1T-TaSe_{2} is widely believed to host a Mott metal-insulator transition in the charge density wave (CDW) phase according to the spectroscopic observation of a band gap that extends across all momentum space. Previous investigations inferred that the occurrence of the Mott phase is limited to the surface only of bulk specimens, but recent analysis on thin samples revealed that the Mott-like behavior, observed in the monolayer, is rapidly suppressed with increasing thickness. Here, we report combined time- and angle-resolved photoemission spectroscopy and theoretical investigations of the electronic structure of 1T-TaSe_{2}. Our experimental results confirm the existence of a state above E_{F}, previously ascribed to the upper Hubbard band, and an overall band gap of ∼0.7  eV at Γ[over ¯]. However, supported by density functional theory calculations, we demonstrate that the origin of this state and the gap rests on band structure modifications induced by the CDW phase alone, without the need for Mott correlation effects.

Download full-text PDF

Source
http://dx.doi.org/10.1103/PhysRevLett.130.156401DOI Listing

Publication Analysis

Top Keywords

charge density
8
density wave
8
cdw phase
8
band gap
8
exploring charge
4
phase
4
wave phase
4
phase 1t-tase_{2}
4
mott
4
1t-tase_{2} mott
4

Similar Publications

The anisotropic properties of materials profoundly influence their electronic, magnetic, optical, and mechanical behaviors and are critical for a wide range of applications. In this study, the anisotropic characteristics of Ni-based van der Waals materials, specifically NiTe and its alloy NiTeSe, utilizing a combination of comprehensive scanning tunneling microscopy (STM), angle-resolved photoemission spectroscopy (ARPES), and density functional theory (DFT) calculations, are explored. Unlike 1T-NiTe, which exhibits trigonal in-plane symmetry, the substitution of Te with Se in NiTe (resulting in the NiTeSe alloy) induces a pronounced in-plane anisotropy.

View Article and Find Full Text PDF

In the field of quantum materials, understanding anomalous behavior under charge degrees of freedom through bond formation is of fundamental importance, with two key concepts: Dimerization and charge order at different cation sites. The coexistence of both dimerization and charge ordering is unusually found in NaRu2O4, even in its metallic state at room temperature. Our work unveils the origin of the interplay of these effects within metallic single-crystalline NaRu2O4.

View Article and Find Full Text PDF

All-solid-state fluoride-ion batteries (FIBs) have attracted extensive attention as candidates for next-generation energy storage devices; however, promising cathodes with high energy density are still lacking. In this study, CuN is investigated as a cathode material for all-solid-state fluoride-ion batteries, which offers enough anionic vacancies around the 2-fold coordinated Cu center for F intercalation, thereby enabling a multielectron-transferred fluorination process. The contribution of both cationic and anionic redox to charge compensation, in particular, the generation of molecular nitrogen species in highly charged states, has been proved by several synchrotron-radiation-based spectroscopic technologies.

View Article and Find Full Text PDF

Photoinduced Fröhlich Interaction-Driven Distinct Electron- and Hole-Polaron Behaviors in Hybrid Organic-Inorganic Perovskites by Ultrafast Terahertz Probes.

ACS Nano

January 2025

School of Information Science and Technology and Department of Optical Science and Engineering and Key Laboratory of Micro and Nano Photonic Structures (MOE), Fudan University, Shanghai 200433, China.

The formation of large polarons resulting from the Fröhlich coupling of photogenerated carriers with the polarized crystal lattice is considered crucial in shaping the outstanding optoelectronic properties in hybrid organic-inorganic perovskite crystals. Until now, the initial polaron dynamics after photoexcitation have remained elusive in the hybrid perovskite system. Here, based on the terahertz time-domain spectroscopy and optical-pump terahertz probe, we access the nature of interplay between photoexcited unbound charge carriers and optical phonons in MAPbBr within the initial 5 ps after excitation and have demonstrated the simultaneous existence of both electron- and hole-polarons, together with the photogenerated carrier dynamic process.

View Article and Find Full Text PDF

The design of interfaces between nanostructured electrodes and advanced electrolytes is critical for realizing advanced electrochemical double-layer capacitors (EDLCs) that combine high charge-storage capacity, high-rate capability, and enhanced safety. Toward this goal, this work presents a novel and sustainable approach for fabricating ionogel-based electrodes using a renewed slurry casting method, in which the solvent is replaced by the ionic liquid (IL), namely 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide (EMIFSI). This method avoids time-consuming and costly electrolyte-filling steps by integrating the IL directly into the electrode during slurry preparation, while improving the rate capability of EDLCs based on non-flammable ILs.

View Article and Find Full Text PDF

Want AI Summaries of new PubMed Abstracts delivered to your In-box?

Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!