Giant Third-Harmonic Optical Generation from Topological Insulator Heterostructures
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Polarization Control via Artificial Optical Nonlinearity in Dielectric Metasurfaces
Nonlinear optical phenomena are generally governed by geometry in matter systems, as they depend on the spatial arrangement of atoms within materials or molecules. Metasurfaces, through precisely designed geometries on a subwavelength scale, allow the optical response of a material to be tailored far beyond its natural properties. Therefore, metasurfaces are highly appealing for enabling the engineering of nonlinear optical interactions. Current studies of nonlinear metasurfaces predominantly focus on the phase control of the generated light. Nonetheless, investigating the tensorial nature of the nonlinearity of metasurfaces and its effect on the polarization of the generated light is critical to fully unlocking a range of applications, such as nonlinear vector beam generation and nonlinear polarization imaging. Here, we study the artificial optical nonlinearity of a dielectric metasurface originating from its meta-atom symmetry and describe the third-order nonlinear behavior by considering the polarization degree of freedom. We establish an effective nonlinear medium model that serves as a design toolbox for developing amorphous silicon-based geometric metasurfaces with customizable features for third-harmonic generation. We further extract quantitative values of the artificial nonlinear susceptibility tensor elements related to the investigated nonlinear process and geometry. The implemented functional devices demonstrate the versatility of dielectric metasurfaces in shaping the emitted light in terms of amplitude, phase, and polarization for the precise engineering of advanced nonlinear architectures targeting applications in nonlinear imaging and complex light generation.
Diffraction↗
Optical Bound States in the Continuum Enabled by Magnetic Resonances Coupled to a Mirror
Dielectric metasurfaces made of high refractive index and low optical loss materials have emerged as promising platforms to achieve high-quality factor modes enabling strong light–matter interaction. Bound states in the continuum have shown potential to demonstrate narrow spectral resonances but often require asymmetric geometry and typically feature strong polarization dependence, complicating fabrication and limiting practical applications. Here, we introduce a novel approach for designing high-quality bound states in the continuum using magnetic dipole resonances coupled to a mirror. The resulting metasurface has simple geometric parameters requiring no broken symmetry. To demonstrate the unique features of our photonic platform we show a record-breaking third harmonic generation efficiency from the metasurface benefiting from the strongly enhanced electric field at high-quality resonances. Our approach mitigates the shortcomings of previous platforms with simple geometry enabling facile and large-area fabrication of metasurfaces paving the way for applications in optical sensing, detection, quantum photonics, and nonlinear devices.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Resonant Chiral Effects in Nonlinear Dielectric Metasurfaces
We study the resonant enhancement of linear and nonlinear chiroptical effects in planar silicon metasurfaces with an in-plane asymmetry supporting multipolar Mie resonances and quasi-bound states in the continuum (quasi-BICs). We demonstrate theoretically and observe in experiment the pronounced linear circular dichroism at the quasi-BIC resonances originating from the interaction of modes with the substrate. We further find that both local field enhancement and third-harmonic signal are large for Mie resonances and some quasi-BIC modes due to the critical coupling. We demonstrate experimentally a strong nonlinear chiroptical response associated with high efficiency of the third-harmonic generation and large nonlinear circular dichroism varying from +0.918 ± 0.049 to –0.771 ± 0.004 for the samples with different asymmetries. We reveal the nonreciprocal nature of nonlinear chirality governed by the microscopic symmetry of nonlinearities and macroscopic symmetries of the meta-atom and metasurface lattice. Here, we believe our results suggest a general strategy for engineering nonlinear chiroptical response in dielectric resonant metasurfaces.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Nonlinear Dispersion Relation and Out‐of‐Plane Second Harmonic Generation in MoSSe and WSSe Janus Monolayers
Janus transition metal dichalcogenides are an emerging class of atomically thin materials with engineered broken mirror symmetry that gives rise to long‐lived dipolar excitons, Rashba splitting, and topologically protected solitons. They hold great promise as a versatile nonlinear optical platform due to their broadband harmonic generation tunability, ease of integration on photonic structures, and nonlinearities beyond the basal crystal plane. Here, second and third harmonic generation in MoSSe and WSSe Janus monolayers is studied. Polarization‐resolved spectroscopy is used to map the full second‐order susceptibility tensor of MoSSe, including its out‐of‐plane components. In addition, the effective third‐order susceptibility and the second‐order nonlinear dispersion close to exciton resonances for both MoSSe and WSSe are measured at room and cryogenic temperatures. This work sets a bedrock for understanding the nonlinear optical properties of Janus transition metal dichalcogenides and probing their use in the next‐generation on‐chip multifaceted photonic devices.
36 MATERIALS SCIENCE↗
Effect of halogenation on the nonlinear optical properties of porthyrin and substituted porphyrins
The effect that fluorine and chlorine substitution has on the nonlinear optical properties of porphyrin, tetramethylporphyrin and tetraphenylporphyrin has been theoretically studied. The calculations of nonlinear optical properties have been obtained by performing finite-field calculations on structures determined by semiempirical methods. In addition, tetra(p-chlorophenyl)porphyrin and tetra(p-bromophenyl)porphyrin were synthesized by the condensation of pyrrol and the appropriate aldehyde. Thin films of polymethylmethacrylate were obtained containing these materials, by spin coating onto glass substrates. The films were characterized by third-harmonic generation. It was determined that the experimental conditions enhance the third-order polarizability of the tetraphenylporphyrins by a factor of about 1.6.
Cardelino, Beatriz H.↗
Phonon-enhanced nonlinearities in hexagonal boron nitride
Abstract Polar crystals can be driven into collective oscillations by optical fields tuned to precise resonance frequencies. As the amplitude of the excited phonon modes increases, novel processes scaling non-linearly with the applied fields begin to contribute to the dynamics of the atomic system. Here we show two such optical nonlinearities that are induced and enhanced by the strong phonon resonance in the van der Waals crystal hexagonal boron nitride (hBN). We predict and observe large sub-picosecond duration signals due to four-wave mixing (FWM) during resonant excitation. The resulting FWM signal allows for time-resolved observation of the crystal motion. In addition, we observe enhancements of third-harmonic generation with resonant pumping at the hBN transverse optical phonon. Phonon-induced nonlinear enhancements are also predicted to yield large increases in high-harmonic efficiencies beyond the third.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Cascaded Optical Nonlinearities in Dielectric Metasurfaces
Since the discovery of the laser, optical nonlinearities have been at the core of efficient light conversion sources. Typically, thick transparent crystals or quasi-phase matched waveguides are utilized in conjunction with phase-matching techniques to select a single parametric process. In recent years, due to the rapid developments in artificially structured materials, optical frequency mixing has been achieved at the nanoscale in subwavelength resonators arrayed as metasurfaces. Phase matching becomes relaxed for these wavelength-scale structures, and all allowed nonlinear processes can, in principle, occur on an equal footing. This could promote harmonic generation via a cascaded (consisting of several frequency mixing steps) process. However, so far, all reported work on dielectric metasurfaces have assumed frequency mixing from a direct (single step) nonlinear process. In this work, we prove the existence of cascaded second-order optical nonlinearities by analyzing the second- and third-wave mixing from a highly nonlinear metasurface in conjunction with polarization selection rules and crystal symmetries. We find that the third-wave mixing signal from a cascaded process can be of comparable strength to that from conventional third-harmonic generation and that surface nonlinearities are the dominant mechanism that contributes to cascaded second-order nonlinearities in our metasurface.
36 MATERIALS SCIENCE↗
Prediction of nonlinear optical properties of organic materials. General theoretical considerations
The prediction of nonlinear optical properties of organic materials is geared to assist materials scientists in the selection of good candidate molecules. A brief summary of the quantum mechanical methods used for estimating hyperpolarizabilities will be presented. The advantages and limitations of each technique will be discussed. Particular attention will be given to the finite-field method for calculating first and second order hyperpolarizabilities, since this method is better suited for large molecules. Corrections for dynamic fields and bulk effects will be discussed in detail, focusing on solvent effects, conformational isomerization, core effects, dispersion, and hydrogen bonding. Several results will be compared with data obtained from third-harmonic-generation (THG) and dc-induced second harmonic generation (EFISH) measurements. These comparisons will demonstrate the qualitative ability of the method to predict the relative strengths of hyperpolarizabilities of a class of compounds. The future application of molecular mechanics, as well as other techniques, in the study of bulk properties and solid state defects will be addressed. The relationship between large values for nonlinear optical properties and large conjugation lengths is well known, and is particularly important for third-order processes. For this reason, the materials with the largest observed nonresonant third-order properties are conjugated polymers. An example of this type of polymer is polydiacetylene. One of the problems in dealing with polydiacetylene is that substituents which may enhance its nonlinear properties may ultimately prevent it from polymerizing. A model which attempts to predict the likelihood of solid-state polymerization is considered, along with the implications of the assumptions that are used. Calculations of the third-order optical properties and their relationship to first-order properties and energy gaps will be discussed. The relationship between monomeric and polymeric third-order optical properties will also be considered.
Cardelino, B.↗
Non-resonant picosecond three-wave mixing in the gas phase
We report on the experimental observation of non-resonant, second-order optical sum-frequency generation (SFG) in five different atomic and molecular gases. The measured signal is attributed to a SFG process by characterizing its intensity scaling and its polarization behavior. We show that the electric quadrupole mechanism cannot explain the observed trends and suggest a mechanism based on symmetry breaking along the incident beam path arising from laser-induced species ground state number density gradients. Our results demonstrate that the SFG is about four orders of magnitude stronger than the third-harmonic generation (THG) and independent from any externally applied electric fields. In conclusion, these features make this method suitable for gas number density measurements at the picosecond time scale in reactive flows and plasmas.
LaCombe, Grayson↗
Modeling of transverse stimulated Raman scattering in KDP/DKDP in large-aperture plates suitable for polarization control
Transverse stimulated Raman scattering (TSRS) in potassium dihydrogen phosphate (KDP) and deuterated potassium dihydrogen phosphate (DKDP) plates for large-aperture, inertial confinement fusion (ICF)-class laser systems is a well-recognized limitation giving rise to parasitic energy conversion and laser-induced damage. The onset of TSRS is manifested in plates exposed to the ultraviolet section of the beam. TSRS amplification is a coherent process that grows exponentially and is distributed nonuniformly in the crystal and at the crystal surfaces. To understand the growth and spatial distribution of TSRS energy in various configurations, a modeling approach has been developed to simulate the operational conditions relevant to ICF-class laser systems. Specific aspects explored in this work include (i) the behavior of TSRS in large-aperture crystal plates suitable for third-harmonic generation and use as wave plates for polarization control in current-generation ICF-class laser system configurations; (ii) methods, and their limitations, of TSRS suppression and (iii) optimal geometries to guide future designs.
47 OTHER INSTRUMENTATION↗
Insights into the Growth Orientation and Phase Stability of Chemical-Vapor-Deposited Two-Dimensional Hybrid Halide Perovskite Films
Chemical vapor deposition (CVD) offers a large-area, scalable, and conformal growth of perovskite thin films without the use of solvents. Low-dimensional organic–inorganic halide perovskites, with alternating layers of organic spacer groups and inorganic perovskite layers, are promising for enhancing the stability of optoelectronic devices. Moreover, their multiple quantum-well structures provide a powerful platform for tuning excitonic physics. Here, in this work, we show that the CVD process is conducive to the growth of 2D hybrid halide perovskite films. Using butylammonium (BA) and phenylethylammonium (PEA) cations, the growth parameters of BA 2 PbI 4 and PEA 2 PbI 4 and mixed halide perovskite films were first optimized. These films are characterized by well-defined grain boundaries and display characteristic absorption and emission features of the 2D quantum wells. X-ray diffraction (XRD) and a noninteger dimensionality model of the absorption spectrum provide insights into the orientation of the crystalline planes. Unlike BA 2 PbI 4 , temperature-dependent photoluminescence measurements from PEA 2 PbI 4 show a single excitonic peak throughout the temperature range from 20 to 350 K, highlighting the lack of defect states. These results further corroborate the temperature-dependent synchrotron-based XRD results. Furthermore, the nonlinear optical properties of the CVD-grown perovskite films are investigated, and a high third harmonic generation efficiency is observed.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Multiphoton and Harmonic Imaging of Microarchitected Materials
Microadditive manufacturing has revolutionized the production of complex, nano- to microscale components across various fields. This work investigates two-photon (2P) and three-photon (3P) fluorescence imaging, as well as third-harmonic generation (THG) microscopy, to examine periodic microarchitected lattice structures fabricated using multiphoton lithography (MPL). By immersing the structures in refractive index matching fluids, we demonstrate high-fidelity 3D reconstructions of both fluorescent structures using 2P and 3P microscopy as well as low-fluorescence structures using THG microscopy. These results show that multiphoton fluorescence (MPF) imaging offers reduced signal decay with respect to depth compared to single-photon techniques in the examined structures. We further demonstrate the ability to nondestructively identify intentional internal modifications of the structure that are not immediately visible with scanning electron microscope (SEM) images and compression-induced fractures, highlighting the potential of these techniques for quality control and defect detection in microadditively manufactured components.
36 MATERIALS SCIENCE↗
Near-zero-index ultra-fast pulse characterization
Transparent conducting oxides exhibit giant optical nonlinearities in the near-infrared window where their linear index approaches zero. Despite the magnitude and speed of these nonlinearities, a “killer” optical application for these compounds has yet to be found. Because of the absorptive nature of the typically used intraband transitions, out-of-plane configurations with short optical paths should be considered. In this direction, we propose an alternative frequency-resolved optical gating scheme for the characterization of ultra-fast optical pulses that exploits near-zero-index aluminium zinc oxide thin films. Besides the technological advantages in terms of manufacturability and cost, our system outperforms commercial modules in key metrics, such as operational bandwidth, sensitivity, and robustness. The performance enhancement comes with the additional benefit of simultaneous self-phase-matched second and third harmonic generation. Because of the fundamental importance of novel methodologies to characterise ultra-fast events, our solution could be of fundamental use for numerous research labs and industries.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Quantum control of Hubbard excitons
Quantum control of the many-body wavefunction is a central challenge in quantum materials research, as it could yield a precise control knob to manipulate emergent phenomena. Floquet engineering, the coherent dressing of quantum states with periodic non-resonant optical fields, has become an important strategy for quantum control. Most applications to solid-state systems have targeted weakly interacting or single-ion states, leaving the manipulation of many-body wavefunctions largely unexplored. Here, in this work, we use Floquet engineering to achieve quantum control of a strongly correlated Hubbard exciton in the one-dimensional Mott insulator Sr 2 CuO 3 . A nonresonant midinfrared optical field coherently dresses the exciton wavefunction, driving its rotation between bright and dark states. We use resonant third-harmonic generation to quantify ultrafast π/2 rotations on the Bloch sphere spanned by these exciton states. Our work advances the quest towards programmable control of correlated states and exciton-based quantum sensing.
36 MATERIALS SCIENCE↗
Nonlinear dynamics of topological Dirac fermions in 2D spin-orbit coupled materials
Abstract The graphene family materials are two-dimensional staggered monolayers with a gapped energy band structure due to intrinsic spin-orbit coupling. The mass gaps in these materials can be manipulated on-demand via biasing with a static electric field, an off-resonance circularly polarized laser, or an exchange interaction field, allowing the monolayer to be driven through a multitude of topological phase transitions. We investigate the dynamics of spin-orbit coupled graphene family materials to unveil topological phase transition fingerprints embedded in the nonlinear regime and show how these signatures manifest in the nonlinear Kerr effect and in third-harmonic generation processes. We show that the resonant nonlinear spectral response of topological fermions can be traced to specific Dirac cones in these materials, enabling characterization of topological invariants in any phase by detecting the cross-polarized component of the electromagnetic field. By shedding light on the unique processes involved in harmonic generation via topological phenomena our findings open an encouraging path towards the development of novel nonlinear systems based on two-dimensional semiconductors of the graphene family.
36 MATERIALS SCIENCE↗
Plasmon-enhanced optical nonlinearity in graphene nanomeshes
Using the density-matrix formalism, here we show that graphene nanomeshes (GNMs)—graphene sheets patterned with antidots—have large plasmon-enhanced nonlinear optical response. GNMs can be designed to behave as quasi-one-dimensional plasmonic crystals in which plasmons with large propagation lengths are efficiently excited. The associated third-order Kerr and third-harmonic-generation susceptibility can be as high as 10 –7 and 10 –9 m 2 V –2 , respectively, over the mid-to-near-infrared frequency range. Furthermore, carrier-density tuning in GNMs can flip the propagation direction of plasmonic waves and enables bidirectional switching of optical signals.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Multidimensional coherent spectroscopy of light-driven states and their collective modes in multiband superconductors
We present a comprehensive theory of light-controlled multiband superconductivity, and apply it to predict distinctive signatures of light-driven superconducting (SC) states in terahertz multidimensional coherent spectroscopy (THz-MDCS) experiments. We first derive gauge-invariant Maxwell-Bloch equations for multiband BCS superconductors with spatial fluctuations. We consider driving electromagnetic fields determined self-consistently by Maxwell's equations. By calculating the THz-MDCS spectra measured experimentally in the clean SC limit, we identify unique signatures of finite-momentum Cooper-pairing states that live longer than the laser pulse. They are controlled by a pair of THz laser pulses with well-defined relative phase (pulse pair). The pseudospin oscillators that describe the properties of these SC states are parametrically driven by both finite-momentum Cooper pairing and by time oscillations of the order-parameter relative phase. We show that such strong parametric driving leads to drastic changes in the THz-MDCS spectral shape from the predictions of third-order nonlinear susceptibility calculations. These spectral changes strongly depend on the interband-to-intraband interaction ratio and on the collective modes of the light-driven state. For negligible interband interaction, the spectra show a transition with increasing field, from traditional pump-probe, four-wave-mixing, and third-harmonic generation peaks determined by the laser frequency to sidebands determined by the excitations of the driven system. These sidebands emerge from difference-frequency Raman processes in the nonequilibrium SC state. For interband couplings weaker than the intraband pairing, we show that the Leggett phase collective mode leads to harmonic sidebands around the traditional pump-probe peaks. Additional Higgs collective mode peaks result from light-induced inversion-symmetry breaking in a thin-film geometry. For strong interband coupling, we find a transition from a nonequilibrium finite Cooper-pair momentum state characterized by hybrid-Higgs amplitude mode peaks in THz-MDCS spectra to a driven state identified experimentally by the emergence of Floquet-type sidebands at bi-Higgs frequencies. Those dominant bi-Higgs-frequency satellites are manifestations of a new order parameter relative phase collective mode that characterizes the nonequilibrium SC state. The predicted interaction- and field-dependent transitions in the spectral profile allow us to propose THz-MDCS experiments for quantum tomography of light-driven superconductivity.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗