Angle-resolved Photoemission Spectroscopy Study Research Articles

Electronic structure and effective mass of pristine and Cl-doped CsPbBr3

Organic–inorganic lead halide perovskites (LHPs) have attracted great interest owing to their outstanding optoelectronic properties. Typically, the underlying electronic structure would determinate the physical properties of materials. But as for now, limited studies have been done to reveal the underlying electronic structure of this material system, comparing to the huge amount of investigations on the material synthesis. The effective mass of the valance band is one of the most important physical parameters which plays a dominant role in charge transport and photovoltaic phenomena. In pristine CsPbBr3, the Fröhlich polarons associated with the Pb–Br stretching modes are proposed to be responsible for the effective mass renormalization. In this regard, it would be very interesting to explore the electronic structure in doped LHPs. Here, we report high-resolution angle-resolved photoemission spectroscopy (ARPES) studies on both pristine and Cl-doped CsPbBr3. The experimental band dispersions are extracted from ARPES spectra along both Γ¯ – M¯ – Γ¯ and X¯ – M¯ – X¯ high symmetry directions. DFT calculations are performed and directly compared with the ARPES data. Our results have revealed the band structure of Cl-doped CsPbBr3 for the first time, which have also unveiled the effective mass renormalization in the Cl-doped CsPbBr3 compound. Doping dependent measurements indicate that the chlorine doping could moderately tune the renormalization strength. These results will help understand the physical properties of LHPs as a function of doping.

Nonsymmorphic symmetry protected nodal lines in layered topological semimetal Ta3GeTe6

Topological semimetals have garnered significant attention due to their distinctive physical properties. However, the ideal material platforms for studying these phenomena remain limited. Here, we report the synthesis and nontrivial topological properties of high-quality van der Waals material Ta3GeTe6. Angle-resolved photoemission spectroscopy studies performed systematically on the as-grown Ta3GeTe6 single crystal along different high-symmetry directions reveal the formation of two nodal lines located near 0.07 and 0.55 eV below EF along the loop X-U-R-S, which arises from band crossings protected by nonsymmorphic symmetry. Furthermore, the nodal lines near the Fermi level along the S-R and S-X directions exhibit a flat feature. The discovery of this material enriches the family of topological nodal line semimetals and provides a promising platform for future investigations into exotic electronic correlation phenomena and potential device applications.

Observation of momentum-dependent charge density wave gap in a layered antiferromagnet {textrm{Gd}}{textrm{Te}}_{3}

Charge density wave (CDW) ordering has been an important topic of study for a long time owing to its connection with other exotic phases such as superconductivity and magnetism. The R{textrm{Te}}_{3} (R = rare-earth elements) family of materials provides a fertile ground to study the dynamics of CDW in van der Waals layered materials, and the presence of magnetism in these materials allows to explore the interplay among CDW and long range magnetic ordering. Here, we have carried out a high-resolution angle-resolved photoemission spectroscopy (ARPES) study of a CDW material {textrm{Gd}}{textrm{Te}}_{3}, which is antiferromagnetic below sim mathrm {12~K}, along with thermodynamic, electrical transport, magnetic, and Raman measurements. Our ARPES data show a two-fold symmetric Fermi surface with both gapped and ungapped regions indicative of the partial nesting. The gap is momentum dependent, maximum along {overline{Gamma }}-mathrm{overline{Z}} and gradually decreases going towards {overline{Gamma }}-mathrm{overline{X}}. Our study provides a platform to study the dynamics of CDW and its interaction with other physical orders in two- and three-dimensions.

Spin- and angle-resolved photoemission spectroscopy study of heptahelicene layers on Cu(111) surfaces.

It has been demonstrated previously that electrons interact differently with chiral molecules depending on their polarization. For enantiomeric pure monolayers of heptahelicene, opposite asymmetries in spin polarization were reported and attributed to the so-called chirality-induced spin selectivity effect. However, these promising proof-of-concept photoemission experiments lack the angular and energy resolution that could provide the necessary insights into the mechanism of this phenomenon. In order to fill in the missing gaps, we provide a detailed spin- and angle-resolved photoemission spectroscopy study of heptahelicene layers on a Cu(111) substrate. Throughout the large accessible energy and angle range, no chirality induced spin asymmetry in photoemission could be observed. Possible reasons for the absence of signatures of the spin-dependent electron transmission through the chiral molecular layer are briefly discussed.

Angle-resolved photoemission spectroscopy study on iron-based superconductors

Angle-resolved photoemission spectroscopy study on iron-based superconductors

High-performance time- and angle-resolved photoemission spectroscopy studies on quantum materials

通过飞秒激光激发固体材料，可利用材料中不同自由度的响应时间尺度研究多体相互作用、追踪超快相变过程、实现光诱导新物态或隐藏态等，是凝聚态物理研究的前沿和重要探索方向。时间分辨角分辨光电子能谱是近十多年发展起来的研究量子材料在飞秒激光激发后超快电子结构动力学的关键实验手段。本文回顾了基于非线性光学晶体和高阶倍频的时间分辨角分辨光电子能谱的基本原理和组成，以及利用其对量子材料的超快电子结构动力学进行的研究。主要包括四个方面的研究进展：（1）量子材料的非占据电子态探测；（2）光诱导的超快电子结构相变；（3）关联电子材料中电声相互作用强度确定；（4）光致新物态。最后，讨论了时间分辨角分辨光电子能谱未来可能的发展方向。

Bulk and surface electronic structure of NiBi3

We present a high-resolution, angle-resolved photoemission spectroscopy study of the normal electronic state of the superconducting ${\mathrm{NiBi}}_{3}$. Our experimental results show a complex Fermi surface structure with many sheets along the $\mathrm{\ensuremath{\Gamma}}\text{\ensuremath{-}}X$ and $\mathrm{\ensuremath{\Gamma}}\text{\ensuremath{-}}Y$ directions of the Brillouin zone. The band structure presents a topological surface state (TSS) at the high symmetry $\mathrm{\ensuremath{\Gamma}}$ point with a surface Dirac point at the energy $\ensuremath{-}0.185$ eV. The Dirac-like cone presents a linear dispersion along ${\mathrm{k}}_{x}$ while it presents saddle-like states along ${\mathrm{k}}_{y}$ located in the vicinity of the surface Dirac point. Our results are in good agreement with results of density functional theory band structure calculations. We also discuss the topological band structure of the ${\mathrm{NiBi}}_{3}$ compound.

Flat band in hole-doped transition metal dichalcogenide observed by angle-resolved photoemission spectroscopy

Layered transition metal dichalcogenides (TMDCs) gained widespread attention because of their electron-correlation-related physics, such as charge density wave (CDW), superconductivity, etc. In this paper, we report the high-resolution angle-resolved photoemission spectroscopy (ARPES) studies on the electronic structure of Ti-doped 1T-Ti x Ta1–x S2 with different doping levels. We observe a flat band that originates from the formation of the star of David super-cell at the x = 5% sample at the low temperature. With the increasing Ti doping levels, the flat band vanishes in the x = 8% sample due to the extra hole carrier. We also find the band shift and variation of the CDW gap caused by the Ti-doping. Meanwhile, the band folding positions and the CDW vector q CDW are intact. Our ARPES results suggest that the localized flat band and the correlation effect in the 1T-TMDCs could be tuned by changing the filling factor through the doping electron or hole carriers. The Ti-doped 1T-Ti x Ta1–x S2 provides a platform to fine-tune the electronic structure evolution and a new insight into the strongly correlated physics in the TMDC materials.

Nonmagnetic Sn doping effect on the electronic and magnetic properties of antiferromagnetic topological insulator MnBi[formula omitted]Te[formula omitted

We investigated the effect of nonmagnetic Sn doping on the electronic and magnetic properties of antiferromagnetic topological insulator MnBi2Te4. We observe that the Sn doping reduces out-of-plane antiferromagnetic (AFM) interactions in Mn1−xSnxBi2Te4 for up to 68% of Sn concentration and above, the system is found to be a paramagnetic. In this way, the anomalous Hall effect observed at a very high critical field of 7.8 T in MnBi2Te4 is reduced to 2 T at 68% of Sn doping. Electrical transport measurements suggest that all compositions are metallic in nature, while the low temperature resistivity is sensitive to the AFM ordering and to the doping-induced disorder. Hall effect study demonstrates that Sn actually dopes electrons into the system, thus, enhancing the electron carrier density almost by two orders at 68% of Sn. In contrast, SnBi2Te4 is found to be a p-type metal. Angle-resolved photoemission spectroscopy (ARPES) studies show that the topological properties are intact at least up to 55% of Sn doping as the Dirac surface states are present near the Fermi level. But in SnBi2Te4 we are unable to detect the surface states due to heavy hole doping. Thus, the Sn doping significantly affects the electronic and magnetic properties of MnBi2Te4.

Interlayer hybridization in a van der Waals quantum spin-Hall insulator/superconductor heterostructure

In this work, we present an angle-resolved photoemission spectroscopy study of a 1T′-WTe2 monolayer epitaxially grown on NbSe2 substrates, a prototypical quantum spin Hall insulator (QSHI)/superconductor heterojunction. Angle-resolved photoemission spectroscopy data indicate the formation of electronic states in the bulk bandgap of WTe2, which are absent in the nearly free-standing WTe2 grown on the highly oriented pyrolytic graphite substrate, where an energy gap of ∼100 meV is reported. The results are explained in terms of hybridization effects promoted by the QSHI–superconductor interaction at WTe2/NbSe2 interfaces, in line with recent scanning probe microscopy investigation and theoretical band structure calculations. Our findings highlight the important role of interlayer interaction on the electronic properties and ultimately on the engineering of topological properties of the QSHI/superconducting heterostructure.

Electronic structure and correlations in planar trilayer nickelate Pr4Ni3O8.

The discovery of superconductivity in planar nickelates raises the question of how the electronic structure and correlations of Ni1+ compounds compare to those of the Cu2+ cuprate superconductors. Here, we present an angle-resolved photoemission spectroscopy (ARPES) study of the trilayer nickelate Pr4Ni3O8, revealing a Fermi surface resembling that of the hole-doped cuprates but with critical differences. Specifically, the main portions of the Fermi surface are extremely similar to that of the bilayer cuprates, with an additional piece that can accommodate additional hole doping. We find that the electronic correlations are about twice as strong in the nickelates and are almost k-independent, indicating that they originate from a local effect, likely the Mott interaction, whereas cuprate interactions are somewhat less local. Nevertheless, the nickelates still demonstrate the strange-metal behavior in the electron scattering rates. Understanding the similarities and differences between these two families of strongly correlated superconductors is an important challenge.

Angle-resolved photoemission spectroscopy study of charge density wave order in the layered semiconductor EuTe4

Layered tellurides have been extensively studied as a platform for investigating the Fermi surface (FS) nesting-driven charge density wave (CDW) states. EuTe4, one of quasi-two-dimensional (quasi-2D) binary rare-earth tetratellurides CDW compounds, with unconventional hysteretic transition, is currently receiving much attention. Here, the CDW modulation vector, momentum and temperature dependence of CDW gaps in EuTe4 are investigated using angle-resolved photoemission spectroscopy. Our results reveal that (i) a FS nesting vector q ~ 0.67 b* drives the formation of CDW state, (ii) a large anisotropic CDW gap is fully open in the whole FS, and maintains a considerable size even at 300 K, leading to appearance of semiconductor properties, (iii) an abnormal non-monotonic increase of CDW gap in magnitude as a function of temperature, (iv) an extra, larger gap opens at a higher binding energy due to the interaction between the different orbits of the main bands.

Fermiology and Origin of T_{c} Enhancement in a Kagome Superconductor Cs(V_{1-x}Nb_{x})_{3}Sb_{5}.

Kagome metals AV_{3}Sb_{5} (A=K, Rb, and Cs) exhibit a characteristic superconducting ground state coexisting with a charge density wave (CDW), whereas the mechanisms of the superconductivity and CDW have yet to be clarified. Here we report a systematic angle-resolved photoemission spectroscopy (ARPES) study of Cs(V_{1-x}Nb_{x})_{3}Sb_{5} as a function of Nb content x, where isovalent Nb substitution causes an enhancement of superconducting transition temperature (T_{c}) and the reduction of CDW temperature (T_{CDW}). We found that the Nb substitution shifts the Sb-derived electron band at the Γ point downward and simultaneously moves the V-derived band around the M point upward to lift up the saddle point (SP) away from the Fermi level, leading to the reduction of the CDW-gap magnitude and T_{CDW}. This indicates a primary role of the SP density of states to stabilize the CDW. The present result also suggests that the enhancement of superconductivity by Nb substitution is caused by the cooperation between the expansion of the Sb-derived electron pocket and the recovery of the V-derived density of states at the Fermi level.

Pseudogap suppression by competition with superconductivity in La-based cuprates

We carried out a comprehensive high-resolution angle-resolved photoemission spectroscopy (ARPES) study of the pseudogap interplay with superconductivity in La-based cuprates. The three systems La2−xSrxCuO4, La1.6−xNd0.4SrxCuO4, and La1.8−xEu0.2SrxCuO4 display slightly different pseudogap critical points in the temperature versus doping phase diagram. We studied the pseudogap evolution into the superconducting state for doping concentrations just below the critical point. In this setting, near optimal doping for superconductivity and in the presence of the weakest possible pseudogap, we uncover how the pseudogap is partially suppressed inside the superconducting state. This conclusion is based on the direct observation of a reduced pseudogap energy scale and re-emergence of spectral weight suppressed by the pseudogap. Altogether these observations suggest that the pseudogap phenomenon in La-based cuprates is in competition with superconductivity for antinodal spectral weight.Received 27 April 2022Accepted 30 August 2022DOI:https://doi.org/10.1103/PhysRevResearch.4.043015Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasElectronic structurePhysical SystemsCupratesTechniquesAngle-resolved photoemission spectroscopyCondensed Matter, Materials & Applied Physics

Large antiferromagnetic fluctuation enhancement of the thermopower at a critical doping in magnetic semimetal Cr1+δTe2

Cr1+dTe2 is a self-intercalated transition metal dichalcogenide that hosts tunable electronic filling and magnetism in its semimetallic band structure. Recent angle-resolved photoemission spectroscopy (ARPES) studies have unveiled a systematic shift in this semimetallic band structure relative to the chemical potential with increased Cr doping. This report presents the temperature and magnetic field dependence of the longitudinal thermopower Sxx for different Cr1+dTe2 compositions. We show that as doping increases, the sign of Sxx changes from positive to negative at the critical doping level of d ~ 0.5. This observed doping-dependent trend in the thermopower is consistent with the evolution of the semimetallic band structure from ARPES. Importantly, an anomalous enhancement of the thermoelectric response is also observed around d~0.5. Combining information from magnetometry and ARPES measurements, existence of the critical nature of the doping level dc (~0.5) is unveiled in magnetic semimetal Cr1+dTe2, where antiferromagnetic fluctuation and near-Fermi-energy pseudogap formation play a potential vital role in enhancing thermoelectric energy conversion.

Exciton optics, dynamics, and transport in atomically thin semiconductors

Atomically thin semiconductors such as transition metal dichalcogenide (TMD) monolayers exhibit a very strong Coulomb interaction, giving rise to a rich exciton landscape. This makes these materials highly attractive for efficient and tunable optoelectronic devices. In this Research Update, we review the recent progress in the understanding of exciton optics, dynamics, and transport, which crucially govern the operation of TMD-based devices. We highlight the impact of hexagonal boron nitride-encapsulation, which reveals a plethora of many-particle states in optical spectra, and we outline the most novel breakthroughs in the field of exciton-polaritonics. Moreover, we underline the direct observation of exciton formation and thermalization in TMD monolayers and heterostructures in recent time-resolved, angle-resolved photoemission spectroscopy studies. We also show the impact of exciton density, strain, and dielectric environment on exciton diffusion and funneling. Finally, we put forward relevant research directions in the field of atomically thin semiconductors for the near future.

Differentiated roles of Lifshitz transition on thermodynamics and superconductivity in La2-xSrxCuO4

The effect of Lifshitz transition on thermodynamics and superconductivity in hole-doped cuprates has been heavily debated but remains an open question. In particular, an observed peak of electronic specific heat is proposed to originate from fluctuations of a putative quantum critical point p* (e.g., the termination of pseudogap at zero temperature), which is close to but distinguishable from the Lifshitz transition in overdoped La-based cuprates where the Fermi surface transforms from hole-like to electron-like. Here we report an in situ angle-resolved photoemission spectroscopy study of three-dimensional Fermi surfaces in La2-xSrxCuO4 thin films (x = 0.06 to 0.35). With accurate kz dispersion quantification, the said Lifshitz transition is determined to happen within a finite range around x = 0.21. Normal state electronic specific heat, calculated from spectroscopy-derived band parameters, reveals a doping-dependent profile with a maximum at x = 0.21 that agrees with previous thermodynamic microcalorimetry measurements. The account of the specific heat maximum by underlying band structures excludes the need for additionally dominant contribution from the quantum fluctuations at p*. A d-wave superconducting gap smoothly across the Lifshitz transition demonstrates the insensitivity of superconductivity to the dramatic density of states enhancement.

A-type antiferromagnetic order in semiconducting EuMg2Sb2 single crystals

Eu-based Zintl-phase materials EuA$_2$Pn$_2$ (A = Mg, In, Cd, Zn; Pn = Bi, Sb, As, P) have generated significant recent interest owing to the complex interplay of magnetism and band topology. Here, we investigated the electronic, magnetic, and electronic properties of the layered Zintl-phase single crystals of EuMg$_2$Sb$_2$ with the trigonal CaAl$_2$Si$_2$ crystal structure (space group $P\bar{3}m1$). Electrical resistivity measurements complemented with angle-resolved photoemission spectroscopy (ARPES) studies find an activated behavior with the intrinsic conductivity at high temperatures indicating a semiconducting electronic ground state with a narrow energy gap of 370 meV. Magnetic susceptibility and zero-field heat-capacity measurements indicate that the compound undergoes antiferromagnetic (AFM) ordering at the Neel temperature $T_{\rm N}$ = 8.0(2) K. Zero-field neutron-diffraction measurements reveal that the AFM ordering is A-type where the Eu ordered moments (Eu$^{2+}$, S= 7/2) arranged in ab-plane layers are aligned ferromagnetically in the ab plane with the Eu moments in adjacent layers aligned antiferromagnetically. We also find that Eu-moment reorientation in the trigonal AFM domains within the ab planes occurs below $T_{\rm N}$ at low fields < 0.05 T due to very small in-plane anisotropy. Although isostructural semimetallic EuMg$_2$Bi$_2$ is reported to host Dirac surface states, the observation of narrow-gap semiconducting behavior in EuMg$_2$Sb$_2$ implies a strong role of spin-orbit coupling in tuning the electronic states of these materials.

Superconducting dome and pseudogap endpoint in Bi2201

Once doped away from their parent Mott insulating state, the hole-doped cuprates enter into many varied and exotic phases. The onset temperature of each phase is then plotted versus $p$---the number of doped holes per copper atom---to form a representative phase diagram. Apart from differences in the absolute temperature scales among the various families, the resultant phase diagrams are strikingly similar. In particular, the $p$ values corresponding to optimal doping (${p}^{\mathrm{opt}}\ensuremath{\sim}0.16$) and to the end of the pseudogap phase $({p}^{*}\ensuremath{\sim}0.19--0.20)$ are essentially the same for all cuprate families bar one: the single-layer Bi-based cuprate ${\mathrm{Bi}}_{2+z\ensuremath{-}y}{\mathrm{Pb}}_{y}{\mathrm{Sr}}_{2\ensuremath{-}x\ensuremath{-}z}{\mathrm{La}}_{x}{\mathrm{CuO}}_{6+\ensuremath{\delta}}$ (Bi2201). This anomaly arises partly due to the complex stoichiometry of this material and also to the different $p$ values inferred from disparate (e.g., bulk or surface) measurements performed on samples with comparable superconducting transition temperatures ${T}_{c}$. Here, by combining measurements of the in-plane resistivity in zero and high magnetic fields with angle-resolved photoemission spectroscopy studies in the superconducting and normal state, we argue that the phase diagram of Bi2201 may in fact be similar to that realized in other families. This study therefore brings Bi2201 into the fold and supports the notion of universality of ${p}^{\mathrm{opt}}$ and ${p}^{*}$ in all hole-doped cuprates.

Magnetotransport and ARPES studies of the topological insulators Sb2Te3 and Bi2Te3 grown by MOCVD on large-area Si substrates

Recently, the topological insulators (TIs) antimony telluride (Sb2Te3) and bismuth telluride (Bi2Te3) are attracting high interest for applications based on spin-charge interconversion mechanisms. Aiming to make a step toward the technology transfer, it is of major importance to achieve and investigate epitaxial quality-TIs on large area Si-based substrates. In view of that, we report here magnetotransport and angle-resolved photoemission spectroscopy (ARPES) studies on Sb2Te3 and Bi2Te3 thin films grown by metal organic chemical vapor deposition (MOCVD) on top of 4″ Si(111) substrates. Clear weak antilocalization (WAL) effects are observed in both TIs, proving the existence of quantum transport mechanism, and the data are successfully interpreted in the framework of the Hikami–Larkin–Nagaoka model. Further, by dedicated magnetotransport experiments, it has been confirmed that the investigated WAL originates from two-dimensional (2D) topological states. ARPES has been performed ex-situ, and in both TIs the gapless Dirac cones have been observed and attributed to the topological surface states. Combining the proofs of the existence of quantum 2D transport as deduced from the analysis of the magnetoconductance curve with the direct observation of the Dirac-like band structure revealed by the ARPES spectra, it is possible to unambiguously confirm the topological nature of our Sb2Te3 and Bi2Te3 thin films. The results obtained on thin films grown by MOCVD on 4’’ Si(111) substrate mark an important step towards the technology transfer of the topological insulators studied in this work.