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We investigate the surface oxidation in a van der Waals ferromagnet Fe3-xGeTe2, a material widely utilized for spintronic applications. While known for its relative air-insensitivity, exposure to air during the handling process (e.g. device or heterostructure fabrication) can lead to reduction or disappearance of its magnetic signal. Comparison of x-ray absorption and x-ray magnetic circular dichroism spectra between pristine and air-exposed Fe3-xGeTe2 confirm a naturally oxidized surface layer on the material. The surface oxide layer has predominantly Fe3+ content. X-ray absorption spectroscopy done on micron-sized exfoliated Fe3-xGeTe2 flakes reveal that the change in the surface chemical properties can be quite significant for thin flakes. The surface modulation of Fe3-xGeTe2 can lead to inaccuracies in characterizing its interfacial magnetic and spin transport properties, and complicate device and heterostructure fabrication processes.

Graphene is an emergent research topic that has attracted a huge amount of research interest ever since its experimental demonstration as a two-dimensional realization of Dirac fermions in 2005. In subsequent years, the research on graphene has rapidly expanded its field not only due to the new paradigm to study relativistic high energy physics in a condensed matter, but also due to its potential in the application for next generation devices. Most of the novel phenomena observed so far in graphene are attributed to its low-energy excitations, which is described by those of relativistic Dirac fermions. This article reviews recent progress in angle-resolved photoemission spectroscopy studies of electron-electron interactions in graphene.

Two-dimensional triangular-lattice antiferromagnets are predicted under some conditions to exhibit a quantum spin liquid ground state with no energy barrier to create emergent, fractionalized spinon excitations that carry spin but no charge. Materials that realize this kind of spin liquid are expected to have a low-energy behaviour described by a spinon Fermi surface. Directly imaging the resulting spinons, however, is difficult due to their chargeless nature. Here we use scanning tunnelling spectroscopy to image density waves consistent with the predictions of spinon density modulation arising from a spinon Fermi surface instability in single-layer 1T-TaSe2. We confirm the existence of a triangular lattice of localized spins in this material by contacting it with a metallic 1H-TaSe2 substrate and measuring the Kondo effect. Spectroscopic imaging of isolated single-layer 1T-TaSe2 reveals long-wavelength super-modulations at Hubbard band energies, consistent with the predicted behaviour of itinerant spinons. These super-modulations allow the direct experimental measurement of the spinon Fermi wavevector, in good agreement with theoretical predictions for a two-dimensional quantum spin liquid. Some quantum spin liquids are expected to have an effective Fermi surface of fractionalized spinon excitations. The two-dimensional spin liquid candidate 1T-TaSe2 has charge density modulations that may be caused by an unstable spinon Fermi surface.

The spontaneous formation of electronic orders is a crucial element for understanding complex quantum states and engineering heterostructures in 2D materials. A novel

The low-energy electron band structure of Cu $$_2$$ Si on Si(111) has been investigated using angle-resolved photoemission spectroscopy. Cu $$_2$$ Si exhibits two Dirac nodal-lines, stemming from the crossing of one electron-pocket with two hole-pockets, that are protected by mirror reflection symmetry. When Cu $$_2$$ Si is placed on Si(111), the hole-pockets and their satellite bands due to the quasi- $$5\times 5$$ periodicity are clearly observed whereas the electron-pocket is observed with very weak spectral intensity. Interestingly, close to the Fermi energy, the hole-pockets exhibit almost linear energy-momentum dispersion when their spectral width is also linearly proportional to energy. These findings indicate that Cu $$_2$$ Si on Si(111) can host Dirac nodal-line fermions, of which low-energy excitations might depart from those of the conventional Fermi liquid.

Author(s): Pham, AT; Vu, TH; Cheng, C; Trinh, TL; Lee, JE; Ryu, H; Hwang, C; Mo, SK; Kim, J; Zhao, LD; Duong, AT; Cho, S | Abstract: High-quality SnSe2 single crystals were successfully synthesized using a temperature gradient method. N-type characteristics and strong anisotropic transport properties of SnSe2 single crystals were exhibited between the ab plane and the c-axis. At 673 K, the power factor (PF) value along the ab plane is 3.43 μW cm-1 K-2, while it is 0.92 μW cm-1 K-2 along the c-axis. The ratio between thermal conductivities along the ab plane (κab) and c-axis (κc) is on the order of 7.6 at 300 K, while this value is about 5.6 at 673 K. The thermoelectric figure of merit (ZT) in the c-axis (0.15) is higher than that (0.1) along the ab plane, according to the ultralow out-of-plane thermal conductivity. The electronic band structure results, which were examined by angle-resolved photoemission spectroscopy (ARPES) predicted the potential of improving the thermoelectric performance of SnSe2 single crystals by electron doping.

Identifying material parameters affecting properties of ferromagnets is key to optimized materials that are better suited for spintronics. Magnetic anisotropy is of particular importance in van der Waals magnets, since it not only influences magnetic and spin transport properties, but also is essential to stabilizing magnetic order in the two-dimensional limit. Here, we report that hole doping effectively modulates the magnetic anisotropy of a van der Waals ferromagnet and explore the physical origin of this effect. Fe3-xGeTe2 nanoflakes show a significant suppression of the magnetic anisotropy with hole doping. Electronic structure measurements and calculations reveal that the chemical potential shift associated with hole doping is responsible for the reduced magnetic anisotropy by decreasing the energy gain from the spin-orbit induced band splitting. Our findings provide an understanding of the intricate connection between electronic structures and magnetic properties in two-dimensional magnets and propose a method to engineer magnetic properties through doping.

The interplay between electron-electron interaction and electron-phonon coupling has been one of the key issues in graphene as it can provide information on the origin of enhanced electron-phonon coupling in graphene by foreign atoms. In ytterbium-decorated graphene on SiC substrate, electron-phonon coupling exhibits strong enhancement compared to that of as-grown graphene. Based on angle-resolved photoemission study, the presence of ytterbium is also found to result in the decrease of Fermi velocity, revealing the enhancement of electron-electron interaction within the Fermi liquid theory. Our finding on the concomitant enhancement of electron-electron interaction and electron-phonon coupling suggests a possibility of the interplay between the two representative many-body interactions in graphene decorated with foreign atoms., 3 figures

Monolayers of two-dimensional van der Waals materials exhibit novel electronic phases distinct from their bulk due to the symmetry breaking and reduced screening in the absence of the interlayer coupling. In this work, we combine angle-resolved photoemission spectroscopy and scanning tunneling microscopy/spectroscopy to demonstrate the emergence of a unique insulating 2 × 1 dimer ground state in monolayer 1T-IrTe

Proximity of two different materials leads to an intricate coupling of quasiparticles so that an unprecedented electronic state is often realized at the interface. Here, we demonstrate a resonance-type many-body ground state in graphene, a non-magnetic two-dimensional Dirac semimetal, when grown on SmB6, a Kondo insulator, via thermal decomposition of fullerene molecules. This ground state is typically observed in three-dimensional magnetic materials with correlated electrons. Above the characteristic Kondo temperature of the substrate, the electron band structure of pristine graphene remains almost intact. As temperature decreases, however, the Dirac fermions of graphene become hybridized with the Sm 4f states. Remarkable enhancement of the hybridization and Kondo resonance is observed with further cooling and increasing charge carrier density of graphene, evidencing the Kondo screening of the Sm 4f local magnetic moment by the conduction electrons of graphene at the interface. These findings manifest the realization of the Kondo effect in graphene by the proximity of SmB6 that is tuned by temperature and charge carrier density of graphene., 4 figures

Recent advances in two-dimensional (2D) crystals make it possible to realize an ideal interface structure that is required for device applications. Specifically, a p-n junction made of 2D crystals is predicted to exhibit an atomically well-defined interface that will lead to high device performance. Using angle-resolved photoemission spectroscopy, a simple surface treatment was shown to allow the possible formation of such an interface. Ta adsorption on the surface of a p-doped SnSe shifts the valence band maximum towards higher binding energy due to the charge transfer from Ta to SnSe that is highly localized at the surface due to the layered structure of SnSe. As a result, the charge carriers of the surface are changed from holes of its bulk characteristics to electrons, while the bulk remains as a p-type semiconductor. This observation suggests that the well-defined interface of a p-n junction with an atomically thin {\it n}-region is formed between Ta-adsorbed surface and bulk., 4 figures

In the past decade, the advent of time-resolved spectroscopic tools has provided a new ground to explore fundamental interactions in solids and to disentangle degrees of freedom whose coupling leads to broad structures in the frequency domain. Time- and angle-resolved photoemission spectroscopy (tr-ARPES) has been utilized to directly study the relaxation dynamics of a metal in the presence of electron-phonon coupling. The effect of photo-excitations on the real and imaginary part of the self-energy as well as the time scale associated with different recombination processes are discussed. In contrast to a theoretical model, the phonon energy does not set a clear scale governing quasiparticle dynamics, which is also different from the results observed in a superconducting material. These results point to the need for a more complete theoretical framework to understand electron-phonon interaction in a photo-excited state., Comment: 4 figures

Identifying material parameters affecting properties of ferromagnets is key to optimized materials that are better suited for spintronics. Magnetic anisotropy is of particular importance in van der Waals magnets, since it not only influences magnetic and spin transport properties, but also is essential to stabilizing magnetic order in the two-dimensional limit. Here, we report that hole doping effectively modulates the magnetic anisotropy of a van der Waals ferromagnet and explore the physical origin of this effect. Fe

We present the electronic characterization of single-layer 1H-TaSe2 grown by molecular beam epitaxy using a combined angle-resolved photoemission spectroscopy, scanning tunneling microscopy/spectroscopy, and density functional theory calculations. We demonstrate that 3 × 3 charge-density-wave (CDW) order persists despite distinct changes in the low energy electronic structure highlighted by the reduction in the number of bands crossing the Fermi energy and the corresponding modification of Fermi surface topology. Enhanced spin-orbit coupling and lattice distortion in the single-layer play a crucial role in the formation of CDW order. Our findings provide a deeper understanding of the nature of CDW order in the two-dimensional limit.

SnTe is a prototypical topological crystalline insulator, in which the gapless surface state is protected by a crystal symmetry. The hallmark of the topological properties in SnTe is the Dirac cones projected to the surfaces with mirror symmetry, stemming from the band inversion near the L points of its bulk Brillouin zone, which can be measured by angle-resolved photoemission. We have obtained the (111) surface of SnTe film by molecular beam epitaxy on BaF2(111) substrate. Photon-energy-dependence of in situ angle-resolved photoemission, covering multiple Brillouin zones in the direction perpendicular tothe (111) surface, demonstrate the projected Dirac cones at the Gamma_bar and M_bar points of the surface Brillouinzone. In addition, we observe a Dirac-cone-like band structure at the Gamma point of the bulk Brillouin zone,whose Dirac energy is largely different from those at the Gamma_bar and M_bar points., 8 pages, 4 figures

A combination of photoemission and scanning tunnelling spectroscopy measurements provide compelling evidence that single layers of 1T'-WTe2 are a class of quantum spin Hall insulator. A quantum spin Hall (QSH) insulator is a novel two-dimensional quantum state of matter that features quantized Hall conductance in the absence of a magnetic field, resulting from topologically protected dissipationless edge states that bridge the energy gap opened by band inversion and strong spin–orbit coupling1,2. By investigating the electronic structure of epitaxially grown monolayer 1T'-WTe2 using angle-resolved photoemission (ARPES) and first-principles calculations, we observe clear signatures of topological band inversion and bandgap opening, which are the hallmarks of a QSH state. Scanning tunnelling microscopy measurements further confirm the correct crystal structure and the existence of a bulk bandgap, and provide evidence for a modified electronic structure near the edge that is consistent with the expectations for a QSH insulator. Our results establish monolayer 1T'-WTe2 as a new class of QSH insulator with large bandgap in a robust two-dimensional materials family of transition metal dichalcogenides (TMDCs).

Chalcogen vacancies are generally considered to be the most common point defects in transition metal dichalcogenide (TMD) semiconductors because of their low formation energy in vacuum and their frequent observation in transmission electron microscopy studies. Consequently, unexpected optical, transport, and catalytic properties in 2D-TMDs have been attributed to in-gap states associated with chalcogen vacancies, even in the absence of direct experimental evidence. Here, we combine low-temperature non-contact atomic force microscopy, scanning tunneling microscopy and spectroscopy, and state-of-the-art ab initio density functional theory and GW calculations to determine both the atomic structure and electronic properties of an abundant chalcogen-site point defect common to MoSe and WS monolayers grown by molecular beam epitaxy and chemical vapor deposition, respectively. Surprisingly, we observe no in-gap states. Our results strongly suggest that the common chalcogen defects in the described 2D-TMD semiconductors, measured in vacuum environment after gentle annealing, are oxygen substitutional defects, rather than vacancies., This work was supported by the Center for Computational Study of Excited State Phenomena in Energy Materials (C2SEPEM), which is funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division under Contract No. DE-AC02-05CH11231, as part of the Computational Materials Sciences Program. Work performed at the Molecular Foundry was also supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under the same contract number. S.B. acknowledges fellowship support by the European Union under FP7-PEOPLE-2012-IOF-327581. S.B. and M.M.U acknowledge Spanish MINECO (MAT2017-88377-C2-1-R). S.R.A acknowledges Rothschild and Fulbright fellowships. B.S. appreciates support from the Swiss National Science Foundation under project number P2SKP2_171770. A.P. and O.V.Y. acknowledge support by the ERC Starting grant “TopoMat” (Grant No. 306504). M.F.C. acknowledges support from the U.S. National Science Foundation under project number EFMA-1542741. C.H. acknowledges support from NRF grant funded by the Korea government (MSIT) (No. 2018R1A2B6004538). DFT calculations were performed at the Swiss National Supercomputing Centre (CSCS) under project s832 and the facilities of Scientific IT and Application Support Center of EPFL. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231 for the GW calculations. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DE-AC02-05CH11231.

Author(s): Ryu, Hyejin; Chen, Yi; Kim, Heejung; Tsai, Hsin-Zon; Tang, Shujie; Jiang, Juan; Liou, Franklin; Kahn, Salman; Jia, Caihong; Omrani, Arash A; Shim, Ji Hoon; Hussain, Zahid; Shen, Zhi-Xun; Kim, Kyoo; Min, Byung Il; Hwang, Choongyu; Crommie, Michael F; Mo, Sung-Kwan | Abstract: Corrections to the original paper are the following: Page 692, line 6, left column. "centered at Λ (-0.5 eV l E l 0)" should be "centered at Λ (E l -1 eV)". Page 692, line 2, right column. "E ∼ -0.5 eV" should be "V ∼ +0.6 V".

The interface between graphene and a ferromagnetic substrate has attracted recent research interests due to its potential for spintronic applications. We report an angle-resolved photoemission spectroscopy study on the interface between graphene and cobalt epitaxially grown on a tungsten substrate. We find that the electron band structure of the interface exhibits clear discontinuities at the crossing points with cobalt 3d bands. These observations indicate strong hybridizations between the electronic states in the interface and provide an important clue to understand the intriguing electromagnetic properties of the graphene/ferromagnet interface.

We report new wide band gap engineering for graphene using slow Cs+ ions, which allows both fine-tuning and on–off switching capability of the band gap in a range suitable for most applications without modifying or deteriorating the relativistic nature of the Dirac fermions. The doping of Cs+ ions opens the band gap up to Eg = 0.68 eV, which can be closed completely by adding neutral Cs atoms, as observed in angle-resolved photoemission spectroscopy. The operating mechanism of this band gap engineering is understood by a simple capacitor model, which is fully supported by the density-functional theory calculations.

We investigate the electronic structure of BaMnBi2 and BaZnBi2 using angle-resolved photoemission spectroscopy and first-principles calculations. Although they share similar structural properties, we show that their electronic structure exhibit dramatic differences. A strong anisotropic Dirac dispersion is revealed in BaMnBi2 with a decreased asymmetry factor compared with other members of AMnBi2 (A = alkali earth or rare earth elements) family. In addition to the Dirac cones, multiple bands crossing the Fermi energy give rise to a complex Fermi surface topology for BaZnBi2. We further show that the strength of hybridization between Bi-p and Mn-d/Zn-s states is the main driver of the differences in electronic structure for these two related compounds.

The interaction between a magnetic impurity, such as cerium (Ce) atom, and surrounding electrons has been one of the core problems in understanding many-body interaction in solid and its relation to magnetism. Kondo effect, the formation of a new resonant ground state with quenched magnetic moment, provides a general framework to describe many-body interaction in the presence of magnetic impurity. In this Letter, a combined study of angle-resolved photoemission (ARPES) and dynamic mean-field theory (DMFT) on Ce-intercalated graphene shows that Ce-induced localized states near Fermi energy, $E_{\rm F}$, hybridized with the graphene $\pi$ band, exhibit gradual increase in spectral weight upon decreasing temperature. The observed temperature dependence follows the expectations from the Kondo picture in the weak coupling limit. Our results provide a novel insight how Kondo physics emerges in the sea of two-dimensional Dirac electrons., Comment: 17 pages, 4 figures

We present the electronic characterization of single-layer 1H-TaSe

The electron band structure of manganese-adsorbed graphene on an SiC(0001) substrate has been studied using angle-resolved photoemission spectroscopy. Upon introducing manganese atoms, the conduction band of graphene completely disappears and the valence band maximum is observed at 0.4 eV below Fermi energy. At the same time, the slope of the valence band decreases, approaching the electron band structure calculated using the local density approximation method. While the former provides experimental evidence of the formation of nearly free-standing graphene on an SiC substrate, concomitant with a metal-to-insulator transition, the latter suggests that its electronic correlations can be modified by foreign atoms. These results pave the way for promising device applications using graphene that is semiconducting and charge neutral., Comment: 16 pages, 3 figures

© 2017 Author(s). We have investigated the electron band structure of graphene epitaxially grown on an SiC substrate using angle-resolved photoemission spectroscopy. The conical energy spectrum of graphene exhibits a minimum slope at ∼50 K, which is accompanied by the minimum separation between its two branches. These observations provide a viable route towards the engineering of the electronic properties of graphene using temperature, while the latter suggests a possible evidence of gap engineering via strain induced by the substrate and modulated by temperature.

The electron band structure of graphene on SrTiO

The interaction between graphene and substrates provides a viable route to enhance the functionality of both materials. Depending on the nature of electronic interaction at the interface, the electron band structure of graphene is strongly influenced, allowing us to make use of the intrinsic properties of graphene or to design additional functionalities in graphene. Here, we present an angle-resolved photoemission study on the interaction between graphene and a platinum substrate. The formation of an interface between graphene and platinum leads to a strong deviation in the electronic structure of graphene not only from its freestanding form but also from the behavior observed on typical metals. The combined study on the experimental and theoretical electron band structure unveils the unique electronic properties of graphene on a platinum substrate, which singles out graphene/platinum as a model system investigating graphene on a metallic substrate with strong interaction.

High quality WSe2 films have been grown on bilayer graphene (BLG) with layer-by-layer control of thickness using molecular beam epitaxy. The combination of angle-resolved photoemission, scanning tunneling microscopy/spectroscopy, and optical absorption measurements reveal the atomic and electronic structures evolution and optical response of WSe2/BLG. We observe that a bilayer of WSe2 is a direct bandgap semiconductor, when integrated in a BLG-based heterostructure, thus shifting the direct-indirect band gap crossover to trilayer WSe2. In the monolayer limit, WSe2 shows a spin-splitting of 475 meV in the valence band at the K point, the largest value observed among all the MX2 (M = Mo, W; X = S, Se) materials. The exciton binding energy of monolayer-WSe2/BLG is found to be 0.21 eV, a value that is orders of magnitude larger than that of conventional three-dimensional semiconductors, yet small as compared to other two-dimensional transition metal dichalcogennides (TMDCs) semiconductors. Finally, our finding regarding the overall modification of the electronic structure by an alkali metal surface electron doping opens a route to further control the electronic properties of TMDCs.

The interaction between two different materials can present novel phenomena that are quite different from the physical properties observed when each material stands alone. Strong electronic correlations, such as magnetism and superconductivity, can be produced as the result of enhanced Coulomb interactions between electrons. Two-dimensional materials are powerful candidates to search for the novel phenomena because of the easiness of arranging them and modifying their properties accordingly. In this work, we report magnetic effects of graphene, a prototypical non-magnetic two-dimensional semi-metal, in the proximity with sulfur, a diamagnetic insulator. In contrast to the well-defined metallic behaviour of clean graphene, an energy gap develops at the Fermi energy for the graphene/sulfur compound with decreasing temperature. This is accompanied by a steep increase of the resistance, a sign change of the slope in the magneto-resistance between high and low fields, and magnetic hysteresis. A possible origin of the observed electronic and magnetic responses is discussed in terms of the onset of low-temperature magnetic ordering. These results provide intriguing insights on the search for novel quantum phases in graphene-based compounds., Comment: 6 pages and 5 figures

The Landau-Fermi liquid picture for quasiparticles assumes that charge carriers are dressed by many-body interactions, forming one of the fundamental theories of solids. Whether this picture still holds for a semimetal like graphene at the neutrality point, i.e., when the chemical potential coincides with the Dirac point energy, is one of the long-standing puzzles in this field. Here we present such a study in quasi-freestanding graphene by using high-resolution angle-resolved photoemission spectroscopy. We see the electron-electron and electron-phonon interactions go through substantial changes when the semimetallic regime is approached, including renormalizations due to strong electron-electron interactions with similarities to marginal Fermi liquid behavior. These findings set a new benchmark in our understanding of many-body physics in graphene and a variety of novel materials with Dirac fermions., Comment: PNAS 2011 ; published ahead of print June 27, 2011

Monolayer transition metal dichalcogenides (TMDCs) in the 1T′ structural phase have drawn a great deal of attention due to the prediction of quantum spin Hall insulator states. The band inversion and the concomitant changes in the band topology induced by the structural distortion from 1T to 1T′ phases are well established. However, the bandgap opening due to the strong spin-orbit coupling (SOC) is only verified for 1T′-WTe2 recently and still debated for other TMDCs. Here we report a successful growth of high-quality monolayer 1T′-MoTe2 on a bilayer graphene substrate through molecular beam epitaxy. Using in situ angle-resolved photoemission spectroscopy (ARPES), we have investigated the low-energy electronic structure and Fermi surface topology. The SOC-induced breaking of the band degeneracy points between the valence and conduction bands is clearly observed by ARPES. However, the strength of SOC is found to be insufficient to open a bandgap, which makes monolayer 1T′-MoTe2 on bilayer graphene a semimetal.

We have investigated structural and vibrational properties of Na nanoclusters self-assembled on the Si(1 1 1)-7×7 surface at room temperature mainly using high-resolution electron-energy-loss spectroscopy. We observe three characteristic loss peaks L1, L2, and L3 ascribed to an interband transition, a local atomic vibration, and another interband transition from an Na nanocluster-induced state, respectively. The spectral change of L1 with Na coverage θ suggests that the S1 dangling bond band is gradually filled up to open a band gap with increasing θ up to 1.1 eV when all three loss peaks completely disappeared. The relatively high loss energy El=243meV of L2 with a narrow linewidth of 32 meV indicates the only Na–Si atomic vibrational mode with Na atoms occupying the tilted on-top sites above Si rest atoms. Furthermore the extremely weak loss peak L3 visible at a coverage range unique only to the Na nanoclusters proves the presence of a Na nanoclusters-induced electronic state N2. These observations provide explanation to most unresolved spectral behavior of earlier photoemission study and evidence for the atomic structure of the Na nanocluster.

Using synchrotron X-ray diffraction we have determined the atomic arrangement of a two-dimensional lattice of thallium (Tl) nanodots self-assembled on the Si(1 1 1)-7 × 7 surface at room temperature. By analyzing a set of in-plane reflections as well as crystal truncation rods, we find that the atomic structure of a single Tl nanodot is best described by a dynamical model where nine Tl atoms are arranged 0.91 ± 0.19 A above the substrate Si adatoms with three central atoms slightly bulging over the surrounding six atoms by about 0.18 A. Our model further suggests that the Tl atoms are quite mobile within the attractive basins of the frozen substrate 7 × 7 surface. The mobile nature of Tl atoms naturally explains the blurred scanning tunnelling microscope images and may also provide a clue to understand the intriguing metallic feature of the Tl nanodots.

We report an unusual behavior of the work function that remains unchanged while increasing the coverage (θ) of thallium (Tl) nanoclusters regularly arranged on a Si(111)-7×7 surface. Such a constant work function with increasing θ is understood in terms of a θ-dependent inter-cluster interaction that cancels the change induced by dipoles due to Tl nanoclusters. The spectral changes of Si 2p and Tl 5d5/2 core-levels as a function of θ strongly indicates the presence of such an inter-clusters interaction, which is further supported by our theoretical calculation revealing a significant charge redistribution.