Nanoscale-femtosecond dielectric response of Mott insulators captured by two-color near-field ultrafast electron microscopy
Abstract
Characterizing and controlling the out-of-equilibrium state of nanostructured Mott insulators hold great promises for emerging quantum technologies while providing an exciting playground for investigating fundamental physics of strongly-correlated systems. Here, we use two-color near-field ultrafast electron microscopy to photo-induce the insulator-to-metal transition in a single VO2 nanowire and probe the ensuing electronic dynamics with combined nanometer-femtosecond resolution (10–21m • s). We take advantage of a femtosecond temporal gating of the electron pulse mediated by an infrared laser pulse, and exploit the sensitivity of inelastic electron-light scattering to changes in the material dielectric function. By spatially mapping the near-field dynamics of an individual nanowire of VO2, we observe that ultrafast photo-doping drives the system into a metallic state on a timescale of ~150 fs without yet perturbing the crystalline lattice. Due to the high versatility and sensitivity of the electron probe, our method would allow capturing the electronic dynamics of a wide range of nanoscale materials with ultimate spatiotemporal resolution.
- Authors:
-
[1];
[2];
[3];
[4];
[5];
[3];
- Nankai Univ., Tianjin (China); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Ecole Polytechnique Federale Lausanne (Switzlerland); Univ. of Geneva (Switzerland)
- Ecole Polytechnique Federale Lausanne (Switzlerland)
- Univ. of California, Berkeley, CA (United States)
- Univ. of Milano-Bicocca, Milano (Italy)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Swiss Federal Institute of Technology Lausanne; Swiss National Science Foundation (SNSF); National Science Foundation (NSF)
- OSTI Identifier:
- 1763998
- Report Number(s):
- BNL-220951-2021-JAAM
Journal ID: ISSN 2041-1723; TRN: US2206126
- Grant/Contract Number:
- SC0012704; 665667; 200020-179157; DMR-1608899
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Fu, Xuewen, Barantani, Francesco, Gargiulo, Simone, Madan, Ivan, Berruto, Gabriele, LaGrange, Thomas, Jin, Lei, Wu, Junqiao, Vanacore, Giovanni Maria, Carbone, Fabrizio, and Zhu, Yimei. Nanoscale-femtosecond dielectric response of Mott insulators captured by two-color near-field ultrafast electron microscopy. United States: N. p., 2020.
Web. doi:10.1038/s41467-020-19636-6.
Fu, Xuewen, Barantani, Francesco, Gargiulo, Simone, Madan, Ivan, Berruto, Gabriele, LaGrange, Thomas, Jin, Lei, Wu, Junqiao, Vanacore, Giovanni Maria, Carbone, Fabrizio, & Zhu, Yimei. Nanoscale-femtosecond dielectric response of Mott insulators captured by two-color near-field ultrafast electron microscopy. United States. https://doi.org/10.1038/s41467-020-19636-6
Fu, Xuewen, Barantani, Francesco, Gargiulo, Simone, Madan, Ivan, Berruto, Gabriele, LaGrange, Thomas, Jin, Lei, Wu, Junqiao, Vanacore, Giovanni Maria, Carbone, Fabrizio, and Zhu, Yimei. Fri .
"Nanoscale-femtosecond dielectric response of Mott insulators captured by two-color near-field ultrafast electron microscopy". United States. https://doi.org/10.1038/s41467-020-19636-6. https://www.osti.gov/servlets/purl/1763998.
@article{osti_1763998,
title = {Nanoscale-femtosecond dielectric response of Mott insulators captured by two-color near-field ultrafast electron microscopy},
author = {Fu, Xuewen and Barantani, Francesco and Gargiulo, Simone and Madan, Ivan and Berruto, Gabriele and LaGrange, Thomas and Jin, Lei and Wu, Junqiao and Vanacore, Giovanni Maria and Carbone, Fabrizio and Zhu, Yimei},
abstractNote = {Characterizing and controlling the out-of-equilibrium state of nanostructured Mott insulators hold great promises for emerging quantum technologies while providing an exciting playground for investigating fundamental physics of strongly-correlated systems. Here, we use two-color near-field ultrafast electron microscopy to photo-induce the insulator-to-metal transition in a single VO2 nanowire and probe the ensuing electronic dynamics with combined nanometer-femtosecond resolution (10–21m • s). We take advantage of a femtosecond temporal gating of the electron pulse mediated by an infrared laser pulse, and exploit the sensitivity of inelastic electron-light scattering to changes in the material dielectric function. By spatially mapping the near-field dynamics of an individual nanowire of VO2, we observe that ultrafast photo-doping drives the system into a metallic state on a timescale of ~150 fs without yet perturbing the crystalline lattice. Due to the high versatility and sensitivity of the electron probe, our method would allow capturing the electronic dynamics of a wide range of nanoscale materials with ultimate spatiotemporal resolution.},
doi = {10.1038/s41467-020-19636-6},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {Fri Nov 13 00:00:00 EST 2020},
month = {Fri Nov 13 00:00:00 EST 2020}
}
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Works referenced in this record:
Double-slit photoelectron interference in strong-field ionization of the neon dimer
journal, January 2019
- Kunitski, Maksim; Eicke, Nicolas; Huber, Pia
- Nature Communications, Vol. 10, Issue 1
Design and implementation of a fs-resolved transmission electron microscope based on thermionic gun technology
journal, September 2013
- Piazza, L.; Masiel, D. J.; LaGrange, T.
- Chemical Physics, Vol. 423
Ultrafast transmission electron microscopy using a laser-driven field emitter: Femtosecond resolution with a high coherence electron beam
journal, May 2017
- Feist, Armin; Bach, Nora; Rubiano da Silva, Nara
- Ultramicroscopy, Vol. 176
Band-Selective Measurements of Electron Dynamics in Using Femtosecond Near-Edge X-Ray Absorption
journal, August 2005
- Cavalleri, A.; Rini, M.; Chong, H. H. W.
- Physical Review Letters, Vol. 95, Issue 6
Quantum coherent optical phase modulation in an ultrafast transmission electron microscope
journal, May 2015
- Feist, Armin; Echternkamp, Katharina E.; Schauss, Jakob
- Nature, Vol. 521, Issue 7551
Calculation of the near fields for the scattering of electromagnetic waves by multiple infinite cylinders at perpendicular incidence
journal, November 2012
- Schäfer, J.; Lee, S. -C.; Kienle, A.
- Journal of Quantitative Spectroscopy and Radiative Transfer, Vol. 113, Issue 16
Attomicroscopy: from femtosecond to attosecond electron microscopy
journal, January 2018
- Hassan, Mohammed Th
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 51, Issue 3
Treating retardation effects in valence EELS spectra for Kramers–Kronig analysis
journal, April 2008
- Stöger-Pollach, M.; Laister, A.; Schattschneider, P.
- Ultramicroscopy, Vol. 108, Issue 5
Ultrastructural Characterization of the Lower Motor System in a Mouse Model of Krabbe Disease
journal, December 2016
- Cappello, Valentina; Marchetti, Laura; Parlanti, Paola
- Scientific Reports, Vol. 6, Issue 1
Photoinduced nanobubble-driven superfast diffusion of nanoparticles imaged by 4D electron microscopy
journal, August 2017
- Fu, Xuewen; Chen, Bin; Tang, Jau
- Science Advances, Vol. 3, Issue 8
Photon-induced near-field electron microscopy
journal, December 2009
- Barwick, Brett; Flannigan, David J.; Zewail, Ahmed H.
- Nature, Vol. 462, Issue 7275
Anomalously low electronic thermal conductivity in metallic vanadium dioxide
journal, January 2017
- Lee, Sangwook; Hippalgaonkar, Kedar; Yang, Fan
- Science, Vol. 355, Issue 6323
Comprehensive study of the metal-insulator transition in pulsed laser deposited epitaxial VO 2 thin films
journal, January 2013
- Fu, Deyi; Liu, Kai; Tao, Tao
- Journal of Applied Physics, Vol. 113, Issue 4
Development of a high brightness ultrafast Transmission Electron Microscope based on a laser-driven cold field emission source
journal, March 2018
- Houdellier, F.; Caruso, G. M.; Weber, S.
- Ultramicroscopy, Vol. 186
Four-Dimensional Electron Microscopy
journal, April 2010
- Zewail, A. H.
- Science, Vol. 328, Issue 5975
Dielectric properties of silicon nitride ceramics produced by free sintering
journal, August 2017
- Lukianova, O. A.; Sirota, V. V.
- Ceramics International, Vol. 43, Issue 11
Four-dimensional electron microscopy: Ultrafast imaging, diffraction and spectroscopy in materials science and biology
journal, April 2016
- Vanacore, G. M.; Fitzpatrick, A. W. P.; Zewail, A. H.
- Nano Today, Vol. 11, Issue 2
Subthreshold firing in Mott nanodevices
journal, May 2019
- del Valle, Javier; Salev, Pavel; Tesler, Federico
- Nature, Vol. 569, Issue 7756
Subparticle Ultrafast Spectrum Imaging in 4D Electron Microscopy
journal, January 2012
- Yurtsever, Aycan; van der Veen, Renske M.; Zewail, Ahmed H.
- Science, Vol. 335, Issue 6064
4D Imaging of Transient Structures and Morphologies in Ultrafast Electron Microscopy
journal, November 2008
- Barwick, B.; Park, H. S.; Kwon, O. -H.
- Science, Vol. 322, Issue 5905
Memristive devices for computing
journal, January 2013
- Yang, J. Joshua; Strukov, Dmitri B.; Stewart, Duncan R.
- Nature Nanotechnology, Vol. 8, Issue 1, p. 13-24
Real-time measurement of the emergence of superconducting order in a high-temperature superconductor
journal, June 2016
- Madan, I.; Kusar, P.; Baranov, V. V.
- Physical Review B, Vol. 93, Issue 22
Instantaneous Band Gap Collapse in Photoexcited Monoclinic due to Photocarrier Doping
journal, November 2014
- Wegkamp, Daniel; Herzog, Marc; Xian, Lede
- Physical Review Letters, Vol. 113, Issue 21
Vanadium dioxide for energy conservation and energy storage applications: Synthesis and performance improvement
journal, February 2018
- Wang, Shancheng; Owusu, Kwadwo Asare; Mai, Liqiang
- Applied Energy, Vol. 211
Femtosecond Structural Dynamics in during an Ultrafast Solid-Solid Phase Transition
journal, November 2001
- Cavalleri, A.; Tóth, Cs.; Siders, C. W.
- Physical Review Letters, Vol. 87, Issue 23
Graphene-layered steps and their fields visualized by 4D electron microscopy
journal, May 2013
- Park, Sang Tae; Yurtsever, Aycan; Baskin, John Spencer
- Proceedings of the National Academy of Sciences, Vol. 110, Issue 23
Observing liquid flow in nanotubes by 4D electron microscopy
journal, June 2014
- Lorenz, U. J.; Zewail, A. H.
- Science, Vol. 344, Issue 6191
New Scattering Information Portal for the light-scattering community
journal, May 2008
- Wriedt, Thomas; Hellmers, Jens
- Journal of Quantitative Spectroscopy and Radiative Transfer, Vol. 109, Issue 8
Sub-phonon-period compression of electron pulses for atomic diffraction
journal, October 2015
- Gliserin, A.; Walbran, M.; Krausz, F.
- Nature Communications, Vol. 6, Issue 1
A photoinduced metal-like phase of monoclinic VO 2 revealed by ultrafast electron diffraction
journal, October 2014
- Morrison, Vance R.; Chatelain, Robert. P.; Tiwari, Kunal L.
- Science, Vol. 346, Issue 6208
Imaging Nanometer Phase Coexistence at Defects During the Insulator–Metal Phase Transformation in VO 2 Thin Films by Resonant Soft X-ray Holography
journal, May 2018
- Vidas, Luciana; Günther, Christian M.; Miller, Timothy A.
- Nano Letters, Vol. 18, Issue 6
Imaging rotational dynamics of nanoparticles in liquid by 4D electron microscopy
journal, February 2017
- Fu, Xuewen; Chen, Bin; Tang, Jau
- Science, Vol. 355, Issue 6324
Coherent Structural Dynamics and Electronic Correlations during an Ultrafast Insulator-to-Metal Phase Transition in
journal, September 2007
- Kübler, C.; Ehrke, H.; Huber, R.
- Physical Review Letters, Vol. 99, Issue 11
4D Visualization of Transitional Structures in Phase Transformations by Electron Diffraction
journal, November 2007
- Baum, P.; Yang, D. -S.; Zewail, A. H.
- Science, Vol. 318, Issue 5851
Photon-induced near-field electron microscopy (PINEM): theoretical and experimental
journal, December 2010
- Park, Sang Tae; Lin, Milo; Zewail, Ahmed H.
- New Journal of Physics, Vol. 12, Issue 12
Ultrafast electron crystallography of the cooperative reaction path in vanadium dioxide
journal, May 2016
- Yang, Ding-Shyue; Baum, Peter; Zewail, Ahmed H.
- Structural Dynamics, Vol. 3, Issue 3
Training and operation of an integrated neuromorphic network based on metal-oxide memristors
journal, May 2015
- Prezioso, M.; Merrikh-Bayat, F.; Hoskins, B. D.
- Nature, Vol. 521, Issue 7550
Ultrafast disordering of vanadium dimers in photoexcited VO 2
journal, November 2018
- Wall, Simon; Yang, Shan; Vidas, Luciana
- Science, Vol. 362, Issue 6414
Heat capacity of VO2 single crystals
journal, April 1973
- Chandrashekhar, G. V.; Barros, H. L. C.; Honig, J. M.
- Materials Research Bulletin, Vol. 8, Issue 4
Nanoscale Engineering in VO 2 Nanowires via Direct Electron Writing Process
journal, January 2017
- Zhang, Zhenhua; Guo, Hua; Ding, Wenqiang
- Nano Letters, Vol. 17, Issue 2
In Situ Atom Scale Visualization of Domain Wall Dynamics in VO2 Insulator-Metal Phase Transition
journal, October 2014
- He, Xinfeng; Xu, Tao; Xu, Xiaofeng
- Scientific Reports, Vol. 4, Issue 1
Photon gating in four-dimensional ultrafast electron microscopy
journal, October 2015
- Hassan, Mohammed T.; Liu, Haihua; Baskin, John Spencer
- Proceedings of the National Academy of Sciences, Vol. 112, Issue 42
Dynamics and control of gold-encapped gallium arsenide nanowires imaged by 4D electron microscopy
journal, November 2017
- Chen, Bin; Fu, Xuewen; Tang, Jau
- Proceedings of the National Academy of Sciences, Vol. 114, Issue 49
Multiphoton Absorption and Emission by Interaction of Swift Electrons with Evanescent Light Fields
journal, May 2010
- García de Abajo, F. Javier; Asenjo-Garcia, Ana; Kociak, Mathieu
- Nano Letters, Vol. 10, Issue 5
meV Resolution in Laser-Assisted Energy-Filtered Transmission Electron Microscopy
journal, December 2017
- Pomarico, Enrico; Madan, Ivan; Berruto, Gabriele
- ACS Photonics, Vol. 5, Issue 3
Photon-induced near-field electron microscopy: Mathematical formulation of the relation between the experimental observables and the optically driven charge density of nanoparticles
journal, January 2014
- Park, Sang Tae; Zewail, Ahmed H.
- Physical Review A, Vol. 89, Issue 1
Photoinduced phase transition in VO_2 nanocrystals: ultrafast control of surface-plasmon resonance
journal, January 2005
- Rini, Matteo; Cavalleri, Andrea; Schoenlein, Robert W.
- Optics Letters, Vol. 30, Issue 5
External-Strain Induced Insulating Phase Transition in VO2 Nanobeam and Its Application as Flexible Strain Sensor
journal, September 2010
- Hu, Bin; Ding, Yong; Chen, Wen
- Advanced Materials, Vol. 22, Issue 45
Ultrafast optical spectroscopy of strongly correlated materials and high-temperature superconductors: a non-equilibrium approach
journal, March 2016
- Giannetti, Claudio; Capone, Massimo; Fausti, Daniele
- Advances in Physics, Vol. 65, Issue 2
Electron microscopy of electromagnetic waveforms
journal, July 2016
- Ryabov, A.; Baum, P.
- Science, Vol. 353, Issue 6297
High-temporal-resolution electron microscopy for imaging ultrafast electron dynamics
journal, May 2017
- Hassan, M. Th.; Baskin, J. S.; Liao, B.
- Nature Photonics, Vol. 11, Issue 7
Simultaneous observation of the quantization and the interference pattern of a plasmonic near-field
journal, March 2015
- Piazza, L.; Lummen, T. T. A.; Quiñonez, E.
- Nature Communications, Vol. 6, Issue 1
On the Optical Properties of Thin‐Film Vanadium Dioxide from the Visible to the Far Infrared
journal, August 2019
- Wan, Chenghao; Zhang, Zhen; Woolf, David
- Annalen der Physik, Vol. 531, Issue 10
Ultrafast dynamics during the photoinduced phase transition in VO2
journal, December 2015
- Wegkamp, Daniel; Stähler, Julia
- Progress in Surface Science, Vol. 90, Issue 4