Electron-electron interactions can render an otherwise conducting material insulating, with the insulator-metal phase transition in correlated-electron materials being the canonical macroscopic manifestation of the competition between charge-carrier itinerancy and localization. The transition can arise from underlying microscopic interactions among the charge, lattice, orbital and spin degrees of freedom, the complexity of which leads to multiple phase-transition pathways. For example, in many transition metal oxides, the insulator-metal transition has been achieved with external stimuli, including temperature, light, electric field, mechanical strain or magnetic field. Vanadium dioxide is particularly intriguing because both the lattice and on-site Coulomb repulsion contribute to the insulator-to-metal transition at 340 K (ref. 8). Thus, although the precise microscopic origin of the phase transition remains elusive, vanadium dioxide serves as a testbed for correlated-electron phase-transition dynamics. Here we report the observation of an insulator-metal transition in vanadium dioxide induced by a terahertz electric field. This is achieved using metamaterial-enhanced picosecond, high-field terahertz pulses to reduce the Coulomb-induced potential barrier for carrier transport. A nonlinear metamaterial response is observed through the phase transition, demonstrating that high-field terahertz pulses provide alternative pathways to induce collective electronic and structural rearrangements. The metamaterial resonators play a dual role, providing sub-wavelength field enhancement that locally drives the nonlinear response, and global sensitivity to the local changes, thereby enabling macroscopic observation of the dynamics. This methodology provides a powerful platform to investigate low-energy dynamics in condensed matter and, further, demonstrates that integration of metamaterials with complex matter is a viable pathway to realize functional nonlinear electromagnetic composites.
An array of passive metamaterial antennas fabricated on all protein-based silk substrates were conformally transferred and adhered to the surface of an apple. This process allows the opportunity for intimate contact of micro- and nanostructures that can probe, and accordingly monitor changes in, their surrounding environment. This provides in situ monitoring of food quality. It is to be noted that this type of sensor consists of all edible and biodegradable components, holding utility and potential relevance for healthcare and food/consumer products and markets.
IntroductionOver the past decade, optical near-field techniques, especially scattering-type scanning near-field optical microscopy Infrared and optical spectroscopy represents one of the most informative methods in advanced materials research. As an important branch of modern optical techniques that has blossomed in the past decade, scattering-type scanning near-field optical microscopy (s-SNOM) promises deterministic characterization of optical properties over a broad spectral range at the nanoscale. It allows ultrabroadband optical (0.5-3000 µm) nanoimaging, and nanospectroscopy with fine spatial (<10 nm), spectral (<1 cm −1 ), and temporal (<10 fs) resolution. The history of s-SNOM is briefly introduced and recent advances which broaden the horizons of this technique in novel material research are summarized. In particular, this includes the pioneering efforts to study the nanoscale electrodynamic properties of plasmonic metamaterials, strongly correlated quantum materials, and polaritonic systems at room or cryogenic temperatures. Technical details, theoretical modeling, and new experimental methods are also discussed extensively, aiming to identify clear technology trends and unsolved challenges in this exciting field of research. and Astronomy. His research interests cover nanoscale and ultrafast electromagnetic responses of strongly correlated electron materials, 2D materials, and metamaterials that span from the near-infrared to terahertz frequencies.tip-sample interactions. In s-SNOM, these difficulties result from at least three factors. First, the well-known antenna effect [48] causes light to be highly confined between the probe apex and the sample surface. The specific geometry of the tip shank plays a significant role in determining the intensity of the scattered signal. [49] Second, in addition to the local optical information, a strong but undesired background signal can be detected. This background signal can be mainly attributed to the light scattering from the tip shank, cantilever, and sample surface. Third, due to the broad momentum distribution of the localized radiation, in some cases, nominally "far-field trivial" Adv. Mater. 2019, 31, 1804774 Figure 1. Far-field (blue) and near-field (yellow) measurements, accessing the propagating field and the evanescent field, respectively.The authors declare no conflict of interest.
Measurements on graphene exfoliated over a substrate prepatterned with shallow depressions demonstrate that graphene does not remain free-standing but instead adheres to the substrate despite the induced biaxial strain. The strain is homogeneous over the depression bottom as determined by Raman measurements. We find higher Raman shifts and Gruneisen parameters of the phonons underlying the G and 2D bands under biaxial strain than previously reported. Interference modeling is used to determine the vertical position of the graphene and to calculate the optimum dielectric substrate stack for maximum Raman signal.
Pump-probe spectroscopy is central for exploring ultrafast dynamics of fundamental excitations, collective modes, and energy transfer processes. Typically carried out using conventional diffraction-limited optics, pump-probe experiments inherently average over local chemical, compositional, and electronic inhomogeneities. Here, we circumvent this deficiency and introduce pump-probe infrared spectroscopy with ∼ 20 nm spatial resolution, far below the diffraction limit, which is accomplished using a scattering scanning near-field optical microscope (s-SNOM). This technique allows us to investigate exfoliated graphene single-layers on SiO2 at technologically significant mid-infrared (MIR) frequencies where the local optical conductivity becomes experimentally accessible through the excitation of surface plasmons via the s-SNOM tip. Optical pumping at near-infrared (NIR) frequencies prompts distinct changes in the plasmonic behavior on 200 fs time scales. The origin of the pump-induced, enhanced plasmonic response is identified as an increase in the effective electron temperature up to several thousand Kelvin, as deduced directly from the Drude weight associated with the plasmonic resonances.
Active, widely tunable optical materials have enabled rapid advances in photonics and optoelectronics, especially in the emerging field of meta-devices. Here, we demonstrate that spatially selective defect engineering on the nanometer scale can transform phase-transition materials into optical metasurfaces. Using ion irradiation through nanometer-scale masks, we selectively defect-engineered the insulator-metal transition of vanadium dioxide, a prototypical correlated phase-transition material whose optical properties change dramatically depending on its state. Using this robust technique, we demonstrated several optical metasurfaces, including tunable absorbers with artificially induced phase coexistence and tunable polarizers based on thermally triggered dichroism. Spatially selective nanoscale defect engineering represents a new paradigm for active photonic structures and devices.
These results reveal that strain engineering can tune emergent functionality towards proximal macroscopic states to enable dynamic ultrafast optical phase switching and control.Precision tuning of the local environment in complex materials provides a route to control macroscopic functionality thereby offering a glimpse into how microscopic interactions conspire toward emergent behavior. Figure 1ashows resistivity measurements for a strained 30 nm LCMO film. In zero applied magnetic field, the film remains insulating at all temperatures (due to strain-enhanced orthorombicity 22 23 as depicted in Fig. 1d). For fields above 3 T the insulating phase collapses becoming a ferromagnetic metal at low temperatures. Figure 1b details the phase diagram of strained LCMO as determined from the field-dependent transport measurements 22 23 . The FM and AFM phases coexist over the range from 0-3 T, depending on temperature. To characterize the time-integrated electrodynamic response of the strained films, the optical conductivity was measured from 100 meV to 5 eV using spectroscopic ellipsometry (Fig. 1c). With decreasing temperature, the film displays spectral weight transfer from a small polaron (~1.5 eV) peak to a sharp well- Fig. 3a).As we now show, photoexcitation recovers the hidden FM phase of the strain- The photoinduced THz conductivity (PTC) is stable as long as the temperature is maintained. Further, the maximum conductivity is the same value as obtained with a strong magnetic field. This is clear from the blue dots of Fig. 1a, where the PTC from pulses, the resistivity continues to decrease by an additional order of magnitude, reaching a minimum after ~20 pulses. Figure 3b plots the photoinduced conductivity versus shot number for different fluences. The 4 mJ/cm 2 (same data as Fig. 3a) saturates at 800 Ω -1 cm -1 , while at lower fluences the conductivity saturates at a lower value. This is important, showing that the conductivity change does not simply arise from the absorbed number of photons. If there were a simple dependence on the number of absorbed photons, the data at lower fluences would saturate to the same conductivity value as the higher fluence data after a sufficient number of pulses. This is clearly not the case and indicates a cooperative process with a photon-absorption threshold. Figure 3c plots the conductivity plateaus from Measuring the conductivity dynamics of the pristine AFI state following singlepulse excitation would provide insight into the photoinduced IMT but is not experimentally feasible on a shot-to-shot basis. Instead, we employed an all-optical single-shot ultrafast spectroscopic method 28 which faithfully represents the conductivity dynamics because of the aforementioned spectral weight transfer. Figure 3d shows the results of single-shot photoinduced reflectivity dynamics (R/R) probing at the peak of the intersite transition (1.7 eV) following 1.55 eV excitation. There is a decrease in R/R consistent with dynamic spectral weight transfer to THz frequencies and the IMT dy...
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