Pseudospin-selective Floquet band engineering in black phosphorus.

Time-periodic light field has emerged as a control knob for manipulating quantum states in solid-state materials1-3, cold atoms4 and photonic systems5 through hybridization with photon-dressed Floquet states6 in the strong-coupling limit, dubbed Floquet engineering. Such interaction leads to tailored properties of quantum materials7-11, for example, modifications of the topological properties of Dirac materials12,13 and modulation of the optical response14-16. Despite extensive research interests over the past decade3,8,17-20, there is no experimental evidence of momentum-resolved Floquet band engineering of semiconductors, which is a crucial step to extend Floquet engineering to a wide range of solid-state materials. Here, on the basis of time and angle-resolved photoemission spectroscopy measurements, we report experimental signatures of Floquet band engineering in a model semiconductor, black phosphorus. On near-resonance pumping at a photon energy of 340-440 meV, a strong band renormalization is observed near the band edges. In particular, light-induced dynamical gap opening is resolved at the resonance points, which emerges simultaneously with the Floquet sidebands. Moreover, the band renormalization shows a strong selection rule favouring pump polarization along the armchair direction, suggesting pseudospin selectivity for the Floquetband engineering as enforced by the lattice symmetry. Our work demonstrates pseudospin-selective Floquet band engineering in black phosphorus and provides important guiding principles for Floquet engineering of semiconductors.

Carbon nanotube electron blackbody and its radiation spectra.

An optical blackbody is an ideal absorber for all incident optical radiation, and the theoretical study of its radiation spectra paved the way for quantum mechanics (Planck's law). Herein, we propose the concept of an electron blackbody, which is a perfect electron absorber as well as an electron emitter with standard energy spectra at different temperatures. Vertically aligned carbon nanotube arrays are electron blackbodies with an electron absorption coefficient of 0.95 for incident energy ranging from 1 keV to 20 keV and standard electron emission spectra that fit well with the free electron gas model. Such a concept might also be generalized to blackbodies for extreme ultraviolet, X-ray, and γ-ray photons as well as neutrons, protons, and other elementary particles.

Evolution of the flat band and the role of lattice relaxations in twisted bilayer graphene.

Magic-angle twisted bilayer graphene exhibits correlated phenomena such as superconductivity and Mott insulating states related to the weakly dispersing flat band near the Fermi energy. Such a flat band is expected to be sensitive to both the moiré period and lattice relaxations. Thus, clarifying the evolution of the electronic structure with the twist angle is critical for understanding the physics of magic-angle twisted bilayer graphene. Here we combine nano-spot angle-resolved photoemission spectroscopy and atomic force microscopy to resolve the fine electronic structure of the flat band and remote bands, as well as their evolution with twist angle from 1.07° to 2.60°. Near the magic angle, the dispersion is characterized by a flat band near the Fermi energy with a strongly reduced band width. Moreover, we observe a spectral weight transfer between remote bands at higher binding energy, which allows to extract the modulated interlayer spacing near the magic angle. Our work provides direct spectroscopic information on flat band physics and highlights the important role of lattice relaxations.

A correlated ferromagnetic polar metal by design.

Polar metals have recently garnered increasing interest because of their promising functionalities. Here we report the experimental realization of an intrinsic coexisting ferromagnetism, polar distortion and metallicity in quasi-two-dimensional Ca3Co3O8. This material crystallizes with alternating stacking of oxygen tetrahedral CoO4 monolayers and octahedral CoO6 bilayers. The ferromagnetic metallic state is confined within the quasi-two-dimensional CoO6 layers, and the broken inversion symmetry arises simultaneously from the Co displacements. The breaking of both spatial-inversion and time-reversal symmetries, along with their strong coupling, gives rise to an intrinsic magnetochiral anisotropy with exotic magnetic field-free non-reciprocal electrical resistivity. An extraordinarily robust topological Hall effect persists over a broad temperature-magnetic field phase space, arising from dipole-induced Rashba spin-orbit coupling. Our work not only provides a rich platform to explore the coupling between polarity and magnetism in a metallic system, with extensive potential applications, but also defines a novel design strategy to access exotic correlated electronic states.

Ultrafast Carrier Relaxation Dynamics in a Nodal-Line Semimetal PtSn4.

Topological Dirac nodal-line semimetals host topologically nontrivial electronic structure with nodal-line crossings around the Fermi level, which could affect the photocarrier dynamics and lead to novel relaxation mechanisms. Herein, by using time- and angle-resolved photoemission spectroscopy, we reveal the previously inaccessible linear dispersions of the bulk conduction bands above the Fermi level in a Dirac nodal-line semimetal PtSn4, as well as the momentum and temporal evolution of the gapless nodal lines. A surprisingly ultrafast relaxation dynamics within a few hundred femtoseconds is revealed for photoexcited carriers in the nodal line. Theoretical calculations suggest that such ultrafast carrier relaxation is attributed to the multichannel scatterings among the complex metallic bands of PtSn4 via electron-phonon coupling. In addition, a unique dynamic relaxation mechanism contributed by the highly anisotropic Dirac nodal-line electronic structure is also identified. Our work provides a comprehensive understanding of the ultrafast carrier dynamics in a Dirac nodal-line semimetal.

Factors affecting long-term changes of meibomian gland in MGD patients.

PURPOSE: To explore the long-term course of patients with meibomian gland dysfunction (MGD), and to analyse potential factors affecting the recovery of meibomian gland (MG) dropout. METHODS: Seventy-nine MGD patients (79 eyes) aged 36.03±15.78 years old who underwent more than one year of follow-up were enrolled in this retrospective study. Corneal fluorescein staining (CFS), tear meniscus height (TMH), noninvasive breakup time (NIBUT), and noncontact meibography at baseline and last visit were collected and analysed. Then an automatic MG analyzer was used to measure the morphological and functional parameters of MGs, including their area ratio (AR), tortuosity index (TI), and signal index (SI). The patients whose AR increased by more than 5% were defined as MG improvement, and AR decreased by more than 5% was MG worsening. RESULTS: A total of 79 patients (79 eyes) were assessed with at least 1-year of follow-up. More than 1/3 of MGD patients (27 eyes, 34.2%) underwent MG improvement, and 30.4% of MGs became worsened. Age (P=0.002), gender (P<0.001), IPL treatment (P=0.013), the change of CFS (P=0.0015), and the recovery of SI (P=0.035) showed significant differences among different recovery groups. Age(P<0.001), female sex (P=0.003), ΔCFS (P<0.001), AR at baseline (P<0.001) were negative correlation with AR recovery, and the change of SI (P=0.003) and IPL treatment (P=0.003) had a positive correlation with it. Among them, age (P=0.038), the change of CFS (P=0.004), and AR at baseline (P=0.007) were confirmed as negatively correlated factors predicting the long-term change of the MG. CONCLUSION: Although the MGD treatment has continued for more than 1 year, only 34.2% of MGD patients were observed to undergo MG improvement. Younger patients and patients with better CFS recovery seem to have more opportunities to improve their MGs.

Floquet Engineering of Black Phosphorus upon Below-Gap Pumping.

Time-periodic light field can dress the electronic states and lead to light-induced emergent properties in quantum materials. While below-gap pumping is regarded favorable for Floquet engineering, so far direct experimental evidence of momentum-resolved band renormalization still remains missing. Here, we report experimental evidence of light-induced band renormalization in black phosphorus by pumping at photon energy of 160 meV, which is far below the band gap, and the distinction between below-gap pumping and near-resonance pumping is revealed. Our Letter demonstrates light-induced band engineering upon below-gap pumping, and provides insights for extending Floquet engineering to more quantum materials.

Facile Synthesis of Helicene-Containing Arenes for Optical Limiting Devices.

A helicene-containing arene and its linear analogue have been successfully synthesized and characterized, where the single-crystal X-ray diffraction analysis indicates that the former can arrange in an offset packing style with a π-π overlap. The introduction of pentagon-rings into the parent skeletons in the resulting compounds can boost the stability, and such helicene-containing molecule possesses higher solubility in organic solvent than the linear analogue. The structural difference has significantly influenced the optical limiting performance. The former in solution and in doped gel glass presents higher optical limiting response towards 532 nm laser than the latter. This study can enrich the functionalization of helicene, which can possess a positive effect in terms of nonlinear optical property.

Electric-field control of tri-state phase transformation with a selective dual-ion switch.

Materials can be transformed from one crystalline phase to another by using an electric field to control ion transfer, in a process that can be harnessed in applications such as batteries, smart windows and fuel cells. Increasing the number of transferrable ion species and of accessible crystalline phases could in principle greatly enrich material functionality. However, studies have so far focused mainly on the evolution and control of single ionic species (for example, oxygen, hydrogen or lithium ions). Here we describe the reversible and non-volatile electric-field control of dual-ion (oxygen and hydrogen) phase transformations, with associated electrochromic and magnetoelectric effects. We show that controlling the insertion and extraction of oxygen and hydrogen ions independently of each other can direct reversible phase transformations among three different material phases: the perovskite SrCoO3-δ (ref. 12), the brownmillerite SrCoO2.5 (ref. 13), and a hitherto-unexplored phase, HSrCoO2.5. By analysing the distinct optical absorption properties of these phases, we demonstrate selective manipulation of spectral transparency in the visible-light and infrared regions, revealing a dual-band electrochromic effect that could see application in smart windows. Moreover, the starkly different magnetic and electric properties of the three phases-HSrCoO2.5 is a weakly ferromagnetic insulator, SrCoO3-δ is a ferromagnetic metal, and SrCoO2.5 is an antiferromagnetic insulator-enable an unusual form of magnetoelectric coupling, allowing electric-field control of three different magnetic ground states. These findings open up opportunities for the electric-field control of multistate phase transformations with rich functionalities.

Population Inversion and Dirac Fermion Cooling in 3D Dirac Semimetal Cd3As2.

Revealing the ultrafast dynamics of three-dimensional (3D) Dirac fermions is critical for both fundamental science and device applications. So far, how the cooling of 3D Dirac fermions differs from that of two-dimensional (2D) and whether there is population inversion are fundamental questions to be answered. Here we reveal the ultrafast dynamics of Dirac fermions in a model 3D Dirac semimetal Cd3As2 by time- and angle-resolved photoemission spectroscopy with a tunable probe photon energy. The energy- and momentum-resolved relaxation rate shows a linear dependence on the energy, suggesting Dirac fermion cooling through intraband relaxation. Moreover, a population inversion is reported based on the observation of accumulated photoexcited carriers in the conduction band with a lifetime of 3.0 ps. Our work provides direct experimental evidence for a long-lived population inversion in a 3D Dirac semimetal, which is in contrast to 2D graphene with a much shorter lifetime.

Siloxene Nanosheets and Their Hybrid Gel Glasses for Broad-Band Optical Limiting.

With the development of laser technology, the research of novel laser protection materials is of great significance. In this work, dispersible siloxene nanosheets (SiNSs) with a thickness of about 1.5 nm are prepared by the top-down topological reaction method. Based on the Z-scan and optical limiting testing under the visible-near IR ranges nanosecond laser, the broad-band nonlinear optical properties of the SiNSs and their hybrid gel glasses are investigated. The results show that the SiNSs have outstanding nonlinear optical properties. Meanwhile, the SiNSs hybrid gel glasses also exhibit high transmittance and excellent optical limiting capabilities. It demonstrates that SiNSs are promising materials for broad-band nonlinear optical limiting and even have potential applications in optoelectronics.

Synthesis, Photoswitching Behavior and Nonlinear Optical Properties of Substituted Tribenzo[a,d,g]coronene.

A family of tribenzocoronene derivatives bearing various substituents (3) were constructed through the Diels-Alder reaction, followed by the Scholl oxidation, where the molecular structure of 3b was determined via single crystal X-ray diffraction analysis. The effect of substitution on the optical and electrochemical property was systematically investigated, with the assistance of theoretical calculations. Moreover, the thin films of the resulting molecules 3b and 3e complexed with fullerene produced strong photocurrent response upon irradiation of white light. In addition, 3b and 3e exhibit a positive nonlinear optical response resulting from the two-photon absorption and excited state absorption processes.

High Quantum Efficiency Rare-Earth-Doped Gd2O2S:Tb, F Scintillators for Cold Neutron Imaging.

High-resolution neutron radiography provides novel and stirring opportunities to investigate the structures of light elements encased by heavy elements. For this study, a series of Gd2O2S:Tb, F particles were prepared using a high-temperature solid phase method and then used as a scintillation screen. Upon reaching 293 nm excitation, a bright green emission originated from the Tb3+ luminescence center. The level of F doping affected the fluorescence intensity. When the F doping level was 8 mol%, the fluorescence intensity was at its highest. The absolute quantum yield of the synthesized particles reached as high as 77.21%. Gd2O2S:Tb, F particles were applied to the scintillation screen, showing a resolution on the neutron radiograph as high as 12 µm. These results suggest that the highly efficient Gd2O2S:Tb, F particles are promising scintillators for the purposes of cold neutron radiography.

N-Doped Nonalternant Nanoribbons with Excellent Nonlinear Optical Performance.

Two novel N-doped nonalternant nanoribbons (NNNR-1 and NNNR-2) featuring multiple fused N-heterocycles and bulky solubilizing groups were prepared via bottom-up solution synthesis. NNNR-2 achieves a total molecular length of 33.8 Å, which represents the longest soluble N-doped nonalternant nanoribbon reported to date. The pentagon subunits and doping of N atoms in NNNR-1 and NNNR-2 have successfully regulated their electronic properties, achieving high electron affinity and good chemical stability enabled by the nonalternant conjugation and electronic effects. When applied a laser pulse of 532 nm, the 13-rings nanoribbon NNNR-2 shows outstanding nonlinear optical (NLO) responses, with the nonlinear extinction coefficient of 374 cm GW-1 , much higher than those of NNNR-1 (96 cm GW-1 ) and the well-known NLO material C60 (153 cm GW-1 ). Our findings indicate that the N-doping of nonalternant nanoribbons is an effective strategy to access another type of excellent material system for high-performance NLO applications, which can be extended to construct numerous heteroatom-doped nonalternant nanoribbons with fine-tunable electronic properties.

Ultra-Broadband Random Laser and White-Light Emissive Carbon Dots/Crystal In-Situ Hybrids.

The continuous white-light emission of carbon dots (CDs) can be applied to producing multicolor laser emissions by one single medium. Meanwhile, the solid-state emission greatly contributes to its practical application. In this work, a strategy to realize the in-situ hybridization of silane-functionalized CDs (SiCDs) and 1,3,5-benzenetricarboxylic acid trimethyl ester (Et3BTC) by a one-pot solvothermal method is reported. Significantly, the SiCDs/Et3BTC hybrid crystals exhibit ultra-broadband random laser emission over the near ultraviolet-visible region under 265 nm nanosecond pulsed laser excitation. The wavelength region of laser emission is achieved from 315 to 600 nm within an emission band of CDs-based materials. It is worth noting that the wavelength range of the laser is wider than the previously reported works. It is proposed that the continuous white-light emission of SiCDs caused by multiple fluorescence centers mainly gives rise to the broadband random laser emission. Moreover, the crystals are conducive to forming resonance and realizing solid-state laser emission. This in-situ method is expected to enable a more convenient, cheaper, and greener approach to prepare luminescent hybrids for application in multicolor laser displays, multi-level laser anti-counterfeiting, supercontinuum light sources, and so on.

Light-Tunable Surface State and Hybridization Gap in Magnetic Topological Insulator MnBi8Te13.

MnBi8Te13 is an intrinsic ferromagnetic (FM) topological insulator with different complex surface terminations. Resolving the electronic structures of different termination surfaces and manipulation of the electronic state are important. Here, by using micrometer spot time- and angle-resolved photoemission spectroscopy (µ-TrARPES), we resolve the electronic structures and reveal the ultrafast dynamics upon photoexcitation. Photoinduced filling of the surface state hybridization gap is observed for the Bi2Te3 quintuple layer directly above MnBi2Te4 accompanied by a nontrivial shift of the surface state, suggesting light-tunable interlayer interaction. Relaxation of photoexcited electrons and holes is observed within 1-2 ps. Our work reveals photoexcitation as a potential control knob for tailoring the interlayer interaction and surface state of MnBi8Te13.

Hydrogen-Rich 2D Halide Perovskite Scintillators for Fast Neutron Radiography.

A fast neutron has strong penetration ability through dense and bulky objects, which makes it an ideal nondestructive technology for detecting voids, cracks, or other defects inside large equipment. However, the lack of effective fast neutron detection materials limits its application. Perovskites have shown excellent optical properties in many areas, but they are absent from fast neutron detection imaging because they cannot directly absorb fast neutrons and emit luminescence. Here, we demonstrate a hydrogen-rich long-chain organic amine modified two-dimensional (2D) perovskite fast neutron scintillator, Mn-(C18H37NH3)2PbBr4(Mn-STA2PbBr4). Its hydrogen density can reach 9.51 × 1028 m-3, and the photoluminescence quantum yield can reach 58.58%, so it is possible to integrate fast neutron absorption and luminescence into a single compound. More importantly, Mn-STA2PbBr4 can be made into a large-area self-supporting fast neutron scintillator plate with satisfactory spatial resolution (0.5 lp/mm (lp: line pairs)). This strategy provides a simple and promising choice for fast neutron scintillator nondestructive testing.

Experimental Evidence of Chiral Symmetry Breaking in Kekulé-Ordered Graphene.

The low-energy excitations of graphene are relativistic massless Dirac fermions with opposite chiralities at valleys K and K^{'}. Breaking the chiral symmetry could lead to gap opening in analogy to dynamical mass generation in particle physics. Here we report direct experimental evidences of chiral symmetry breaking (CSB) from both microscopic and spectroscopic measurements in a Li-intercalated graphene. The CSB is evidenced by gap opening at the Dirac point, Kekulé-O type modulation, and chirality mixing near the gap edge. Our work opens up opportunities for investigating CSB related physics in a Kekulé-ordered graphene.

Quasicrystalline 30° twisted bilayer graphene as an incommensurate superlattice with strong interlayer coupling.

The interlayer coupling can be used to engineer the electronic structure of van der Waals heterostructures (superlattices) to obtain properties that are not possible in a single material. So far research in heterostructures has been focused on commensurate superlattices with a long-ranged Moiré period. Incommensurate heterostructures with rotational symmetry but not translational symmetry (in analogy to quasicrystals) are not only rare in nature, but also the interlayer interaction has often been assumed to be negligible due to the lack of phase coherence. Here we report the successful growth of quasicrystalline 30° twisted bilayer graphene (30°-tBLG), which is stabilized by the Pt(111) substrate, and reveal its electronic structure. The 30°-tBLG is confirmed by low energy electron diffraction and the intervalley double-resonance Raman mode at 1383 cm-1 Moreover, the emergence of mirrored Dirac cones inside the Brillouin zone of each graphene layer and a gap opening at the zone boundary suggest that these two graphene layers are coupled via a generalized Umklapp scattering mechanism-that is, scattering of a Dirac cone in one graphene layer by the reciprocal lattice vector of the other graphene layer. Our work highlights the important role of interlayer coupling in incommensurate quasicrystalline superlattices, thereby extending band structure engineering to incommensurate superstructures.

Size-Dependent Nonlinear Optical Properties of Gd2O2S:Tb3+ Scintillators and Their Doped Gel Glasses.

With the advancement of ultra-fast and high-energy pulsed laser output, lasers have caused serious harm to precision instruments and human eyes. Therefore, the development of optical limiting materials with a fast response, low optical limiting threshold, and high damage threshold are important. In this work, for the first time, it is reported that phosphors Gd2O2S:Tb3+(GOS) displays exceptional functionality in laser protection. GOS with sizes of 11 µm, 1 µm, and 0.45 µm are prepared. Based on the optical limiting and Z-scan technology systems under 532 nm and 1064 nm nanosecond laser excitation, the nonlinear optical properties of GOS are investigated. It is found that GOS exhibits outstanding optical limiting properties. In addition, the optical limiting response of GOS is size-dependent. Concerning the largest particle size, GOS has the best nonlinear optical response, while the precursor shows no nonlinear optical performance. Meanwhile, GOS doped gel glass also displays excellent optical limiting properties with high transmittance, which preliminarily validates the application of GOS and other scintillators in nonlinear optics and encourages more research to better realize the potential of GOS.