Journal
NANO LETTERS
Volume 21, Issue 21, Pages 9052-9060Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c02638
Keywords
Quantum Materials; Ultrafast Nanospectroscopy; Vanadium Dioxide; s-SNOM; Phase Transition; Nucleation and Growth
Categories
Funding
- Center on Precision-Assembled Quantum Materials through US National Science Foundation (NSF) Materials Research Science and Engineering Centers [DMR-2011738]
- NSF EFMA [1741660]
- DARPA DRINQS Program [D18AC00014]
- Institute of Information & Communications Technology Planning & Evaluation (IITP) grant - Korean government (MSIT) on MIT [2017-0-00830]
- ARO MURI Grant [W911NF-16-1-0361]
- National Science Foundation [DMR-1904576]
- Emerging Frontiers & Multidisciplinary Activities
- Directorate For Engineering [1741660] Funding Source: National Science Foundation
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Transient nanotextured heterogeneity in vanadium dioxide (VO2) thin films during a light-induced insulator-to-metal transition (IMT) was investigated, revealing hidden disorder and inequivalent twin domain structures. Coexisting metallic and insulating regions were observed during the IMT, anchored to twin domain interfaces and grain boundaries. Photoinduced nucleation was deterministically anchored to predefined nanoscopic regions, allowing monitoring of emergent metallicity in space and time.
We investigate transient nanotextured heterogeneity in vanadium dioxide (VO2) thin films during a light-induced insulator-to-metal transition (IMT). Timeresolved scanning near-field optical microscopy (Tr-SNOM) is used to study VO2 across a wide parameter space of infrared frequencies, picosecond time scales, and elevated steady-state temperatures with nanoscale spatial resolution. Room temperature, steady-state, phonon enhanced nano-optical contrast reveals preexisting hidden disorder. The observed contrast is associated with inequivalent twin domain structures. Upon thermal or optical initiation of the IMT, coexisting metallic and insulating regions are observed. Correlations between the transient and steady-state nano-optical textures reveal that heterogeneous nucleation is partially anchored to twin domain interfaces and grain boundaries. Ultrafast nanoscopic dynamics enable quantification of the growth rate and bound the nucleation rate. Finally, we deterministically anchor photoinduced nucleation to predefined nanoscopic regions by locally enhancing the electric field of pump radiation using nanoantennas and monitor the on-demand emergent metallicity in space and time.
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