Nano-resonator integrated with two-dimensional materials (e.g. transition metal dichalcogenides) have recently emerged as a promising nano-optoelectronic platform. Here we demonstrate resonatorenhanced second-harmonic generation (SHG) in tungsten diselenide using a silicon photonic crystal cavity. By pumping the device with the ultrafast laser pulses near the cavity mode at the telecommunication wavelength, we observe a near visible SHG with a narrow linewidth and near unity linear polarization, originated from the coupling of the pump photon to the cavity mode. The observed SHG is enhanced by factor of ~200 compared to a bare monolayer on silicon. Our results imply the efficacy of cavity integrated monolayer materials for nonlinear optics and the potential of building a silicon-compatible second-order nonlinear integrated photonic platform.
We demonstrate enhanced second harmonic generation in a gallium phosphide photonic crystal waveguide with a measured external conversion efficiency of 5$times10^{-7}$/W. Our results are promising for frequency conversion of on-chip integrated emitters having broad spectra or large inhomogeneous broadening, as well as for frequency conversion of ultrashort pulses.
A hallmark of wave-matter duality is the emergence of quantum-interference phenomena when an electronic transition follows different trajectories. Such interference results in asymmetric absorption lines such as Fano resonances, and gives rise to secondary effects like electromagnetically induced transparency (EIT) when multiple optical transitions are pumped. Few solid-state systems show quantum interference and EIT, with quantum-well intersubband transitions in the IR offering the most promising avenue to date to devices exploiting optical gain without inversion. Quantum interference is usually hampered by inhomogeneous broadening of electronic transitions, making it challenging to achieve in solids at visible wavelengths and elevated temperatures. However, disorder effects can be mitigated by raising the oscillator strength of atom-like electronic transitions - excitons - which arise in monolayers of transition-metal dichalcogenides (TMDCs). Quantum interference, probed by second-harmonic generation (SHG), emerges in monolayer WSe2, without a cavity, splitting the SHG spectrum. The splitting exhibits spectral anticrossing behaviour, and is related to the number of Rabi flops the strongly driven system undergoes. The SHG power-law exponent deviates strongly from the canonical value of 2, showing a Fano-like wavelength dependence which is retained at room temperature. The work opens opportunities in solid-state quantum-nonlinear optics for optical mixing, gain without inversion and quantum-information processing.
Monolayer transition metal dichalcogenides, coupled to metal plasmonic nanocavities, have recently emerged as new platforms for strong light-matter interactions. These systems are expected to have nonlinear optical properties that will enable them to be used as entangled photon sources, compact wave-mixing devices, and other elements for classical and quantum photonic technologies. Here we report the first experimental investigation of the nonlinear properties of these strongly coupled systems, by observing second harmonic generation from a WSe2 monolayer strongly coupled to a single gold nanorod. The pump frequency dependence of the second harmonic signal displays a pronounced splitting that can be explained by a coupled oscillator model with second-order nonlinearities. Rigorous numerical simulations utilizing a nonperturbative nonlinear hydrodynamic model of conduction electrons support this interpretation and reproduce experimental results. Our study thus lays the groundwork for understanding the nonlinear properties of strongly coupled nanoscale systems.
We describe an approach based on topology optimization that enables automatic discovery of wavelength-scale photonic structures for achieving high-efficiency second-harmonic generation (SHG). A key distinction from previous formulation and designs that seek to maximize Purcell factors at individual frequencies is that our method not only aims to achieve frequency matching (across an entire octave) and large radiative lifetimes, but also optimizes the equally important nonlinear--coupling figure of merit $bar{beta}$, involving a complicated spatial overlap-integral between modes. We apply this method to the particular problem of optimizing micropost and grating-slab cavities (one-dimensional multilayered structures) and demonstrate that a variety of material platforms can support modes with the requisite frequencies, large lifetimes $Q > 10^4$, small modal volumes $sim (lambda/n)^3$, and extremely large $bar{beta} gtrsim 10^{-2}$, leading to orders of magnitude enhancements in SHG efficiency compared to state of the art photonic designs. Such giant $bar{beta}$ alleviate the need for ultra-narrow linewidths and thus pave the way for wavelength-scale SHG devices with faster operating timescales and higher tolerance to fabrication imperfections.
We study second harmonic generation in nonlinear, GaAs gratings. We find large enhancement of conversion efficiency when the pump field excites the guided mode resonances of the grating. Under these circumstances the spectrum near the pump wavelength displays sharp resonances characterized by dramatic enhancements of local fields and favorable conditions for second harmonic generation, even in regimes of strong linear absorption at the harmonic wavelength. In particular, in a GaAs grating pumped at 1064nm, we predict second harmonic conversion efficiencies approximately five orders of magnitude larger than conversion rates achievable in either bulk or etalon structures of the same material.
Taylor K. Fryett
,Kyle L. Seyler
,Jiajiu Zheng
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(2016)
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"Silicon photonic crystal cavity enhanced second-harmonic generation from monolayer WSe2"
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Taylor Fryett
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