Spin polarized excitons induced by spin injection from magnetic ion to a single quantum dot, has been considered as a basic unit of quantum information transfer between spin and photon for spin-photonic applications. However, this state-of-the-art technology has only been found with limited coupling strength and weak excitonic emission. Here, we demonstrate a spin-polarized self-trapped exciton naturally formed in the zero-dimensional lattice of cesium copper iodide. Upon excitation, the conversion from Cu + ion to spin-1/2 Cu 2+ ion results in an in-situ self-trapped exciton, which facilitates a local Jahn-Teller distortion and guarantees the strong spin-exciton coupling and near-unity excitonic emission efficiency. Consequently, a giant Zeeman splitting of −53 meV and an effective excitonic g-factor of −93.5 are observed from magneto-photoluminescence. More importantly, this nano-scale coupling can also be driven by an external electric field, which generates electroluminescence with a circular polarization of 44.5% at 4.2 K and 8% at 300 K. The spin-optic properties of this copper compound will stimulate the fabrication of next-generation spin-photonic devices based on self-trapped excitons.

GaAsBi nanowires have emerged as a promising material platform for optoelectronics in the near-infrared spectral range, combining the optoelectronic advantages of semiconductor nanowires with the high-band gap tunability of the GaAsBi alloy. The considerable size mismatch between bismuth and arsenic atoms leads to lattice disorder in GaAsBi, causing the localization of excitons/carriers at Bi cluster states. Understanding the impact of this localization on exciton-carrier dynamics is vital for technological implementation. In this study, we use time-resolved photoluminescence spectroscopy to investigate these important effects in GaAs/GaAsBi core/shell nanowires. We find that the emission from Bi cluster states exhibits stretched exponential decay behavior, arising from exciton-hole hopping between cluster states. Moreover, the revealed Bi cluster states are found to be surprisingly deep, with binding energies exceeding 300 meV-much larger than that typically observed in planar GaAsBi. Notably, this strong localization persists even up to room temperature. Finally, we demonstrate that postgrowth thermal annealing can lead to a redistribution of Bi atoms, enhancing the rate of intercluster hopping and reducing the rate of nonradiative recombination. These results highlight a critical role of localization in exciton/carrier dynamics and emphasize the distinctive differences between nanowire and planar structures as well as the need for proper understanding and control of the atomic arrangement in highly mismatched alloys.

To realize the optical transfer of electron spin information, developing a semiconductor layer for efficient transport of spin-polarized electrons to the active layers is necessary. In this study, electron spin transport from a GaAs/Al0.3Ga0.7As superlattice (SL) barrier to In0.5Ga0.5As quantum dots (QDs) is investigated at room temperature through a combination of time-resolved photoluminescence and rate equation analysis, separating the two transport processes from the GaAs layer around the QDs and SL barrier. The electron transport time in the SL increases for a thicker quantum well (QW) of SL due to the weaker wavefunction overlap between adjacent QWs. Additionally, the degree of conservation of spin polarization during transport varies with QW thickness. Rate equation analysis demonstrates an electron transport from SL to QDs while maintaining a high spin polarization for thick QWs. The achieved spin-conserved electron transport can be attributed to the combination of electron transport being sufficiently faster than the spin relaxation in SL and the suppressed spin relaxation in the p-doped GaAs layer capping the QDs. The findings indicate that SL is a promising candidate as an electron spin transport layer for optical spin devices.

Due to its attractive electronic properties, the GaNAs alloy is considered a promising material for optoelectronic applications in the near-infrared spectral region. Unfortunately, nitrogen incorporation is also known to lead to material degradation due to the formation of non-radiative defects and strong band tailing effects caused by alloy disorder. In this study, we show that post-growth hydrogenation of GaNAs-based nanowires (NWs) can largely suppress these unwanted effects. First, we find that this treatment results in a more homogeneous electronic structure due to the passivation of nitrogen-related band tail states, without affecting the bandgap energy of the material. Additionally, hydrogenation reduces the density of quantum emitters that are spontaneously formed in dilute nitride NWs upon N incorporation. This leads to spectrally isolated emission lines from these emitters, which is important for creating high-purity single-photon sources. Finally, the treatment improves the overall optical quality of the material, giving an up to threefold increase in the intensity of band-to-band emission after hydrogenation. Our findings, therefore, highlight the potential of hydrogenation as a viable approach for improving material quality and tailoring the optoelectronic properties of GaNAs NWs without compromising their emission wavelength, paving the way for their integration into telecom-compatible photonic devices.

This work investigates exciton localization and dynamics in semiconductor GaNAsP nanowires (NWs) with varying nitrogen concentrations. Through detailed time-resolved photoluminescence studies, we identify a nitrogen composition-dependent difference in exciton transfer between localized states formed due to alloy disorder. With [N] = 0.1%, the localized states exhibit cluster-like, non-interacting behavior, whereas at [N] = 1.1%, a continuous band of localized states is observed. Additionally, the phosphorous incorporation in the NWs appears to enhance the exciton spatial confinement compared to behaviors observed in phosphorous-free GaNAs NWs, emphasizing the role of the alloy composition in the nature of exciton localization. Temperature is highlighted as a significant factor affecting exciton mobility, enabling efficient transfer between the localized states at higher temperatures. This, in turn, influences exciton lifetimes. Our findings, therefore, shed light on the nature of exciton dynamics in GaNAsP NWs, enriching our understanding of these materials and paving the way for their applications in optoelectronics.

Lead-free halide double perovskites (HDPs) have emerged as a new generation of thermochromic materials. However, further materials development and mechanistic understanding are required. Here, a highly stable HDP Cs2NaFeCl6 single crystal is synthesized, and its remarkable and fully reversible thermochromism with a wide color variation from light-yellow to black over a temperature range of 10 to 423 K is investigated. First-principles, density functional theory (DFT)-based calculations indicate that the thermochromism in Cs2NaFeCl6 is an effect of electron-phonon coupling. The temperature sensitivity of the bandgap in Cs2NaFeCl6 is up to 2.52 meVK(-1) based on the Varshni equation, which is significantly higher than that of lead halide perovskites and many conventional group-IV, III-V semiconductors. Meanwhile, this material shows excellent environmental, thermal, and thermochromic cycle stability. This work provides valuable insights into HDPs' thermochromism and sheds new light on developing efficient thermochromic materials.

Solution-processable semiconductors with antiferromagnetic (AFM) order are attractive for future spintronics and information storage technology. Halide perovskites containing magnetic ions have emerged as multifunctional materials, demonstrating a cross-link between structural, optical, electrical, and magnetic properties. However, stable optoelectronic halide perovskites that are antiferromagnetic remain sparse, and the critical design rules to optimize magnetic coupling still must be developed. Here, we combine the complementary magnetometry and electron-spin-resonance experiments, together with first-principles calculations to study the antiferromagnetic coupling in stable Cs2(Ag:Na)FeCl6 bulk semiconductor alloys grown by the hydrothermal method. We show the importance of nonmagnetic monovalence ions at the BI site (Na/Ag) in facilitating the superexchange interaction via orbital hybridization, offering the tunability of the Curie-Weiss parameters between -27 and -210 K, with a potential to promote magnetic frustration via alloying the nonmagnetic BI site (Ag:Na ratio). Combining our experimental evidence with first-principles calculations, we draw a cohesive picture of the material design for B-site-ordered antiferromagnetic halide double perovskites.

We provide direct evidence for a spin-active V4+ defect center, likely in the form of a VO2+ complex, predominantly introduced in single crystals of vanadium-doped Cs2NaInCl6 halide double perovskites grown by the solution-processed hydrothermal method. The defect has C-4v point group symmetry, exhibiting an electron paramagnetic resonance (EPR) spectrum arising from an effective electron spin of S = 1/2 and a nuclear spin of I = 7/2 (corresponding to V-51 with nearly 100% natural abundance). The determined electron g-factor and hyperfine parameter values are g(perpendicular to)= 1.973, g(parallel to) = 1.945, A(perpendicular to) = 180 MHz, and A(parallel to) = 504 MHz, with the principal axis z along a < 001 > crystallographic axis. The controlled growth of V-doped Cs2NaInCl6 in an oxygen-free environment is shown to suppress the V4+ EPR signal. The defect model is suggested to have a VOCl5 octahedral coordination, where one of the nearest-neighbor Cl- of V is replaced by O2-, with octahedral compression along the V-O axis. This VO complex formation competes with the isolated V3+ substitution of In3+, which in turn provides a means for the charge-state tuning of V ions. This finding calls for a better understanding and control of defect formation in solution-grown halide double perovskites, which is critical for optimizing and tailoring material design for solution-processable optoelectronics and spintronics.

Transition metal (TM) ions incorporated into a host from a wide bandgap semiconductor are recognized as a promising system for quantum technologies with enormous potential. In this work, we report on a TM color center in β-Ga2O3 with physical properties attractive for quantum information applications. The center is found to emit at 1.316 μm and exhibits weak coupling to phonons, with optically addressable higher-lying excited states, beneficial for single-photon emission within the telecom range (O-band). Using magneto-photoluminescence (PL) complemented by time-resolved PL measurements, we identify the monitored emission to be internal 1E→3A2 spin-forbidden transitions of a 3d8 TM ion with a spin-triplet ground state—a possible candidate for a spin qubit. We tentatively attribute this color center to a complex involving a sixfold coordinated Cu3+ ion.

In this study, we report a significant enhancement in the performance of GaNAs-based single nanowire lasers through optimization of growth conditions, leading to a lower lasing threshold and higher operation temperatures. Our analysis reveals that these improvements in the laser performance can be attributed to a decrease in the density of localized states within the material. Furthermore, we demonstrate that owing to their excellent nonlinear optical properties, these nanowires support self-frequency conversion of the stimulated emission through second harmonic generation (SHG) and sum-frequency generation (SFG), providing coherent light emission in the cyan-green range. Mode-specific differences in the self-conversion efficiency are revealed and explained by differences in the light extraction efficiency of the converted light caused by the electric field distribution of the fundamental modes. Our work, therefore, facilitates the design and development of multiwavelength coherent light generation and higher-temperature operation of GaNAs nanowire lasers, which will be useful in the fields of optical communications, sensing, and nanophotonics.

Reversible optical property changes in lead-free perovskites have recently received great interest due to their potential applications in smart windows, sensors, data encryption, and various on-demand devices. However, it is challenging to achieve remarkable color changes in their thin films. Here, methylamine gas (CH3NH2, MA(0)) induced switchable optical bleaching of bismuth (Bi)-based perovskite films is demonstrated for the first time. By exposure to an MA(0) atmosphere, the color of Cs2AgBiBr6 (CABB) films changes from yellow to transparent, and the color of Cs3Bi2I9 (CBI) films changes from dark red to transparent. More interestingly, the underlying reason is found to be the interactions between MA(0) and Bi3+ with the formation of an amorphous liquefied transparent intermediate phase, which is different from that of lead-based perovskite systems. Moreover, the generality of this approach is demonstrated with other amine gases, including ethylamine (C2H5NH2, EA(0)) and butylamine (CH3(CH2)(3)NH2, BA(0)), and another compound, Cs3Sb2I9, by observing a similar reversible optical bleaching phenomenon. The potential for the application of CABB and CBI films in switchable smart windows is investigated. This study provides valuable insights into the interactions between amine gases and lead-free perovskites, opening up new possibilities for high-efficiency optoelectronic and stimuli-responsive applications of these emerging Bi-based materials.

We propose a new and unconventional concept of defect-enabled remote spin filtering and demonstrate its capability to generate nearly fully spin-polarized electrons in InAs/GaAs quantum dots and the resulting chiral light. This represents the highest room-temperature conduction-electron spin polarization ever reported in any semiconductor by any approach, paving the way for a range of potential opto-spintronic applications such as spin-LEDs, spin lasers, spin-polarized single-photon sources, and spin-photon interfaces.

Semiconducting nanowires (NWs) fabricated from III–V materials have gained significant attention for their application in advanced optoelectronic devices. Here, the growth of GaAs/GaInNAs/GaAs core-multishell NWs with a triple quantum-well structure, having about 2% N and 20% In, is reported. The NWs are grown via selective area plasma-assisted molecular beam epitaxy on patterned Si(111) substrates with SiO2 mask holes. The nucleation and growth of the GaAs nanowires' core are carried out by Ga-induced vapor–liquid–solid growth at the open holes. Finely controlled, vertically aligned, regular core-multishell NWs with uniform wire length and diameter are obtained with a 96% yield and targeted nitrogen concentrations of 0%, 2%, and 3%. The GaInNAs NWs exhibit a spectral red shift relative to the GaAs NWs' peak. Their emission wavelength increases with the N content reaching up to 1.26 μm, which makes them a promising tool in telecommunication light sources.

Photon energy upconversion, i.e. the conversion of several low-energy photons to a photon of higher energy, offers significant potential for nano-optoelectronics and nanophotonics applications. The primary challenge is to achieve high upconversion efficiency and a broad device performance range, enabling effective upconversion even at low excitation power. This study demonstrates that core/shell semiconductor nanowire heterostructures can exhibit upconversion efficiencies exceeding what was previously reported for semiconductor nanostructures even at a low excitation power of 100 mW/cm2, by a two-photon absorption process through conduction band states of the narrow-bandgap nanowire shell region. By engineering the electric-field distribution of the excitation light inside the NWs, upconversion efficiency can be further improved by eight times. This work showcases the effectiveness of the proposed approach in achieving efficient photon upconversion using core/shell NW heterostructures, resulting in some of the highest upconversion efficiencies reported in semiconductor nanostructures. Additionally, it offers design guidelines for enhancing energy upconversion efficiency.

β-Ga2O3 is a wide bandgap semiconductor that is attractive for various applications, including power electronics, transparent conductive electrodes, etc. Electrical and optical properties of Ga2O3 are affected by the presence of dopants/contaminants and/or intrinsic defects. Here, we investigate the electrical and optical properties of transition metals like Co and Cr since they are often unintentionally present during the growth or used as intentional dopants. This is done by using magnetic resonance spectroscopy and magneto-optical characterization techniques. We determine spin- Hamiltonian parameters of the Cr3+ ground-state and first excited-state as well as the spin-Hamiltonian parameters of Co2+.

GaAsBi nanowires represent a novel and promising material platform for future nano-photonics. However, the growth of high-quality GaAsBi nanowires and GaAsBi alloy is still a challenge due to a large miscibility gap between GaAs and GaBi. In this work we investigate effects of Bi incorporation on lattice dynamics and carrier recombination processes in GaAs/GaAsBi core/shell nanowires grown by molecular-beam epitaxy. By employing photoluminescence (PL), PL excitation, and Raman scattering spectroscopies complemented by scanning electron microscopy, we show that increasing Bi-beam equivalent pressure (BEP) during the growth does not necessarily result in a higher alloy composition but largely affects the carrier localization in GaAsBi. Specifically, it is found that under high BEP, bismuth tends either to be expelled from a nanowire shell towards its surface or to form larger clusters within the GaAsBi shell. Due to these two processes the bandgap of the Bi-containing shell remains practically independent of the Bi BEP, while the emission spectra of the NWs experience a significant red shift under increased Bi supply as a result of the localization effect.

Nonlinear effects and dynamics are found in a wide range of research fields. In magnetic materials, nonlinear spin dynamics enables ultrafast manipulation of spin, which promises high-speed nonvolatile information processing and storage for future spintronic applications. However, a nonlinear spin response is not yet demonstrated in a nonmagnetic material that lacks strong magnetic interactions. Dilute nitride III-V materials, e.g., (Ga, N)As, have the ability to amplify the conduction-electron-spin polarization by filtering out minority spins via spin-polarized defect states at room temperature. Here, by employing coupled rate equations, we theoretically demonstrate the emergence of a nonlinear spin response in such a defect-enabled room-temperature spin amplifier. Furthermore, we showcase the proposed spin nonlinearity in a (Ga, N)As-InAs quantum dot (QD) coupled all-semiconductor nanostructure, by measuring the higher-harmonic generation, which converts the modulation of excitation polarization into the second-, third-, and fourth-order harmonic oscillations of the QD's photoluminescence intensity and polarization. The observed spin nonlinearity originates from defect-mediated spin-dependent recombination, which can be conveniently tuned with an external magnetic field and can potentially operate at a speed exceeding 1 GHz. The demonstrated spin nonlinearity could pave the way for nonlinear spintronic and optospintronic device applications based on nonmagnetic semiconductors with simultaneously achievable high operation speed and nonlinear response.

Phonon-phonon and electron/exciton-phonon coupling play a vitally important role in thermal, electronic, as well as optical properties of metal halide perovskites. In this work, we evaluate phonon anharmonicity and coupling between electronic and vibrational excitations in novel double perovskite Cs2NaFeCl6 single crystals. By employing comprehensive Raman measurements combined with first-principles theoretical calculations, we identify four Raman-active vibrational modes. Polarization properties of these modes imply Fm3̅m symmetry of the lattice, indicative for on average an ordered distribution of Fe and Na atoms in the lattice. We further show that temperature dependence of the Raman modes, such as changes in the phonon line width and their energies, suggests high phonon anharmonicity, typical for double perovskite materials. Resonant multiphonon Raman scattering reveals the presence of high-lying band states that mediate strong electron-phonon coupling and give rise to intense nA1g overtones up to the fifth order. Strong electron-phonon coupling in Cs2NaFeCl6 is also concluded based on the Urbach tail analysis of the absorption coefficient and the calculated Fröhlich coupling constant. Our results, therefore, suggest significant impacts of phonon-phonon and electron-phonon interactions on electronic properties of Cs2NaFeCl6, important for potential applications of this novel material.

We report the firstobservation of second harmonic generation (SHG)from halide double perovskites single crystals, a promising classof materials for low-cost and versatile optoelectronic applications,owing to their enormous structural flexibility and environmental friendliness.We show that the SHG efficiency of these materials with centrosymmetriccrystalline structures critically depends on the measurement temperature.At high temperatures, it is determined by a surface contribution butincreases by up to 3 orders of magnitude at low temperatures (T < 137 K for Cs2NaFeCl6 and T < 250 K for Cs2AgBiBr6) underlight illumination within several minutes. We attribute this enhancementto the build-up of a light-induced electric field within the near-surfaceregion, which generates an additional contribution to the SHG process.This DC electric field is found to be predominantly oriented orthogonallyto the sample surface, as deduced from the six-fold rotational symmetryof the SHG azimuthal pattern. The electric field formation is explainedby photoinduced charge transfer from deep surface-related states totraps in the bulk region or vice versa, mainly driven by diffusion.Furthermore, the inscribed electric field can be maintained for hoursat low temperatures and can only be erased by raising the temperaturedue to carrier detrapping. Our findings, therefore, highlight theimportance of the surface states in double perovskites, which couldbe utilized for enhancing the nonlinear properties of these centrosymmetricmaterials.