We present a detailed exposition of the design for time- and angle-resolved photoemission spectroscopy using a UV probe laser source that combines the nonlinear effects of \b{eta}-BaB2O4 and KBe2BO3F2 optical crystals. The photon energy of the probe laser can be switched between 6.0 and 7.2 eV, with the flexibility to operate each photon energy setting under two distinct resolution configurations. Under the fully optimized energy resolution configuration, we achieve an energy resolution of 8.5 meV at 6.0 eV and 10 meV at 7.2 eV. Alternatively, switching to the other configuration enhances temporal resolution, yielding a temporal resolution of 72 fs for 6.0 eV and 185 fs for 7.2 eV. We validated the performance and reliability of our system by applying it to measuring two typical materials: the topological insulator MnBi2Te4 and excitonic insulator candidate Ta2NiSe5.
Time- and angle-resolved photoemission spectroscopy (trARPES) is a powerful spectroscopic method to measure the ultrafast electron dynamics directly in momentum-space. However, band gap materials with exceptional strong Coulomb interaction such as monolayer transition metal dichlacogenides (TMDC) exhibit tightly bound excitons, which dominate their optical properties. This rises the question whether excitons, in particular their formation and relaxation dynamics, can be detected in photoemission. Here, we develope a fully microscopic theory of the temporal dynamics of excitonic time- and angle…
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 computation…
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 …
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, …
The interaction between light and novel two-dimensional electronic states holds promise to realize new fundamental physics and optical devices. Here, we use pump-probe photoemission spectroscopy to study the optically-excited Dirac surface states in the bulk-insulating topological insulator Bi2Te2Se, and reveal optical properties that are in sharp contrast to those of bulk-metallic topological insulators. We observe a gigantic optical life-time exceeding 4 micro-sec for the surface states in Bi2Te2Se, whereas the life-time in most topological insulators such as Bi2Se3 has been limited to a few…
Momentum transfer in the ponderomotive potential of near-infrared laser pulses leads to sizable energy shifts and electron-wavepacket squeezing in time-resolved ARPES
We report high-resolution spin-resolved photoemission spectroscopy (Spin-ARPES) measurements on the parent compound Sb of the recently discovered 3D topological insulator Bi1-xSbx [D. Hsieh et al., Nature 452, 970 (2008)]. By modulating the incident photon energy, we are able to map both the bulk and (111) surface band structure, from which we directly demonstrate that the surface bands are spin polarized by the spin-orbit interaction and connect the bulk valence and conduction bands in a topologically non-trivial way. A unique asymmetric Dirac surface state gives rise to a k-splitting of its …
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…
We identify features in the angle-resolved photoemission spectra (ARPES) arising from the periodic pattern characteristic for graphene heterostructure with hexagonal boron nitride (hBN). For this, we model ARPES spectra and intensity maps for five microscopic models used previously to describe moire superlattice in graphene/hBN systems. We show that detailed analysis of these features can be used to pin down the microscopic mechanism of the interaction between graphene and hBN. We also analyze how the presence of a moire-periodic strain in graphene or scattering of photoemitted electrons off h…
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…
We consider a ground-state wide-gap band insulator turning into a nonequilibrium excitonic insulator (NEQ-EI) upon visiting properly selected and physically relevant highly excited states. The NEQ-EI phase, characterized by self-sustained oscillations of the complex order parameter, neatly follows from a Nonequilibrium Green's Function treatment on the Konstantinov-Perel' contour. We present the first {\em ab initio} band structure of LiF, a ground-state bulk insulator, in different NEQ-EI states and show that these states can be generated by currently available pump pulses. We highlight two g…
We have performed spin- and angle-resolved photoemission spectroscopy of the topological insulator Pb(Bi,Sb)2Te4 (Pb124) and observed significant out-of-plane spin polarization on the hexagonally warped Dirac-cone surface state. To put this into context, we carried out quantitative analysis of the warping strengths for various topological insulators (Pb124, Bi2Te3, Bi2Se3, and TlBiSe2) and elucidated that the out-of-plane spin polarization Pz is systematically correlated with the warping strength. However, the magnitude of Pz is found to be only half of that expected from the kp theory when th…
The single-particle spectral function measures the density of electronic states (DOS) in a material as a function of both momentum and energy, providing central insights into phenomena such as superconductivity and Mott insulators. While scanning tunneling microscopy (STM) and other tunneling methods have provided partial spectral information, until now only angle-resolved photoemission spectroscopy (ARPES) has permitted a comprehensive determination of the spectral function of materials in both momentum and energy. However, ARPES operates only on electronic systems at the material surface and…
Spin-split two-dimensional electronic states have been observed on ultrathin Sn(001) films grown on InSb(001) substrates. Angle-resolved photoelectron spectroscopy (ARPES) performed on these films revealed Dirac-cone-like linear dispersion around the $\barΓ$ point of surface Brillouin zone, suggesting nearly massless electrons belonging to 2D surface states. The states disperse across a bandgap between bulk-like quantum well states in the films. Moreover, both circular dichroism of ARPES and spin-resolved ARPES studies show helical spin polarization of the Dirac-cone-like surface states, sugge…
We report high-resolution spin-resolved photoemission spectroscopy (Spin-ARPES) measurements on the parent compound Sb of the first discovered 3D topological insulator Bi{1-x}Sb{x} [D. Hsieh et al., Nature 452, 970 (2008) Submitted 2007]. By modulating the incident photon energy, we are able to map both the bulk and (111) surface band structure, from which we directly demonstrate that the surface bands are spin polarized by the spin-orbit interaction and connect the bulk valence and conduction bands in a topologically non-trivial way. A unique asymmetric Dirac surface state gives rise to a $k$…
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…
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)…
First direct observation of Spin-textures in Topological Insulators : Spin-resolved ARPES as a probe of topological quantum spin Hall effect and Berry's phase
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 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…
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）
In pump-probe time and angle-resolved photoemission spectroscopy (TR-ARPES) experiments the presence of the pump pulse adds a new level of complexity to the photoemission process in comparison to conventional ARPES. This is evidenced by pump-induced vacuum space-charge effects and surface photovoltages, as well as multiple pump excitations due to internal reflections in the sample-substrate system. These processes can severely affect a correct interpretation of the data by masking the out-of-equilibrium electron dynamics intrinsic to the sample. In this study, we show that such effects indeed …
Progress in performing angle-resolved photoemission spectroscopy (ARPES) with high spatial resolution in the order of 1~$μ$m or less (nanoARPES) has opened the possibility to map the spectral function of solids on this tiny scale and thereby obtain detailed information on the materials' \emph{local} electronic band structure and many-body interactions. Recently, nanoARPES has been used to study simple electronic devices, based on two-dimensional materials, with the possibility of tuning the carrier type and density by field effect-gating, and while passing a current through the device. It was …
