Terahertz (THz) wave science and technology have found countless applications in biomedical imaging, security screening, and non-destructive testing as they approach maturity. However, due to the challenge of high ambient moisture absorption, the development of remote open-air broadband THz spectroscopy technology is lagging behind the compelling need that exists in homeland security, astronomy and environmental monitoring. Furthermore the underlying physical mechanisms behind the interaction between the THz wave and laser-induced plasma which responds strongly to electromagnetic waves, have not been fully understood.
This thesis aims to explain the light-plasma interaction at THz frequencies within a semiclassical framework along with experimental study of the femtosecond-laser-induced nitrogen plasma fluorescence under the illumination of sing-cycle THz pulses. The results indicate that THz radiation-enhanced-emission-of-fluorescence (REEF) is dominated by electron kinetics in the THz field and the electron-impact excitation of gas molecules/ions. The information of the time-dependent THz field can be recovered from the measured time-resolved THz-REEF from single-color laser induced plasma with the help of the bias as local oscillator. The calculations and experimental verification lead to a more complete understanding of the science behind these effects and push forward to extend their capabilities in related applications such as remote THz sensing, plasma diagnostics and ultrafast photoluminescence modulation.
Systematic studies in selected gases including neon, argon, krypton, xenon, methane (CH4), ethane (C2H6), propane (C3H8), and n-butane (C4H10) gases were performed to obtain an improved understanding of the THz-REEF. The dependences of the enhanced fluorescence on the THz field, laser excitation intensity, gas pressure, and intrinsic atomic properties were experimentally characterized. Both narrow line emission and broad continuum emission of the gas plasma are enhanced by the THz field. Their fluorescence enhancement ratios and time-resolved enhanced fluorescence are largely dependent on the scattering cross section and ionization potential of atoms.
For the first time, we demonstrate a novel ‘all-optical’ technique of broadband THz wave remote sensing by coherently manipulating the fluorescence emission from asymmetrically ionized gas plasma that interacts with THz waves. By studying the ultrafast electron dynamics under the single cycle THz radiation, we found that the fluorescence emission from laser-induced air plasma is highly dependent on the THz electric field and the symmetry of the electron drift velocity distribution created by two-color laser fields. The time-resolved THz-REEF can be tailored by switching the relative two-color phase and laser polarizations. Owing to the high atmospheric transparency and omni-directional emission pattern of fluorescence, this technique can be used to measure THz pulses at standoff distances with minimal water vapor absorption and unlimited directionality for optical signal collection. The coherent THz wave detection at a distance of 10 meter has been demonstrated. The combination of this method and previously demonstrated remote THz generation would eventually make remote THz spectroscopy available.
We also introduce a unique plasma diagnostic method utilizing the terahertz-wave-enhanced fluorescence emission from the excited atoms or molecules. The electron relaxation time and plasma density were deduced through applying the electron impact excitation/ionization and electron-ion recombination processes to the measured time-delay-dependent enhanced fluorescence. The electron collision dynamics of nitrogen plasma excited at different gas pressures and laser pulse energies have been systematically investigated. This plasma diagnostic method offers picosecond temporal resolution and is capable of omni-directional optical signal collection.
The ultrafast quenching dynamics of laser-pulse-induced photoluminescence in semiconductors under the radiation of single-cycle terahertz pulses has been studied. It is found that the quenching in both of cadmium telluride (CdTe) and gallium arsenide (GaAs) is linearly proportional to the intensity of incident terahertz waves and reaches up to 17% and 4% respectively at the peak intensity of 13 MW/cm2. The THz-wave-induced heating of the carriers and lattice and the subsequent decreased efficiency of photocarrier generation and recombination are most likely to be responsible for the quenching. This is potentially useful for the applications of a non-invasive ultrafast light modulator for photoluminescence devices with picoseconds switching time in the fields of the light-emitting devices and optical communication.