Twist angle-dependent valley polarization switching in heterostructures.

The twist engineering of moiré superlattice in van der Waals heterostructures of transition metal dichalcogenides can manipulate valley physics of interlayer excitons (IXs), paving the way for next-generation valleytronic devices. However, the twist angle-dependent control of excitonic potential on valley polarization is not investigated so far in electrically controlled heterostructures and the physical mechanism underneath needs to be explored. Here, we demonstrate the dependence of both polarization switching and degree of valley polarization on the moiré period. We also find the mechanisms to reveal the modulation of twist angle on the exciton potential and the electron-hole exchange interaction, which elucidate the experimentally observed twist angle-dependent valley polarization of IXs. Furthermore, we realize the valley-addressable devices based on polarization switch. Our work demonstrates the manipulation of the valley polarization of IXs by tunning twist angle in electrically controlled heterostructures, which opens an avenue for electrically controlling the valley degrees of freedom in twistronic devices.

Charge transport mechanisms of PbSnSe2 and observation of transition from direct to Fowler-Nordheim tunneling.

In this study, we report the observation of various conduction mechanisms in mechanically exfoliated PbSnSe2 based on temperature-dependent current and voltage characteristics. A transition from direct tunneling to Fowler-Nordheim tunneling in PbSnSe2 was observed at 2.63 V. At lower temperatures, the 3D Mott variable range hopping model fits the data, yielding a density of states of ∼8.80 × 1020 eV-1 cm-3 at 2 V. The values of Whop and Rhop were 64 meV and 22.7 nm, respectively, at 250 K. The Poole-Frenkel conduction was observed in the Au/PbSnSe2/Au device and the dielectric constant of PbSnSe2 was calculated to be 1.4. At intermediate voltages, a space charge limited current with an exponential distribution of traps was observed and a trap density of ∼9.53 × 1013 cm-3 and a trap characteristic temperature of 430 K were calculated for the Au/PbSnSe2/Au device.

Revealing broken valley symmetry of quantum emitters in WSe2 with chiral nanocavities.

Single photon emission of quantum emitters (QEs) carrying internal degrees of freedom such as spin and angular momentum plays an important role in quantum optics. Recently, QEs in two-dimensional semiconductors have attracted great interest as promising quantum light sources. However, whether those QEs are characterized by the same valley physics as delocalized valley excitons is still under debate. Moreover, the potential applications of such QEs still need to be explored. Here we show experimental evidence of valley symmetry breaking for neutral QEs in WSe2 monolayer by interacting with chiral plasmonic nanocavities. The anomalous magneto-optical behaviour of the coupled QEs suggests that the polarization state of emitted photon is modulated by the chiral nanocavity instead of the valley-dependent optical selection rules. Calculations of cavity quantum electrodynamics further show the absence of intrinsic valley polarization. The cavity-dependent circularly polarized single-photon output also offers a strategy for future applications in chiral quantum optics.

Photoinduced Phase Transition in Infinite-Layer Nickelates.

The quantum phase transition caused by regulating the electronic correlation in strongly correlated quantum materials has been a research hotspot in condensed matter science. Herein, a photon-induced quantum phase transition from the Kondo-Mott insulating state to the low temperature metallic one accompanying with the magnetoresistance changing from negative to positive in the infinite-layer NdNiO2 films is reported, where the antiferromagnetic coupling among the Ni1+ localized spins and the Kondo effect are effectively suppressed by manipulating the correlation of Ni-3d and Nd-5d electrons under the photoirradiation. Moreover, the critical temperature Tc of the superconducting-like transition exhibits a dome-shaped evolution with the maximum up to ≈42 K, and the electrons dominate the transport process proved by the Hall effect measurements. These findings not only make the photoinduction a promising way to control the quantum phase transition by manipulating the electronic correlation in Mott-like insulators, but also shed some light on the possibility of the superconducting in electron-doped nickelates.

Controllable spin-resolved photon emission enhanced by a slow-light mode in photonic crystal waveguides on a chip.

We report the slow-light enhanced spin-resolved in-plane emission from a single quantum dot (QD) in a photonic crystal waveguide (PCW). The slow light dispersions in PCWs are designed to match the emission wavelengths of single QDs. The resonance between two spin states emitted from a single QD and a slow light mode of a waveguide is investigated under a magnetic field with Faraday configuration. Two spin states of a single QD experience different degrees of enhancement as their emission wavelengths are shifted by combining diamagnetic and Zeeman effects with an optical excitation power control. A circular polarization degree up to 0.81 is achieved by changing the off-resonant excitation power. Strongly polarized photon emission enhanced by a slow light mode shows great potential to attain controllable spin-resolved photon sources for integrated optical quantum networks on chip.

Magnetoelectric coupling in multiferroics probed by optical second harmonic generation.

Magnetoelectric coupling, as a fundamental physical nature and with the potential to add functionality to devices while also reducing energy consumption, has been challenging to be probed in freestanding membranes or two-dimensional materials due to their instability and fragility. In this paper, we report a magnetoelectric coupling probed by optical second harmonic generation with external magnetic field, and show the manipulation of the ferroelectric and antiferromagnetic orders by the magnetic and thermal fields in BiFeO3 films epitaxially grown on the substrates and in the freestanding ones. Here we define an optical magnetoelectric-coupling constant, denoting the ability of controlling light-induced nonlinear polarization by the magnetic field, and found the magnetoelectric-coupling was suppressed by strain releasing but remain robust against thermal fluctuation for freestanding BiFeO3.

The Evolution of Band Topology in Two-Dimensional Weyl Half-Metals.

Two-dimensional ferromagnetic Weyl half-metals that are robust against spin-orbital coupling were theoretically proposed recently, in which the nodal points and the nodal loops are protected by specific symmetries. As the symmetry of a ferromagnetic material is highly dependent on the magnetization orientation, here we predict a family of two-dimensional ferromagnetic Weyl half-metals, Mn2X3 (X = S, Se, Te) monolayers, to investigate the band topology under different magnetization orientations in the presence of spin-orbital coupling. The Curie temperatures (∼1000 K) were estimated to be much higher than room temperature due to the strong double exchange interaction and the suppression of spin fluctuation for the two-sublayer structure. Taking a Mn2Te3 monolayer as an example, we demonstrated the evolution of the nodal points and the nodal loops in the presence of spin-orbital coupling via manipulating magnetization orientation. Our work provides a family of high temperature two-dimensional ferromagnetic Weyl half-metals for investigating the nontrivial band topology.

Single charge control of localized excitons in heterostructures with ferroelectric thin films and two-dimensional transition metal dichalcogenides.

Single charge control of localized excitons (LXs) in two-dimensional transition metal dichalcogenides (TMDCs) is crucial for potential applications in quantum information processing and storage. However, traditional electrostatic doping method by applying metallic gates onto TMDCs may cause inhomogeneous charge distribution, optical quenching, and energy loss. Herein, by locally controlling the ferroelectric polarization of the ferroelectric thin film BiFeO3 (BFO) with a scanning probe, we can deterministically manipulate the doping type of monolayer WSe2 to achieve p-type and n-type doping. This nonvolatile approach can maintain the doping type and hold the localized excitonic charges for a long time without applied voltage. Our work demonstrated that the ferroelectric polarization of BFO can control the charges of LXs effectively. Neutral and charged LXs have been observed in different ferroelectric polarization regions, confirmed by magnetic optical measurement. Highly circular polarization degree with 90% photon emission from these quantum emitters was achieved in high magnetic fields. Controlling the single charge of LXs in a non-volatile way shows a great potential for deterministic photon emission with desired charge states for photonic long-term memory.

Manipulating the electronic structure and physical properties in monolayer Mo2I3Br3via strain and doping.

Identifying new two-dimensional intrinsic ferromagnets with high transition temperatures is a key step of improving device performance. Here we used first-principles calculations to demonstrate that the monolayer Janus Mo2I3Br3 is an intrinsic ferromagnetic bipolar semiconductor with a large out-of-plane spin orientation. The calculated phonon dispersion and ab initio molecular dynamic simulations indicate the stability dynamically and thermally. Furthermore, we investigated the effect of electrostatic doping or in-plane biaxial strain on the electronic structures and magnetic and optical properties of monolayer Mo2I3Br3. We find that the magnetic anisotropy energy and Curie temperature are enhanced more than 4 and 2 times with the hole doping compared with those in the pristine monolayer Mo2I3Br3, respectively. The calculated electronic structures show that the stable half-metallic states are formed by electron or hole doping due to the strong spin polarization of the electronic states around the Fermi level. Furthermore, the spin orientation in the metallic channel of the doped monolayer Mo2I3Br3 can be flipped with the increase of electron doping concentration. In addition, the magnetic anisotropy energy and Curie temperature can also be effectively manipulated by in-plane biaxial strain. The spin polarization of the conduction band minimum can be reversed by the tensile strain of 3% for the monolayer Mo2I3Br3, transforming it into an indirect band gap semiconductor. Finally, the calculated large and tunable optical absorption coefficient indicates that monolayer Mo2I3Br3 is a promising candidate for potential optoelectronic applications. Our results may open up more opportunities for few-layer van der Waals crystals in magnetic storage, spintronics, and optoelectronic devices.

Enhanced Valley Polarization in WS2 /LaMnO3 Heterostructure.

Monolayer transition metal dichalcogenides have attracted great attention for potential applications in valleytronics. However, the valley polarization degree is usually not high because of the intervalley scattering. Here, a largely enhanced valley polarization up to 80% in monolayer WS2 under nonresonant excitation at 4.2 K is demonstrated using WS2 /LaMnO3 thin film heterostructure, which is much higher than that for monolayer WS2 on SiO2 /Si substrate with a valley polarization of 15%. Furthermore, the greatly enhanced valley polarization can be maintained to a high temperature of about 160 K with a valley polarization of 53%. The temperature dependence of valley polarization is strongly correlated with the thermomagnetic curve of LaMnO3 , indicating an exciton-magnon coupling between WS2 and LaMnO3 . A simple model is introduced to illustrate the underlying mechanisms. The coupling of WS2 and LaMnO3 is further confirmed with an observation of two interlayer excitons with opposite valley polarizations in the heterostructure, resulting from the spin-orbit coupling induced splitting of the conduction bands in monolayer transition metal dichalcogenides. The results provide a pathway to control the valleytronic properties of transition metal dichalcogenides by means of ferromagnetic van der Waals engineering, paving a way to practical valleytronic applications.

Strong Light-Matter Interactions between Gap Plasmons and Two-Dimensional Excitons under Ambient Conditions in a Deterministic Way.

Strong exciton-plasmon interactions between layered two-dimensional (2D) semiconductors and gap plasmons show a great potential to implement cavity quantum electrodynamics under ambient conditions. However, achieving a robust plasmon-exciton coupling with nanocavities is still very challenging, because the layer area is usually small in the conventional approaches. Here, we report on a robust strong exciton-plasmon coupling between the gap mode of a bowtie and the excitons in MoS2 layers with gold-assisted mechanical exfoliation and nondestructive wet transfer techniques for a large-area layer. Due to the ultrasmall mode volume and strong in-plane field, the estimated effective exciton number contributing to the coupling is largely reduced. With a corrected exciton transition dipole moment, the exciton numbers are extracted as being 40 for the case of a single layer and 48 for eight layers. Our work paves the way to realize strong coupling with 2D materials with a small number of excitons at room temperature.

Optimization and robustness of the topological corner state in second-order topological photonic crystals.

The second-order topological photonic crystal with the 0D corner state provides a new way to investigate cavity quantum electrodynamics and develop topological nanophotonic devices with diverse functionalities. Here, we report on the optimization and robustness of the topological corner state in the second-order topological photonic crystal both in theory and in experiment. The topological nanocavity is formed based on the 2D generalized Su-Schrieffer-Heeger model. The quality factor of the corner state is optimized theoretically and experimentally by changing the gap between two photonic crystals or just modulating the position or size of the airholes surrounding the corner. The fabricated quality factors are further optimized by the surface passivation treatment which reduces surface absorption. A maximum quality factor of the fabricated devices is about 6000, which is the highest value ever reported for the active topological corner state. Furthermore, we demonstrate the robustness of the corner state against strong disorders including the bulk defect, edge defect, and even corner defect. Our results lay a solid foundation for further investigations and applications of the topological corner state, such as the investigation of a strong coupling regime and the development of optical devices for topological nanophotonic circuitry.

Self-Catalyzed AlGaAs Nanowires and AlGaAs/GaAs Nanowire-Quantum Dots on Si Substrates.

Self-catalyzed AlGaAs nanowires (NWs) and NWs with a GaAs quantum dot (QD) were monolithically grown on Si(111) substrates via solid-source molecular beam epitaxy. This growth technique is advantageous in comparison to the previously employed Au-catalyzed approach, as it removes Au contamination issues and renders the structures compatible with complementary metal-oxide-semiconductor (CMOS) technology applications. Structural studies reveal the self-formation of an Al-rich AlGaAs shell, thicker at the NW base and thinning towards the tip, with the opposite behavior observed for the NW core. Wide alloy fluctuations in the shell region are also noticed. AlGaAs NW structures with nominal Al contents of 10, 20, and 30% have strong room temperature photoluminescence, with emission in the range of 1.50-1.72 eV. Individual NWs with an embedded 4.9 nm-thick GaAs region exhibit clear QD behavior, with spatially localized emission, both exciton and biexciton recombination lines, and an exciton line width of 490 µeV at low temperature. Our results demonstrate the properties and behavior of the AlGaAs NWs and AlGaAs/GaAs NWQDs grown via the self-catalyzed approach for the first time and exhibit their potential for a range of novel applications, including nanolasers and single-photon sources.

Emergent Magnetic Phenomenon with Unconventional Structure in Epitaxial Manganate Thin Films.

A variety of emergent phenomena are enabled by interface engineering in the complex oxides heterostructures. While extensive attention is attracted to LaMnO3 (LMO) thin films for observing the control of functionalities at its interface with substrate, the nature of the magnetic phases in the thin film is, however, controversial. Here, it is reported that the ferromagnetism in two and five unit cells thick LMO films epitaxially deposited on (001)-SrTiO3 substrates, a ferromagnetic/ferromagnetic coupling in eight and ten unit cells ones, and a striking ferromagnetic/antiferromagnetic pinning effect with apparent positive exchange bias in 15 and 20 unit cells ones are observed. This novel phenomenon in both 15 and 20 unit cells films indicates a coexistence of three magnetic orderings in a single LMO film. The high-resolution scanning transmission electron microscopy suggests a P21/n to Pbnm symmetry transition from interface to surface, with the spatial stratification of MnO6 octahedral morphology, corresponding to different magnetic orderings. These results can shed some new lights on manipulating the functionality of oxides by interface engineering.

Enhanced emission from a single quantum dot in a microdisk at a deterministic diabolical point.

We report on controllable cavity modes by controlling the backscattering by two identical scatterers. Periodic changes of the backscattering coupling between two degenerate cavity modes are observed with the changing angle between two scatterers and elucidated by a theoretical model using two-mode approximation and numerical simulations. The periodically appearing single-peak cavity modes indicate mode degeneracy at diabolical points. Interactions between single quantum dots and cavity modes are then investigated. Enhanced emission of a quantum dot with a six-fold intensity increase is obtained in a microdisk at a diabolical point. This method to control cavity modes allows large-scale integration, high reproducibility and flexible design of the size, the location, the quantity and the shape for scatterers, which can be applied for integrated photonic structures with scatterer-modified light-matter interaction.

Strong Triplet-Exciton-LO-Phonon Coupling in Two-Dimensional Layered Organic-Inorganic Hybrid Perovskite Single Crystal Microflakes.

Two-dimensional (2D) layered hybrid perovskites provide an ideal platform for studying the properties of excitons. Here, we report on a strong triplet-exciton and longitudinal-optical (LO) phonon coupling in 2D (C6H5CH2CH2NH3, PEA)2PbBr4 perovskites. The triplet excitons exhibit strong photoluminescence (PL) in thick perovskite microflakes, and the PL is not detectable for monolayer microflakes. The coupling strength of the triplet exciton-LO phonon is approximately two to three times greater than that of the singlet exciton-LO phonon with a LO phonon energy of about 21 meV. This difference might due to the different locations of singlet excitons located in the well and triplet excitons located in the barrier in the 2D layered perovskite. Revealing the strong coupling of triplet exciton-LO phonon provides a fundamental understanding of many-body interaction in hybrid perovskites, which is useful to develop and optimize the optoelectronic devices based on 2D perovskites in the future.

Tunable electronic structure and magnetic anisotropy in bilayer ferromagnetic semiconductor Cr2Ge2Te6.

The emergence of ferromagnetism in two-dimensional van der Waals materials has aroused broad interest. However, the ferromagnetic instability has been a problem remained. In this work, by using the first-principles calculations, we identified the critical ranges of strain and doping for the bilayer Cr2Ge2Te6 within which the ferromagnetic stability can be enhanced. Beyond the critical range, the tensile strain can induce the phase transition from the ferromagnetic to the antiferromagnetic, and the direction of magnetic easy axis can be converted from out-of-plane to in-plane due to the increase of compressive strain, or electrostatic doping. We also predicted an electron doping range, within which the ferromagnetism can be enhanced, while the ferromagnetic stability was maintained. Moreover, we found that the compressive strain can reverse the spin polarization of electrons at the conduction band minimum, so that two categories of half-metal can be induced by controlling electrostatic doping in the bilayer Cr2Ge2Te6. These results should shed a light on achieving ferromagnetic stability for low-dimensional materials.

Low-threshold topological nanolasers based on the second-order corner state.

Topological lasers are immune to imperfections and disorder. They have been recently demonstrated based on many kinds of robust edge states, which are mostly at the microscale. The realization of 2D on-chip topological nanolasers with a small footprint, a low threshold and high energy efficiency has yet to be explored. Here, we report the first experimental demonstration of a topological nanolaser with high performance in a 2D photonic crystal slab. A topological nanocavity is formed utilizing the Wannier-type 0D corner state. Lasing behaviour with a low threshold of approximately 1 µW and a high spontaneous emission coupling factor of 0.25 is observed with quantum dots as the active material. Such performance is much better than that of topological edge lasers and comparable to that of conventional photonic crystal nanolasers. Our experimental demonstration of a low-threshold topological nanolaser will be of great significance to the development of topological nanophotonic circuitry for the manipulation of photons in classical and quantum regimes.

Diabolical points in coupled active cavities with quantum emitters.

In single microdisks, embedded active emitters intrinsically affect the cavity modes of the microdisks, resulting in trivial symmetric backscattering and low controllability. Here we demonstrate macroscopic control of the backscattering direction by optimizing the cavity size. The signature of the positive and negative backscattering directions in each single microdisk is confirmed with two strongly coupled microdisks. Furthermore, diabolical points are achieved at the resonance of the two microdisks, which agrees well with theoretical calculations considering the backscattering directions. Diabolical points in active optical structures pave the way for an implementation of quantum information processing with geometric phase in quantum photonic networks.

Enhanced Strong Interaction between Nanocavities and p-shell Excitons Beyond the Dipole Approximation.

Large coupling strengths in exciton-photon interactions are important for the quantum photonic network, while strong cavity-quantum dot interactions have been focused on s-shell excitons with small coupling strengths. Here we demonstrate strong interactions between cavities and p-shell excitons with a great enhancement by the in situ wave-function control. The p-shell excitons are demonstrated with much larger wave-function extents and nonlocal interactions beyond the dipole approximation. Then the interaction is tuned from the nonlocal to the local regime by the wave function shrinking, during which the enhancement is obtained. A large coupling strength of 210 µeV has been achieved, indicating the great potential of p-shell excitons for coherent information exchange. Furthermore, we propose a distributed delay model to quantitatively explain the coupling strength variation, revealing the intertwining of excitons and photons beyond the dipole approximation.