Optical nonlinearities in solids reveal information about both the in-plane rotational and out-of-plane inversion symmetries of a crystal. In the van der Waals material hexagonal boron nitride (hBN) both these symmetries and the linear vibrational pr
operties have led to the rich physics of mid-infrared phonon-polaritons. However, the role of strong electron-phonon nonlinearities requires further study. In this work, we investigate both theoretically and experimentally the rich interplay of phonon anharmonicity and symmetry in phonon-polariton mediated nonlinear optics. We show that large enhancements (>30x) of third-harmonic generation occur for incident femtosecond pulses that are resonant with the hBN transverse optical phonons. In addition, we predict and observe large transient sub-picosecond duration second-harmonic signals during resonant excitation, which in equilibrium is forbidden by symmetry. This surprising result indicates that instantaneous crystal inversion symmetry breaking can be optically induced and controlled via phonon interactions by both the power and polarization of the pump laser.
Strong field-confinement, long-lifetime resonances, and slow-light effects suggest that meta surfaces are a promising tool for nonlinear optical applications. These nanostructured devices have been utilized for relatively high efficiency solid-state
high-harmonic generation platforms, four-wave mixing, and Raman scattering experiments, among others. Here we report the first all-dielectric metasurface to enhance harmonic generation from a surrounding gas, achieving as much as a factor of 45 increase in the overall yield for Argon atoms. When compared to metal nanostructures, dielectrics are more robust against damage for high power applications such as those using atomic gases. We employ dimerized high-contrast gratings fabricated in silicon-on-insulator that support bound states in the continuum, a resonance feature accessible in broken-symmetry planar devices. Our 1D gratings maintain large mode volumes, overcoming one of the more severe limitations of earlier device designs and greatly contributing to enhanced third- and fifth- harmonic generation. The interaction lengths that can be achieved are also significantly greater than the 10s of nm to which earlier solid-state designs were restricted. We perform finite-difference time-domain simulations to fully characterize the wavelength, linewidth, mode profile, and polarization dependence of the resonances. Our experiments confirm these predictions and are consistent with other nonlinear optical properties. The tunable wavelength dependence and quality-factor control we demonstrate in these devices make them an attractive tool for the next generation of high-harmonic sources, which are anticipated to be pumped at longer wavelengths and with lower peak power, higher repetition rate lasers.
Solids with topologically robust electronic states exhibit unusual electronic and optical transport properties that do not exist in other materials. A particularly interesting example is chiral charge pumping, the so-called chiral anomaly, in recentl
y discovered topological Weyl semimetals, where simultaneous application of parallel DC electric and magnetic fields creates an imbalance in the number of carriers of opposite topological charge (chirality). Here, using time-resolved terahertz measurements on the Weyl semimetal TaAs in a magnetic field, we optically interrogate the chiral anomaly by dynamically pumping the chiral charges and monitoring their subsequent relaxation. Theory based on Boltzmann transport shows that the observed effects originate from an optical nonlinearity in the chiral charge pumping process. Our measurements reveal that the chiral population relaxation time is much greater than 1 ns. The observation of terahertz-controlled chiral carriers with long coherence times and topological protection suggests the application of Weyl semimetals for quantum optoelectronic technology.
Hot electron effects in graphene are significant because of graphenes small electronic heat capacity and weak electron-phonon coupling, yet the dynamics and cooling mechanisms of hot electrons in graphene are not completely understood. We describe a
novel photocurrent spectroscopy method that uses the mixing of continuous-wave lasers in a graphene photothermal detector to measure the frequency dependence and nonlinearity of hot-electron cooling in graphene as a function of the carrier concentration and temperature. The method offers unparalleled sensitivity to the nonlinearity, and probes the ultrafast cooling of hot carriers with an optical fluence that is orders of magnitude smaller than in conventional time-domain methods, allowing for accurate characterization of electron-phonon cooling near charge neutrality. Our measurements reveal that near the charge neutral-point the nonlinear power dependence of the electron cooling is dominated by disorder-assisted collisions, while at higher carrier concentrations conventional momentum-conserving cooling prevails in the nonlinear dependence. The relative contribution of these competing mechanisms can be electrostatically tuned through the application of a gate voltage -- an effect that is unique to graphene.
