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.

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.

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.

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.

Generation of 0.19-mJ THz pulses in LiNbO3 driven by 800-nm femtosecond laser.

A cylindrical lens telescope tilted-pulse-front pumping scheme was proposed for high energy terahertz (THz) pulse generation. This scheme allows higher pump energy to be used with lower saturation effects under high pump fluence, and higher THz generation efficiency was achieved within large range of pump energy. The optimum pump pulse duration and crystal cooling temperature for THz generation in LiNbO3 (LN) crystal were also researched systematically. Excited by 800-nm laser, up to 0.19 mJ THz pulse energy and 0.27% conversion efficiency was demonstrated under 800-nm 400-fs laser excitation with ~100-mJ pulse energy and 150-K LN cooling temperature.

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.

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.

Silica-Coated Gold Nanorods with High Photothermal Efficiency and Biocompatibility as a Contrast Agent for In Vitro Terahertz Imaging.

The application of terahertz imaging in biomedical diagnostics is limited by the poor imaging contrast due to the strong absorption of terahertz waves by water molecules in the living body. To resolve this problem, gold nanorods (GNRs) have been considered as a possible contrast agent. However, the conventional preparation of GNRs requires using cetyltrimethylammonium bromide (CTAB) as a stabilizing surfactant, which is toxic to animals at high exposures. In this work, a modified seed-mediated growth method was proposed to synthesize silica-coated GNRs, which exhibited better stability and biocompatibility and the same cellular uptake efficiency as compared to those of uncoated GNRs. Moreover, silica-coated GNRs showed higher photothermal efficiency caused by the localized surface plasmon resonance that increased the terahertz reflection amplitude. In particular, the in vitro terahertz imaging of prostate cancer cells demonstrated noticeably higher contrast when silica-coated GNRs were used as a contrast agent. Hence, this study suggests a stable, biocompatible, and efficient contrast-enhancing agent for terahertz imaging, which can expand the scope of its clinical applications.

Time-resolved single-shot terahertz time-domain spectroscopy for ultrafast irreversible processes.

Pulsed terahertz spectroscopy is suitable for spectroscopic diagnostics of ultrafast events. However, the study of irreversible or single shot ultrafast events requires ability to record transient properties at multiple time delays, i.e., time resolved at single shot level, which is not available currently. Here by angular multiplexing use of femtosecond laser pulses, we developed and demonstrated a time resolved, transient terahertz time domain spectroscopy technique, where burst mode THz pulses were generated and then detected in a single shot measurement manner. The burst mode THz pulses contain 2 sub-THz pulses, and the time gap between them is adjustable up to 1 ns with picosecond accuracy, thus it can be used to probe the single shot event at two different time delays. The system can detect the sub-THz pulses at 0.1 THz-2.5 THz range with signal to noise ratio (SNR) of ∼400 and spectrum resolution of 0.05 THz. System design was described here, and optimizations of single shot measurement of THz pulses were discussed in detail. Methods to improve SNR were also discussed in detail. A system application was demonstrated where pulsed THz signals at different time delays of the ultrafast process were successfully acquired within single shot measurement. This time resolved transient terahertz time domain spectroscopy technique provides a new diagnostic tool for irreversible or single shot ultrafast events where dynamic information can be extracted at terahertz range within one-shot experiment.

Terahertz pulsed spectroscopy of paraffin-embedded brain glioma.

The refractive indices, absorption coefficients, and complex dielectric constants of paraffin-embedded brain glioma and normal brain tissues have been measured by a terahertz time-domain spectroscopy (THz-TDS) system in the 0.2- to 2.0-THz range. The spectral differences between gliomas and normal brain tissues were obtained. Compared with normal brain tissue, our results indicate that paraffin-embedded brain gliomas have a higher refractive index, absorption coefficient, and dielectric constant. Based on these results, the best THz frequencies for different methods of paraffin-embedded brain glioma imaging, such as intensity imaging, coherent imaging with continuum THz sources, and THz pulsed imaging with short-pulsed THz sources, are analyzed.