in Cl-Doped Bi2Se3
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(English)Manuscript (preprint) (Other (popular science, discussion, etc.))
Abstract [en]

Controlling the carrier density and band alignment in three-dimensional topological insulators remains a central challenge due to intrinsic defect-induced n-type doping. In Bi2Se3, selenium vacancies typically shift the Fermi level into the bulk conduction band, complicating access to the intrinsic surface transport regime. Here, we investigate the effect of chlorine incorporation on the electronic structure of Bi2Se3 single crystals using angle-resolved photoemission spectroscopy (ARPES). Across nominal Cl concentrations of 0.25%-1.0%, the topological surface state remains gapless and well-defined, while the band structure shifts systematically toward higher binding energy, indicating enhanced electron doping. Quantitative analysis of the Fermi surface areas reveals an increase in the enclosed momentum-space area of both the topological surface state and conduction-band-derived states with increasing Cl content. Hall measurements further confirm an increase in bulk carrier density, consistent with donor behavior of Cl incorporation. Time-dependent ARPES measurements tracking the surface electronic evolution after cleaving demonstrate a significantly reduced energy shift under prolonged XUV exposure in Cl-doped samples compared to pristine Bi2Se3, indicating reduced sensitivity to adsorption-induced band bending and suggesting a modification of the near-surface defect landscape. Despite the increased carrier density, the bulk band gap remains essentially unchanged, while the relative energy position of the Dirac point within the gap evolves modestly with Cl concentration.

National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:kth:diva-381337 (URN)
Note

QC 20260521

Available from: 2026-05-13 Created: 2026-05-13 Last updated: 2026-05-21Bibliographically approved
2. Laser Induced Transient Grating on Studying Dynamics in Bilayer Graphene
Open this publication in new window or tab >>Laser Induced Transient Grating on Studying Dynamics in Bilayer Graphene
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(English)Manuscript (preprint) (Other academic)
National Category
Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-381338 (URN)
Note

QC 20260520

Available from: 2026-05-13 Created: 2026-05-13 Last updated: 2026-05-20Bibliographically approved
3. Topological stability and ultra-fast lattice contraction by optical excitation in a topological crystalline insulatorStatus: Manuscript under preparation
Open this publication in new window or tab >>Topological stability and ultra-fast lattice contraction by optical excitation in a topological crystalline insulatorStatus: Manuscript under preparation
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(English)Manuscript (preprint) (Other academic)
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:kth:diva-381339 (URN)
Note

QC 20260520

Available from: 2026-05-13 Created: 2026-05-13 Last updated: 2026-05-20Bibliographically approved
4. Fabrication of atomically flat cleavage planes with ultrafast laser scribing
Open this publication in new window or tab >>Fabrication of atomically flat cleavage planes with ultrafast laser scribing
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

The preparation of extensive, atomically flat surfaces remains a central challenge in modern quantum materials research, as many crystals lack natural cleavage planes suitable for advanced surface-sensitive investigations. Here, we demonstrate that laser scribing guided by an ultrafast laser can be applied to facilitate easy cleavage along a desired crystallographic plane under ultra-high vacuum. The method is validated on two brittle materials, SrTiO3 and Si. The technique allows precise spatial localization of the cleaving site and produces extensive, uniformly oriented, and atomically flat surfaces, as verified by scanning electron microscopy (SEM) and atomic force microscopy (AFM). When applied to SrTiO3, the technique enables angle-resolved photoemission spectroscopy (ARPES) measurements of surface electronic states characteristic of the two-dimensional electron liquid (2DEL) hosted at its bare (100) surface. Moreover, ultrafast laser scribing is significantly faster than focused ion beam (FIB) techniques for preparing cleavable planes, offering a more accessible and efficient approach. Owing to its broad applicability, this method establishes a powerful and general framework to prepare high-quality surfaces for advanced photoemission and microscopic investigations of quantum phenomena.

National Category
Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-381341 (URN)
Note

QC 20260520

Available from: 2026-05-13 Created: 2026-05-13 Last updated: 2026-05-20Bibliographically approved

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