Ultrafast Mid-Infrared Nanoscopy of Strained Vanadium Dioxide Nanobeams.

Long regarded as a model system for studying insulator-to-metal phase transitions, the correlated electron material vanadium dioxide (VO2) is now finding novel uses in device applications. Two of its most appealing aspects are its accessible transition temperature (∼341 K) and its rich phase diagram. Strain can be used to selectively stabilize different VO2 insulating phases by tuning the competition between electron and lattice degrees of freedom. It can even break the mesoscopic spatial symmetry of the transition, leading to a quasiperiodic ordering of insulating and metallic nanodomains. Nanostructuring of strained VO2 could potentially yield unique components for future devices. However, the most spectacular property of VO2--its ultrafast transition--has not yet been studied on the length scale of its phase heterogeneity. Here, we use ultrafast near-field microscopy in the mid-infrared to study individual, strained VO2 nanobeams on the 10 nm scale. We reveal a previously unseen correlation between the local steady-state switching susceptibility and the local ultrafast response to below-threshold photoexcitation. These results suggest that it may be possible to tailor the local photoresponse of VO2 using strain and thereby realize new types of ultrafast nano-optical devices.

[1]  S. Wolf,et al.  THz spectroscopy of VO2 epitaxial films: controlling the anisotropic properties through strain engineering , 2012 .

[2]  R. Haglund,et al.  Ultrafast changes in lattice symmetry probed by coherent phonons , 2010, Nature Communications.

[3]  Hanspeter Helm,et al.  Metal-insulator phase transition in a VO2 thin film observed with terahertz spectroscopy , 2006 .

[4]  L. Lauhon,et al.  Increased Yield and Uniformity of Vanadium Dioxide Nanobeam Growth via Two-Step Physical Vapor Transport Process , 2012 .

[5]  Ahmed H. Zewail,et al.  4D Visualization of Transitional Structures in Phase Transformations by Electron Diffraction , 2007, Science.

[6]  M. Kawasaki,et al.  Collective bulk carrier delocalization driven by electrostatic surface charge accumulation , 2012, Nature.

[7]  H. Bandulet,et al.  Phase diagram of the ultrafast photoinduced insulator-metal transition in vanadium dioxide , 2012 .

[8]  M. Raschke,et al.  Inhomogeneity of the ultrafast insulator-to-metal transition dynamics of VO2 , 2015, Nature Communications.

[9]  S. Parkin,et al.  Suppression of Metal-Insulator Transition in VO2 by Electric Field–Induced Oxygen Vacancy Formation , 2013, Science.

[10]  H. Ehrke,et al.  Coherent structural dynamics and electronic correlations during an ultrafast insulator-to-metal phase transition in VO2. , 2007, Physical review letters.

[11]  Kunio Okimura,et al.  Characterization of structural dynamics of VO2 thin film on c-Al2O3 using in-air time-resolved x-ray diffraction , 2010 .

[12]  H. Bandulet,et al.  Terahertz conductivity of the metal-insulator transition in a nanogranular VO2 film , 2010 .

[13]  C. N. Lau,et al.  Ultrafast and nanoscale plasmonic phenomena in exfoliated graphene revealed by infrared pump-probe nanoscopy. , 2014, Nano letters.

[14]  L. Sorba,et al.  Ultrafast multi-terahertz nano-spectroscopy with sub-cycle temporal resolution , 2014 .

[15]  Angel Rubio,et al.  Instantaneous band gap collapse in photoexcited monoclinic VO2 due to photocarrier doping. , 2014, Physical review letters.

[16]  D J Hilton,et al.  Enhanced photosusceptibility near Tc for the light-induced insulator-to-metal phase transition in vanadium dioxide. , 2007, Physical review letters.

[17]  Junqiao Wu,et al.  Strain and temperature dependence of the insulating phases of VO2 near the metal-insulator transition , 2012 .

[18]  Joyeeta Nag,et al.  Ultrafast phase transition via catastrophic phonon collapse driven by plasmonic hot-electron injection. , 2014, Nano letters.

[19]  Judson D Ryckman,et al.  Ultra-compact silicon photonic devices reconfigured by an optically induced semiconductor-to-metal transition. , 2013, Optics express.

[20]  Masayoshi Tonouchi,et al.  Cutting-edge terahertz technology , 2007 .

[21]  Hongkun Park,et al.  Strain-induced self organization of metal-insulator domains in single-crystalline VO2 nanobeams. , 2006, Nano letters.

[22]  Mohamed Chaker,et al.  A photoinduced metal-like phase of monoclinic VO2 revealed by ultrafast electron diffraction , 2014, Science.

[23]  M. Goldflam,et al.  Anisotropic electronic state via spontaneous phase separation in strained vanadium dioxide films. , 2013, Physical review letters.

[24]  Byung-Gyu Chae,et al.  Mott Transition in VO2 Revealed by Infrared Spectroscopy and Nano-Imaging , 2007, Science.

[25]  Jed I. Ziegler,et al.  Control of plasmonic nanoantennas by reversible metal-insulator transition , 2015, Scientific Reports.

[26]  Evgheni Strelcov,et al.  In situ monitoring of the growth, intermediate phase transformations and templating of single crystal VO2 nanowires and nanoplatelets. , 2011, ACS nano.

[27]  J C Grossman,et al.  Strain engineering and one-dimensional organization of metal-insulator domains in single-crystal vanadium dioxide beams. , 2009, Nature nanotechnology.

[28]  J. C. Kieffer,et al.  Evidence for a structurally-driven insulator-to-metal transition in VO 2 : A view from the ultrafast timescale , 2004, cond-mat/0403214.

[29]  A I Lichtenstein,et al.  Dynamical singlets and correlation-assisted Peierls transition in VO2. , 2005, Physical review letters.

[30]  M. Raschke,et al.  Nano-optical investigations of the metal-insulator phase behavior of individual VO(2) microcrystals. , 2010, Nano letters.

[31]  Wei Chen,et al.  New aspects of the metal-insulator transition in single-domain vanadium dioxide nanobeams. , 2009, Nature nanotechnology.

[32]  D. Mittleman,et al.  The metal-insulator transition in VO2 studied using terahertz apertureless near-field microscopy , 2007 .

[33]  Fritz Keilmann,et al.  Ultrafast dynamics of surface plasmons in InAs by time-resolved infrared nanospectroscopy. , 2014, Nano letters.

[34]  Martin Dressel,et al.  Electrodynamics of correlated electron materials , 2011, 1106.2309.

[35]  John D. Budai,et al.  Metallization of vanadium dioxide driven by large phonon entropy , 2014, Nature.

[36]  Stuart S. P. Parkin,et al.  Control of the metal–insulator transition in vanadium dioxide by modifying orbital occupancy , 2013, Nature Physics.

[37]  H. Bechtel,et al.  Phase transition in bulk single crystals and thin films of VO2 by nano-infrared spectroscopy and imaging , 2015, 1506.04786.

[38]  C. La-o-vorakiat,et al.  New Insights into the Diverse Electronic Phases of a Novel Vanadium Dioxide Polymorph: A Terahertz Spectroscopy Study , 2015, Scientific Reports.

[39]  Tohru Suemoto,et al.  Photoinduced metallic state in VO2 proved by the terahertz pump-probe spectroscopy , 2008 .

[40]  E. Bakkers,et al.  Nanoscale free-carrier profiling of individual semiconductor nanowires by infrared near-field nanoscopy. , 2010, Nano letters.

[41]  M. Raschke,et al.  Nano-optical imaging and spectroscopy of order, phases, and domains in complex solids , 2012 .

[42]  Xin Zhang,et al.  Terahertz-field-induced insulator-to-metal transition in vanadium dioxide metamaterial , 2012, Nature.

[43]  John B. Goodenough,et al.  The two components of the crystallographic transition in VO2 , 1971 .

[44]  Patrick Georges,et al.  Femtosecond laser excitation of the semiconductor‐metal phase transition in VO2 , 1994 .

[45]  F. J. Morin,et al.  Oxides Which Show a Metal-to-Insulator Transition at the Neel Temperature , 1959 .

[46]  L. Boeri,et al.  Optical properties of V 1 − x Cr x O 2 compounds under high pressure , 2008 .

[47]  Swanson,et al.  Femtosecond vibrational dynamics of self-trapping in a quasi-one-dimensional system , 2000, Physical review letters.

[48]  David H. Cobden,et al.  Measurement of a solid-state triple point at the metal–insulator transition in VO2 , 2013, Nature.

[49]  M. Veenendaal,et al.  Ultrafast photoinduced insulator-to-metal transitions in vanadium dioxide , 2013 .

[50]  Nevill Francis Mott,et al.  Metal-insulator transition in vanadium dioxide , 1975 .

[51]  Byung-Gyu Chae,et al.  Monoclinic and correlated metal phase in VO(2) as evidence of the Mott transition: coherent phonon analysis. , 2006, Physical review letters.

[52]  J. Eroms,et al.  A direct comparison of CVD-grown and exfoliated MoS2 using optical spectroscopy , 2013, 1310.8470.

[53]  R. F. Haglund,et al.  Ultrafast insulator-metal phase transition in VO 2 studied by multiterahertz spectroscopy , 2011, 1104.2984.

[54]  Allen,et al.  VO2: Peierls or Mott-Hubbard? A view from band theory. , 1994, Physical review letters.