ABSTRACT
Spontaneous symmetry breaking (SSB) is key for our understanding of phase transitions and the spontaneous emergence of order. In this work, we report that, for a two-dimensional (2D) periodic metasurface with gain, SSB occurs in the lasing transition. We study diffractive hexagonal plasmon nanoparticle lattices, where the K-points in momentum space provide two modes that are degenerate in frequency and identically distributed in space. Using femtosecond pulses to energize the gain medium, we simultaneously capture single-shot real-space and Fourier-space images of laser emission. By combining Fourier and real space, we resolve the two order parameters for which symmetry breaking simultaneously occurs: spatial parity and U(1) (rotational) symmetry breaking, evident respectively as random relative mode amplitude and phase. The methodology reported in this work is generally applicable to 2D plasmonic and dielectric metasurfaces and opens numerous opportunities for the study of SSB and the emergence of spatial coherence in metaphotonics.
ABSTRACT
Temporal dynamics of confined optical fields can provide valuable insights into light-matter interactions in complex optical systems, going beyond their frequency-domain description. Here, we present a new experimental approach based on interferometric autocorrelation (IAC) that reveals the dynamics of optical near-fields enhanced by collective resonances in periodic metasurfaces. We focus on probing the resonances known as waveguide-plasmon polaritons, which are supported by plasmonic nanoparticle arrays coupled to a slab waveguide. To probe the resonant near-field enhancement, our IAC measurements make use of enhanced two-photon excited luminescence (TPEL) from semiconductor quantum dots deposited on the nanoparticle arrays. Thanks to the incoherent character of TPEL, the measurements are only sensitive to the fundamental optical fields and therefore can reveal clear signatures of their coherent temporal dynamics. In particular, we show that the excitation of a high-Q collective resonance gives rise to interference fringes at time delays as large as 500 fs, much greater than the incident pulse duration (150 fs). Based on these signatures, the basic characteristics of the resonances can be determined, including their Q factors, which are found to exceed 200. Furthermore, the measurements also reveal temporal beating between two different resonances, providing information on their frequencies and their relative contribution to the field enhancement. Finally, we present an approach to enhance the visibility of the resonances hidden in the IAC curves by converting them into spectrograms, which greatly facilitates the analysis and interpretation of the results. Our findings open up new perspectives on time-resolved studies of collective resonances in metasurfaces and other multiresonant systems.
ABSTRACT
Lead-halide perovskites offer excellent properties for lighting and display applications. Nanopatterning perovskite films could enable perovskite-based devices with designer properties, increasing their performance and adding novel functionalities. We demonstrate the potential of nanopatterning for achieving light emission of a perovskite film into a specific angular range by introducing periodic sol-gel structures between the injection and emissive layer by using substrate conformal imprint lithography (SCIL). Structural and optical characterization reveals that the emission is funnelled into a well-defined angular range by optical resonances, while the emission wavelength and the structural properties of the perovskite film are preserved. The results demonstrate a flexible and scalable approach to the patterning of perovskite layers, paving the way toward perovskite LEDs with designer angular emission patterns.
