Coherent light control of a metastable hidden state

Julian Maklar; Jit Sarkar; Shuo Dong; Yaroslav A. Gerasimenko; Tommaso Pincelli; Samuel Beaulieu; Patrick S. Kirchmann; Jonathan A. Sobota; Shuolong Yang; Dominik Leuenberger; Robert G. Moore; Zhi Xun Shen; Martin Wolf; Dragan Mihailovic; Ralph Ernstorfer; Laurenz Rettig

doi:10.1126/SCIADV.ADI4661

Coherent light control of a metastable hidden state

Julian Maklar, Jit Sarkar, Shuo Dong, Yaroslav A. Gerasimenko, Tommaso Pincelli, Samuel Beaulieu, Patrick S. Kirchmann, Jonathan A. Sobota, Shuolong Yang, Dominik Leuenberger, Robert G. Moore, Zhi Xun Shen, Martin Wolf, Dragan Mihailovic, Ralph Ernstorfer, Laurenz Rettig

Research output: Contribution to journal › Article › peer-review

9 Scopus citations

Abstract

Metastable phases present a promising route to expand the functionality of complex materials. Of particular interest are light-induced metastable phases that are inaccessible under equilibrium conditions, as they often host new, emergent properties switchable on ultrafast timescales. However, the processes governing the trajectories to such hidden phases remain largely unexplored. Here, using time- and angle-resolved photoemission spectroscopy, we investigate the ultrafast dynamics of the formation of a hidden quantum state in the layered dichalcogenide 1T-TaS₂ upon photoexcitation. Our results reveal the nonthermal character of the transition governed by a collective charge-density-wave excitation. Using a double-pulse excitation of the structural mode, we show vibrational coherent control of the phase-transition efficiency. Our demonstration of exceptional control, switching speed, and stability of the hidden state are key for device applications at the nexus of electronics and photonics.

Original language	English
Article number	adi4661
Journal	Science Advances
Volume	9
Issue number	47
DOIs	https://doi.org/10.1126/SCIADV.ADI4661
State	Published - Nov 2023
Externally published	Yes

Funding

discussions. Funding: This work was funded by the Max Planck Society, the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant no. ERC-2015-CoG-682843 and OPTOlogic 899794), the German Research Foundation (DFG) under the Emmy Noether program (grant no. RE 3977/1), the SFB/TRR 227 Ultrafast Spin Dynamics (projects A09 and B07, project-ID 328545488), the priority program SPP2244 (project-ID 443366970), and the DFG research unit FOR 1700. T.P. acknowledges financial support from the Alexander von Humboldt Foundation. The work by P.S.K., J.A.S., S.Y., D.L., R.G.M., and Z.-X.S. at Stanford and SLAC was supported by the Department of Energy, Office of Basic Energy Sciences, Division of Materials Science and Engineering. D.L. acknowledges support from the Swiss National Science Foundation, under fellowship no. P300P2_151328. S.Y. acknowledges support from the Stanford Graduate Fellowship. Author contributions: L.R., D.M., and J.M. Acknowledgments:W ethankP .Sutar(JožefStefanInstitute)forprovidingthesamples.W e thankT .Ritschel(T echnische UniversitätDresden),M.A.Sentef,D.B.Shin(MPIfortheStructure andDynamicsofMatter),M.Müller,andL.Jiajun(PaulScherrerInstitut)forenlightening discussions.Funding:ThisworkwasfundedbytheMaxPlanckSociety,theEuropeanResearch Council (ERC) under the European Union’s Horizon 2020 research and innovation progr am (grantno.ERC-2015-CoG-682843andOPTOlogic899794),theGermanResearchFoundation (DFG)undertheEmmyNoetherprogram(grantno.RE3977/1),theSFB/TRR227UltrafastSpin Dynamics(projectsA09andB07,project-ID328545488),thepriorityprogramSPP2244(project-ID 443366970), and theDFG researchunit FOR 1700. T .P . acknowledges financialsupport from theAlexandervonHumboldtFoundation.TheworkbyP .S.K., J.A.S.,S.Y ., D.L.,R.G.M.,andZ.-X.S. atStanfordandSLA CwassupportedbytheDepartmentofEnergy,OfficeofBasicEnergy Sciences,DivisionofMaterialsScienceandEngineering.D.L.acknowledgessupportfromthe SwissNationalScienceFoundation,underfellowshipno.P300P2_151328.S.Y .acknowledges supportfromtheStanfordGraduateFellowship.Authorcontributions:L.R.,D.M.,andJ.M. conceivedtheexperiment.J.M.,S.D.,J.S.,T .P ., S.B.,andL.R.carriedouttheXUVtrARPES experiments.P .S.K., J.A.S.,S.Y ., D.L.,andR.G.M.carriedoutthe6-eVlaserARPESexperiments.Y . A.G.conductedandanalyzedtheSTMexperiments.J.M.analyzedthedatawithsupportfromL. R.andJ.S.J.M.wrotethemanuscriptwithsupportfromL.R.,Y .A.G., andD.M.L.R.,R.E.,M.W ., and Z.-X.S.pro vided theexperimentalinfrastructure.Allauthorscommentedonthepaper. Competinginterests:Theauthorsdeclarethattheyhav enocompetinginterests.Dataand materialsavailability:Alldataneededtoevaluatetheconclusionsinthepaperarepresentin the paper and/or the Supplementary Materials. The corresponding raw data files are publicly available at the Zenodo data repository under DOI 10.5281/zenodo.8238530.

Funders	Funder number
SFB
TRR 227 Ultrafast Spin Dynamics	328545488, B07
U.S. Department of Energy
Alexander von Humboldt-Stiftung
Stanford University
Basic Energy Sciences
Horizon 2020 Framework Programme
Division of Materials Sciences and Engineering
European Research Council
Deutsche Forschungsgemeinschaft	443366970, FOR 1700, grantno.RE3977/1, projectsA09andB07,project-ID328545488
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung	P300P2_151328
Max-Planck-Gesellschaft
China Scholarship Council
Horizon 2020	899794, ERC-2015-CoG-682843

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title = "Coherent light control of a metastable hidden state",

abstract = "Metastable phases present a promising route to expand the functionality of complex materials. Of particular interest are light-induced metastable phases that are inaccessible under equilibrium conditions, as they often host new, emergent properties switchable on ultrafast timescales. However, the processes governing the trajectories to such hidden phases remain largely unexplored. Here, using time- and angle-resolved photoemission spectroscopy, we investigate the ultrafast dynamics of the formation of a hidden quantum state in the layered dichalcogenide 1T-TaS2 upon photoexcitation. Our results reveal the nonthermal character of the transition governed by a collective charge-density-wave excitation. Using a double-pulse excitation of the structural mode, we show vibrational coherent control of the phase-transition efficiency. Our demonstration of exceptional control, switching speed, and stability of the hidden state are key for device applications at the nexus of electronics and photonics.",

author = "Julian Maklar and Jit Sarkar and Shuo Dong and Gerasimenko, {Yaroslav A.} and Tommaso Pincelli and Samuel Beaulieu and Kirchmann, {Patrick S.} and Sobota, {Jonathan A.} and Shuolong Yang and Dominik Leuenberger and Moore, {Robert G.} and Shen, {Zhi Xun} and Martin Wolf and Dragan Mihailovic and Ralph Ernstorfer and Laurenz Rettig",

note = "Publisher Copyright: Copyright {\textcopyright} 2023 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).",

year = "2023",

month = nov,

doi = "10.1126/SCIADV.ADI4661",

language = "English",

volume = "9",

journal = "Science Advances",

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T1 - Coherent light control of a metastable hidden state

AU - Maklar, Julian

AU - Sarkar, Jit

AU - Dong, Shuo

AU - Gerasimenko, Yaroslav A.

AU - Pincelli, Tommaso

AU - Beaulieu, Samuel

AU - Kirchmann, Patrick S.

AU - Sobota, Jonathan A.

AU - Yang, Shuolong

AU - Leuenberger, Dominik

AU - Moore, Robert G.

AU - Shen, Zhi Xun

AU - Wolf, Martin

AU - Mihailovic, Dragan

AU - Ernstorfer, Ralph

AU - Rettig, Laurenz

N1 - Publisher Copyright: Copyright © 2023 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

PY - 2023/11

Y1 - 2023/11

N2 - Metastable phases present a promising route to expand the functionality of complex materials. Of particular interest are light-induced metastable phases that are inaccessible under equilibrium conditions, as they often host new, emergent properties switchable on ultrafast timescales. However, the processes governing the trajectories to such hidden phases remain largely unexplored. Here, using time- and angle-resolved photoemission spectroscopy, we investigate the ultrafast dynamics of the formation of a hidden quantum state in the layered dichalcogenide 1T-TaS2 upon photoexcitation. Our results reveal the nonthermal character of the transition governed by a collective charge-density-wave excitation. Using a double-pulse excitation of the structural mode, we show vibrational coherent control of the phase-transition efficiency. Our demonstration of exceptional control, switching speed, and stability of the hidden state are key for device applications at the nexus of electronics and photonics.

AB - Metastable phases present a promising route to expand the functionality of complex materials. Of particular interest are light-induced metastable phases that are inaccessible under equilibrium conditions, as they often host new, emergent properties switchable on ultrafast timescales. However, the processes governing the trajectories to such hidden phases remain largely unexplored. Here, using time- and angle-resolved photoemission spectroscopy, we investigate the ultrafast dynamics of the formation of a hidden quantum state in the layered dichalcogenide 1T-TaS2 upon photoexcitation. Our results reveal the nonthermal character of the transition governed by a collective charge-density-wave excitation. Using a double-pulse excitation of the structural mode, we show vibrational coherent control of the phase-transition efficiency. Our demonstration of exceptional control, switching speed, and stability of the hidden state are key for device applications at the nexus of electronics and photonics.

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VL - 9

JO - Science Advances

JF - Science Advances

IS - 47

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ER -

Coherent light control of a metastable hidden state

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