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Register a new userCoherent Acoustic Perturbation of Second-Harmonic-Generation in NiO
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We investigate the structural and magnetic origins of the unusual ultrafast second-harmonicgeneration (SHG) response of femtosecond-laser-excited nickel oxide (NiO) previously attributed to oscillatory reorientation dynamics of the magnetic structure induced by d-d excitations. Using time-resolved x-ray diffraction from the (3/2 3/2 3/2) magnetic planes, we show that changes in the magnitude of the magnetic structure factor following ultrafast optical excitation are limited to $Delta<F_m>/<F_m>$ = 1.5% in the first 30 ps. An extended investigation of the ultrafast SHG response reveals a strong dependence on wavelength as well as characteristic echoes, both of which give evidence for an acoustic origin of the dynamics. We therefore propose an alternative mechanism for the SHG response based on perturbations of the nonlinear susceptibility via optically induced strain in a spatially confined medium. In this model, the two observed oscillation periods can be understood as the times required for an acoustic strain wave to traverse one coherence length of the SHG process in either the collinear or anti-collinear geometries.
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The valley degeneracy of electron states in graphene stimulates intensive research of valley-related optical and transport phenomena. While many proposals on how to manipulate valley states have been put forward, experimental access to the valley polarization in graphene is still a challenge. Here, we develop a theory of the second optical harmonic generation in graphene and show that this effect can be used to measure the degree and sign of the valley polarization. We show that, at the normal incidence of radiation, the second harmonic generation stems from imbalance of carrier populations in the valleys. The effect has a specific polarization dependence reflecting the trigonal symmetry of electron valley and is resonantly enhanced if the energy of incident photons is close to the Fermi energy.
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Inspired by concepts developed for fermionic systems in the framework of condensed matter physics, topology and topological states are recently being explored also in bosonic systems. The possibility of engineering systems with unidirectional wave propagation and protected against disorder is at the heart of this growing interest. Topogical acoustic effects have been observed in a variety of systems, most of them based on kHz-MHz sound waves, with typical wavelength of the order of the centimeter. Recently, some of these concepts have been successfully transferred to acoustic phonons in nanoscaled multilayered systems. The reported demonstration of confined topological phononic modes was based on Raman scattering spectroscopy, yet the resolution did not suffice to determine lifetimes and to identify other acoustic modes in the system. Here, we use time-resolved pump-probe measurements using an asynchronous optical sampling (ASOPS) technique to overcome these resolution limitations. By means of one-dimensional GaAs/AlAs distributed Bragg reflectors (DBRs) as building blocks, we engineer high frequency ($sim$ 200 GHz) topological acoustic interface states. We are able to clearly distinguish confined topological states from stationary band edge modes. The detection scheme reflects the symmetry of the modes directly through the selection rules, evidencing the topological nature of the measured confined state. These experiments enable a new tool in the study of the more complex topology-driven phonon dynamics such as phonon nonlinearities and optomechanical systems with simultaneous confinement of light and sound.
Valley polarization in graphene breaks inversion symmetry and therefore leads to second-harmonic generation. We present a complete theory of this effect within a single-particle approximation. It is shown that this may be a sensitive tool to measure the valley polarization created, e.g., by polarized light and, thus, can be used for a development of ultrafast valleytronics in graphene.
The two-dimensional ferroelectrics GeS, GeSe, SnS and SnSe are expected to have large spontaneous in-plane electric polarization and enhanced shift-current response. Using density functional methods, we show that these materials also exhibit the largest effective second harmonic generation reported so far. It can reach magnitudes up to $10$ nm/V which is about an order of magnitude larger than that of prototypical GaAs. To rationalize this result we model the optical response with a simple one-dimensional two-band model along the spontaneous polarization direction. Within this model the second-harmonic generation tensor is proportional to the shift-current response tensor. The large shift current and second harmonic responses of GeS, GeSe, SnS and SnSe make them promising non-linear materials for optoelectronic applications.
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