Photoemission Spectroscopy Measurements Research Articles

UOTe: Kondo-Interacting Topological Antiferromagnet in a Van der Waals Lattice.

Since the initial discovery of 2D van der Waals (vdW) materials, significant effort has been made to incorporate the three properties of magnetism, band structure topology, and strong electron correlations-to leverage emergent quantum phenomena and expand their potential applications. However, the discovery of a single vdW material that intrinsically hosts all three ingredients has remained an outstanding challenge. Here, the discovery of a Kondo-interacting topological antiferromagnet is reported in the vdW 5f electron system UOTe. It has a high antiferromagnetic (AFM) transition temperature of 150K, with a unique AFM configuration that breaks the combined parity and time reversal (PT) symmetry in an even number of layers while maintaining zero net magnetic moment. This angle-resolved photoemission spectroscopy (ARPES) measurements reveal Dirac bands near the Fermi level, which combined with the theoretical calculations demonstrate UOTe as an AFM Dirac semimetal. Within the AFM order, the presence of the Kondo interaction is observed, as evidenced by the emergence of a 5f flat band near the Fermi level below 100 K and hybridization between the Kondo band and the Dirac band. The density functional theory calculations in its bilayer form predict UOTe as a rare example of a fully-compensated AFM Cherninsulator.

Revealing light-induced charge density wave melting and carrier redistribution in 1T-TiSe2

Abstract Capturing the ultrafast dynamics over a large momentum space is critical for revealing the relationship between the electronic and structural modulation in quantum materials. Here, by performing time- and angle-resolved photoemission spectroscopy measurements at Synergetic Extreme Condition User Faclity (SECUF) equipped with extreme ultraviolet light source, we reveal the ultrafast dynamics of a charge density wave (CDW) material 1T-TiSe2 upon photo-excitation. The pump-induced CDW melting is revealed from two aspects, a gap closing of CDW at the Brillouin zone (BZ) center and a weakening of the CDW folded band at the BZ boundary. By comparing the transient electronic structure and spectral weight over a large momentum space, we further reveal the carrier redistribution involving excitation of electrons from the Γ point to the M point. Our work provides a comprehensive picture on the physics and ultrafast dynamics of a CDW material across the entire BZ.

Molecular beam epitaxy and band structures of type-II antiferromagnetic semiconductor EuTe thin films

The rare-earth Eu-based compounds with a unique half-filled 4f orbital have attracted an amount of research interest recently. Here, we synthesized EuTe(001) single-crystal thin films on SrTiO3(001) substrate via molecular beam epitaxy (MBE). The scanning tunneling microscopy and x-ray diffraction results indicate that the grown EuTe thin films orientated as EuTe[100]//SrTiO3[110] in plane. In the angle-resolved photoemission spectroscopic (ARPES) measurements, the grown EuTe films show a semiconductive band structure with the valence band maximum lying on the center point of the Brillouin zone. The bandgap size of EuTe was further identified by the optical transmission spectra as 2.2 eV. The antiferromagnetic transition temperature of the grown EuTe film is 10.5 K measured by a superconductive quantum interference device (SQUID). Our results provide important information on the fundamental electronic structures for the further research and applications of the Eu-based compounds.

Unexpected band structure changes within the higher-temperature antiferromagnetic state of CeBi

The interest in the rare-earth monopnictides was boosted after the discovery of unconventional surface-state pairs in antiferromagnetically ordered NdBi. In contrast to other materials in which such states were reported, CeBi is known to have multiple antiferromagnetic phases. In this study, we perform angle-resolved photoemission spectroscopy (ARPES) measurements in conjunction with density functional theory (DFT) calculations to investigate the evolution of the electronic structure of CeBi upon a series of antiferromagnetic (AFM) transitions. We find evidence for a new AFM transition in addition to two previously known from transport studies. We demonstrate the development of an additional Dirac state in the ( + − + − ) ordered phase and a transformation of unconventional surface-state pairs in the ( + + − − ) ordered phase. This revises the phase diagram of this intriguing material, where there are now three distinct AFM states below TN in zero magnetic field instead of two as it was previously thought.

Observation of Highly Spin-Polarized Dangling Bond Surface States in Rare-Earth Pnictide Tellurides.

To generate and manipulate spin-polarized electronic states in solids are crucial for modern spintronics. The textbook routes employ quantum well states or Shockley/topological type surface states whose spin degeneracy is lifted by strong spin-orbit coupling and inversion symmetry breaking at the surface/interface. The resultant spin polarization is usually truncated because of the intertwining between multiple orbitals. Here a unique type of surface states is realized, namely, dangling bond surface states in a family of ternary rare-earth pnictide tellurides RePnTe (Re = La, Gd, Ce; Pn = Sb, Bi), with robust band structure and sizeable spin splitting. Spin and angle-resolved photoemission spectroscopy measurements reveal high spin polarization and distinct spin-momentum locking texture, which, according to the theoretical analysis, arise from local site asymmetry and surface-purified spin-orbital texture. The work extends the so-called "hidden spin polarization" from the bulk to the surface, presenting an intriguing spin-orbital-momentum-layer locking phenomenon, which may shed lights on potential spintronic applications.

Observation of doping-induced spin–orbit coupling in gold cluster assembly to carrier-tuneable semiconductors and Schottky behaviors

The doping influenced carrier dynamics to maneuvering n-type to p-type semiconducting gold cluster assembly have been assessed. The resonance photoemission spectroscopic measurements corroborate an incremental rise in the density of states at the valence edge, the overlap of valence states due to doping, and the presence of distinct spin–orbit splitting and coupling in manganese-doping (Au7Mn) compared to gold clusters (Au8), originating from the relativistic effect resulted in a semiconducting property. The work function dependent current–voltage characteristics in metal–semiconductor configuration show Ohmic and Schottky behaviors assorting p-type carriers in Au7Mn in contrast to the n-type Au8 and are presenting an atomic cluster based fast electronic device.

Observation of kagome-like bands in two-dimensional semiconducting Cr8Se12

The kagome lattice is a versatile platform for investigating correlated electronic states. However, its realization in two-dimensional (2D) semiconductors for tunable device applications is still challenging. An alternative strategy to create kagome-like bands is to realize a coloring-triangle (CT) lattice in semiconductors through a distortion of a modified triangular lattice. Here, we report the observation of low-energy kagome-like bands in a semiconducting 2D transition metal chalcogenide—Cr8Se12 with a thickness of 7 atomic layers—which exhibits a CT lattice and a bandgap of 0.8 eV. The Cr-deficient layer beneath the topmost Se-full layer is partially occupied with 2/3 occupancy, yielding a √3 × √3 Cr honeycomb network. Angle-resolved photoemission spectroscopy measurements and first-principles investigations reveal the surface kagome-like bands near the valence band maximum, which are attributed to topmost Se pz orbitals modulated by the honeycomb Cr.

Epitaxial growth and band offsets of β -(ScxGa1− x)2O3 thin films grown on (100) β -Ga2O3 substrate

β-(ScxGa1−x)2O3 (x = 0–0.36) thin films were epitaxially grown on (100) β-Ga2O3 substrates by oxygen-radical-assisted pulsed-laser deposition. β-(ScxGa1−x)2O3 epilayers were coherently strained up to x = 0.30, although the presence of a structural disorder was implied when x > 0.2. The bandgap energies measured by reflection electron energy loss spectroscopy increased from 4.56 to 5.25 eV with increasing Sc content. In β-(ScxGa1−x)2O3 epilayers, a slightly negative bandgap bowing behavior with a bowing parameter of −0.4 eV was observed, resulting in a larger bandgap increase than in β-(AlxGa1−x)2O3 epilayers with identical x. X-ray photoemission spectroscopy measurement revealed that the valence-band and conduction-band offsets of β-(Sc0.17Ga0.83)2O3 epilayer with respect to β-Ga2O3 were 0.0 and 0.3 eV, respectively.

Peeling-induced interfacial roughness and charging for enhanced triboelectric power generation

To date, there have been a lot of efforts to enhance the conversion efficiency of triboelectric nanogenerators (TENGs) via physical and chemical modifications of the polymer surface. Herein, we report that a facile peeling of polymer from a substrate can enhance the triboelectric power output. The peeling of spin-coated polydimethylsiloxane (PDMS) from glass and polytetrafluoroethylene (PTFE) substrates has revealed a considerable increase in interfacial roughness and lateral friction. Surface-sensitive X-ray photoemission spectroscopy and non-contact current measurements have also revealed the transfer of counter-material and interfacial charging. The surface roughness of peeled PDMS is significant for the PTFE substrate, while the surface charge is significant for the glass substrate. The triboelectric output power density for peeled PDMS from the substrate is similar, 10.3 µW/cm2, but significantly larger than that for as-grown PDMS (2.2 µW/cm2). The peeling strength of PDMS significantly increases for glass compared to PTFE after the oxygen plasma treatment of substrates. The triboelectric charge of peeled PDMS from a plasma-treated glass substrate is almost 1.3 times larger than that from a PTFE substrate. This work implies that peeling polymer from a rough substrate with a large adhesion force would be a facile and effective way to increase the triboelectric power output, without any delicate surface treatments.

Ferroelectric Semimetals with α-Bi/SnSe van der Waals Heterostructures and Their Topological Currents.

We show that proximity effects can be utilized to engineer van der Waals heterostructures (vdWHs) displaying semimetallic spin-ferroelectricity locking, where ferroelectricity and semimetallic spin states are confined to different layers, but are correlated by means of proximity effects. Our findings are supported by first principles calculations involving α-Bi/SnSe bilayers. We show that such systems support ferroelectrically switchable nonlinear anomalous Hall effect originating from large Berry curvature dipoles as well as direct and inverse spin Hall effects with giant bulk spin-charge interconversion efficiencies. The giant efficiencies are consequences of the proximity-induced semimetallic nature of low energy electron states, which are shown to behave as two-dimensional pseudo-Weyl fermions by means of symmetry analysis and first principles calculations as well as direct angle-resolved photoemission spectroscopy measurements.

Magnetotransport and angle-resolved photoemission spectroscopy of MnSb12Te19: a new member of MnSb2nTe3n+1 family

The quest for intrinsically ferromagnetic topological materials is a focal point in the study of topological phases of matter, as intrinsic ferromagnetism plays a vital role in realizing exotic properties such as the anomalous Hall effect (AHE) in quasi-two-dimensional materials, and this stands out as one of the most pressing concerns within the field. Here, we investigate a novel higher order member of the MnSb2nTe3n+1family, MnSb12Te19, for the first time combining magnetotransport and angle-resolved photoemission spectroscopy (ARPES) measurements. Our magnetic susceptibility experiments identify ferromagnetic transitions at temperatureTc= 18.7 K, consistent with our heat capacity measurements (T= 18.8 K). The AHE is observed for the field along thec-axis belowTc. Our study of Shubinikov-de-Haas oscillations provides evidence for Dirac fermions withπBerry phase. Our comprehensive investigation reveals that MnSb12Te19exhibits a FM ground state along with AHE, and hole-dominated transport properties consistent with ARPES measurements.

Interplay between disorder and electronic correlations in compositionally complex alloys

Owing to their exceptional mechanical, electronic, and phononic transport properties, compositionally complex alloys, including high-entropy alloys, represent an important class of materials. However, the interplay between chemical disorder and electronic correlations, and its influence on electronic structure-derived properties, remains largely unexplored. This is addressed for the archetypal CrMnFeCoNi alloy using resonant and valence band photoemission spectroscopy, electrical resistivity, and optical conductivity measurements, complemented by linear response calculations based on density functional theory. Utilizing dynamical mean-field theory, correlation signatures and damping in the spectra are identified, highlighting the significance of many-body effects, particularly in states distant from the Fermi edge. Electronic transport remains dominated by disorder and potentially short-range order, especially at low temperatures, while visible-spectrum optical conductivity and high-temperature transport are influenced by short quasiparticle lifetimes. These findings improve our understanding of element-specific electronic correlations in compositionally complex alloys and facilitate the development of advanced materials with tailored electronic properties.

Hole-Carrier-Dominant Transport in 2D Single-Crystal Copper.

In 2D noble metals like copper, the carrier scattering at grain boundaries has obscured the intrinsic nature of electronic transport. However, it is demonstrated that the intrinsic nature of transport by hole carriers in 2D copper can be revealed by growing thin films without grain boundaries. As even a slight deviation from the twin boundary is perceived as grain boundaries by electrons, it is only through the thorough elimination of grain boundaries that the hidden hole-like attribute of 2D single-crystal copper can be unmasked. Two types of Fermi surfaces, a large hexagonal Fermi surface centered at the zone center and the triangular Fermi surface around the zone corner, tightly matching to the calculated Fermi surface topology, confirmed by angle-resolved photoemission spectroscopy (ARPES) measurements and vivid nonlinear Hall effects of the 2D single-crystal copper account for the presence of hole carriers experimentally. This breakthrough suggests the potential to manipulate the majority carrier polarity in metals by means of grain boundary engineering in a 2D geometry.

Characterization of MoS2:Nb sputtered thin films. An application as hole transport layer in Cu2ZnSnS4/Si tandem solar cells

MoS2:Nb films deposited by radio-frequency magnetron sputtering are investigated in view of their application in infrared (IR)-transparent contacts for tandem photovoltaic devices.This material is already known to give a good electrical contact with p-type chalcogenide semiconductors, which are typically grown onto opaque molybdenum metallic contacts and a MoS2 layer spontaneously forms at the back interface during the on-top semiconductor growth. Our study explores a different approach, which involves the direct growth of IR-transparent MoS2:Nb films via sputtering inside complete photovoltaic devices, like Cu2ZnSnS4 (CZTS)-based single junction solar cells and CZTS/Si tandem devices. Films deposited at different sputtering pressures are compared by analysing their microstructure, morphology, chemical composition, optical and electrical properties. The effects of post-deposition sulfurization treatments are also investigated. We find that MoS2:Nb films deposited at around 0.1 Pa exhibit compactness but show a notable sulfur deficit ([S]/[Mo]≈1.4), a significant sub-bandgap optical absorptance and lack of crystallinity. Increasing the Ar pressure to 1 Pa raises the [S]/[Mo] ratio to 2.2, yielding crystalline films with good IR-transparency, although with a porous morphology. Despite 0.5 wt% Nb-doping of the sputtering target, the as-deposited films demonstrate n-type conductivity likely due to uncontrolled impurities and intrinsic defects. Ultraviolet Photoemission Spectroscopy measurements suggest that films’ work function higher than 5 eV can be obtained with a post-deposition sulfurization, making these materials suitable as Hole Transport Layer in photovoltaic applications. A similar increase in work function is expected in the CZTS/MoS2 junctions, since the sputtered MoS2:Nb films undergo a sulfurization process needed to obtain the overlying polycrystalline CZTS absorber.CZTS solar cells produced with sputtered MoS2 and Transparent Conductive Oxides contacts on glass substrates, despite plagued by severe adhesion problems, show the potentiality to give efficiencies comparable to reference devices with standard Mo back contact. Fabrication of CZTS/Si tandem devices on textured silicon bottom cells yields a maximum efficiency of 4.4 %, primarily hindered by the low quality of the CZTS film on textured substrates. Nonetheless, optoelectronic characterizations based on both spectrophotometric and quantum efficiency measurements confirm a good IR transparency of the MoS2-based intermediate contacts and the desired electrical behaviour.

Quantum-Confined Lifshitz Transition on Weyl Semimetal Td-MoTe2.

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 Td-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.

Observation of the multiple magnetic phases in double perovskite Pr1.8La0.2CoFeO6

The structural and magnetic properties of the double perovskite Pr1.8La0.2CoFeO6 have been investigated. The X-ray diffraction study shows that the system acquires room-temperature orthorhombic phase with the Pnma space group. The X-ray photoemission spectroscopy (XPS) measurement confirmed that the B-site ions are present in mixed valence states i.e. Co has been found in Co2+ and Co3+ valance states whereas Fe has been found in Fe3+/Fe4+. Magnetic measurements of the system confirm the existence of several fascinating magnetic behaviors, such as long-range canted antiferromagnetism withTN ∼ 271 K, giant exchange bias, and re-entrant cluster glass phase (TG ∼ 33 K). Field-dependent magnetization shows a large spontaneous exchange bias; HSEB∼ 1.8 kOe and giant conventional exchange bias, HCEB∼ 2.4 kOe at 5 K. Antiferromagnetic materials with large exchange bias can be utilized in high-density spintronic devices. Temperature-dependent Raman study demonstrates that the observed phonon mode exhibits anomalous behavior close to the magnetic transition temperature. Analysis of anomalous softening of phonon mode below TN, clarifies the presence of significant spin-phonon coupling while the magnetostriction effect does not play any significant role in the observed phonon anomaly.

(Invited) Internal Photoemission (IPE) Spectroscopy Measurement of Interfacial Energy Barriers in Operating Metal/Insulator/Metal (MIM) and Metal/Ferroelectric/Metal (MFM) Devices

Metal-insulator-metal (MIM) and Metal/Ferroelectric/Metal (MFM) devices find application as high speed tunnel diodes for rectenna based energy harvesting and sensing of IR radiation, hot-electron transistors, single electron transistors, resistive random access memory (RRAM), back end of line (BEOL) capacitors, and ferroelectric tunnel junction (FTJ) diodes. Precise knowledge of band-offsets / energy barriers (φBn) at metal/insulator interfaces is critical for understanding, predicting, and optimizing charge transport in these devices.The Schottky-Mott rule, which neglects charge transfer across interfaces, states that the difference between the Fermi level of a metal (EF) and the conduction band of an insulator should vary simply with the metal vacuum work function (ΦM,vac) and the insulator electron affinity (χi) so that φBn = ΦM,vac - χi. In induced gap state theory, charge transfer at intrinsic interface traps creates an interfacial dipole that drives the EF towards the charge neutral level of the insulator (ECNL,i) the energy at which the dominant character of the interface states switches from donor-like to acceptor-like. A metal on an insulator will thus behave as if it has an effective work function (ΦM-eff) where ΦM,eff = ECNL,I + S(ΦM,vac - ECNL,i), where S = dφBn / dΦM,vac.1 Empirically, S = 1 / (1 + 0.1(εopt - 1)2), so that as the optical dielectric constant of the insulator (εhf) increases, S decreases from an ideal 1 towards 0 so that the insulator more effectively "pins" EFM at ECNL-i.2 Despite some success of MIGS theory, it is difficult to calculate or determine ECNL for a given material and it is observed that actual φBn's often deviate substantially from predictions. Indeed, φBn's depends on material processing, extrinsic effects (such as interfacial and near-interfacial trapped charge arising from point defects), dipoles (due to interfacial chemical reactions), and scavenging of oxygen from the insulator. Therefore, it is necessary to directly measure φBn for the specific metal/insulator or metal/ferroelectric combination in use. Internal photoemission (IPE) spectroscopy is an electro-optical technique that allows measurement of φBn at both metal interfaces in operating MIM & MFM devices.3-5 IPE is the only technique capable of measuring barrier heights, in-situ, in operating device structures. To date, relatively little work has been reported on IPE of these devices.6-12 In this invited talk, IPE spectroscopy measurements are described and measurements are presented of φBn's in MIM structures between insulators (Al2O3, HfO2, SiO2, NiO, CoOx) and ferroelectric HfZrOx deposited via atomic layer deposition (ALD) and various metals including ALD Ru, sputtered thin film amorphous metals (ZrCuAlNi, TaWSi, and TaNiSi), and benchmark metals (TaN, Al, and Au). Comparisons with electrical measurements on the same devices are found to be qualitatively consistent with φBns determined via IPE, even when inconsistent with Schottky model predictions, pointing to various non-idealities present in the materials and their interfaces and demonstrating the power of IPE for understanding and optimizing MIM & MFM device operation. C. Yeo, T.J. King, and C. Hu, J. Appl. Phys. 92, 7266 (2002).Mönch, Phys. Rev. Lett. 58, 1260 (1987).K. Adamchuk and V. V. Afanas’ev, Prog. Surf. Sci. 41, 111 (1992).V. Afanas’ev and A. Stesmans, J. Appl. Phys. 102, 081301 (2007).V. Nguyen, O. A. Kirillov, and J. S. Suehle, Thin Solid Films 519, 2811 (2011).Afanas’ev, N. Kolomiiets, M. Houssa, and A. Stesmans, Phys. Status Solidi A 215, 1700865 (2017).V. Afanas’ev et al., Appl. Phys. Lett. 98, 132901 (2011).A. Jenkins, T. Klarr, D. Z. Austin, W. Li, N. V. Nguyen, and J. F. Conley Jr., Phys. Status Solidi RRL – Rapid Res. Lett. 12, 1700437 (2018).A. Jenkins, J. M. McGlone, J. F. Wager, and J. F. Conley, Jr., J. Appl. Phys. 125, 055301 (2019).A. Jenkins, T. Klarr, J. M. McGlone, J. F. Wager, and J. F. Conley Jr., ECS Trans. 85, 729 (2018).A. Jenkins, K.E.K. Holden, S.W. Smith, M.T. Brumbach, M.D. Henry, C. Weiland, J.C. Woicik, S.T. Jaszewski, J.F. Ihlefeld, and J.F. Conley. ACS AMI 13, 14634 (2021).L. Peterson, T. Mimura, J. Ihlefeld, and J.F. Conley Jr., "Internal Photoemission (IPE) Spectroscopy Measurement of Electrode Energy Barriers in Pristine, Woken, and Poled Ferroelectric HZO MFM Devices," in the American Vacuum Society (AVS) Workshop for Innovative Nano Devices and Systems (WINDS) Book of s, Kona, HI, Dec. 2023.

Robustness of linear bands in epitaxial planar silicene heterostructure against surface doping

In this study, we investigate the electronic structure of epitaxial planar silicene heterostructure grown on ultrathin gold films on the Si(111) substrates, covered by 0.1 monolayer of silver, antimony and lead. Angle-Resolved Photoemission Spectroscopy measurements reveal that the electronic structure of planar silicene, that shows bands with linear dispersion, remains largely unaffected by the presence of these dopants, with only a slight energy shift observed in the case of antimony. Density functional theory calculations corroborate these experimental observations, confirming the robustness of the epitaxial planar silicene heterostructure against surface doping. The results suggest that the intrinsic electronic properties of planar silicene are well-protected against surface contamination.

Quasi-Homoepitaxial Growth of Highly Strained Alkali-Metal Ultrathin Films on Kagome Superconductors.

Applying lattice strain to thin films, a critical factor to tailor their properties such as stabilizing a structural phase unstable at ambient pressure, generally necessitates heteroepitaxial growth to control the lattice mismatch with substrate. Therefore, while homoepitaxy, the growth of thin film on a substrate made of the same material, is a useful method to fabricate high-quality thin films, its application to studying strain-induced structural phases is limited. Contrary to this general belief, here the quasi-homoepitaxial growth of Cs and Rb thin films is reported with substantial in-plane compressive strain. This is achieved by utilizing the alkali-metal layer existing in bulk crystal of kagome metals AV3Sb5 (A=Cs and Rb) as a structural template. The angle-resolved photoemission spectroscopy measurements reveal the formation of metallic quantum well states and notable thickness-dependent quasiparticle lifetime. Comparison with density functional theory calculations suggests that the obtained thin films crystalize in the face-centered cubic structure, which is typically stable only under high pressure in bulk crystals. These findings provide a useful approach for synthesizing highly strained thin films by quasi-homoepitaxy, and pave the way for investigating many-body interactions in Fermi liquids with tunable dimensionality.

Emergence of two distinct phase transitions in monolayer CoSe2 on graphene

Dimensional modifications play a crucial role in various applications, especially in the context of device miniaturization, giving rise to novel quantum phenomena. The many-body dynamics induced by dimensional modifications, including electron-electron, electron-phonon, electron-magnon and electron-plasmon coupling, are known to significantly affect the atomic and electronic properties of the materials. By reducing the dimensionality of orthorhombic CoSe2 and forming heterostructure with bilayer graphene using molecular beam epitaxy, we unveil the emergence of two types of phase transitions through angle-resolved photoemission spectroscopy and scanning tunneling microscopy measurements. We disclose that the 2 × 1 superstructure is associated with charge density wave induced by Fermi surface nesting, characterized by a transition temperature of 340 K. Additionally, another phase transition at temperature of 160 K based on temperature dependent gap evolution are observed with renormalized electronic structure induced by electron-boson coupling. These discoveries of the electronic and atomic modifications, influenced by electron-electron and electron-boson interactions, underscore that many-body physics play significant roles in understanding low-dimensional properties of non-van der Waals Co-chalcogenides and related heterostructures.Graphical