Photoluminescence Polarization Research Articles

Degree of polarization of luminescence from InP under SiN stripes: fits to FEM simulations

Fits of 3D finite element method (FEM) simulations to the degree of polarization (DOP) of photoluminescence (PL) measured on facets under SiN stripes on InP substrates are presented. The measured data is low noise and the fits are remarkably good; lobes owing to defects (perhaps dislocations) can be seen in false colour maps of the residues from the least squares fits. It is found that the vast majority (estimated to be > 99%) of the DOP patterns can be attributed to an initial condition for the FEM simulations of biaxial strain in the SiN stripes. In addition to the fits of FEM simulations to the data and discussion of the fits: fits of error functions to PL data to find the resolution of the optical system and the location of the top surface, quantities that are required in fits of 3D FEM simulations to the data, are presented; as is presented some historical information on analysis of luminescent III-V materials and devices by analysis of the DOP of the luminescence, and some information on the dependence of the DOP of luminescence on strain for InP.

Persistent room-temperature valley polarization in graphite-filtered WS2 monolayer

Transition metal dichalcogenide (TMD) monolayers (1L) in the 2H-phase are two-dimensional semiconductors with two valleys in their band structure that can be selectively populated using circularly polarized light. The choice of the substrate for monolayer TMDs is an essential factor for the optoelectronic properties and for achieving a high degree of valley polarization at room temperature (RT). In this work, we investigate the RT valley polarization of monolayer WS2 on different substrates. A degree of polarization of photoluminescence (PL) in excess of 27% is found from neutral excitons in 1L-WS2 on graphite at RT, under resonant excitation. Using chemical doping through photochlorination we modulate the polarization of the neutral exciton emission from 27% to 38% for 1L-WS2/graphite. We show that the valley polarization strongly depends on the interplay between doping and the choice of the supporting layer of TMDs. Time-resolved PL measurements, corroborated by a rate equation model accounting for the bright exciton population in the presence of a dark exciton reservoir support our findings. These results suggest a pathway towards engineering valley polarization and exciton lifetimes in TMDs, by controlling the carrier density and/or the dielectric environment at ambient conditions.

Layer-dependent optically induced spin polarization in InSe

Optical control of spin in semiconductors has been pioneered using nanostructures of III-V and II-VI semiconductors, but the emergence of two-dimensional van der Waals materials offers an alternative low-dimensional platform for spintronic phenomena. Indium selenide (InSe), a group-III monochalcogenide van der Waals material, has shown promise for opto-electronics due to its high electron mobility, tunable direct bandgap, and quantum transport. There are predictions of spin-dependent optical selection rules suggesting potential for all-optical excitation and control of spin in a two-dimensional layered material. Despite these predictions, layer-dependent optical spin phenomena in InSe have yet to be explored. Here, we present measurements of layer-dependent optical spin dynamics in few-layer and bulk InSe. Polarized photoluminescence reveals layer-dependent optical orientation of spin, thereby demonstrating the optical selection rules in few-layer InSe. Spin dynamics are also studied in many-layer InSe using time-resolved Kerr rotation spectroscopy. By applying out-of-plane and in-plane static magnetic fields for polarized emission measurements and Kerr measurements, respectively, the $g$-factor for InSe was extracted. Further investigations are done by calculating precession values using a $\textbf{k} \cdot \textbf{p}$ model, which is supported by \textit{ab-initio} density functional theory. Comparison of predicted precession rates with experimental measurements highlights the importance of excitonic effects in InSe for understanding spin dynamics. Optical orientation of spin is an important prerequisite for opto-spintronic phenomena and devices, and these first demonstrations of layer-dependent optical excitation of spins in InSe lay the foundation for combining layer-dependent spin properties with advantageous electronic properties found in this material.

Nanoimprinted 2D-Chiral Perovskite Nanocrystal Metasurfaces for Circularly Polarized Photoluminescence.

The versatile hybrid perovskite nanocrystals (NCs) are one of the most promising materials for optoelectronics by virtue of their tunable bandgaps and high photoluminescence (PL) quantum yields. However, their inherent crystalline chemical structure limits the chiroptical properties achievable with the material. The production of chiral perovskites has become an active field of research for its promising applications in optics, chemistry, or biology. Typically, chiral halide perovskites are obtained by the incorporation of different chiral moieties in the material. Unfortunately, these chemically modified perovskites have demonstrated moderate values of chiral PL so far. Here, a general and scalable approach is introduced to produce chiral PL from arbitrary nanoemitters assembled into 2D-chiral metasurfaces. The fabrication via nanoimprinting lithography employs elastomeric molds engraved with chiral motifs covering millimeter areas that are used to pattern two types of unmodified colloidal perovskite NC inks: green-emissive CsPbBr3 and red-emissive CsPbBr1 I2 . The perovskite 2D-metasurfaces exhibit remarkable PL dissymmetry factors (glum ) of 0.16 that can be further improved up to glum of 0.3 by adding a high-refractive-index coating on the metasurfaces. This scalable approach to produce chiral photoluminescent thin films paves the way for the seamless production of bright chiral light sources for upcoming optoelectronic applications.

Anisotropically Fused Clusters Form a 2D Superatomic Sheet Exhibiting Polarized Light Emission

Polarized light emission is desirable for a number of optoelectronic applications and is difficult to realize in conventional semiconductors. Here we take advantage of the tunability in structure, symmetry, and functionality of superatomic semiconductors, i.e., crystalline arrays of atomically precise polyatomic clusters. We report the in-plane anisotropy in electronic and optical properties in the van der Waals two-dimensional (2D) superatomic semiconductor CsRe6Se8I3. Consistent with structural anisotropy within the 2D plane, CsRe6Se8I3 shows linearly polarized photoluminescence (PL) emission at room temperature. By lowering the temperature, we observe a new PL peak with nearly orthogonal linear polarization without an accompanying structural phase transition. Theoretical calculations together with spectroscopic measurements suggest that the high- and low-temperature PL peaks originate, respectively, from direct and indirect excitons. These results demonstrate rich optical properties of superatomic solids, which may be precisely programmed with the hierarchical design of the constituent clusters and the intercluster bonding.

Circularly Polarized Photoluminescence from Nanostructured Arrays of Light Emitters

Strategically designed metamaterials can influence the properties of light emitters in several ways, including shaping of the directionality and polarization of luminescence. These properties, however, are limited in systems where the luminophores uniformly coat the metamaterial. Here, we study and design metamaterials composed of both Au nanobars and nanopatterned light emitters. We systematically investigate the role of spatial averaging, dipole orientation, chirality, near-field effects, and other factors for these multimaterial systems. Finally, we discuss multiple design routes to create metasurfaces that can emit photoluminescence of any circular polarization at any arbitrary angle. These systems simultaneously exhibit high photoluminescence intensity and tailored, directional, and polarized photoluminescence.

Observation of optical anisotropy and a linear dichroism transition in layered silicon phosphide.

The investigation of in-plane two-dimensional (2D) anisotropic materials has garnered significant attention due to their exceptional electronic, optical, and mechanical characteristics. The anisotropic optical properties and angle-dependent photodetectors based on 2D anisotropic materials have been extensively studied. However, novel in-plane anisotropic materials still need to be explored to satisfy for distinct environments and devices. Here, we report the remarkable anisotropic behavior of excitons and demonstrate a unique linear-dichroism transition of absorption between ultraviolet and visible light in layered silicon phosphide (SiP) through the analysis of polarization photoluminescence (PL) and absorbance spectra. Its high absorption linear dichroism ratio of 1.16 at 388 nm, 1.15 at 532 nm, and 1.19 at 733 nm is revealed, suggesting the brilliant non-isotropic responses. The robust periodic variation of the A1 and A2 Raman modes in 2D SiP materials allows for the determination of their crystal orientation. Furthermore, the presence of indirect excitons with phonon sidebands in the temperature-dependent PL spectra exhibits non-monotonic energy shifts with increasing temperature, which is attributed to an enhanced electron-phonon interaction and thermal expansion. Our findings provide valuable insights into the fundamental physical properties of layered SiP and offer guidelines for designing polarization-sensitive photodetectors and angle-dependent devices based on 2D anisotropic materials.

Twist-angle-dependent momentum-space direct and indirect interlayer excitons in WSe2/WS2 heterostructure.

Interlayer excitons (ILEs) in the van der Waals (vdW) heterostructures of type-II band alignment transition metal dichalcogenides (TMDCs) have attracted significant interest owing to their unique exciton properties and potential in quantum information applications. However, the new dimension that emerges with the stacking of structures with a twist angle leads to a more complex fine structure of ILEs, presenting both an opportunity and a challenge for the regulation of the interlayer excitons. In this study, we report the evolution of interlayer excitons with the twist angle in the WSe2/WS2 heterostructure and identify the direct (indirect) interlayer excitons by combining photoluminescence (PL) and density functional theory (DFT) calculations. Two interlayer excitons with opposite circular polarization assigned to the different transition paths of K-K and Q-K were observed. The nature of the direct (indirect) interlayer exciton was confirmed by circular polarization PL measurement, excitation power-dependent PL measurement and DFT calculations. Furthermore, by applying an external electric field to regulate the band structure of the WSe2/WS2 heterostructure and control the transition path of the interlayer excitons, we could successfully realize the regulation of interlayer exciton emission. This study provides more evidence for the twist-angle-based control of heterostructure properties.

Polarized emission from unidirectionally oriented semiconductor nanorods in light-emitting devices

Unidirectional ordering of colloidal semiconductor nanorods (NRs) is key to taking advantage of anisotropic optical properties of NRs in solid-state devices. In this study, we report long-range orientation of colloidal CdSe/CdS heterostructure NRs by spin coating a mixture of NRs and poly(9-vinylcarbazole) (PVK) molecules on an off-center position of a substrate. Addition of 1,2-dichlorobenzene slows the evaporation of solvent resulting in better orientation with contrast ratio of 2.5 in linear photoluminescence polarization and 2.0 in electroluminescence. Our calculation reveals that the stabilization of the NR assembly is likely a result of depletion energy during spin coating. The retarded evaporation enables the depletion interaction to come into play in the process of NR stacking, hence highly oriented and closely packed NR films. Our findings on unidirectionally assembled NRs in uniform film offer an insight for ordering of anisotropic colloidal nanoparticles.

Photoluminescence Polarization of MAPbBr3 Perovskite Nanostructures. Can the Dielectric Contrast Effect Explain It?

The dielectric contrast effect is usually evoked to explain anisotropy of optical properties of elongated nanoobjects, for example, semiconductor nanowires. We applied two-dimensional polarization imaging microscopy to measure the polarization of photoluminescence (PL) excitation and PL intensity of nanoaggregates of in-situ formed MAPbBr3 perovskite nanoparticles in a stretched polymeric matrix. Scanning electron microscopy images of these objects were also acquired to characterize their sizes and shapes. We find that individual perovskite aggregates with sizes of 100–300 nm often possess a PL excitation polarization degree as high as 0.5–0.9, which is up to three times higher than the polarization degree of absorption predicted by the dielectric contrast effect. Small aggregates of nanoparticles possess an emission polarization degree substantially higher than that of excitation. Computer simulations of many possible scenarios show that the dielectric contrast alone cannot quantitatively explain the polarization properties of the studied objects. We propose energy transfer to localized emitting sites and the dependence of PL yield on excitation power density as possible factors strongly influencing the polarization properties of PL emission and PL excitation, respectively.

Electrochemically Switchable Circularly Polarized Photoluminescence within Self-Assembled Conducting Polymer Helical Microfibers.

Achieving electrically and/or electrochemically controlled circularly polarized photoluminescence (CPL) is challenging due to the non-electroactive characteristics of most chiral materials and the non-electrosensitive feature of materials' chiroptical signals. Here we found that the CPL of self-assembled conducting polyaniline (PANI) helical microfibers could be reversibly switched by applying an alternating electrical bias. The conducting polymer is not the fluorophore but can transfer its chirality to the coassembled aggregation-induced emission (AIE) fluorescent molecules. The electrochemically switchable CPL is derived from the reversible transformation of the chirality of the polyaniline microfibers, which is probably due to the change in the molecular interchain distance upon doping/dedoping. Subsequently, we have demonstrated double-layer information encryption based on the electrochemically reversible CPL and conductance.

New Spin-Polarized Electron Source Based on Alkali Antimonide Photocathode.

New spin-dependent photoemission properties of alkali antimonide semiconductor cathodes are predicted based on the detected optical spin orientation effect and DFT band structure calculations. Using these results, the Na_{2}KSb/Cs_{3}Sb heterostructure is designed as a spin-polarized electron source in combination with the Al_{0.11}Ga_{0.89}As target as a spin detector with spatial resolution. In the Na_{2}KSb/Cs_{3}Sb photocathode, spin-dependent photoemission properties were established through detection of a high degree of photoluminescence polarization and high polarization of the photoemitted electrons. It was found that the multi-alkali photocathode can provide electron beams with emittance very close to the limits imposed by the electron thermal energy. The vacuum tablet-type sources of spin-polarized electrons have been proposed for accelerators, which can exclude the construction of the photocathode growth chambers for photoinjectors.

Photoluminescence microscopy as a noninvasive characterization method for defects in gallium oxide and aluminum gallium oxide epitaxial films

Herein we utilize polarized photoluminescence (PL) microscopy and spectral analysis to locate and characterize many different types of µm-scale extended defects present in melt-grown bulk crystals and metal-organic vapor-phase epitaxy (MOVPE)-grown epitaxial thin films of β-Ga2O3 and β-(Al,Ga)2O3. These include pits, divots, mounds, scratches, rotation domain boundaries, stacking faults, cracks, and other defect categories. Some types of µm-scale defects simply decrease overall PL yield, while others emit different spectra than single crystal regions. We combine PL microscopy with atomic force microscopy (AFM) and scanning electron microscopy (SEM) to provide detailed characteristics of these different types of features which can arise from both bulk crystal growth, surface preparation, and epitaxial growth processes. We show that sample quality (in terms of extended defects) can be determined by using PL and that attributing spectral features to isolated point defects is invalid unless the sample is proven to not contain extended defects.

Engineering WS2 exciton polarization by an anisotropic organic substrate

Controlling the polarization of the emitted light at room temperature is critical for the transition metal dichalcogenides monolayer based photonic devices. One way is to integrate the complicated man-made photonic structures with the monolayer where the photoluminescence (PL) couples with linearly polarized radiation. However, the PL polarization of the monolayer is fixed and cannot be tuned in these structures. In this work, through transferring the WS2 monolayer onto a simple organic β-perylene (Pe) layer, we show the PL of the WS2 monolayer can be linearly polarized by virtue of the coupling with the anisotropic modes, which are created due to the reflection of photons between the surface of the Pe substrate. More importantly, we demonstrate tunable linearly polarized excitonic emission from the WS2 monolayer by varying the thickness of the β-Pe substrate. Our work paves the way to engineer the exciton polarization of 2D materials without complicated fabrication structures at room temperature.

Valley-magnetophonon resonance for interlayer excitons

Heterobilayers consisting of MoSe2 and WSe2 monolayers can host optically bright interlayer excitons with intriguing properties such as ultralong lifetimes and pronounced circular polarization of their photoluminescence due to valley polarization, which can be induced by circularly polarized excitation or applied magnetic fields. Here, we report on the observation of an intrinsic valley-magnetophonon resonance for localized interlayer excitons promoted by invervalley hole scattering. It leads to a resonant increase of the photoluminescence polarization degree at the same field of 24.2 Tesla for H-type and R-type stacking configurations despite their vastly different excitonic energy splittings. As a microscopic mechanism of the hole intervalley scattering we identify the scattering with chiral TA phonons of MoSe2 between excitonic states mixed by the long-range electron hole exchange interaction.

Intrinsic circularly polarized exciton emission in a twisted van der Waals heterostructure

We report the emergence of a significant degree of intrinsic circular polarization of exciton photoluminescence in a twisted ${\mathrm{MoSe}}_{2}/{\mathrm{WSe}}_{2}$ heterostructure upon nonresonant driving with a linearly polarized laser. The effect is not related to the polarization of the incident light. Moreover, it is present at zero magnetic field, and reacts perceptibly to a perpendicularly applied magnetic field that, unexpectedly, can strongly diminish this effect. The giant magnitude of the polarization, which cannot be explained by natural optical activity or circular dichroism of the twisted lattice, suggests a kinematic origin arising from an emergent pyromagnetic symmetry in our structure, which we exploit to gain insight into the microscopic optical processes of our device.

Laser-Patterned Submicrometer Bi2Se3-WS2 Pixels with Tunable Circular Polarization at Room Temperature.

Characterizing and manipulating the circular polarization of light is central to numerous emerging technologies, including spintronics and quantum computing. Separately, monolayer tungsten disulfide (WS2) is a versatile material that has demonstrated promise in a variety of applications, including single photon emitters and valleytronics. Here, we demonstrate a method to tune the photoluminescence (PL) intensity (factor of ×161), peak position (38.4 meV range), circular polarization (39.4% range), and valley polarization of a Bi2Se3-WS2 2D heterostructure using a low-power laser (0.762 μW) in ambient conditions. Changes are spatially confined to the laser spot, enabling submicrometer (814 nm) features, and are long-term stable (>334 days). PL and valley polarization changes can be controllably reversed through laser exposure in a vacuum, allowing the material to be erased and reused. Atmospheric experiments and first-principles calculations indicate oxygen diffusion modulates the exciton radiative vs nonradiative recombination pathways, where oxygen absorption leads to brightening and desorption to darkening.

Optical Rashba Effect in a Light-Emitting Perovskite Metasurface.

The Rashba effect, i.e., the splitting of electronic spin-polarized bands in the momentum space of a crystal with broken inversion symmetry, has enabled the realization of spin-orbitronic devices, in which spins are manipulated by spin-orbit coupling. In optics, where the helicity of light polarization represents the spin degree of freedom for spin-momentum coupling, the optical Rashba effect is manifested by the splitting of optical states with opposite chirality in the momentum space. Previous realizations of the optical Rashba effect relied on passive devices determining the surface plasmon or light propagation inside nanostructures, or the directional emission of chiral luminescence when hybridized with light-emitting media. An active device underpinned by the optical Rashba effect is demonstrated here, in which a monolithic halide perovskite metasurface emits highly directional chiral photoluminescence. An all-dielectric metasurface design with broken in-plane inversion symmetry is directly embossed into the high-refractive-index, light-emitting perovskite film, yielding a degree of circular polarization of photoluminescence of 60% at room temperature.

Photoluminescence of Double Quantum Wells: Asymmetry and Excitation Laser Wavelength Effects

Circularly polarized photoluminescence (PL) spectroscopy measured at 19 K on GaAs/AlGaAs symmetric and asymmetric double quantum wells (DQW) is reported. The PL is obtained by exciting the sample with a circularly polarized (left or right) laser in order to create an initial unbalanced distribution of electron spins in the conduction band and, in this way, obtain the electron spin lifetime . The effects of the excitation laser wavelength are estimated by exciting with laser wavelengths of 701.0, 787.0, 801.5, and 806.5 nm. The increase of with the excitation wavelength is attributed to the lower initial quasimomentum k of the excited carriers, which also reduces spin–orbit relaxation processes. is found to be higher in asymmetric DQWs: this is attributed to the wider QWs in these samples, which reduces spin relaxation due to the Dresselhaus mechanism. In addition, a smaller contribution from the Rashba mechanism is also detected by comparing samples with built‐in electric fields of different orientations defined by doped barrier layers.

Observation of 3D Biexcitons in Pristine-Quality CH3 NH3 PbBr3 Single Crystals.

Halide perovskites (HPs) are fascinating materials whose optoelectronic properties are arguably excitonic. In the HP family, biexcitons are known to exist only in low dimensions where exciton-exciton binding is strongly enhanced by quantum and dielectric confinements. In this paper, however, it is shown that they indeed do exist in 3D bulk CH3 NH3 PbBr3 (MAPbBr3 ) single crystals if the pristine crystal quality is ensured for subtle binding of two excitons. The existence of biexcitons is clearly evidenced below 30 K with a binding energy of ≈3.9 ± 0.3 meV according to i) exciton-biexciton population dynamics, ii) giant resonant two-photon excitation of biexcitons, iii) inverted Boltzmann-type spectral feature, and iv) zero degree of circular polarization in the biexciton photoluminescence. Because of the polariton effect, the two-photon resonance occurs at the excited biexciton state from which longitudinal-transverse splitting is calculated to be 3.7 meV. The discovery of the 3D biexcitons underscores the very quality of HP crystals for generating various many-body excitonic phases in MAPbBr3 and its analogues toward the improved understanding of their fundamental properties and highly efficient optoelectronic applications.