Ultrafast Nanoimaging of the Photoinduced Phase Transition Dynamics in VO2

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• 作者：Sven A. Dönges ; Omar Khatib ; Brian T. O’Callahan ; Joanna M. Atkin ; Jae Hyung Park ; David Cobden ; Markus B. Raschke
• 刊名：Nano Letters
• 出版年：2016
• 出版时间：May 11, 2016
• 年：2016
• 卷：16
• 期：5
• 页码：3029-3035
• 全文大小：490K
• 年卷期：0
• ISSN：1530-6992

文摘

Many phase transitions in correlated matter exhibit spatial inhomogeneities with expected yet unexplored effects on the associated ultrafast dynamics. Here we demonstrate the combination of ultrafast nondegenerate pump–probe spectroscopy with far from equilibrium excitation, and scattering scanning near-field optical microscopy (s-SNOM) for ultrafast nanoimaging. In a femtosecond near-field near-IR (NIR) pump and mid-IR (MIR) probe study, we investigate the photoinduced insulator-to-metal (IMT) transition in nominally homogeneous VO₂ microcrystals. With pump fluences as high as 5 mJ/cm², we can reach three distinct excitation regimes. We observe a spatial heterogeneity on ∼50–100 nm length scales in the fluence-dependent IMT dynamics ranging from <100 fs to ∼1 ps. These results suggest a high sensitivity of the IMT with respect to small local variations in strain, doping, or defects that are difficult to discern microscopically. We provide a perspective with the distinct requirements and considerations of ultrafast spatiotemporal nanoimaging of phase transitions in quantum materials.