Time and angular resolved photoelectron spectroscopy is a powerful technique to measure electron dynamics in solids. Recent advances in this technique have facilitated band and energy resolved observations of the effect that excited phonons, have on the electronic structure. Here, we show with the help of \textit{ab initio} simulations that the Fourier analysis of time-resolved measurements of solids with excited phonon modes leads, in fact, to an observation of the band- and mode-resolved electron-phonon coupling directly from the experimental data and without need for theoretical computations.
Angle-resolved photoelectron spectroscopy (ARPES) is the main experimental tool to explore electronic structure of solids resolved in the electron momentum k . Soft-X-ray ARPES (SX-ARPES), operating in a photon energy range around 1 keV, benefits from enhanced probing depth compared to the conventional VUV-range ARPES, and elemental/chemical state specificity achieved with resonant photoemission. These advantages make SX-ARPES ideally suited for buried heterostructure and impurity systems, which are at the heart of current and future electronics. These applications are illustrated here with a …
Indirect transitions of electrons in graphene and graphite are investigated by means of angle-resolved photoemission spectroscopy (ARPES) with several different incident photon energies and light polarizations. The theoretical calculations of the indirect transition for graphene and graphite are compared with the experimental measurements for highly-oriented pyrolytic graphite and a single-crystal of graphite. The dispersion relations for the transverse optical (TO) and the out-of-plane longitudinal acoustic (ZA) phonon modes of graphite and the TO phonon mode of graphene can be extracted from…
Photo-induced charge separation in transition metal dichalcogenide heterobilayers is being explored for moiré excitons, spin-valley polarization, and quantum phases of excitons/electrons. While different momentum spaces may be critically involved in charge separation dynamics, little is known directly from experiments. Here we determine momentum-resolved electron dynamics in the WS2/MoS2 heterobilayer using time and angle resolved photoemission spectroscopy (TR-ARPES). Upon photoexcitation in the K valleys, we detect electrons in M/2, M, and Q valleys/points on time scales as short as ~70 fs, …
Angle-resolved photoemission spectroscopy (ARPES), an experimental technique based on the photoelectric effect, is arguably the most powerful method for probing the electronic structure of solids. The past decade has witnessed notable progress in ARPES, including the rapid development of soft-X-ray ARPES, time-resolved ARPES, spin-resolved ARPES and spatially resolved ARPES, as well as considerable improvements in energy and momentum resolution. Consequently , ARPES has emerged as an indispensable experimental probe in the study of topological materials, which have characteristic non-trivial b…
The dynamics of photo-generated electron-hole pairs in solids are dictated by many-body interactions such as electron-electron and electron-phonon scattering. Hence, understanding and controlling these scattering channels is crucial for many optoelectronic applications, ranging from light harvesting to optical amplification. Here we measure the formation and relaxation of the photo-generated non-thermal carrier distribution in monolayer graphene with time- and angle-resolved photoemission spectroscopy. Using sub 10fs pulses we identify impact ionization as the primary scattering channel, which…
I present a fully abinitio scheme to model transient spectroscopy signals in presence of strongly bound excitons. Using LiF as a prototype material, I show that the scheme is able to capture the exciton signature both in time-resolved ARPES and transient absorption experiments. The approach is completely general and can become the reference scheme for modelling pump and probe experiment in a wide range of materials.
We develop a general theory to model the angle-resolved photoemission spectroscopy (ARPES) of commensurate and incommensurate van der Waals (vdW) structures, formed by lattice mismatched and/or misaligned stacked layers of two-dimensional materials. The present theory is based on a tight-binding description of the structure and the concept of generalized umklapp processes, going beyond previous descriptions of ARPES in incommensurate vdW structures, which are based on continuous, low-energy models, being limited to structures with small lattice mismatch/misalignment. As applications of the gen…
First-principles methods for time-resolved angular resolved photoelectron spectroscopy play a pivotal role in providing interpretation and microscopic understanding of the complex experimental data and in exploring novel observables or observation conditions that may be achieved in future experiments. Here we describe an efficient, reliable and scalable first-principles method for tr-ARPES based on time-dependent density functional theory including propagation and surface effects usually discarded in the widely used many-body techniques based on computing the non-equilibrium spectral function …
The linewidths of the electronic bands originating from the electron-phonon coupling in graphene are analyzed based on model tight-binding calculations and experimental angle-resolved photoemission spectroscopy (ARPES) data. Our calculations confirm the prediction that the high-energy optical phonons provide the most essential contribution to the phonon-induced linewidth of the two upper occupied $σ$ bands near the $\barΓ$-point. For larger binding energies of these bands, as well as for the $π$ band, we find evidence for a substantial lifetime broadening from interband scattering $π\rightarro…
Photogeneration and signatures of coherent phonons in time-resolved photoemission spectroscopy: First-principles time-dependent adiabatic GW approach
Institute of Atomic and Molecular Sciences, Academia Sinica（原子分子科学研究所，中央研究院）；Physics Division, National Center of Theoretical Sciences（理论科学中心物理部）；Mork Family Department of Chemical Engineering and Materials Science, University of Southern California（南加州大学莫克家族化学工程与材料科学系）；Department of Physics, University of California at Berkeley（加州大学伯克利分校物理系）；Materials Sciences Division, Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室材料科学部）
Soft-X-ray ARPES (SX-ARPES) with its enhanced probing depth and chemical specificity allows access to fundamental electronic structure characteristics - momentum-resolved spectral function, band structure, Fermi surface - of systems difficult and even impossible for the conventional ARPES such as three-dimensional materials, buried interfaces and impurities. After a recap of the spectroscopic abilities of SX-ARPES, we review its applications to oxide interfaces, focusing on the paradigm LaAlO3-SrTiO3 interface. Resonant SX-ARPES at the Ti L-edge accentuates photoemission response of the mobile…
Long-Lived Coherence between Incoherent Excitons revealed by Time-Resolved ARPES: An Exact Solution
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China（合肥微尺度物质科学国家研究中心，中国科学技术大学）；Dipartimento di Fisica, Università di Roma Tor Vergata（罗马托尔维加塔大学物理系）；INFN, Sezione di Roma Tor Vergata（意大利国家核物理研究所，罗马托尔维加塔分部）
Angle-resolved photoemission spectroscopy using a micro-focused beam spot (micro-ARPES) is becoming a powerful tool to elucidate key electronic states of exotic quantum materials. We have developed a versatile micro-ARPES system based on synchrotron radiation beam focused with a Kirkpatrick-Baez mirror optics. The mirrors are monolithically installed on a stage, which is driven with five-axes motion, and are vibrationally separated from the ARPES measurement system. Spatial mapping of the Auphotolithography pattern on Si signifies the beam spot size of 10 $μ$m (horizontal) x 12 $μ$m (vertical)…
Excitons in WSe2 time-resolved ARPES: particle or oscillation?
Istituto di Struttura della Materia and Division of Ultrafast Processes in Materials (FLASHit) of the National Research Council（国家研究委员会物质结构研究所及材料超快过程分部（FLASHit））；Laboratory of Ultrafast Spectroscopy (LSU) and Lausanne Centre for Ultrafast Science (LACUS), École Polytechnique Fédérale de Lausanne (EPFL)（洛桑联邦理工学院超快光谱实验室（LSU）与洛桑超快科学中心（LACUS））
With its direct correspondence to electronic structure, angle-resolved photoemission spectroscopy (ARPES) is a ubiquitous tool for the study of solids. When extended to the temporal domain, time-resolved (TR)-ARPES offers the potential to move beyond equilibrium properties, exploring both the unoccupied electronic structure as well as its dynamical response under ultrafast perturbation. Historically, ultrafast extreme ultraviolet (XUV) sources employing high-order harmonic generation (HHG) have required compromises that make it challenging to achieve a high energy resolution - which is highly …
Angle-resolved photoemission spectroscopy (ARPES) is a powerful experimental technique for directly probing electron dynamics in solids. The energy vs. momentum dispersion relations and the associated spectral broadenings measured by ARPES provide a wealth of information on quantum many-body interaction effects. In particular, ARPES allows studies of the Coulomb interaction among electrons (electron-electron interactions) and the interaction between electrons and lattice vibrations (electron-phonon interactions). Here, we report ab initio simulations of the ARPES spectra of graphene including …
We show that the intensity of pumped states near Weyl point is different when pumped with left- and right-handed circular polarized light, which leads to a special circular dichroism (CD) in time-dependent angle resolved photoemission spectra (ARPES). We derive the expression for the CD of time-dependent ARPES, which is directly related to the chirality of Weyl fermions. Based on the above derivation, we further propose a method to determine the chirality for a given Weyl point from the CD of time-dependent ARPES. The corresponding CD spectra for TaAs has then been calculated from the first pr…
Time-resolved, angle-resolved photoemission spectroscopy (TR-ARPES) is a one-particle spectroscopic technique that can probe excitons (two-particle excitations) in momentum space. We present an ab initio, time-domain GW approach to TR-ARPES and apply it to monolayer MoS$_2$. We show that photoexcited excitons may be measured and quantified as satellite bands, as well as leading to the renormalization of the quasiparticle bands. These features are explained in terms of an exciton- Floquet phenomenon induced by an exciton time-dependent bosonic field, which is orders of magnitude stronger than l…
We obtain analytical expressions for the electron self-energy and the electron-phonon coupling in electron-doped graphene using electron-phonon matrix elements extracted from density functional theory simulations. From the electron self-energies we calculate angle resolved photoemission spectra. We demonstrate that the measured kink at $\approx -0.2$ eV from the Fermi level is actually composed of two features, one at $\approx -0.195$ eV due to the twofold degenerate E$_{2g}$ mode, and a second one at $\approx -0.16$ eV due to the A$_{1}^{'}$ mode. The electron-phonon coupling extracted from t…
We have performed high-resolution angle-resolved photoemission spectroscopy (ARPES) on trigonal tellurium consisting of helical chains in the crystal. Through the band-structure mapping in the three-dimensional Brillouin zone, we found a definitive evidence for the band splitting originating from the chiral nature of crystal. A direct comparison of the band dispersion between the ARPES results and the first-principles band-structure calculations suggests the presence of Weyl nodes and tiny spin-polarized hole pockets around the H point. The present result opens a pathway toward studying the in…
We present a novel theoretical approach to simulate spin, time and angular-resolved photoelectron spectroscopy (ARPES) from first principles that is applicable to surfaces, thin films, few layer systems, and low-dimensional nanostructures. The method is based on a general formulation in the framework of time-dependent density functional theory (TDDFT) to describe the real time-evolution of electrons escaping from a surface under the effect of any external (arbitrary) laser field. By extending the so called t-SURFF method to periodic systems one can calculate the final photoelectron spectrum by…
Recent improvements to spatial resolution in angle-resolved photo-emission spectroscopy (ARPES) have made it common to perform measurements with a very brief dwell time, for the purpose of mapping the spectral function over large surface regions. However, rapid measurement modalities can suffer a grid-like intensity modulation due to a wire mesh that is typically placed in front of the ARPES detector to block stray electrons. Here, we explore Fourier-based methods that can effectively remove this artifact, and improve the quality of ARPES images obtained in rapid scanning modes. An open source…
Time-resolved Raman spectroscopy has been applied to probe the anharmonic coupling and electron-phonon interaction of optical phonons in graphite. From the decay of the transient anti-Stokes scattering of the G-mode following ultrafast excitation, we measured a lifetime of 2.2+/-0.1ps for zone-center optical phonons. We also observed a transient stiffening of G-mode phonons, an effect attributed to the reduction of the electron-phonon coupling for high electronic temperatures.
Orbital-resolved anisotropic electron pockets in electron-doped SrTiO3 observed by ARPES
NTT Basic Research Laboratories, NTT Corporation（NTT基础研究所）；Department of Electrical Engineering and Information Systems, The University of Tokyo（东京大学电气信息工程系）；Center for Spintronics Research Network, The University of Tokyo（东京大学自旋网络研究中心）
Sub-tesla on-chip nanomagnetic metamaterial platform for angle-resolved photoemission spectroscopy
Yale University（耶鲁大学）；Rice University（莱斯大学）；Boston College（波士顿学院）；Princeton University（普林斯顿大学）；University of Maine（缅因大学）；University of Minnesota（明尼苏达大学）；Georgia Institute of Technology（佐治亚理工学院）；Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory（斯坦福同步辐射光源，SLAC国家加速器实验室）
The quest for mapping the femtosecond dynamics of the electronic band structure of complex materials via Time- and Angle-Resolved Photoelectron Spectroscopy (TR-ARPES) over their full First Brillouin Zone is pushing the development of schemes to efficiently generate ultrashort photon pulses in the VUV-range of photon energies. At present, the critical aspect is to combine a high photon energy with high photoemission count rates and a small pulse-bandwidth, necessary to achieve high energy resolution in ARPES, while preserving a good time resolution and mitigating space-charge effects. Here we …
Recently, Kobayashi et al. (arXiv:1608.07718; ref. 1) have proposed an alternative interpretation of our angle-resolved photoemission spectroscopy (ARPES) results for the dilute ferromagnetic semiconductor (Ga,Mn)As. They claim that our ARPES data [Sci. Rep. 6, 27266 (2016); ref. 2] can be explained by locating the Fermi level EF above the valence-band top, supporting the impurity-band model of ferromagnetic (Ga,Mn)As. In this comment, we show that the assignment of bands' positions in respect to EF by Kobayashi et al. is not consistent with our data. By comparing the ARPES result to band-stru…
In this letter we report measurements of the coupling between Dirac fermion quasiparticles (DFQs) and phonons on the (001) surface of the strong topological insulator Bi2Se3. While most contemporary investigations of this coupling have involved examining the temperature dependence of the DFQ self-energy via angle-resolved photoemission spectroscopy (ARPES) measurements, we employ inelastic helium atom scattering to explore, for the first time, this coupling from the phonon perspective. Using a Hilbert transform, we are able to obtain the imaginary part of the phonon self-energy associated with…
Angle-resolved photoemission spectroscopy (ARPES) is the key momentum-resolved technique for direct probing of the electronic structure of a material. However, since it is very surface-sensitive, it has been applied to a relatively small set of complex oxides that can be easily cleaved in ultra-high vacuum. Here we describe a new multi-module system at Brookhaven National Laboratory (BNL) in which an oxide molecular beam epitaxy (OMBE) is interconnected with an ARPES and a spectroscopic-imaging scanning tunneling microscopy (SI-STM) module. This new capability largely expands the range of comp…
The electronic structure of $p$-type doped \BiTe is studied by angle resolved photoemission spectroscopy (ARPES) to experimentally confirm the mechanism responsible for the high thermoelectric figure of merit. Our ARPES study shows that the band edges are located off the $Γ$-Z line in the Brillouin zone, which provides direct observation that the spin-orbit interaction is a key factor to understand the electronic structure and the corresponding thermoelectric properties of \BiTe. Successive time dependent ARPES measurement also reveals that the electron-like bands crossing E$_F$ near the $\und…
We have studied the O 2p valence-band structure of Nb-doped SrTiO3, in which a dilute concentration of electrons are doped into the d0 band insulator, by angle-resolved photoemission spectroscopy (ARPES) measurements. We found that ARPES spectra at the valence band maxima at the M [k = (pi/a, pi/a, 0)]and R [k = (pi/a, pi/a, pi/a)] points start from ~ 3.3 eV below the Fermi level (EF), consistent with the indirect band gap of 3.3 eV and the EF position at the bottom of the conduction band. The peak position of the ARPES spectra were, however, shifted toward higher binding energies by ~ 500 meV…
Despite the intensive efforts for determining the mechanism that causes high-temperature superconductivity in copper oxide materials, no consensus on the pairing mechanism has been reached. Recent advances in high resolution angle-resolved photoemission spectroscopies have suggested that a sizeable electron-phonon coupling exists as the principal cause for kinks in the dispersion relations (energy versus wave vector) of the electronic states. Here, we report on a systematic study about the influence of the electron-phonon coupling parameter "$λ$" in the electronic quasiparticle dispersions alo…
Ultrafast signatures of Dirac / flat-band hybrid states from time-resolved ARPES
University of Regensburg（雷根斯堡大学）；Christian-Albrechts-Universität zu Kiel（基尔大学）；Deutsches Elektronen-Synchrotron DESY（德国电子同步辐射中心）；Chemnitz University of Technology（开姆尼茨工业大学）
For solid-state materials, the electronic structure, E(k), is critical in determining a crystal's physical properties. By experimentally detecting the electronic structure, the fundamental physics can be revealed. Angle-resolved photoemission spectroscopy (ARPES) is a powerful technique for directly observing the electronic structure with energy- and momentum-resolved information. Over the past decades, major improvements in the energy and momentum resolution, alongside the extension of ARPES observables to spin (SpinARPES), micrometer or nanometer lateral dimensions (MicroARPES/NanoARPES), an…
Angle-resolved photoemission spectroscopy (ARPES) has played an important role in determining the band structure and the superconducting gap structure of iron-based superconductors. Here from the ARPES perspective, we briefly review the main results from our group in the recent years on the iron-based superconductors and their parent compounds, and depict our current understanding on the antiferromagnetism and superconductivity in these materials.
Time-resolved ARPES in pumped excitonic systems: Floquet physics induced by excitonic fields
Dipartimento di Fisica “E.R. Caianiello”, Università degli Studi di Salerno（萨莱诺大学 E.R. 卡亚涅洛物理系）；CNR-SPIN, Unità di Salerno（意大利国家研究委员会 SPIN 研究所萨莱诺分部）；CNISM, Unità di Salerno, Università degli Studi di Salerno（萨莱诺大学 CNISM 研究所萨莱诺分部）
Plasma discharge lamps are widely utilized in the practice of angle-resolved photoemission spectroscopy (ARPES) experiments as narrow-linewidth ultraviolet photon sources. However, many emission lines such as Ar-I, Ne-I, and Ne-II have closely spaced doublet emission lines, which result in superimposed replica on the measured ARPES spectra. Here, we present a simple method for subtracting the contribution of these doublet emission lines from photoemission spectra. Benchmarking against ARPES spectra of well-characterized 2D materials, we demonstrate that this algorithm manages to subtract the d…
Various technical developments enlarged the potential of angle-resolved photo emission (ARPES) tremendously during the last one or two decades. In particular improved momentum and energy resolution as well as the use of photon energies from few eV up to several keV makes ARPES a rather unique tool to investigate the electronic properties of solids and surfaces. Obviously, this rises the need for a corresponding theoretical formalism that allows to accompany experimental ARPES studies in an adequate way. As will be demonstrated by several examples this goal could be achieved by various recent d…
Angle-resolved photoemission spectroscopy with sub-micrometer spatial resolution (μ-ARPES), has become a powerful tool for studying quantum materials. To achieve sub-micrometer or even nanometer-scale spatial resolution, it is important to focus the incident light beam (usually from the synchrotron radiation) using X-ray optics such as the zone plate or ellipsoidal capillary mirrors. Recently, we developed a laser-based μ-ARPES with spin-resolution (LMS-ARPES). The 177 nm laser beam is achieved by frequency doubling a 355 nm beam using a KBBF crystal and subsequently focused using an optical l…
Altermagnetism, ARPES, symmetry, non-relativistic band splitting
Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences（中国科学院上海微系统与信息技术研究所）；University of Chinese Academy of Sciences（中国科学院大学）；National Synchrotron Radiation Laboratory and School of Nuclear Science and Technology, University of Science and Technology of China（中国科学技术大学核科学与技术学院及国家同步辐射实验室）；Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute（上海先进应用研究院上海同步辐射光源）
Combining Angle resolved photoelectron spectroscopy (ARPES) and a $μ$-focused Laser, we have performed scanning ARPES microscopy measurements of the domain population within the nematic phase of FeSe single crystals. We are able to demonstrate a variation of the domain population density on a scale of a few 10 $μ$m while constraining the upper limit of the single domain size to less than 5 $μm$. This experiment serves as a demonstration of how combining the advantages of high resolution Laser ARPES and an ultimate control over the spatial dimension can improve investigations of materials by re…
Free-standing exfoliated monolayer graphene is an ultra-thin flexible membrane, which exhibits out of plane deformation or corrugation. In this paper, a technique is described to measure the band structure of such free-standing graphene by angle-resolved photoemission. Our results show that photoelectron coherence is limited by the crystal corrugation. However, by combining surface morphology measurements of the graphene roughness with angle-resolved photoemission, energy dependent quasiparticle lifetime and bandstructure measurements can be extracted. Our measurements rely on our development …
The crystallographic stacking order in multilayer graphene plays an important role in determining its electronic structure. In trilayer graphene, rhombohedral stacking (ABC) is particularly intriguing, exhibiting a flat band with an electric-field tunable band gap. Such electronic structure is distinct from simple hexagonal stacking (AAA) or typical Bernal stacking (ABA), and is promising for nanoscale electronics, optoelectronics applications. So far clean experimental electronic spectra on the first two stackings are missing because the samples are usually too small in size (um or nm scale) …
