Minah Seo

Ultrafast Phase Transition via Catastrophic Phonon Collapse Driven by Plasmonic Hot-Electron Injection

Ultrafast photoinduced phase transitions could revolutionize data-storage and telecommunications technologies by modulating signals in integrated nanocircuits at terahertz speeds. In quantum phase-changing materials (PCMs), microscopic charge, lattice, and orbital degrees of freedom interact cooperatively to modify macroscopic electrical and optical properties. Although these interactions are well documented for bulk single crystals and thin films, little is known about the ultrafast dynamics of nanostructured PCMs when interfaced to another class of materials as in this case to active plasmonic elements. Here, we demonstrate how a mesh of gold nanoparticles, acting as a plasmonic photocathode, induces an ultrafast phase transition in nanostructured vanadium dioxide (VO2) when illuminated by a spectrally resonant femtosecond laser pulse. Hot electrons created by optical excitation of the surface-plasmon resonance in the gold nanomesh are injected ballistically across the Au/VO2 interface to induce a subpicosecond phase transformation in VO2. Density functional calculations show that a critical density of injected electrons leads to a catastrophic collapse of the 6 THz phonon mode, which has been linked in different experiments to VO2 phase transition. The demonstration of subpicosecond phase transformations that are triggered by optically induced electron injection opens the possibility of designing hybrid nanostructures with unique nonequilibrium properties as a critical step for all-optical nanophotonic devices with optimizable switching thresholds.

Highly sensitive and selective sugar detection by terahertz nano-antennas.

Molecular recognition and discrimination of carbohydrates are important because carbohydrates perform essential roles in most living organisms for energy metabolism and cell-to-cell communication. Nevertheless, it is difficult to identify or distinguish various carbohydrate molecules owing to the lack of a significant distinction in the physical or chemical characteristics. Although there has been considerable effort to develop a sensing platform for individual carbohydrates selectively using chemical receptors or an ensemble array, their detection and discrimination limits have been as high in the millimolar concentration range. Here we show a highly sensitive and selective detection method for the discrimination of carbohydrate molecules using nano-slot-antenna array-based sensing chips which operate in the terahertz (THz) frequency range (0.5–2.5 THz). This THz metamaterial sensing tool recognizes various types of carbohydrate molecules over a wide range of molecular concentrations. Strongly localized and enhanced terahertz transmission by nano-antennas can effectively increase the molecular absorption cross sections, thereby enabling the detection of these molecules even at low concentrations. We verified the performance of nano-antenna sensing chip by both THz spectra and images of transmittance. Screening and identification of various carbohydrates can be applied to test even real market beverages with a high sensitivity and selectivity.

Mapping carrier diffusion in single silicon core-shell nanowires with ultrafast optical microscopy.

Recent success in the fabrication of axial and radial core-shell heterostructures, composed of one or more layers with different properties, on semiconductor nanowires (NWs) has enabled greater control of NW-based device operation for various applications. (1-3) However, further progress toward significant performance enhancements in a given application is hindered by the limited knowledge of carrier dynamics in these structures. In particular, the strong influence of interfaces between different layers in NWs on transport makes it especially important to understand carrier dynamics in these quasi-one-dimensional systems. Here, we use ultrafast optical microscopy (4) to directly examine carrier relaxation and diffusion in single silicon core-only and Si/SiO(2) core-shell NWs with high temporal and spatial resolution in a noncontact manner. This enables us to reveal strong coherent phonon oscillations and experimentally map electron and hole diffusion currents in individual semiconductor NWs for the first time.

Understanding ultrafast carrier dynamics in single quasi-one-dimensional Si nanowires

We use femtosecond optical pump-probe spectroscopy to study ultrafast carrier dynamics in single quasi-one-dimensional silicon nanowires. By isolating individual nanowires, we avoid complications resulting from the broad size and alignment distribution in nanowire ensembles, allowing us to directly probe ultrafast carrier dynamics. Spatially-resolved experiments demonstrate the influence of surface-mediated mechanisms on carrier dynamics in a single NW, while polarization-resolved experiments reveal a clear anisotropy in carrier lifetimes measured parallel and perpendicular to the long axis of the NW, due to density-dependent Auger recombination. These results suggest the possibility of tailoring carrier relaxation in a single nanowire for a desired application.

Metallic MXene Saturable Absorber for Femtosecond Mode-Locked Lasers

2D transition metal carbides, nitrides, and carbonitides called MXenes have attracted much attention due to their outstanding properties. However, MXenes potential in laser technology is not explored. It is demonstrated here that Ti3 CN, one of MXene compounds, can serve as an excellent mode-locker that can produce femtosecond laser pulses from fiber cavities. Stable laser pulses with a duration as short as 660 fs are readily obtained at a repetition rate of 15.4 MHz and a wavelength of 1557 nm. Density functional theory calculations show that Ti3 CN is metallic, in contrast to other 2D saturable absorber materials reported so far to be operative for mode-locking. 2D structural and electronic characteristics are well conserved in their stacked form, possibly due to the unique interlayer coupling formed by MXene surface termination groups. Noticeably, the calculations suggest a promise of MXenes in broadband saturable absorber applications due to metallic characteristics, which agrees well with the experiments of passively Q-switched lasers using Ti3 CN at wavelengths of 1558 and 1875 nm. This study provides a valuable strategy and intuition for the development of nanomaterial-based saturable absorbers opening new avenues toward advanced photonic devices based on MXenes.

Ultrafast Optical Microscopy of Single Monolayer Molybdenum Disulfide Flakes

We use ultrafast optical microscopy to investigate carrier dynamics in single flakes of atomically thin molybdenum disulfide. By tuning the probe wavelength through the bandgap, we reveal the influence of layer thickness on carrier dynamics.

Ultrafast optical wide field microscopy

An ultrafast optical microscope capable of rapidly and sensitively acquiring wide field optical images with sub-100 femtosecond temporal resolution and micrometer spatial resolution is demonstrated for the first time.

Ultrasensitive Detection of Residual Pesticides Using THz Near-Field Enhancement

We present a novel type of highly sensitive and selective detection method for residual pesticide molecules including, e.g., methomyl using nanoscale metamaterials based terahertz (THz) time-domain spectroscopy (TDS) system. Nanoscale slot-antenna-based metamaterials were designed for the strong THz resonance at a certain frequency, where the specific molecule has intramolecular or intermolecular collective vibrational mode. Enhanced THz near-field via a nano-antenna metamaterial strongly increases absorption cross section, and this leads to the detection sensitivity up to parts-per-billion level even in a solution state of pesticide sample. Measured transmittance and reflectance spectrum results show excellent performances in both sensitivity and selectivity. We also imaged reflected THz signals though our THz nano-metamaterials in a nondestructive manner to simply detect the contained residual pesticide at the surface of an apple as it is, without any treatment. This observation can offer the possibility for further various applications as prompt and accurate molecule sensing tools in real time.

Observation of terahertz-radiation-induced ionization in a single nano island

Terahertz (THz) electromagnetic wave has been widely used as a spectroscopic probe to detect the collective vibrational mode in vast molecular systems and investigate dielectric properties of various materials. Recent technological advances in generating intense THz radiation and the emergence of THz plasmonics operating with nanoscale structures have opened up new pathways toward THz applications. Here, we present a new opportunity in engineering the state of matter at the atomic scale using THz wave and a metallic nanostructure. We show that a medium strength THz radiation of 22 kV/cm can induce ionization of ambient carbon atoms through interaction with a metallic nanostructure. The prepared structure, made of a nano slot antenna and a nano island located at the center, acts as a nanogap capacitor and enhances the local electric field by two orders of magnitudes thereby causing the ionization of ambient carbon atoms. Ionization and accumulation of carbon atoms are also observed through the change of the resonant condition of the nano slot antenna and the shift of the characteristic mode in the spectrum of the transmitted THz waves.

Nano metamaterials for ultrasensitive Terahertz biosensing

As a candidate for a rapid detection of biomaterials, terahertz (THz) spectroscopy system can be considered with some advantage in non-destructive, label-free, and non-contact manner. Because protein-ligand binding energy is in the THz range, especially, most important conformational information in molecular interactions can be captured by THz electromagnetic wave. Based on the THz time-domain spectroscopy system, THz nano-metamaterial sensing chips were prepared for great enhancing of detection sensitivity. A metamaterial sensing chip was designed for increasing of absorption cross section of the target sample, related to the transmitted THz near field enhancement via the composition of metamaterial. The measured THz optical properties were then analyzed in terms of refractive index and absorption coefficient, and compared with simulation results. Also, virus quantification regarding various concentrations of the viruses was performed, showing a clear linearity. The proposed sensitive and selective THz detection method can provide abundant information of detected biomaterials to help deep understanding of fundamental optical characteristics of them, suggesting rapid diagnosis way especially useful for such dangerous and time-sensitive target biomaterials.