VO2 Films Decorated with an MXene Interface for Decreased-Power-Triggered Terahertz Modulation.

VO2, which exhibits semiconductor-metal phase transition characteristics occurring on a picosecond time scale, holds great promise for ultrafast terahertz modulation in next-generation communication. However, as of now, there is no reported prototype for an ultrafast device. The temperature effect has been proposed as one of the major obstacles. Consequently, reducing the excitation threshold for the phase transition would be highly significant. The traditional strategy typically involves chemical doping, but this approach often leads to a decrease in phase transition amplitude and a slower transition speed. In this work, we proposed a design featuring a highly conductive MXene interfacial layer between the VO2 film and the substrate. We demonstrate a significant reduction in the phase transition threshold for both temperature and laser-induced phase transition by adjusting the conductivity of the MXene layers with varying thicknesses. Our observations show that the phase transition temperature can be decreased by 9 °C, while the pump fluence for laser excitation can be reduced by as high as 36%. The ultrafast phase transition process on a picosecond scale, as revealed by the optical-pump terahertz-probe method, suggests that the MXene layers have minimal impact on the phase transition speed. Moreover, the reduced phase transition threshold can remarkably alleviate the photothermal effect and inhibit temperature rise and diffusion in VO2 triggered by laser. This study offers a blueprint for designing VO2/MXene hybrid films with reduced phase transition thresholds. It holds significant potential for the development of low-power, intelligent optical and electrical devices including, but not limited to, terahertz modulators based on phase transition phenomena.

Mesoporous black TiO2 hollow shells with controlled cavity size for enhanced visible light photocatalysis.

Black TiO2 formed by introducing lattice disorder into pristine TiO2 has a narrowed band gap and suppresses the recombination of charge carriers. This provides a potential strategy for visible light photocatalysis. However, the microstructural design of black TiO2 for a higher optimization of visible light is still in high demand. In this work, we proposed the preparation of black TiO2 hollow shells with controllable cavity diameters using silica spheres as templates for the cavities and the NaBH4 reduction method. The decreased cavity size resulted in a hollow shell with an enhanced visible-light absorption and improved photocatalytic performance. Moreover, we demonstrated that this cavity can be combined with gold nanoparticles (AuNPs) to form AuNPs@black TiO2 yolk-shells. The AuNPs provided additional visible light absorption and promoted the separation of photogenerated carriers in the yolk-shell structures. This further improved the photocatalysis, the degradation rate of Cr(VI) can reach 0.066 min-1. Our work evaluated the effect of the cavity size on the photocatalytic performance of hollow and yolk-shell structures and provided concepts for the further enhancement of visible-light photocatalysis.

Impact of the uniaxial strain on terahertz modulation characteristics in flexible epitaxial VO2 film across the phase transition.

Exploring flexible electronics is on the verge of innovative breakthroughs in terahertz (THz) communication technology. Vanadium dioxide (VO2) with insulator-metal transition (IMT) has excellent application potential in various THz smart devices, but the associated THz modulation properties in the flexible state have rarely been reported. Herein, we deposited an epitaxial VO2 film on a flexible mica substrate via pulsed-laser deposition and investigated its THz modulation properties under different uniaxial strains across the phase transition. It was observed that the THz modulation depth increases under compressive strain and decreases under tensile strain. Moreover, the phase-transition threshold depends on the uniaxial strain. Particularly, the rate of the phase transition temperature depends on the uniaxial strain and reaches approximately 6 °C/% in the temperature-induced phase transition. The optical trigger threshold in laser-induced phase transition decreased by 38.9% under compressive strain but increased by 36.7% under tensile strain, compared to the initial state without uniaxial strain. These findings demonstrate the uniaxial strain-induced low-power triggered THz modulation and provide new insights for applying phase transition oxide films in THz flexible electronics.

Thermal and mechanical THz modulation of flexible all-dielectric metamaterial.

The implementation of Terahertz (THz) modulation is critical for applications in high-speed wireless communications, security screening and so on. Therefore, it is particularly significant to obtain THz wave modulation devices with stable and flexible performance, easy manipulation of the modulation method, and multi-functionality. Here, we propose a flexible all-dielectric metamaterial by embedding zirconia (ZrO2) microspheres into a vanadium dioxide/polydimethylsiloxane (VO2/PDMS) composite, which can achieve thermal and mechanical tuning of THz wave transmission. When the temperature of the ZrO2/VO2/PDMS metamaterial increases, VO2 changes from the insulating phase to the metallic phase, and the 1st (at 0.304 THz) and 2nd (at 0.414 THz) order magnetic resonances exhibit the tunability of 20 GHz and 15 GHz, respectively. When stretched, the 1st and 2nd order magnetic resonances show the tunability of 12 GHz and 10 GHz, respectively. In the meantime, there are accompanying changes in transmittance at the resonances. The ZrO2/VO2/PDMS all-dielectric metamaterial presented in this work provides an alternative strategy for developing actively tunable, flexible, and versatile THz devices. In addition, it has the merits of simple preparation and low cost, promising large-area and rapid preparation of meta-arrays.

Volatile and Nonvolatile Switching of Phase Change Material Ge2Sb2Te5 Revealed by Time-Resolved Terahertz Spectroscopy.

Phase change materials exhibit unique advantages in reconfigurable photonic devices due to drastic tunability of photoelectric properties. Here, we systematically investigate the thermal equilibrium process and the ultrafast dynamics of Ge2Sb2Te5 (GST) driven by femtosecond (fs) pulses, using time-resolved terahertz spectroscopy. Both fs-pulse-driven crystallization and amorphization are demonstrated, and the threshold of photoinduced crystallization (amorphization) is determined to be 8.4 mJ/cm2 (10.1 mJ/cm2). The ultrafast carrier dynamics reveal that the cumulative photothermal effect plays a crucial role in the ultrafast crystallization, and modulation depth of volatile (nonvolatile) THz has switching limits up to 30% (15%). A distinctive phonon absorption at 1.1 THz is observed, providing fingerprint spectrum evidence of crystalline lattice formation driven by intense fs pulses. Finally, multistate volatile (nonvolatile) THz switching is implemented by tuning optical pump fluence. These results provide insight into the photoinduced phase change of GST and offer benefits for all optical THz functional devices.

Active control of terahertz waves based on p-Si hybrid PIT metasurface device under avalanche breakdown.

Active control of terahertz waves is a critical application for terahertz devices. Silicon is widely used in large-scale integrated circuit and optoelectronic devices, and also shows great potential in the terahertz field. In this paper, a p-Si hybrid metasurface device is proposed and its terahertz characteristics under avalanche breakdown effect is investigated. In the study, a plasmon-induced transparency (PIT) effect caused by the near-field coupling of the bright mode and the dark mode is observed in the transmission spectrum. Due to avalanche breakdown effect, the resonance of the PIT metamaterial disappears as the current increased. Carriers existed in the interface between the metasurface and substrate result to a dipole resonance suppression. When the current continues increasing, the maximal modulation depth can reach up to 99.9%, caused by the avalanche effect of p-Si. Experimental results demonstrate that the avalanche breakdown p-Si can achieve a performance modulation depth, bringing much more possibilities for terahertz devices.

Ghost spintronic THz-emitter-array microscope.

Terahertz (THz) waves show great potential in nondestructive testing, biodetection and cancer imaging. Despite recent progress in THz wave near-field probes/apertures enabling raster scanning of an object's surface, an efficient, nonscanning, noninvasive, deep subdiffraction imaging technique remains challenging. Here, we demonstrate THz near-field microscopy using a reconfigurable spintronic THz emitter array (STEA) based on the computational ghost imaging principle. By illuminating an object with the reconfigurable STEA followed by computing the correlation, we can reconstruct an image of the object with deep subdiffraction resolution. By applying an external magnetic field, in-line polarization rotation of the THz wave is realized, making the fused image contrast polarization-free. Time-of-flight (TOF) measurements of coherent THz pulses further enable objects at different distances or depths to be resolved. The demonstrated ghost spintronic THz-emitter-array microscope (GHOSTEAM) is a radically novel imaging tool for THz near-field imaging, opening paradigm-shifting opportunities for nonintrusive label-free bioimaging in a broadband frequency range from 0.1 to 30 THz (namely, 3.3-1000 cm-1).

Enhancing terahertz molecular fingerprint detection by a dielectric metagrating.

Terahertz (THz) sensing of molecular fingerprint enables wide applications in biomedicine and security detection. Conventional detection approaches face big barriers in trace analysis of analyte due to the difficulties of enhancing the broadband molecular absorption. In order to achieve strong broadband wave-matter interaction for the analyte, we propose a method based on THz wave angular scanning on a dielectric metagrating. In virtue of the guided-mode resonance, one can strengthen the local electric field in various trace-amount analytes by tuning the polarization and incident angle, which leads to significant enhancement on the broadband signal of molecular fingerprint. The study paves the way for more applications of THz trace-amount detection.

Ultrasensitive specific sensor based on all-dielectric metasurfaces in the terahertz range.

An ultrasensitive specific sensor based on all-dielectric metasurfaces in the terahertz range was proposed. The designed metasurfaces consist of multi pairs of tilted silicon bars on a SiO2 substrate with a high-Q Fano resonance feature. The peak of this high Q Fano resonance can form a wide reflection spectrum band by scanning the angle of the incident THz waves. Utilizing this angle-scanning strategy, we designed a metasurface sensor and its reflection spectrum band can cover the absorption peak of tyrosine and santonin. By depositing different thicknesses of tyrosine and santonin on the sensor, we have successfully identified them with a detection limit of 6.7 µg cm-2 and 59.35 µg cm-2, respectively. The performance of the sensor with high sensitivity has been analyzed in detail, showing an exciting prospect for identification of 'fingerprint' spectra in the terahertz region.

Giant dual-mode graphene-based terahertz modulator enabled by Fabry-Perot assisted multiple reflection.

We report a high-performance terahertz (THz) modulator with dual operation mode. For the pulse operation mode, the proposed THz modulator has the advantage of high modulation depth (MD) and can operate in a broadband frequency range. We have experimentally achieved a MD larger than 90% for the fifth-order pulse THz echo at 0.8 THz, and the MD stays larger than 75% in a broadband frequency range larger than 1 THz, whereas, for the coherent operation mode, the Fabry-Perot (F-P) interference effect has been taken into consideration and a MD larger than 75% at 0.76 THz has also been realized.

Terahertz wave near-field compressive imaging with a spatial resolution of over λ/100.

We demonstrate terahertz (THz) wave near-field imaging with a spatial resolution of ∼4.5 µm using single-pixel compressive sensing enabled by femtosecond-laser (fs-laser) driven vanadium dioxide (VO2)-based spatial light modulator. By fs-laser patterning a 180 nm thick VO2 nanofilm with a digital micromirror device, we spatially encode the near-field THz evanescent waves. With single-pixel Hadamard detection of the evanescent waves, we reconstructed the THz wave near-field image of an object from a serial of encoded sequential measurements, yielding improved signal-to-noise ratio by one order of magnitude over a raster-scanning technique. Further, we demonstrate that the acquisition time was compressed by a factor of over four with 90% fidelity using a total variation minimization algorithm. The proposed THz wave near-field imaging technique inspires new and challenging applications such as cellular imaging.

Giant impact of self-photothermal on light-induced ultrafast insulator-to-metal transition in VO2 nanofilms at terahertz frequency.

Ultrafast detection and switching of light are key processes in high-speed optoelectronic devices. However, the performances of VO2-based optoelectronics are strongly degraded by photothermal. The mechanism of the latter is still unclear. Here, by using femtosecond-laser (fs-laser) driven kinetic terahertz wave absorption, we quantitatively separate slow photothermal response and ultrafast photodoping response (e.g. light-induced insulator-to-metal transition) from second- to picosecond-timescales, and discover the competing interplay between them. With self-photothermal (mainly determined by fs-laser pulse repetition rate and pump fluence), the ultrafast transition time was degraded by 190% from 50 ps to 95 ps, the ultrafast transition threshold was decreased to 82% from 11mJ/cm2 to 9mJ/cm2, while the amplitudes of the two photoresponse are competing. Percolation theory, along with the macroscopic conductivity response, is used to explain the competing interplay. Our findings are relevant for designing and optimizing VO2-based ultrafast optoelectronic devices.

Sub-wavelength tight-focusing of terahertz waves by polarization-independent high-numerical-aperture dielectric metalens.

A focusing device is one of the key elements for terahertz applications, including homeland security, medicine, industrial inspection, and other fields. Sub-wavelength tight-focusing of terahertz waves is attractive for microscopy and spectroscopy. Flat optical lenses based on metasurfaces have shown potential in diffraction-limit focusing and advantages of ultrathin thickness and lightweight for large-aperture optics. However previously reported THz metalenses suffered from either polarization-dependency or small numerical aperture (NA), which greatly limits their focusing performance. In this paper, to achieve high-NA and polarization-free operation, we proposed a polarization-independent dielectric metasurface with a sub-wavelength period of 0.4λ. A planar terahertz lens based on such metasurface was designed for a wavelength of λ = 118.8 µm with a focal length of 100λ, a radius of 300λ, and a high NA of 0.95, which was fabricated with a silicon-on-insulator wafer. The experimental results demonstrate a tight focal spot with sub-wavelength full widths at half-maxima of 0.45λ and 0.61λ in the x and y directions, respectively, on the focal plane. In the x direction, the size of 0.45λ is even smaller than the diffraction limit 0.526λ (0.5λ/NA). Such a metalens is favorable for sub-wavelength tight-focusing terahertz waves with different polarizations, due to its polarization independence. The metalens has potential applications in THz imaging, spectroscopy, information processing, and communications, among others.

Ultrasensitive specific terahertz sensor based on tunable plasmon induced transparency of a graphene micro-ribbon array structure.

We proposed an ultrasensitive specific terahertz sensor consisting of two sets of graphene micro-ribbon with different widths. The interference between the plasmon resonances of the wide and narrow graphene micro-ribbons gives rise to the plasmon induced transparency (PIT) effect and enables ultrasensitive sensing in terahertz region. The performances of the PIT sensor have been analyzed in detail considering the thickness and refractive index sensing applications using full wave electromagnetic simulations. Taking advantage of the electrical tunability of graphene's Fermi level, we demonstrated the specific sensing of benzoic acid with detection limit smaller than 6.35 µg/cm2. The combination of specific identification and enhanced sensitivity of the PIT sensor opens exciting prospects for bio/chemical molecules sensing in the terahertz region.

Realizing a terahertz far-field sub-diffraction optical needle with sub-wavelength concentric ring structure array.

The terahertz (THz) lens is an essential and strategic element of THz optical systems, while a conventional THz lens cannot even reach high resolution due to the diffraction limit. Optical super-oscillation paves a way to generate sub-diffraction hotspots in the far field, and demonstrates the capacity for resolution improvement of microscopic imaging in the visible range. However, there are few demonstrations of THz lenses for focusing hotspots or needles based on super-oscillation. We propose and experimentally demonstrate a far-field sub-diffraction focusing planar lens, consisting of a sub-wavelength concentric ring structure array, for a wavelength of 118.8 µm with focal length 420λ and radius 160λ. Utilizing the silicon-etching process, a sub-diffraction focusing lens is fabricated. The experimental results show that the planar lens can generate a sub-diffraction needle with length 19.7λ in the focal region along the optic axis. Moreover, the smallest focal spot, with a transverse size of 1.212λ, is smaller than the diffraction limit of 1.476λ. The proposed sub-diffraction optical needle planar lens can substitute for its traditional counterpart, and it has great potential in super-resolution tomography THz imaging systems.

All-dielectric metalens for terahertz wave imaging.

Terahertz wave imaging offers promising properties for non-destructive testing applications in the areas of homeland security, medicine, and industrial inspection. However, conventional optical lenses are heavy and bulky and difficult to integrate. An all-dielectric metasurface provides an attractive way to realize a planar lens of light weight that is ultrathin and offers ease of integration. Terahertz lenses based on various metasurfaces have been studied, especially for the application of wave focusing, while there are few experimental demonstrations of terahertz wave imaging lenses based on an all-dielectric metasurface. In the present work, we propose a metalens based on an all-dielectric metasurface with a sub-wavelength unit size of 0.39λ for terahertz wave imaging and experimentally demonstrate its performance in focusing and imaging. A large numerical aperture metalens was fabricated with a focal length of 300λ, radius of 300λ, and numerical aperture of 0.707. The experimental results show that the lens can focus THz waves with an incident angle up to 48°. More importantly, clear terahertz wave images of different objects were obtained for both different cases of forward- and inverse-incident directions, which demonstrate the reversibility of the metalens for imaging. Such a metalens provides a way for realization of all-planar-lens THz imaging system, and might find application in terahertz wave imaging, information processing, microscopy, and others.

Label-free monitoring of cell death induced by oxidative stress in living human cells using terahertz ATR spectroscopy.

We demonstrated that attenuated total reflectance terahertz time-domain spectroscopy (ATR THz-TDS) is able to monitor oxidative stress response of living human cells, which is proven in this work that it is an efficient non-invasive, label-free, real-time and in situ monitoring of cell death. Furthermore, the dielectric constant and dielectric loss of cultured living human breast epithelial cells, and along with their evolution under oxidative stress response induced by high concentration of H2O2, were quantitatively determined in the work. Our observation and results were finally confirmed using standard fluorescence-labeled flow cytometry measurements and visible fluorescence imaging.

Dual-mode tunable terahertz generation in lithium niobate driven by spatially shaped femtosecond laser.

A new approach for dual-mode (namely broadband mode and narrowband mode) terahertz (THz) pulses generation in a single lithium niobate (LN) crystal excited by spatially shaped tilted-pulse-front femtosecond (fs) laser pulse was proposed and experimentally demonstrated. The two THz emission modes are generated simultaneously while spatially separated. Both central frequency and bandwidth of narrowband THz emission is controllable by in situ tuning the spatial modulation period and beam size of the fs-laser, and the broadband (0.1-1.5 THz) THz emission keeps almost unchanged while tuning the narrowband emission. Further optimization achieves the narrowband THz emission with energy spectral density up to 0.27 µJ/THz and with bandwidth narrowly down to 23 GHz. Such dual-mode THz source is useful for nonlinear THz optics, such as selected resonant THz excitation with broadband THz probe spectroscopy of crystalline matters.

Terahertz Spectroscopic Diagnosis of Myelin Deficit Brain in Mice and Rhesus Monkey with Chemometric Techniques.

While myelin deficit of the central nervous system leads to several severe diseases, the definitive diagnostic means are lacking. We proposed and performed terahertz time-domain spectroscopy (THz-TDS) combined with chemometric techniques to discriminate and evaluate the severity of myelin deficit in mouse and rhesus monkey brains. The THz refractive index and absorption coefficient of paraffin-embedded brain tissues from both normal and mutant dysmyelinating mice are shown. Principal component analysis of time-domain THz signal (PCA-tdTHz) and absorption-refractive index relation of THz spectrum identified myelin deficit without exogenous labeling or any pretreatment. Further, with the established PCA-tdTHz, we evaluated the severity of myelin deficit lesions in rhesus monkey brain induced by experimental autoimmune encephalomyelitis, which is the most-studied animal model of multiple sclerosis. The results well matched the pathological analysis, indicating that PCA-tdTHz is a quick, powerful, evolving tool for identification and evaluation myelin deficit in preclinical animals and potentially in para-clinical human biopsy.

Optimization of terahertz generation from LiNbO3 under intense laser excitation with the effect of three-photon absorption.

We proposed a three-dimensional model to simulate terahertz generation from LiNbO3 crystal under intense laser excition (up to ~50 mJ/cm2). The impact of three-photon absorption, which leads to free carrier generation and free carrier saturation (when pump fluence above ~10 mJ/cm2) on terahertz generation was investigated. And further with this model, we stated the optimized experimental conditions (incident postion, beam diameter, and pulse duration, etc) for maximum generation efficiency in commonly-used tilted-pulse-front scheme. Red shift of spectrum, spatial distribution "splitting" effects of emitted THz beam, and primilary experimental verification under intense laser excitation are given.