Jaeyoung Kim

Excitons are bosonic quasiparticles with a variety of applications in optoelectronics, photosynthesis, and dissipationless informatics, and their lifetime can become sufficiently long to form a quantum condensate. While exciton condensation has been predicted to occur as a ground state of a solid, so-called an excitonic insulator, whose material realization has been elusive. Here we report the observation of direct photoemission signals from excitons in a ground state of a very recent excitonic insulator candidate Ta 2 Pd 3 Te 5 below its metal-insulator transition temperature using orbital-selective angle-resolved photoemission spectroscopy. It is confirmed that the excitons have a lower energy than the valence band maximum to possibly drive the phase transition. This measurement further discloses the size and the unusual odd parity of the exciton wave function. The present finding opens an avenue toward applications of coherent excitons in solid systems and searching for exotic quantum phases of exciton condensates.

Excitons in semiconductors and molecules are widely utilized in photovoltaics and optoelectronics, and high-temperature coherent quantum states of excitons can be realized in artificial electron-hole bilayers and an exotic material of an excitonic insulator (EI). Here, we investigate the band gap evolution of a putative high-temperature EI Ta2NiSe5 upon surface doing by alkali adsorbates with angle-resolved photoemission and density functional theory (DFT) calculations. The conduction band of Ta2NiSe5 is filled by the charge transfer from alkali adsorbates, and the band gap decreases drastically upon the increase of metallic electron density. Our DFT calculation, however, reveals that there exist both structural and excitonic contributions to the band gap tuned. While electron doping reduces the band gap substantially, it alone is not enough to close the band gap. In contrast, the structural distortion induced by the alkali adsorbate plays a critical role in the gap closure. This work indicates a combined electronic and structural nature for the EI phase of the present system and the complexity of surface doping beyond charge transfer.

Adsorption of alkali atoms onto material surfaces is widely utilized for controlling electronic properties and is particularly effective for two-dimensional materials. While tuning the chemical potential and band gap and creating quantum-confined states are well established for alkali adsorption on semiconductors, the effects on semimetallic systems remain largely elusive. Here, utilizing angle-resolved photoemission spectroscopy measurements and density functional theory calculations, we disclose the creation of two-dimensional electron gas and the quantum-confined Lifshitz transition at the surface of a Weyl semimetal T_d-MoTe₂ by potassium adsorption. Electrons from potassium adatoms are shown to be transferred mainly to the lowest unoccupied band within the gapped part of the Brillouin zone, which, in turn, induces strong surface band bending and quantum confinement in the topmost layer. The quantum-confined topmost layer evolves from a semimetal to a strong metal with a Lifshitz transition departing substantially from the bulk band. The present finding and its underlying mechanism can be exploited for the creation of electronic heterojunctions in van der Waals semimetals.

We demonstrate the systematic tuning of a trivial insulator into a Mott insulator and a Mott insulator into a correlated metallic and a pseudogap state, which emerge in a quasi-two-dimensional electronic system of 1T-TaS₂ through strong electron correlation. The band structure evolution is investigated upon surface doping by alkali adsorbates for two distinct phases occurring at around 220 and 10 K by angle-resolved photoelectron spectroscopy. We find contrasting behaviors upon doping that corroborate the fundamental difference of two electronic states: while the antibonding state of the spin-singlet insulator at 10 K is partially occupied to produce an emerging Mott insulating state, the presumed Mott insulating state at 220 K evolves into a correlated metallic state and then a pseudogap state. The work indicates that surface doping onto correlated 2D materials can be a powerful tool to systematically engineer a wide range of correlated electronic phases.

We report on the Tomonaga-Luttinger liquid (TLL) behavior in fully degenerate 1D Dirac Fermions. A ternary van der Waals material Nb9Si4Te18 incorporates in-plane NbTe2 chains, which produce a 1D Dirac band crossing Fermi energy. Tunneling conductance of electrons confined within NbTe2 chains is found to be substantially suppressed at Fermi energy, which follows a power law with a universal temperature scaling, hallmarking a TLL state. The obtained Luttinger parameter of similar to 0.15 indicates a strong electron-electron interaction. The TLL behavior is found to be robust against atomic-scale defects, which might be related to the Dirac electron nature. These findings, combined with the tunability of the compound and the merit of a van der Waals material, offer a robust, tunable, and integrable platform to exploit non-Fermi liquid physics.

We investigate the interaction between two magnetic layers separated with a normal metal insertion layer (Ti, Pt, and Ru) using x-ray ferromagnetic resonance (XFMR). We measure the amplitude and phase of the ferromagnetic resonance of both layers. Our results indicate that a ferromagnetic exchange coupling between two layers is a dominant coupling mechanism for a thick insertion metal layer. Based on the exchange coupling model, we extract the smallest value of the indirect exchange coefficient of 1.2 μJ/m2, which corresponds to an exchange field of about 0.36 mT. While this value is difficult to measure with other experimental tools, we were able to measure the small value because XFMR detects a resonance phenomenon of a thin layer generated by an oscillating indirect exchange and the Oersted fields with a phase and layer resolved observation.

Metal-organic complex exhibiting spin crossover (SCO) behavior has drawn attention for its functionality as a nanoscale spin switch. The spin states in the metal ions can be tuned by external stimuli such as temperature or light. This article demonstrates a soft X-ray–induced excited spin state trapping (SOXEISST) effect in Hofmann-like SCO coordination polymers of Fe^II(4-methylpyrimidine)₂[Au(CN)₂]₂ and Fe^II(pyridine)₂[Ni(CN)₄]. A soft X-ray absorption spectroscopy (XAS) study on these polymers showed that the high spin configuration (HS; S = 2) was prevalent in Fe²⁺ ions during the measurement even at temperatures much lower than the critical temperatures (>170 K), manifesting HS trapping due to the X-ray irradiation. This is in strong contrast to the normal SCO behavior observed in Fe^II(1,10-phenanthroline)₂(NCS)₂, implying that the structure of the ligand chains in the polymers with relatively loose Fe-N coordination might allow a structural adaptation to stabilize the metastable HS state under the soft X-ray irradiation.