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Photo-induced transient structural state in PdSe2
KTH, School of Engineering Sciences (SCI), Applied Physics, Light and Matter Physics.ORCID iD: 0009-0009-2209-2966
KTH, School of Engineering Sciences (SCI), Applied Physics, Light and Matter Physics.ORCID iD: 0000-0002-7833-3943
KTH, School of Engineering Sciences (SCI), Applied Physics, Light and Matter Physics.ORCID iD: 0000-0003-3670-9807
KTH, School of Engineering Sciences (SCI), Applied Physics, Light and Matter Physics.
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

Two-dimensional palladium diselenide (PdSe2) exhibits unique electronic andstructural properties arising from its puckered pentagonal lattice and strong interlayer coupling. The directional Pd–Se bonding and anisotropic phonon modes make PdSe2 an ideal platform for exploring light–matter interactions and photoinduced structural dynamics. Here, we report a reversible photoinduced structural state transition in PdSe2 occurring on the picosecond timescale. Using ultrafast transmission electron microscopy, we reveal a structural transformation characterized by an in-plane rotationof planar (PdSe4)2- units, researching a metastable state that persists for nanoseconds before relaxing back to the ground state. Time- and angle-resolved photoemission spectroscopy reveals transient electronic excitations consistent with photodoping,which serves as the driving force for the transition. These results demonstrate coherent coupling between electronic and lattice degrees of freedom in PdSe2, establishing it asa prototype system for optical control of metastable structural phases in low-dimensional materials.

National Category
Condensed Matter Physics
Research subject
Physics, Material and Nano Physics
Identifiers
URN: urn:nbn:se:kth:diva-375829OAI: oai:DiVA.org:kth-375829DiVA, id: diva2:2031116
Note

QC 20260123

Available from: 2026-01-22 Created: 2026-01-22 Last updated: 2026-01-23Bibliographically approved
In thesis
1. Ultrafast structural dynamics in quantum materials
Open this publication in new window or tab >>Ultrafast structural dynamics in quantum materials
2026 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Strain provides a powerful route for manipulating quantum states in topological materials by coupling lattice distortions to spin, charge, and topological degrees of freedom. While static approaches such as strain engineering, stacking, and twisting have expanded access to new quantum phases, reversible and programmable control of such states on ultrafast timescales remains a central challenge. This thesis addresses this gap by investigating ultrafast structural dynamics and strain modulation in van der Waals materials using ultrafast electron microscopy (UEM), which combines nanometer spatial resolution with picosecond temporal resolution.

We begin by studying strain wave propagation and interference in defective samples. The interaction between static strain fields and photoexcited coherent acoustic phonons is studied in the Weyl semimetal WTe2. Local standing waves are generated at defect sites where static and dynamic strain couple, enabling deterministic modulation of strain at tens of nanometer scales. Finite-element simulations complement UEM imaging and elucidate the mechanisms of light-induced transient strain engineering. By employing spatially structured femtosecond optical fields, we further confine lattice oscillations into programmable phonon cavities with tunable dimensions, symmetries, and frequencies. UEM directly images these phonon dynamics, including confined out-of-plane oscillations and in-plane Lamb waves, establishing a platform for coherent phonon engineering and programmable transient lattice control at the nanoscale.

We then extend the study into the metastable structural phase control. We demonstrate a photoinduced ultrafast structural transition in PdSe2, occurring within tens of picoseconds and followed by long-lived metastable states persisting on nanosecond timescales. This behavior highlights the potential of pentagonal-layered materials as optically switchable platforms for phase control. We further realize femtosecond laser-driven topological phase patterning in WTe2 by engineering transient optical gratings. This approach enables selective and reversible transitions between topological and trivial phases, with real-space imaging revealing strain-mediated interface dynamics. These studies of metastable structure control pave the way for optically addressable quantum and topological devices.

Finally, we report the direct observation of moiré pattern dynamics under transient strain in twisted van der Waals homostructure. Time-resolved dark-field imaging reveals coherent oscillations of moiré contrast at phonon frequencies, spatially correlated with bent regions. These results demonstrate the coupling between lattice vibrations and emergent functionality in van der Waals junctions.

Together, this work establishes a general framework for spatiotemporal ultrafast structural control in layered materials. By bridging structured light excitation with lattice dynamics, it opens new pathway toward optically reconfigurable quantum phases, topological textures, and novel device functionalities.

Abstract [sv]

Strain utgör en kraftfull metod för att manipulera kvanttillstånd i topologiska material genom att koppla gitterdeformationer till spinn-, laddnings- och topologiska frihetsgrader. Även om statiska metoder såsom strain-ingenjörskonst, stapling och vridning har utökat tillgången till nya kvantfaser, kvarstår reversibel och programmerbar kontroll av sådana tillstånd på ultrafasta tidsskalor som en central utmaning. Denna avhandling adresserar detta genom att undersöka ultrafasta strukturdynamiker och strain-modulering i van der Waals-material med hjälp av ultrafast elektronmikroskopi (UEM), som kombinerar rumslig upplösning på nanometernivå med temporal upplösning på pikosekundnivå.

Arbetet inleds med studier av utbredning och interferens av strainvågor i defekta prover. Samspelet mellan statiska strainfält och fotoexciterade koherenta akustiska fononer undersöks i Weyl-semimetallen WTe₂. Lokala stående vågor genereras vid defektplatser där statisk och dynamisk strain kopplas samman, vilket möjliggör deterministisk modulering av strain på längdskalor om tiotals nanometer. Finita element-simuleringar kompletterar UEM-avbildning och klargör mekanismerna bakom ljusinducerad transient strain-ingenjörskonst. Genom att använda rumsligt strukturerade femtosekundoptiska fält kan gitteroscillationer dessutom begränsas till programmerbara fononkaviteter med justerbara dimensioner, symmetrier och frekvenser. UEM avbildar direkt dessa fonondynamiker, inklusive begränsade ut-ur-planet-oscillationer och in-plan Lamb-vågor, vilket etablerar en plattform för koherent fonon-ingenjörskonst och programmerbar transient gitterkontroll på nanoskala.

Studien utvidgas därefter till kontroll av metastabila strukturella faser. Vi demonstrerar en fotoinducerad ultrafast strukturell fasövergång i PdSe₂, som sker inom tiotals pikosekunder och följs av långlivade metastabila tillstånd som kvarstår på nanosekundtidsskalor. Detta beteende belyser potentialen hos pentagonalt skiktade material som optiskt switchbara plattformar för fasstyrning. Vidare realiseras topologisk fas-mönstring i WTe₂ driven av femtosekundlasrar genom att konstruera transienta optiska gitter. Detta möjliggör selektiva och reversibla övergångar mellan topologiska och triviala faser, där realrumsavbildning avslöjar strain-medierad dynamik vid gränsytor. Dessa studier av metastabil strukturkontroll banar väg för optiskt adresserbara kvant- och topologiska enheter.

Slutligen rapporterar vi direkt observation av moiré-mönsterdynamik under transient strain i tvistade van der Waals-homostrukturer. Tidsupplöst mörkfältsavbildning visar koherenta oscillationer i moiré-kontrasten vid fononfrekvenser, rumsligt korrelerade med böjda regioner. Dessa resultat demonstrerar kopplingen mellan gittervibrationer och framväxande funktionalitet i van der Waals-kopplingar.

Sammantaget etablerar detta arbete ett generellt ramverk för spatiotemporal ultrafast strukturell kontroll i skiktade material. Genom att sammanföra strukturerad ljusexcitation med gitterdynamik öppnas nya vägar mot optiskt rekonfigurerbara kvantfaser, topologiska texturer och nya enhetsfunktionaliteter.

Place, publisher, year, edition, pages
KTH Royal Institute of Technology, 2026
Series
TRITA-SCI-FOU ; 2025:65
Keywords
Ultrafast electron microscopy, femtosecond laser, phonon dynamics, structural phase, van der Waals materials, Ultrasnabb elektronmikroskopi, femtosekundlaser, fonondynamik, strukturellfas, van der Waals-material
National Category
Condensed Matter Physics
Research subject
Physics, Material and Nano Physics
Identifiers
urn:nbn:se:kth:diva-375833 (URN)978-91-8106-477-3 (ISBN)
Public defence
2026-02-13, FA31 Roslagstullsbacken 21, https://kth-se.zoom.us/j/68248144408 , Stockholm, 10:00 (English)
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Supervisors
Note

QC 2026-01-22

Available from: 2026-01-22 Created: 2026-01-22 Last updated: 2026-02-10Bibliographically approved

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Wu, JianyuBerntsen, Magnus H.Cao, GaolongNiedermayr, ArthurWeissenrieder, Jonas

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