Single-cycle THz pulses with amplitudes exceeding 1 MV/cm generated by optical rectification in LiNbO3

Using the tilted-pulse-intensity-front scheme, we generate single-cycle terahertz (THz) pulses by optical rectification of femtosecond laser pulses in LiNbO3. In the THz generation setup, the condition that the image of the grating coincides with the tilted-optical-pulse front is fulfilled to obtain optimal THz beam characteristics and pump-to-THz conversion efficiency. The designed focusing geometry enables tight focus of the collimated THz beam with a spot size close to the diffraction limit, and the maximum THz electric field of 1.2 MV/cm is obtained

Nonlinear magnetization dynamics of antiferromagnetic spin resonance induced by intense terahertz magnetic field

We report on the nonlinear magnetization dynamics of a HoFeO3 crystal induced by a strong terahertz magnetic field resonantly enhanced with a split ring resonator and measured with magneto-optical Kerr effect microscopy. The terahertz magnetic field induces a large change (~40%) in the spontaneous magnetization. The frequency of the antiferromagnetic resonance decreases in proportion to the square of the magnetization change. A modified Landau-Lifshitz-Gilbert equation with a phenomenological nonlinear damping term quantitatively reproduced the nonlinear dynamics

High-order harmonic generation in graphene: Nonlinear coupling of intraband and interband transitions

We investigate high-order harmonic generation (HHG) in graphene with a quantum master equation approach. The simulations reproduce the observed enhancement in HHG in graphene under elliptically polarized light [N. Yoshikawa et al., Science 356, 736 (2017)]. On the basis of a microscopic decomposition of the emitted high-order harmonics, we find that the enhancement in HHG originates from an intricate nonlinear coupling between the intraband and interband transitions that are respectively induced by perpendicular electric field components of the elliptically polarized light. Furthermore, we reveal that contributions from different excitation channels destructively interfere with each other. This finding suggests a path to potentially enhance the HHG by blocking a part of the channels and canceling the destructive interference through band-gap or chemical potential manipulation

Sub-Cycle Optical Response Caused by Dressed State with Phase-Locked Wavefunctions

The coherent interaction of light with matter imprints the phase information of the light field on the wavefunction of the photon-dressed electronic state. Driving electric field, together with a stable phase that is associated with the optical probe pulses, enables the role of the dressed state in the optical response to be investigated. We observed optical absorption strengths modulated on a sub-cycle timescale in a GaAs quantum well in the presence of a multi-cycle terahertz driving pulse using a near-infrared probe pulse. The measurements were in good agreement with the analytical formula that accounts for the optical susceptibilities caused by the dressed state of excitons, which indicates that the output probe intensity was coherently reshaped by the excitonic sideband emissions

Size-controlled quantum dots reveal the impact of intraband transitions on high-order harmonic generation in solids

Since the discovery of high-order harmonic generation (HHG) in solids1,2,3, much effort has been devoted to understand its generation mechanism and both inter- and intraband transitions are known to be essential1,2,3,4,5,6,7,8,9,10. However, intraband transitions are affected by the electronic structure of a solid, and how they contribute to nonlinear carrier generation and HHG remains an open question. Here we use mid-infrared laser pulses to study HHG in CdSe and CdS quantum dots, where quantum confinement can be used to control the intraband transitions. We find that both HHG intensity per excited volume and generated carrier density increase when the average quantum dot size is increased from about 2 to 3 nm. We show that the reduction in sub-bandgap energy in larger quantum dots enhances intraband transitions, and this—in turn—increases the rate of photocarrier injection by coupling with interband transitions, resulting in enhanced HHG

Metamaterial-Enhanced Nonlinear Terahertz Spectroscopy

We demonstrate large nonlinear terahertz responses in the gaps of metamaterial split ring resonators in several materials and use nonlinear THz transmission and THz-pump/THz-probe spectroscopy to study the nonlinear responses and dynamics. We use the field enhancement in the SRR gaps to initiate high-field phenomena at lower incident fields. In vanadium dioxide, we drive the insulator-to-metal phase transition with high-field THz radiation. The film conductivity increases by over two orders of magnitude and the phase transition occurs on a several picosecond timescale. In gallium arsenide, we observe high-field transport phenomena, including mobility saturation and impact ionization. The carrier density increases by up to ten orders of magnitude at high fields. At the highest fields, we demonstrate THz-induced damage in both vanadium dioxide and gallium arsenide.United States. Dept. of Energy (DOE-BES, grant DE-FG02- 09ER46643)United States. Office of Naval Research (ONR Grant No. N00014-09-1-1103