Illuminating signatures of gapless topology and correlations: contrasting nonlinear optical responses
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Material Science↗
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Optical Response and Transport in Condensed and Warm Dense Matter from First Principles
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Robinson, Brian Patrick [Sandia National Laborator↗
Nonlinear Spectroscopy of Collective Modes in an Excitonic Insulator
The nonlinear optical response of an excitonic insulator coupled to lattice degrees of freedom is shown to depend in strong and characteristic ways on whether the insulating behavior originates primarily from electron-electron or electron-lattice interactions. Linear response optical signatures of the massive phase mode and the amplitude (Higgs) mode are identified. Upon nonlinear excitation resonant to the phase mode, a new in-gap mode at twice the phase mode frequency is induced, leading to a huge second harmonic response. Excitation of in-gap phonon modes leads to different and much smaller effects. A Landau-Ginzburg theory analysis explains these different behaviors and reveals that a parametric resonance of the strongly excited phase mode is the origin of the photoinduced mode in the electron-dominant case. Here, the difference in the nonlinear optical response serves as a measure of the dominant mechanism of the ordered phase.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Exploiting universal nonlocal dispersion in optically active materials for spectro-polarimetric computational imaging
Recent years have seen significant advancements in exploring novel light-matter interactions such as hyperbolic dispersion within natural crystals. However, current studies have predominantly concentrated on local optical response of materials characterized by a dielectric tensor without spatial dispersion. Here, we investigate the nonlocal response in optically-active crystals with screw symmetries, revealing their lossless, super-dispersive properties compared to traditional optical response functions. We leverage this universal nonlocal dispersion, i.e. the dispersion of optical rotatory power, to explore a novel spectral de-multiplexing scheme compared to conventional gratings, prisms and metasurfaces. We design and demonstrate an ‘Nonlocal-Cam’ - a camera that exploits nonlocal dispersion through sampling of polarized spectral states and the application of computational spectral reconstruction algorithms. The Nonlocal-Cam captures information in both laboratory and outdoor field experiments which is unavailable to traditional intensity cameras - the spectral texture of polarization. Merging the fields of nonlocal electrodynamics and computational imaging, our work paves the way for exploiting nonlocal optics of optically active materials in a variety of applications, from biological microscopy to physics-driven machine vision and remote sensing.
Wang, Xueji [Purdue Univ., West Lafayette, IN (Uni↗
Physics‐Informed Machine Learning for Inverse Design of Optical Metamaterials
Optical metamaterials manipulate light through various confinement and scattering processes, offering unique advantages like high performance, small form factor and easy integration with semiconductor devices. However, designing metasurfaces with suitable optical responses for complex metamaterial systems remains challenging due to the exponentially growing computation cost and the ill‐posed nature of inverse problems. To expedite the computation for the inverse design of metasurfaces, a physics‐informed deep learning (DL) framework is used. A tandem DL architecture with physics‐based learning is used to select designs that are scientifically consistent, have low error in design prediction, and accurate reconstruction of optical responses. The authors focus on the inverse design of a representative plasmonic device and consider the prediction of design for the optical response of a single wavelength incident or a spectrum of wavelength in the visible light range. The physics‐based constraint is derived from solving the electromagnetic wave equations for a simplified homogenized model. The model converges with an accuracy up to 97% for inverse design prediction with the optical response for the visible light spectrum as input, and up to 96% for optical response of single wavelength of light as input, with optical response reconstruction accuracy of 99%.
Sarkar, Sulagna↗
Excitonic Interactions and Mechanism for Ultrafast Interlayer Photoexcited Response in van der Waals Heterostructures
Optical dynamics in van der Waals heterobilayers is of fundamental scientific and practical interest. Based on a time-dependent adiabatic GW approach, we discover a new many-electron (excitonic) channel for converting photoexcited intralayer to interlayer excitations and the associated ultrafast optical responses in heterobilayers, which is conceptually different from the conventional single-particle picture. We find strong electron-hole interactions drive the dynamics and enhance the pump-probe optical responses by an order of magnitude with a rise time of ~300 fs in MoSe 2 /WSe 2 heterobilayers, in agreement with experiment.
74 ATOMIC AND MOLECULAR PHYSICS↗
Lattice Resonances of Nanohole Arrays for Quantum Enhanced Sensing
We report periodic arrays of nanoholes perforated in metallic thin films interact strongly with light and produce large electromagnetic near-field enhancements in their vicinity. As a result, the optical response of these systems is very sensitive to changes in their dielectric environment, thus making them an exceptional platform for the development of compact optical sensors. Given that these systems already operate at the shot-noise limit when used as optical sensors, their sensing capabilities can be enhanced beyond this limit by probing them with quantum light, such as squeezed or entangled states. Motivated by this goal, here, we present a comparative theoretical analysis of the quantum enhanced sensing capabilities of metallic nanohole arrays with one and two holes per unit cell. Through a detailed investigation of their optical response, we find that the two-hole array supports resonances that are narrower and stronger than its one-hole counterpart, and therefore have a higher fundamental sensitivity limit as defined by the quantum Cramer-Rao bound. We validate the optical response of the analyzed arrays with experimental measurements of the reflectance of representative samples. The results of this work advance our understanding of the optical response of these systems and pave the way for developing sensing platforms capable of taking full advantage of the resources offered by quantum states of light.
74 ATOMIC AND MOLECULAR PHYSICS↗
Generalized analytical and numerical modeling of optical second harmonic generation in anisotropic crystals and complex heterostructures using #SHAARP package
Optical second harmonic generation (SHG) is a nonlinear optical effect widely used for nonlinear optical microscopy and laser frequency conversion. The closed-form analytical solution of the nonlinear optical responses is essential for evaluating the optical responses of new materials whose optical properties are unknown a priori. Many approximations have therefore been employed in the existing analytical approaches, such as slowly varying approximation, weak reflection of the nonlinear polarization, transparent medium, high crystallographic symmetry, Kleinman symmetry, easy crystal orientation along a high-symmetry direction, phase matching conditions and negligible interference among nonlinear waves, which may lead to large errors in the reported material properties. To avoid these approximations, here we have developed an open-source package named Second Harmonic Analysis of Anisotropic Rotational Polarimetry (#SHAARP) for single interface (si) and in multilayers (ml) for homogeneous crystals. The reliability and accuracy are established by experimentally benchmarking with both the SHG polarimetry and Maker fringes predicted from the package using standard materials. SHAARP.si and SHAARP.ml are available through GitHub https://github.com/Rui-Zu/SHAARP and https://github.com/bzw133/SHAARP.ml, respectively.
complex systems↗
No One Size Fits All: Semiconductor Nanocrystal Sizing Curves
Although colloidal quantum dots or nanocrystals (NCs) are now long past their infancy, there remain basic issues that must be addressed to fully establish their fundamental, size-dependent properties. This is especially true for model systems such as CdSe where confinement effects are responsible for changes in their optical response and where significant effort has been invested in developing theories of their underlying electronic structure. Surprisingly, there still appears to be a lack of consensus on one of the most fundamental metrics for NCs, their sizing curves. As shown here, these are empirical functions that link the size of isotropically shaped semiconductor NCs (such as the diameter, d, for spherical NCs and edge length, l, for cube-shaped ones) to corresponding changes in optical response.
36 MATERIALS SCIENCE↗
Light-induced shift current vortex crystals in moiré heterobilayers
Transition metal dichalcogenide (TMD) moiré superlattices provide an emerging platform to explore various light-induced phenomena. Recently, the discoveries of novel moiré excitons have attracted great interest. The nonlinear optical responses of these systems are however still underexplored. Here, we report investigation of light-induced shift currents (a second-order response generating DC current from optical illumination) in the WSe 2 /WS 2 moiré superlattice. We identify a striking phenomenon of the formation of shift current vortex crystals—i.e., two-dimensional periodic arrays of moiré-scale current vortices and associated magnetic fields with remarkable intensity under laboratory laser setup. Furthermore, we demonstrate high optical tunability of these current vortices—their location, shape, chirality, and magnitude can be tuned by the frequency, polarization, and intensity of the incident light. Electron-hole interactions (excitonic effects) are found to play a crucial role in the generation and nature of the shift current intensity and distribution. Our findings provide a promising all-optical control route to manipulate nanoscale shift current density distributions and magnetic field patterns, as well as shed light on nonlinear optical responses in moiré quantum matter and their possible applications.
36 MATERIALS SCIENCE↗
Nonlocal Coherent Optical Nonlinearities of a Macroscopic Quantum System
The optical responses of solids are typically understood to be local in space. Whether locality holds for the optical response of a macroscopic quantum system has, however, been largely unexplored. Here, we use multidimensional coherent spectroscopy at the optical diffraction limit to demonstrate nonlocal optical nonlinearities in a semiconductor microcavity. In conclusion, these nonlocal optical responses are both coherent and quantum in nature, deriving from the macroscopic length scale of confined exciton-polariton wave functions.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Excitonic Anisotropy in Single‐Crystalline 2D Silver Phenylchalcogenides
2D materials exhibiting in‐plane anisotropy enable new applications in directional energy transport and polarized optical response. Silver phenylchalcogenides (AgEPh) – including mithrene (AgSePh), tethrene (AgTePh), and thiorene (AgSPh) – represent an exciting new addition to this family, with optical response spanning the visible to near‐UV. Here, excitonic anisotropy is predicted and characterized in this family of materials using a combination of ab initio theory and optical micro‐spectroscopy of single‐crystalline flakes. Using density functional theory and GW with the Bethe–Salpeter equation calculations, it is revealed that all AgEPh compounds exhibit anisotropic electronic band structure and host multiple delocalized excitons with in‐plane anisotropy. Room‐temperature polarization‐resolved optical micro‐spectroscopy shows that orthogonally polarized excitons with similar energy lead to nearly isotropic absorption in AgSPh, whereas energy separation between excitonic resonances in AgSePh and AgTePh leads to strong absorption and emission anisotropy. Cryogenic reflectance micro‐spectroscopy further reveals exciton fine structure in AgSePh, reconciling the discrepancies between room‐temperature experiments and theoretical predictions. Finally, it is demonstrated that the optical response of thicker AgEPh crystals is influenced by photonic effects arising from finite crystal size. Overall, this work advances the understanding of the relationship between anisotropic structure, composition, and excitonic properties in AgEPh, providing a foundation for technological integration.
2D↗
Full complex amplitude control of second-harmonic generation via electrically tunable intersubband polaritonic metasurfaces
Nonlinear intersubband polaritonic metasurfaces based on coupling of the intersubband nonlinear optical response of quantum-engineered semiconductor heterostructures and electromagnetic modes of nanoresonators provide efficient frequency mixing with moderate pump intensities. The resonant nonlinear optical response, represented as a complex function, can be modulated via Stark tuning of intersubband transition energies under applied voltages. However, achieving full complex amplitude control (both phase and magnitude) remains challenging. In this work, we present and experimentally validate electrically tunable nonlinear intersubband polaritonic metasurfaces that achieve complete complex amplitude control for second-harmonic generation (SHG). Through a design featuring two in-plane flipped meta-atoms per unit cell, we achieve complete electrical control of both the amplitude and phase of the metasurface second-order nonlinear susceptibility, with a tuning range of 0 to 30 nm V −1 for the magnitude and 0-2π for the phase of the nonlinear optical response. Using these properties, we achieve complete on-off SHG modulation and beam diffraction tuning through electrically controlled amplitude and phase gratings.
Science & Technology - Other Topics↗
Active Plasmonics and Active Chiral Plasmonics through Orientation-Dependent Multipolar Interactions
While most active plasmonic efforts focus on responsive metamaterials to modulate optical response, we present a simple alternative based on applied orientation control that can likely be implemented for many passive plasmonic materials. Passive plasmonic motifs are simpler to prepare but cannot be altered postfabrication. Here, we show that such systems can be easily manipulated through substrate orientation control to generate both active plasmonic and active chiral plasmonic responses. Using gold nanocrescents as our model platform, we demonstrate tuning of optical extinction from -21% to +36% at oblique incidence relative to normal incidence. Variation of substrate orientation in relation to incident polarization is also demonstrated to controllably switch chiroptical handedness (e.g., Δg = ± 0.55). These active plasmonic responses arise from the multipolar character of resonant modes. In particular, we correlate magnetoelectric and dipole–quadrupole polarizabilities with different light-matter orientation-dependence in both near- and far-field localized surface plasmon activity. Additionally, the attribution of far-field optical response to higher-order multipoles highlights the sensitivity offered by these orientation-dependent characterization techniques to probe the influence of localized electromagnetic field gradients on a plasmonic response. The sensitivity afforded by orientation-dependent optical characterization is further observed by the manifestation in both plasmon and chiral plasmon responses of unpredicted structural nanocrescent variance (e.g., left- and right-tip asymmetry) not physically resolved through topographical imaging.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Giant optical nonlinearity of Fermi polarons in atomically thin semiconductors
In this study, realizing strong nonlinear optical responses is a long-standing goal of both fundamental and technological importance. Recently, substantial efforts have been focused on exploring excitons in solids to achieve nonlinearities even down to few-photon levels. However, a crucial tradeoff arises as strong light–matter interactions require large oscillator strength and short radiative lifetime of excitons, which limits their nonlinearity. Here we experimentally demonstrate strong nonlinear optical responses with large oscillator strength by exploiting the coupling between excitons and carriers in an atomically thin semiconductor. By controlling the electric field and electrostatic doping of trilayer WSe 2 , we observe the hybridization between intralayer and interlayer excitons and the formation of Fermi polarons. Substantial optical nonlinearity is observed under continuous-wave and pulsed laser excitation, where the Fermi polaron resonance blueshifts by as much as ~10 meV. Intriguingly, we observe a remarkable asymmetry in the optical nonlinearity between electron and hole doping, which is tunable by the applied electric field. We attribute these features to the optically induced valley polarization due to the interactions between excitons and free charges. Our results establish atomically thin heterostructures as a highly versatile platform for engineering nonlinear optical response with applications to classical and quantum optoelectronics.
2d materials↗
Dynamically Tunable Terahertz Emission Enabled by Anomalous Optical Phonon Responses in Lead Telluride
Lead telluride (PbTe), a narrow bandgap semiconductor commonly used in infrared detectors, exhibits anomalous vibrational and structural properties, making it appealing for thermoelectrics. Despite significant fundamental interest in the microscopic origins of its unusual vibrational properties, the optical functionalities stemming from phonons and electron–phonon coupling in PbTe have not been closely investigated. This work reports measurements of terahertz (THz) radiation from a PbTe single crystal following ultrafast optical excitation and investigates IR-active phonon responses as a function of excitation fluence and temperature. We uncover a spectrally tunable THz emission peak enabled by an epsilon-near-zero response of the coupled plasmon–longitudinal optical phonon mode that can be dynamically shifted via tuning photocarrier density. Spectral tunability (Δω/ω = 25%) is significant and beyond what has been achieved by any other THz emitter. In addition, the emitted THz fields reveal signatures of a zone center transverse optical phonon anomaly and unveil a new mode at 0.3 THz that diminishes in amplitude under increasing photocarrier density. Temperature-dependent measurements suggest that the transverse-like modes at 1 and 1.5 THz are possibly of different origins. These results indicate that the unusual phononic properties in PbTe are tunable via photoexcitation and enable new optical functionalities in THz applications, such as spectrally tunable emitters and all-optical modulators.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Ultra-wide bandgap β-Ga 2 O 3 films: Optical, phonon, and temperature response properties
Optical and phonon interactions of Ga 2 O 3 thin films with nanocrystalline morphology were studied at extreme temperatures. The films were grown using a sputtering technique and analyzed via temperature response transmission, Raman scattering, and high-resolution deep-UV photoluminescence (PL). Raman modes indicated that the structure corresponds to the β-phase. The optical-gap at the range of 77–620 K exhibited a redshift of ~200 meV, with a temperature coefficient of ~0.4 meV/K. The optical-gap at room-temperature is 4.85 eV. The electron–phonon interaction model at that temperature range pointed to a low energy phonon, ~31 meV, that is involved in the thermal properties of the optical-gap. Detailed Urbach energy analysis indicated that defects are the dominant mechanism controlling the band-edge characteristics even at an elevated temperature regime where phonon dominance is usually expected. Defects are attributed to the disordered forms of graphite that were detected via Raman scattering and to the granular morphology of the film. A deep-UV laser with an above bandgap exaction line of 5.1 eV was employed to map the PL of the films. The highly resolved spectra, even at room-temperature, show a strong emission of ~3.56 eV attributed to self-trapped holes (STHs). The STH is discussed and modeled in terms of the self-trapped exciton. Moreover, a very distinct but low-intensity emission was found at 4.85 eV that agrees with the value of the optical-gap and is attributed to bandgap recombination. The intensity ratio between the STH and that of the bandgap was found to be 6:1.
36 MATERIALS SCIENCE↗
(Cd,Mg)Te crystals for picosecond-response optical-to-x-ray radiation detectors
We demonstrate a photodetector sensitive to both optical and x-ray picosecond pulses based on our in-house grown cadmium magnesium telluride (Cd,Mg)Te single crystal. Specifically, we developed In-doped Cd0.96Mg0.04Te material and discuss its femtosecond optical photoresponse, as well as the detector performance, such as <100-pA dark current and up to 0.22-mA/W responsivity for 780-nm wavelength optical radiation. The detector exposed to Ti fluorescence (K alpha) x-ray pulses at 4.5 keV, generated by a free-electron laser beam with the central energy of 9.8 keV and <100 fs pulse width, exhibited readout-electronics-limited 200-ps full-width-at-half-maximum photoresponse, demonstrating that it is suitable for coarse timing in free-electron laser x-ray/optical femtosecond pump–probe spectroscopy applications.
Instruments & Instrumentation↗