Polarization-resolved Measurements Research Articles

Out-of-plane polarization induces a picosecond photoresponse in rhombohedral stacked bilayer WSe2.

Constructing van der Waals materials with spontaneous out-of-plane polarization through interlayer engineering expands the family of two-dimensional ferroelectrics and provides an excellent platform for enhancing the photoelectric conversion efficiency. Here, we reveal the effect of spontaneous polarization on ultrafast carrier dynamics in rhombohedral stacked bilayer WSe2. Using precise stacking techniques, a 3R WSe2-based vertical heterojunction was successfully constructed and confirmed by polarization-resolved second harmonic generation measurements. Through output characteristics and the scanning photocurrent map under zero bias, we reveal a non-zero short-circuit current in the graphene/3R WSe2/graphene heterojunction region, demonstrating the bulk photovoltaic effect. Furthermore, the out-of-plane polarization enables the 3R WSe2 heterojunction region to achieve an ultrafast intrinsic photoresponse time of approximately 3 ps. The ultrafast response time remains consistent across varying detection powers, demonstrating environmental stability and highlighting the potential in optoelectronic applications. Our study presents an effective strategy for enhancing the response time of photodetectors.

Ultrafast Time-Domain Spectroscopy Reveals Coherent Vibronic Couplings upon Electronic Excitation in Crystalline Organic Thin Films.

The coherent coupling between electronic excitations and vibrational modes of molecules largely affects the optical and charge transport properties of organic semiconductors and molecular solids. To analyze these couplings by means of ultrafast spectroscopy, highly ordered crystalline films with large domains are particularly suitable because the domains can be addressed individually, hence allowing azimuthal polarization-resolved measurements. Impressive examples of this are highly ordered crystalline thin films of perfluoropentacene (PFP) molecules, which adopt different molecular orientations on different alkali halide substrates. Here, we report polarization-resolved time-domain vibrational spectroscopy with 10 fs time resolution and Raman spectroscopy of crystalline PFP thin films grown on NaF(100) and KCl(100) substrates. Coherent oscillations in the time-resolved spectra reveal vibronic coupling to a high-frequency, 25 fs, in-plane deformation mode that is insensitive to the optical polarization, while the coupling to a lower-frequency, 85 fs, out-of-plane ring bending mode depends significantly on the crystalline and molecular orientation. Comparison with calculated Raman spectra of isolated PFP molecules in vacuo supports this interpretation and indicates a dominant role of solid-state effects in the vibronic properties of these materials. Our results represent a first step toward uncovering the role of anisotropic vibronic couplings for singlet fission processes in crystalline molecular thin films.

Submicron Embedded Air/GaN Diffraction Gratings for Photonic Applications

AbstractThe integration of photonic elements with nitride optoelectronic structures allows control of emitted light properties, which is advantageous for achieving, e.g., a single wavelength lasing. Positioning of the photonic structures on the top surface of GaN‐based devices is problematic, in particular, for deposition of a metal contact to p‐type top layer. In this work, custom‐shaped submicron air channels arranged periodically 150 nm below the sample surface, forming an air/GaN diffraction grating embedded within a volume of the structure is proposed and fabricated. The fabrication process includes selective area Si ion implantation, GaN regrowth using plasma‐assisted molecular beam epitaxy, ultra‐high‐pressure annealing for efficient electrical activation of implanted Si without diffusion, and electrochemical etching for the removal of selectively doped material. Embedded air/GaN diffraction gratings with periodicity of 460 and 631 nm are shown. Width of air channels ranges from 46 to 320 nm. Angle and polarization resolved reflectivity measurements combined with theoretical modeling confirm the designed optical performance of the embedded diffraction gratings in the GaN volume. The presented design and fabrication of custom‐shaped, fully integrated photonic structures buried below the surface paves the way for novel type constructions of optoelectronic devices, such as compact distributed feedback laser diodes

Origin of Exciton-Polariton Interactions and Decoupled Dark States Dynamics in 2D Hybrid Perovskite Quantum Wells.

The realization of efficient optical devices depends on the ability to harness strong nonlinearities, which are challenging to achieve with standard photonic systems. Exciton-polaritons formed in hybrid organic-inorganic perovskites offer a promising alternative, exhibiting strong interactions at room temperature (RT). Despite recent demonstrations showcasing a robust nonlinear response, further progress is hindered by an incomplete understanding of the microscopic mechanisms governing polariton interactions in perovskite-based strongly coupled systems. Here, we investigate the nonlinear properties of quasi-2D dodecylammonium lead iodide perovskite (n3-C12) crystals embedded in a planar microcavity. Polarization-resolved pump-probe measurements reveal the contribution of indirect exchange interactions assisted by dark states formation. Additionally, we identify a strong dependence of the unique spin-dependent interaction of polaritons on sample detuning. The results are pivotal for the advancement of polaritonics, and the tunability of the robust spin-dependent anisotropic interaction in n3-C12 perovskites makes this material a powerful choice for the realization of polaritonic circuits.

Anisotropic carrier dynamics and laser-fabricated luminescent patterns on oriented single-crystal perovskite wafers

Perovskite materials and their applications in optoelectronics have attracted intensive attentions in recent years. However, in-depth understanding about their anisotropic behavior in ultrafast carrier dynamics is still lacking. Here we explore the ultrafast dynamical evolution of photo-excited carriers and photoluminescence based on differently-oriented MAPbBr3 wafers. The distinct in-plane polarization of carrier relaxation dynamics of the (100), (110) and (111) wafers and their out-of-plane anisotropy in a picosecond time scale were found by femtosecond time- and polarization-resolved transient transmission measurements, indicating the relaxation process dominated by optical/acoustic phonon interaction is related to photoinduced transient structure rearrangements. Femtosecond laser two-photon fabricated patterns exhibit three orders of magnitude enhancement of emission due to the formation of tentacle-like microstructures. Such a ultrafast dynamic study carried on differently-oriented crystal wafers is believed to provide a deep insight about the photophysical process of perovskites and to be helpful for developing polarization-sensitive and ultrafast-response optoelectronic devices.

Carbon-Related Quantum Emitter in Hexagonal Boron Nitride with Homogeneous Energy and 3-Fold Polarization.

Most hexagonal boron nitride (hBN) single-photon emitters (SPEs) studied to date suffer from variable emission energy and unpredictable polarization, two crucial obstacles to their application in quantum technologies. Here, we report an SPE in hBN with an energy of 2.2444 ± 0.0013 eV created via carbon implantation that exhibits a small inhomogeneity of the emission energy. Polarization-resolved measurements reveal aligned absorption and emission dipole orientations with a 3-fold distribution, which follows the crystal symmetry. Photoluminescence excitation (PLE) spectroscopy results show the predictability of polarization is associated with a reproducible PLE band, in contrast with the non-reproducible bands found in previous hBN SPE species. Photon correlation measurements are consistent with a three-level model with weak coupling to a shelving state. Our ab initio excited-state calculations shed light on the atomic origin of this SPE defect, which consists of a pair of substitutional carbon atoms located at boron and nitrogen sites separated by a hexagonal unit cell.

Robust valley quantum coherence in synthetic 3R-phase MoS2: A material for future valley based devices

Two-dimensional layered transition metal dichalcogenides (TMDCs) offer the ideal platform to optically initialize the qubits utilizing the superposition of valley polarized photons. However, in the commonly available 2H phase TMDCs, thickness sensitive crystal inversion symmetry demands the precise control over the number of layers, which makes the study of valley physics challenging. On the other hand, 3R-polymorphic phase TMDCs are non-centrosymmetric irrespective of the number of layers and therefore retain valley degree of freedom for all the thicknesses. Here, using polarization resolved photoluminescence measurements under linearly polarized excitations, we demonstrate the coherent superposition of the valley photons (known as valley coherence) in synthetic 3R-phase MoS2 with different numbers of layers ranging from 3 layers to 11 layers. With near-resonant excitation (633 nm for AX0), the degree of linear polarization (a measure of the valley coherence) is observed up to 70% at 80 K measurement temperatures and is found to be layer thickness independent. Robust valley coherence is attributed to the high optical quality and the 3R crystal symmetry of the MoS2. Using angle resolved polarization dependent measurements, it is established that the net dipolar emission aligns with the polarization orientations of the incident laser, which signifies the valley coherence to be independent of the crystal orientation. This study paves the way toward using 3R-phase MoS2 as a key material for the development of future quantum technologies utilizing valley polarized photons.

Nonlinear THz Generation through Optical Rectification Enhanced by Phonon-Polaritons in Lithium Niobate Thin Films.

We investigate nonlinear THz generation from lithium niobate films and crystals of different thicknesses by optical rectification of near-infrared femtosecond pulses. A comparison between numerical studies and polarization-resolved measurements of the generated THz signal reveals a 2 orders of magnitude enhancement in the nonlinear response compared to optical frequencies. We show that this enhancement is due to optical phonon modes at 4.5 and 7.45 THz and is most pronounced for films thinner than 2 μm where optical-to-THz conversion is not limited by self-absorption. These results shed new light on the employment of thin film lithium niobate platforms for the development of new integrated broadband THz emitters and detectors. This may also open the door for further control (e.g., polarization, directivity, and spectral selectivity) of the process in nanophotonic structures, such as nanowires and metasurfaces, realized in the thin film platform. We illustrate this potential by numerically investigating optical-to-THz conversion driven by localized surface phonon-polariton resonances in sub-wavelength lithium niobate rods.

Nonlocal resonances in pedestal high-index-contrast metasurfaces based on a silicon-on-insulator platform

Subwavelength control of the electromagnetic field distribution represents one of the current challenges in photonics research. In this field, diffractive metasurfaces with spatially extended (i.e., nonlocal) resonant modes have recently gained great interest for their versatility in molding the electromagnetic field beyond the approximation of independent resonators. In this framework, we design a high-contrast nonlocal metasurface featuring modes situated in the third operating spectral window of optical communications. The optical properties of the fabricated metasurface are investigated by linear spectroscopy and numerical simulations. Our analysis allows to discern the magnetic and electric nature of the bounded modes by means of polarization-resolved reflectance measurements. Our results represent a step toward integrated nano-photonics in the telecom regime and open promising opportunities for the development of compact nonlinear optical devices.

Sensitivity of gold nanoparticles Second Harmonic scattering to surrounding medium change

Gold nanoparticles are widely used in sensing, notably in colorimetry-based methods, where a color change is associated to the Surface Plasmon Resonance peak shift due to a binding event or an environment modification in the vicinity of the nanoparticles. In this work, we explore the sensitivity of the Second Harmonic response from gold nanoparticles of two different diameters as this response stems principally from the nanoparticle surface at small sizes as opposed to the whole volume of the nanoparticle at larger sizes. The origin of this response is therefore different from that involved in the colorimetric response, the latter being of volume origin. Upon addition of Glycerol to an aqueous solution of nanoparticles, Surface Plasmon Resonance peak shifts are first observed but they cannot fully explain the Second Harmonic intensity changes recorded. Hence, in order to gain further insights into the origin of the changes observed in the experimental data, polarization-resolved Second Harmonic measurements are performed. A mechanism where first a modification of the first hyperpolarizability of the nanoparticles due to the presence of glycerol occurs followed by nanoparticle aggregation is then proposed. The potential alternative use of this nonlinear optical method of Second Harmonic scattering for sensing purposes is then discussed in light of a figure of merit proposed to describe the sensing sensitivity observed.

Polarization-Sensitive Photodetection of Anisotropic 2D Black Arsenic

A lateral phototransistor structure based on mechanically exfoliated multilayer black arsenic (b-As) is produced to test its in-plane anisotropy of photoelectrical properties. First, the morphology and structure of the b-As flake are investigated with respect to light polarization and crystal structure orientation. Then, the Raman modes, demonstrating a strong anisotropic nature of twofold symmetry for in-plane vibrations and fourfold symmetry for out-of-plane vibrations, allow us to define the armchair and zigzag crystal directions. The lateral photodetector structure has been prepared by depositing polar-oriented electrodes with an angular step of 45° correlated along the b-As crystal directions. Angle-resolved electrical transport and polarization-resolved photocurrent measurements show its strong in-plane anisotropic photoelectrical properties when conductance and photocurrent are about 2 times higher across the armchair direction than the zigzag one. The respective photoresponsivity at 980 nm is 0.44 and 0.19 A/W with the dichroic ratio of 2.3. The intrinsic linear dichroism conversion is responsible for the unique orientation selection behavior in polarization-dependent photodetection. The results show that multilayer b-As is a potentially useful material for application in innovative polarization-sensitive photodetectors.

Imaging Low-Temperature Phases of Ice with Polarization-Resolved Hyperspectral Stimulated Raman Scattering Microscopy.

Water freezes into various phases of ice under different cryogenic temperatures and pressure conditions, such as ice Ih and ice XI at normal pressure. Vibrational imaging with high spectral, spatial, and polarization resolutions could provide detailed information on ice, including the phases and crystal orientations at the microscopic level. Here, we report in situ stimulated Raman scattering (SRS) imaging of ice to analyze the vibrational spectral changes of the OH stretching modes associated with the phase transition between ice Ih and ice XI. In addition, polarization-resolved measurements were performed to reveal the microcrystal orientations of the two phases of ice, with the spatial-dependent anisotropy pattern indicating the inhomogeneous distribution of their orientations. Furthermore, the angular patterns were theoretically explained by third-order nonlinear optics with the known crystal symmetries of the ice phases. Our work may provide new opportunities to investigate many intriguing physical chemistry properties of ice under low-temperature conditions.

Optical properties of circular Bragg gratings with labyrinth geometry to enable electrical contacts

We present an optical study of various device designs for electrically contactable circular Bragg grating cavities in labyrinth geometries. To create an electrical connection between the central disk and the surrounding membrane, which are separated through air gaps, we introduce connections between the adjacent rings. We propose to rotate these connections, creating a labyrinth-like structure, to disable waveguiding and keep the mode confinement. To investigate how different arrangements and sizes of the connections affect the optical properties and to find the optimal design, six different layouts with either threefold or fourfold symmetry and one with twofold symmetry are investigated experimentally and by numerical simulations. Reflectivity measurements and simulations show that rotating the connections improves the mode confinement, far-field pattern, and Purcell factor compared to layouts with connections arranged in straight lines. We compare results between different layouts for different connection widths and perform polarization resolved measurements to investigate whether the connections create asymmetries in the photonic confinement that would impede the performance of the device.

Polarization anisotropy and valence band ordering in semipolar (112¯2) AlInN/GaN heterostructures

Semipolar $(11\overline{2}2)$ AlInN/GaN heterostructures on GaN templates were studied using photoluminescence (PL) spectroscopy both at 15 K and at room temperature. The polarization-resolved PL measurements revealed a dominant polarization along the $[11\overline{2}\overline{3}] {c}^{\ensuremath{'}}$ and a weaker signal along the $[1\overline{1}00] m$-direction, i.e., the two in-plane directions of the semipolar $(11\overline{2}2)$ growth plane. We observed slightly different polarization degrees of $0.34\ifmmode\pm\else\textpm\fi{}0.01, 0.25\ifmmode\pm\else\textpm\fi{}0.02$, and $0.20\ifmmode\pm\else\textpm\fi{}0.01$ at room temperature, respectively, depending on the degree of strain relaxation in the $[1\overline{1}00]$ direction. From a theoretical model based on a $\mathbf{k}\ifmmode\cdot\else\textperiodcentered\fi{}\mathbf{p}$ calculation, we find that the transition from the conduction band (CB) to the uppermost valence band (VB) is C for AlInN similar to AlN, followed by the transition A from the CB to the second VB, for a wide range of compositions. Thus, the in-plane transition matrix elements from the CB to the two topmost VBs near the $\mathrm{\ensuremath{\Gamma}}$ point of the Brillouin zone are dominated by ${M}_{[11\overline{2}\overline{3}]}$ for the C transition and by ${M}_{[1\overline{1}00]}$ for the A transition. For the samples under consideration with an energy splitting of about $18\ifmmode\pm\else\textpm\fi{}1\phantom{\rule{4pt}{0ex}}\mathrm{meV}$, there is sizable thermal occupation of the second VB at room temperature, reasonably explaining the experimental results. The results show that AlInN possesses a band structure similar to AlN, which might explain the strong Stokes shift and the large variation in the band-gap values reported previously.

Surface vs bulk contribution to the second-harmonic generation in AlGaAs nanoresonators

We address the surface vs bulk origin of the second-order optical nonlinearity in AlGaAs nanocylinders through polarization-resolved measurements. By comparing numerical simulations accounting just for bulk second-order nonlinearity with experimental results, we show that the surface contribution to second-harmonic generation (SHG) cannot be neglected and depends on the resonant conditions of the nanocylinder. Additionally, our analysis suggests that bulk and surface SHG are competing effects, and that their interference might influence the overall efficiency.

Gate-Tunable Helical Currents in Commensurate Topological Insulator/Graphene Heterostructures.

van der Waals heterostructures made from graphene and three-dimensional topological insulators promise very high electron mobilities, a nontrivial spin texture, and a gate-tunability of electronic properties. Such a combination of advantageous electronic characteristics can only be achieved through proximity effects in heterostructures, as graphene lacks a large enough spin-orbit interaction. In turn, the heterostructures are promising candidates for all-electrical control of proximity-induced spin phenomena. Here, we explore epitaxially grown interfaces between graphene and the lattice-matched topological insulator Bi2Te2Se. For this heterostructure, spin-orbit coupling proximity has been predicted to impart an anisotropic and electronically tunable spin texture. Polarization-resolved second-harmonic generation, Raman spectroscopy, and time-resolved magneto-optic Kerr microscopy are combined to demonstrate that the atomic interfaces align in a commensurate symmetry with characteristic interlayer vibrations. By polarization-resolved photocurrent measurements, we find a circular photogalvanic effect which is drastically enhanced at the Dirac point of the proximitized graphene. We attribute the peculiar gate-tunability to the proximity-induced interfacial spin structure, which could be exploited for, e.g., spin filters.

Sub-diffraction-limit Fourier-plane laser scanning microscopy

Resolving features that are smaller than the diffraction limit is an intricate yet fascinating challenge that many scientists are working on. Heretofore, most techniques that can circumvent this resolution limit, such as super-resolution microscopy or electron microscopy, lead to a permanent modification of the sample. Consequently, noninvasive approaches are of special interest. Here we introduce an all-linear far-field measurement and imaging modality for the investigation of ensembles of sub-diffraction-limit sized nanostructures. Our technique is based on laser scanning, polarization resolved Fourier-plane measurements and optimizing a theoretical model of the investigated system to resemble the measurement. As an experimental demonstration, we apply this method to gold nanoparticle clusters and derive their positions and respective sizes with an accuracy down to several nanometers, even if multiple particles are located directly adjacent. Our technique showcases the capabilities of microscopy techniques when combined with careful analysis of light scattered off a specimen.

Boosting Second-Harmonic Generation in Monolayer Rhenium Disulfide by Reversible Laser Patterning

Active modification and control of transition metal dichalcogenides (TMDs) properties are highly desirable for next-generation optoelectronic applications. In particular, controlling one of the most important characteristics of TMDs─their crystal structure and symmetry─may open means for manipulating their optical nonlinearities and electrical transport properties. Here, we show that a monolayer ReS2, which does not have a broken inversion symmetry due to its stable 1T′-distorted phase and correspondingly shows only weak second-harmonic generation (SHG), can produce a significantly enhanced (∼2 orders of magnitude) SHG upon reversible laser patterning. This enhancement can be explained by the laser-induced transition from centrosymmetric 1T′ to noncentrosymmetric 2H-phase. This hypothesis is confirmed by polarization-resolved SHG measurements, which reveal a gradual change from the 2-fold to 6-fold symmetry profiles upon laser patterning. Additionally, we found that laser patterning of the bilayer ReS2 samples, contrary to the monolayers, leads to a substantially reduced SHG signal. This result corroborates the 1T′-to-2H laser-induced phase transition. Finally, we show that the laser-induced patterning is reversible by heat. These results open a possibility to actively and reversibly control the crystal structure of mono- and few-layer ReS2 and thus its optical and electronic properties.

Quasi-BIC Mode Lasing in a Quadrumer Plasmonic Lattice.

Plasmonic lattices of metal nanoparticles have emerged as an effective platform for strong light–matter coupling, lasing, and Bose–Einstein condensation. However, the full potential of complex unit cell structures has not been exploited. On the other hand, bound states in continuum (BICs) have attracted attention, as they provide topologically protected optical modes with diverging quality factors. Here, we show that quadrumer nanoparticle lattices enable lasing in a quasi-BIC mode with a highly out-of-plane character. By combining theory with polarization-resolved measurements of the emission, we show that the lasing mode has a topological charge. Our analysis reveals that the mode is primarily polarized out-of-plane as a result of the quadrumer structure. The quality factors of the out-of-plane BIC modes of the quadrumer array can be exceedingly high. Our results unveil the power of complex multiparticle unit cells in creating topologically protected high-Q modes in periodic nanostructures.

Angle-Resolved Spectrophotometry for the Optical Characterization of Material Surfaces

Surface reflectance is a practical metric of the optical performance of a material. Applications, such as glass manufacturing, light sensing, satellite reflectors, and photovoltaics, depend on their reflectance properties and generalized optical performance. Reflectance measurements are rarely reported comprehensively, with only a single angle of incidence common in most datasets. Here, we present a new spectrophotometry system capable of performing angle-, wavelength-, and polarization-resolved reflectance measurements on various surfaces. Data from such a system yields significant information regarding the everyday, real-world performance of said materials. We perform exemplar studies by characterizing several standard thin-film antireflectance coatings and comparing the results to their known theoretical optical response. We also present results from measurements on an optical insulating material as well as a selection of wall paints to showcase the versatility of the technique. We highlight the parallels between measurement and theory, while analyzing the realistic implications of the measurements on their respective material’s practical performance under real-world conditions.