Ultrafast X-ray imaging of the light-induced phase transition in VO2

Allan S. Johnson; Daniel Perez-Salinas; Khalid M. Siddiqui; Sungwon Kim; Sungwook Choi; Klara Volckaert; Paulina E. Majchrzak; Søren Ulstrup; Naman Agarwal; Kent Hallman; Richard F. Haglund; Christian M. Günther; Bastian Pfau; Stefan Eisebitt; Dirk Backes; Francesco Maccherozzi; Ann Fitzpatrick; Sarnjeet S. Dhesi; Pierluigi Gargiani; Manuel Valvidares; Nongnuch Artrith; Frank de Groot; Hyeongi Choi; Dogeun Jang; Abhishek Katoch; Soonnam Kwon; Sang Han Park; Hyunjung Kim; Simon E. Wall

doi:10.1038/s41567-022-01848-w

Ultrafast X-ray imaging of the light-induced phase transition in VO₂

Allan S. Johnson^*, Daniel Perez-Salinas, Khalid M. Siddiqui, Sungwon Kim, Sungwook Choi, Klara Volckaert, Paulina E. Majchrzak, Søren Ulstrup, Naman Agarwal, Kent Hallman, Richard F. Haglund, Christian M. Günther, Bastian Pfau, Stefan Eisebitt, Dirk Backes, Francesco Maccherozzi, Ann Fitzpatrick, Sarnjeet S. Dhesi, Pierluigi Gargiani, Manuel ValvidaresNongnuch Artrith, Frank de Groot, Hyeongi Choi, Dogeun Jang, Abhishek Katoch, Soonnam Kwon, Sang Han Park, Hyunjung Kim, Simon E. Wall^*

^*Corresponding author for this work

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

Abstract

Using light to control transient phases in quantum materials is an emerging route to engineer new properties and functionality, with both thermal and non-thermal phases observed out of equilibrium. Transient phases are expected to be heterogeneous, either through photo-generated domain growth or by generating topological defects, and this impacts the dynamics of the system. However, this nanoscale heterogeneity has not been directly observed. Here we use time- and spectrally resolved coherent X-ray imaging to track the prototypical light-induced insulator-to-metal phase transition in vanadium dioxide on the nanoscale with femtosecond time resolution. We show that the early-time dynamics are independent of the initial spatial heterogeneity and observe a 200 fs switch to the metallic phase. A heterogeneous response emerges only after hundreds of picoseconds. Through spectroscopic imaging, we reveal that the transient metallic phase is a highly orthorhombically strained rutile metallic phase, an interpretation that is in contrast to those based on spatially averaged probes. Our results demonstrate the critical importance of spatially and spectrally resolved measurements for understanding and interpreting the transient phases of quantum materials.

Original language	English
Pages (from-to)	215-220
Number of pages	6
Journal	Nature Physics
Volume	19
Issue number	2
DOIs	https://doi.org/10.1038/s41567-022-01848-w
Publication status	Published - Feb 2023

Bibliographical note

Publisher Copyright:
© 2022, The Author(s).

Funding

We acknowledge the support of J. Turner and A. Reid with an early iteration of this experiment. This work was funded through the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Programme (grant agreement no. 758461) and PGC2018-097027-B-I00 project funded by MCIN/AEI/10.13039/501100011033/FEDER ‘A way to make Europe’ and CEX2019-000910-S (MCIN/AEI/10.13039/501100011033), Fundació Cellex, Fundació Mir-Puig, and Generalitat de Catalunya (AGAUR grant no. 2017 SGR 1341, CERCA programme) and by the Independent Research Fund Denmark under the Sapere Aude programme (grant no. 9064-00057B) and VILLUM FONDEN under the Young Investigator Program (grant no. 15375). S.Kim., S.C. and H.K. acknowledge support from the National Research Foundation of Korea (NRF-2021R1A3B1077076). Part of this work was carried out with the support of Diamond Light Source, instrument I06 (proposal MM22048). K.H. and R.F.H. were supported by the US National Science Foundation (EECS-1509740). N. Artrith thanks the Dutch National e-Infrastructure and the SURF Cooperative for computational resources that were used for the DFT XAS simulations. A.S.J. acknowledges support of a fellowship from ‘la Caixa’ Foundation (ID 100010434), fellowship code LCF/BQ/PR21/11840013, and support from the Marie Skłodowska-Curie grant agreement no. 754510 (PROBIST) and the Agencia Estatal de Investigacion (the R&D project CEX2019-000910-S, funded by MCIN/AEI/10.13039/501100011033, Plan National FIDEUA PID2019-106901GB-I00, FPI). We acknowledge the support of J. Turner and A. Reid with an early iteration of this experiment. This work was funded through the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Programme (grant agreement no. 758461) and PGC2018-097027-B-I00 project funded by MCIN/AEI/10.13039/501100011033/FEDER ‘A way to make Europe’ and CEX2019-000910-S (MCIN/AEI/10.13039/501100011033), Fundació Cellex, Fundació Mir-Puig, and Generalitat de Catalunya (AGAUR grant no. 2017 SGR 1341, CERCA programme) and by the Independent Research Fund Denmark under the Sapere Aude programme (grant no. 9064-00057B) and VILLUM FONDEN under the Young Investigator Program (grant no. 15375). S.Kim., S.C. and H.K. acknowledge support from the National Research Foundation of Korea (NRF-2021R1A3B1077076). S. Kwon acknowledges support from the National Research Foundation of Korea (NRF-2020R1A2C1007416). Part of this work was carried out with the support of Diamond Light Source, instrument I06 (proposal MM22048). K.H. and R.F.H. were supported by the US National Science Foundation (EECS-1509740). N. Artrith thanks the Dutch National e-Infrastructure and the SURF Cooperative for computational resources that were used for the DFT XAS simulations. A.S.J. acknowledges support of a fellowship from ‘la Caixa’ Foundation (ID 100010434), fellowship code LCF/BQ/PR21/11840013, and support from the Marie Skłodowska-Curie grant agreement no. 754510 (PROBIST) and the Agencia Estatal de Investigacion (the R&D project CEX2019-000910-S, funded by MCIN/AEI/10.13039/501100011033, Plan National FIDEUA PID2019-106901GB-I00, FPI).

Funders	Funder number
SURF
National Science Foundation	EECS-1509740
Fundación Cellex
VILLUM FONDEN	15375
“la Caixa” Foundation	100010434, LCF/BQ/PR21/11840013
Horizon 2020 Framework Programme	MCIN/AEI/10.13039/501100011033, 758461, PGC2018-097027-B-I00, CEX2019-000910-S
H2020 Marie Skłodowska-Curie Actions	754510
European Research Council
Generalitat de Catalunya
Agència de Gestió d'Ajuts Universitaris i de Recerca	2017 SGR 1341
National Research Foundation of Korea	NRF-2021R1A3B1077076, MM22048
Agencia Estatal de Investigación	FIDEUA PID2019-106901GB-I00
Danmarks Frie Forskningsfond	9064-00057B
Fundación Mig-Puig

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Cite this

Johnson, A. S., Perez-Salinas, D., Siddiqui, K. M., Kim, S., Choi, S., Volckaert, K., Majchrzak, P. E., Ulstrup, S., Agarwal, N., Hallman, K., Haglund, R. F., Günther, C. M., Pfau, B., Eisebitt, S., Backes, D., Maccherozzi, F., Fitzpatrick, A., Dhesi, S. S., Gargiani, P., ... Wall, S. E. (2023). Ultrafast X-ray imaging of the light-induced phase transition in VO₂. Nature Physics, 19(2), 215-220. https://doi.org/10.1038/s41567-022-01848-w

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title = "Ultrafast X-ray imaging of the light-induced phase transition in VO2",

abstract = "Using light to control transient phases in quantum materials is an emerging route to engineer new properties and functionality, with both thermal and non-thermal phases observed out of equilibrium. Transient phases are expected to be heterogeneous, either through photo-generated domain growth or by generating topological defects, and this impacts the dynamics of the system. However, this nanoscale heterogeneity has not been directly observed. Here we use time- and spectrally resolved coherent X-ray imaging to track the prototypical light-induced insulator-to-metal phase transition in vanadium dioxide on the nanoscale with femtosecond time resolution. We show that the early-time dynamics are independent of the initial spatial heterogeneity and observe a 200 fs switch to the metallic phase. A heterogeneous response emerges only after hundreds of picoseconds. Through spectroscopic imaging, we reveal that the transient metallic phase is a highly orthorhombically strained rutile metallic phase, an interpretation that is in contrast to those based on spatially averaged probes. Our results demonstrate the critical importance of spatially and spectrally resolved measurements for understanding and interpreting the transient phases of quantum materials.",

author = "Johnson, {Allan S.} and Daniel Perez-Salinas and Siddiqui, {Khalid M.} and Sungwon Kim and Sungwook Choi and Klara Volckaert and Majchrzak, {Paulina E.} and S{\o}ren Ulstrup and Naman Agarwal and Kent Hallman and Haglund, {Richard F.} and G{\"u}nther, {Christian M.} and Bastian Pfau and Stefan Eisebitt and Dirk Backes and Francesco Maccherozzi and Ann Fitzpatrick and Dhesi, {Sarnjeet S.} and Pierluigi Gargiani and Manuel Valvidares and Nongnuch Artrith and {de Groot}, Frank and Hyeongi Choi and Dogeun Jang and Abhishek Katoch and Soonnam Kwon and Park, {Sang Han} and Hyunjung Kim and Wall, {Simon E.}",

note = "Publisher Copyright: {\textcopyright} 2022, The Author(s).",

year = "2023",

month = feb,

doi = "10.1038/s41567-022-01848-w",

language = "English",

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Johnson, AS, Perez-Salinas, D, Siddiqui, KM, Kim, S, Choi, S, Volckaert, K, Majchrzak, PE, Ulstrup, S, Agarwal, N, Hallman, K, Haglund, RF, Günther, CM, Pfau, B, Eisebitt, S, Backes, D, Maccherozzi, F, Fitzpatrick, A, Dhesi, SS, Gargiani, P, Valvidares, M, Artrith, N , de Groot, F, Choi, H, Jang, D, Katoch, A, Kwon, S, Park, SH, Kim, H & Wall, SE 2023, 'Ultrafast X-ray imaging of the light-induced phase transition in VO₂', Nature Physics, vol. 19, no. 2, pp. 215-220. https://doi.org/10.1038/s41567-022-01848-w

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