Visible Surface Plasmon Modes in Single Bi₂Te₃ Nanoplate

Searching for new plasmonic building blocks which offer tunability and design flexibility beyond noble metals is crucial for advancing the field of plasmonics. Herein, we report that solution-synthesized hexagonal Bi₂Te₃ nanoplates, in the absence of grating configurations, can exhibit multiple plasmon modes covering the entire visible range, as observed by transmission electron microscopy (TEM)-based electron energy-loss spectroscopy (EELS) and cathodoluminescence (CL) spectroscopy. Moreover, different plasmon modes are observed in the center and edge of the single Bi₂Te₃ nanoplate and a breathing mode is discovered for the first time in a non-noble metal. Theoretical calculations show that the plasmons observed in the visible range are mainly due to strong spin–orbit coupling induced metallic surface states of Bi₂Te₃. The versatility of shape- and size-engineered Bi₂Te₃ nanocrystals suggests exciting possibilities in plasmonics-enabled technology

Molecular Alignment and Electronic Structure of <i>N</i>,<i>N</i>′‑Dibutyl-3,4,9,10-perylene-tetracarboxylic-diimide Molecules on MoS₂ Surfaces

The molecular orientation of organic semiconductors on a solid surface could be an indispensable factor to determine the electrical performance of organic-based devices. Despite its fundamental prominence, a clear description of the emergent two-dimensional layered material–organic interface is not fully understood yet. In this study, we reveal the molecular alignment and electronic structure of thermally deposited <i>N</i>,<i>N</i>′-dibutyl-3,4,9,10-perylene-dicarboximide (PTCDI-C4) molecules on natural molybdenum disulfide (MoS₂) using near-edge X-ray absorption fine structure spectroscopy (NEXAFS). The average tilt angle determination reveals that the anisotropy in the π* symmetry transition of the carbon <i>K</i>-edge (284–288 eV range) is present at the sub-monolayer regime. Supported by ultraviolet photoelectron spectroscopy (UPS), X-ray photoelectron spectroscopy (XPS), and resonant photoemission spectroscopy (RPES) measurements, we find that our spectroscopic measurements indicate a weak charge transfer established at the PTCDI-C4/MoS₂ interface. Sterical hindrance due to the C4 alkyl chain caused tilting of the molecular plane at the initial thin film deposition. Our result shows a tunable interfacial alignment of organic molecules on transition metal dichalcogenide surfaces effectively enhancing the electronic properties of hybrid organic–inorganic heterostructure devices

Direct Observation of Room-Temperature Stable Magnetism in LaAlO₃/SrTiO₃ Heterostructures

Along with an unexpected conducting interface between nonmagnetic insulating perovskites LaAlO₃ and SrTiO₃ (LaAlO₃/SrTiO₃), striking interfacial magnetisms have been observed in LaAlO₃/SrTiO₃ heterostructures. Interestingly, the strength of the interfacial magnetic moment is found to be dependent on oxygen partial pressures during the growth process. This raises an important, fundamental question on the origin of these remarkable interfacial magnetic orderings. Here, we report a direct evidence of room-temperature stable magnetism in a LaAlO₃/SrTiO₃ heterostructure prepared at high oxygen partial pressure by using element-specific soft X-ray magnetic circular dichroism at both Ti L_3,2 and O K edges. By combining X-ray absorption spectroscopy at both Ti L_3,2 and O K edges and first-principles calculations, we qualitatively ascribe that this strong magnetic ordering with dominant interfacial Ti³⁺ character is due to the coexistence of LaAlO₃ surface oxygen vacancies and interfacial (Ti_Al–Al_Ti) antisite defects. On the basis of this new understanding, we revisit the origin of the weak magnetism in LaAlO₃/SrTiO₃ heterostructures prepared at low oxygen partial pressures. Our calculations show that LaAlO₃ surface oxygen vacancies are responsible for the weak magnetism at the interface. Our result provides direct evidence on the presence of room-temperature stable magnetism and a novel perspective to understand magnetic and electronic reconstructions at such strategic oxide interfaces

Tailoring the Optical and Electronic Properties of 2D Hybrid Dion–Jacobson Copper Chloride Perovskites

The upsurge of low-dimensional Dion–Jacobson (DJ) phase perovskites has brought significant interest in view of their appealing stability against harsh environmental conditions as well as their promising performance in optoelectronic applications. Few reports to date have concentrated on the fundamental relationship of fine-tuning the control of diamine-based perovskite single crystals toward their electronic properties and optical behaviors. Here, we demonstrate that cationic control is proposed to regulate the role of hydrogen bonding of organic ligands with the edge-sharing [CuCl6]4– octahedral layers, leading to strong differences in the material excitonic profile and tunability of their electronic properties. Interestingly, we observe a significant reduction of photoluminescence intensity upon controlling the Cu2+/Cu+ proportion in this hybrid system. According to the photoemission measurements, variation in the oxidation states of Cu cations plays a crucial role in stabilizing the diammonium-based perovskite geometric structure. Interestingly, we find that the electronic signatures of the singlet spin-state and high-energy region transition are not influenced by the thermal effect, as probed by temperature-dependent X-ray absorption spectroscopy (XAS) at elevated temperature. Density functional calculations suggest that such an electronic difference originates from the hydrogen bonding reduction that altered the magnitude of the octahedral distortion within the DJ layered structure. As a result, the 3+NHC4H9NH3+ conformation produces a non-negligible interaction toward tuning the optical and electronic properties of DJ copper-based perovskites

The Mechanism of Electrolyte Gating on High‑<i>T</i>_<i>c</i> Cuprates: The Role of Oxygen Migration and Electrostatics

Electrolyte gating is widely used to induce large carrier density modulation on solid surfaces to explore various properties. Most of past works have attributed the charge modulation to electrostatic field effect. However, some recent reports have argued that the electrolyte gating effect in VO₂, TiO₂, and SrTiO₃ originated from field-induced oxygen vacancy formation. This gives rise to a controversy about the gating mechanism, and it is therefore vital to reveal the relationship between the role of electrolyte gating and the intrinsic properties of materials. Here, we report entirely different mechanisms of electrolyte gating on two high-<i>T</i>_<i>c</i> cuprates, NdBa₂Cu₃O_7−δ (NBCO) and Pr_2–<i>x</i>Ce_<i>x</i>CuO₄ (PCCO), with different crystal structures. We show that field-induced oxygen vacancy formation in CuO chains of NBCO plays the dominant role, while it is mainly an electrostatic field effect in the case of PCCO. The possible reason is that NBCO has mobile oxygen in CuO chains, while PCCO does not. Our study helps clarify the controversy relating to the mechanism of electrolyte gating, leading to a better understanding of the role of oxygen electro migration which is very material specific