Temperature evolution of quasiparticle dispersion dynamics in semimetallic 1T-TiTe2 via high-resolution angle-resolved photoemission spectroscopy and ultrafast optical pump-probe spectroscopy
High-resolution angle-resolved photoemission spectroscopy and ultrafast optical pump-probe spectroscopy were used to study semimetallic 1T - TiTe2 quasiparticle dispersion and dynamics. A kink and a flat band, having the same energy scale and temperature-dependent behaviors along the G-M direction, were detected. Both manifested at low temperatures but blurred as temperature increased. The kink was formed by an electron-phonon coupling. And the localized flat band might be closely related to an electron-phonon coupling. Ultrafast optical spectroscopy identified multiple distinct time scales in the 10-300 K range. Quantitative analysis of the fastest decay process evidenced a significant lifetime temperature dependence at high temperatures, while this starts to change slowly below ~ 100 K where an anomalous Hall coefficient occurred. At low temperature, a coherent A1g phonon mode with a frequency of ~ 4.36 THz was extracted. Frequency temperature dependence suggests that phonon hardening occurs as temperature falls and anharmonic effects can explain it. Frequency fluence dependence indicates that the phonons soften as fluence increases.
The thermoelectric effects of topological semimetals have attracted tremendous research interest because many topological semimetals are excellent thermoelectric materials and thermoelectricity serves as one of their most important potential applications. In this work, we reveal the transient photothermoelectric response of Dirac semimetallic Cd3As2, namely the photo-Seebeck effect and photo-Nernst effect, by studying the terahertz (THz) emission from the transient photocurrent induced by these effects. Our excitation polarization and power dependence confirm that the observed THz emission is …
By correlating time- and angle-resolved photoemission and time-resolved transverse- magneto- optical Kerr effect measurements, both at extreme ultraviolet wavelengths, we uncover the universal nature of the ultrafast photoinduced magnetic phase transition in Ni. This allows us to explain the ultrafast magnetic response of Ni at all laser fluences - from a small reduction of the magnetization at low laser fluences, to complete quenching at high laser fluences. Both probe methods exhibit the same demagnetization and recovery timescales. We further show that the ultrafast demagnetization in Ni is…
A Weyl semimetal is a new type of topological quantum phase with intriguing physics near the Weyl nodes. Although the equilibrium state of Weyl semimetals has been investigated, the ultrafast dynamics near the Weyl node in the nonequilibrium state is still missing. Here by performing time and angle resolved photoemission spectroscopy on type-II Weyl semimetal MoTe$_2$, we reveal the dispersion of the unoccupied states and identify the Weyl node at 70 meV above E$_F$. Moreover, by tracking the ultrafast relaxation dynamics near the Weyl node upon photo-excitation with energy, momentum and tempo…
We reveal an ultrafast purely electronic phase transition in \TNS, which is a plausible excitonic insulator, after excited by an ultrafast infrared laser pulse. Specifically, the order parameter of the strong electron-hole binding shrinks with enhancing the pump pulse, and above a critical pump fluence, a photo-excited semimetallic state is experimentally identified with the absence of ultrafast structural transition. In addition, the bare valence and conduction bands and also the effective exciton binding energy in \TNS~are determined. These findings and detailed analysis suggest a bare noneq…
Techniques in time- and angle-resolved photoemission spectroscopy have facilitated a number of recent advances in the study of quantum materials. We review developments in this field related to the study of incoherent nonequilibrium electron dynamics, the analysis of interactions between electrons and collective excitations, the exploration of dressed-state physics, and the illumination of unoccupied band structure. Future prospects are also discussed.
We analyze the effect of electron-phonon coupling on photoemission properties and ultrafast response of doped monolayer MoS2. The analysis is based on combined DFT and many-body (Eliashberg theory) approaches. In particular, we have calculated the electronic and phonon spectra, the electron-phonon coupling and the electronic spectral function of the system at different values of doping. We have also analyzed the emissive properties and the response of the system to femtosecond (fs) laser pulses. It is shown that position of the emission peak of undoped system is in agreement with the experimen…
Two-dimensional (2D) materials with puckered layer morphology are promising candidates for next-generation opto-electronics devices owing to their anisotropic response to external perturbations and wide band gap tunability with the number of layers. Among them, PdSe2 is an emerging 2D transition-metal dichalcogenide with band gap ranging from 1.3 eV in the monolayer to a predicted semimetallic behavior in the bulk. Here we use angle-resolved photoemission spectroscopy to explore the electronic band structure of PdSe2 with energy and momentum resolution. Our measurements reveal the semiconducti…
The transport of optically excited, hot electrons in heterostructures is analyzed by femtosecond, time-resolved two-photon photoelectron emission spectroscopy (2PPE) for epitaxial Au/Fe/MgO(001). We compare the temporal evolution of the 2PPE intensity upon optically pumping Fe or Au, while the probing occurs on the Au surface. In the case of Fe-side pumping, assuming independent relaxation in the Fe and Au layers, we determine the hot electron relaxation times in these individual layers by an analysis of the Au layer thickness dependence of the observed, effective electron lifetimes in the het…
Time-resolved soft-X-ray photoemission spectroscopy is used to simultaneously measure the ultrafast dynamics of core-level spectral functions and excited states upon excitation of excitons in WSe$_2$. We present a many-body approximation for the Green's function, which excellently describes the transient core-hole spectral function. The relative dynamics of excited-state signal and core levels reveals a delayed core-hole renormalization due to screening by excited quasi-free carriers, revealing an excitonic Mott transition. These findings establish time-resolved core-level photoelectron spectr…
In order to exploit the intriguing optical properties of graphene it is essential to gain a better understanding of the light-matter interaction in the material on ultrashort timescales. Exciting the Dirac fermions with intense ultrafast laser pulses triggers a series of processes involving interactions between electrons, phonons and impurities. Here we study these interactions in epitaxial graphene supported on silicon carbide (semiconducting) and iridium (metallic) substrates using ultrafast time- and angle-resolved photoemission spectroscopy (TR-ARPES) based on high harmonic generation. For…
By using constrained density functional theory modeling, we demonstrate that ultrafast optical pumping unveils hidden charge orders in group VI monolayer transition metal ditellurides. We show that irradiation of the insulating 2H phases stabilizes multiple transient charge density wave orders with light-tunable distortion, periodicity, electronic structure and bandgap. Moreover, optical pumping of the semimetallic 1T' phases generates a transient charge ordered metallic phase composed of 2D diamond clusters. For each transient phase we identify the critical fluence at which it is observed and…
We characterize the topological insulator Bi$_2$Se$_3$ using time- and angle- resolved photoemission spectroscopy. By employing two-photon photoemission, a complete picture of the unoccupied electronic structure from the Fermi level up to the vacuum level is obtained. We demonstrate that the unoccupied states host a second, Dirac surface state which can be resonantly excited by 1.5 eV photons. We then study the ultrafast relaxation processes following optical excitation. We find that they culminate in a persistent non-equilibrium population of the first Dirac surface state, which is maintained…
In high-temperature superconductivity, the process that leads to the formation of Cooper pairs, the fundamental charge carriers in any superconductor, remains mysterious. We use a femtosecond laser pump pulse to perturb superconducting Bi2Sr2CaCu2O8+δ, and study subsequent dynamics using time- and angle-resolved photoemission and infrared reflectivity probes. Gap and quasiparticle population dynamics reveal marked dependencies on both excitation density and crystal momentum. Close to the d-wave nodes, the superconducting gap is sensitive to the pump intensity and Cooper pairs recombine slowly.…
Time- and Angle-resolved photoelectron spectroscopy from surfaces can be used to record the dynamics of electrons and holes in condensed matter on ultrafast time scales. However, ultrafast photoemission experiments using extreme-ultraviolet (XUV) light have previously been limited by either space-charge effects, low photon flux, or limited tuning range. In this article, we describe space-charge-free XUV photoelectron spectroscopy experiments with up to 5 nA of average sample current using a tunable cavity-enhanced high-harmonic source operating at 88 MHz repetition rate. The source delivers $ …
We use time- and angle-resolved photoemission to measure the nodal non-equilibrium electronic states in various dopings of Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$. We find that the initial pump-induced transient signal of these ungapped states is strongly affected by the onset of the superconducting gap at $T_c$, superconducting pairing fluctuations at $T_p$, and the pseudogap at $T^*$. Moreover, $T_p$ marks a suggestive threshold in the fluence-dependent transient signal, with the appearance of a critical fluence below $T_p$ that corresponds to the energy required to break apart all Cooper pairs. These…
Coherent excitation of materials via ultrafast laser pulses can have interesting, observable dynamics in time-resolved photoemission measurements. The broad spectral width of ultrafast pump pulses can coherently excite multiple exciton energy levels. When such coherently excited states are probed by means of photoemission spectroscopy, interference between the polarization of different exciton levels can lead to observable coherent exciton beats. Here, we present the theoretical formalism for evaluating the Time- and Angle- Resolved Photoemission Spectra (tr-ARPES) arising from the coherently …
Ultrafast dynamics of graphite is investigated by time-resolved photoemission spectroscopy. We observe spectral features of direct photoexcitations, non-thermal electron distributions, and recovery dynamics occurring with two time scales having distinct pump-power dependences. Additionally, we find an anomalous increase of the spectral intensity around the Fermi level, and we attribute this to spectral broadenings due to coupled optical phonons in the transient. The fingerprints of the coupled optical phonons occur from the temporal region where the electronic temperature is still not definabl…
The femtosecond evolution of the electronic temperature of laser-excited gold nanoparticles is measured, by means of ultrafast time-resolved photoemission spectroscopy induced by extreme-ultraviolet radiation pulses. The temperature of the electron gas is deduced by recording and fitting high-resolution photo emission spectra around the Fermi edge of gold nanoparticles providing a direct, unambiguous picture of the ultrafast electron-gas dynamics. These results will be instrumental to the refinement of existing models of femtosecond processes in laterally-confined and bulk condensed-matter sys…
We present a novel method to measure transient photovoltage at nanointerfaces using ultrafast electron diffraction. In particular, we report our results on the photoinduced electronic excitations and their ensuing relaxations in a hydroxyl-terminated silicon surface, a standard substrate for fabricating molecular electronics interfaces. The transient surface voltage is determined by observing Coulomb refraction changes induced by the modified space-charge barrier within a selectively probed volume by femtosecond electron pulses. The results are in agreement with ultrafast photoemission studies…
Time- and angle-resolved photoemission spectroscopy accesses the ultrafast evolution of quasiparticles and many-body interactions in solid-state systems. However, the momentum- and energy-resolved transient photoemission intensity may not be unambiguously related to the intrinsic relaxation dynamics of photoexcited electrons. In fact, interpretation of the time-dependent photoemission signal can be affected by the transient evolution of both the one-electron removal spectral function as well as the photoemission dipole matrix elements. Here we investigate the topological insulator Bi$_{1.1}$Sb…
We present energy-momentum mapping of surface Dirac photocurrent in the topological insulator Sb$_2$Te$_3$ by means of time- and angle-resolved two-photon photoemission spectroscopy combined with polarization-variable mid-infrared pulse laser. It is demonstrated that the direct optical transition from the occupied to the unoccupied part of the surface Dirac-cone permits the linear and circular photogalvanic effect which thereby enables us to coherently control the surface electric-current by laser polarization. Moreover, the surface current mapping directly visualizes ultrafast current dynamic…
We present the development of the first ultrafast transmission electron microscope (UTEM) driven by localized photoemission from a field emitter cathode. We describe the implementation of the instrument, the photoemitter concept and the quantitative electron beam parameters achieved. Establishing a new source for ultrafast TEM, the Göttingen UTEM employs nano-localized linear photoemission from a Schottky emitter, which enables operation with freely tunable temporal structure, from continuous wave to femtosecond pulsed mode. Using this emission mechanism, we achieve record pulse properties in …
The dynamics of excited electrons and holes in single layer (SL) MoS$_2$ have so far been difficult to disentangle from the excitons that dominate the optical response of this material. Here, we use time- and angle-resolved photoemission spectroscopy for a SL of MoS$_2$ on a metallic substrate to directly measure the excited free carriers. This allows us to ascertain a direct quasiparticle band gap of 1.95 eV and determine an ultrafast (50 fs) extraction of excited free carriers via the metal in contact with the SL MoS$_2$. This process is of key importance for optoelectronic applications that…
Electronic interactions associated with atomic adsorbates on transition metal dichalcogenides such as MoS2 can induce massive electronic reconstruction that results in the formation of a new type of heavily doped transition metal dichalcogenide that exhibits characteristics of a two-dimensional electron gas. The impact of quantum confinement and reduced dimensionality on the carrier dynamics in such two-dimensional systems is at present not known, but is of paramount importance if they are to find application in optoelectronic devices. Here we show by a combination of angle-resolved photoemiss…
Ultrafast charge separation after photoexcitation is a common phenomenon in various van-der-Waals (vdW) heterostructures with great relevance for future applications in light harvesting and detection. Theoretical understanding of this phenomenon converges towards a coherent mechanism through charge transfer states accompanied by energy dissipation into strongly coupled phonons. The detailed microscopic pathways are material specific as they sensitively depend on the band structures of the individual layers, the relative band alignment in the heterostructure, the twist angle between the layers,…
Using a time-resolved magneto-optical Kerr effect (TR-MOKE) microscope, we observed ultrafast demagnetization of inverse-spinel-type NiCo2O4 (NCO) epitaxial thin films of the inverse spinel type ferrimagnet NCO with perpendicular magnetic anisotropy. This microscope uses a pump-probe method, where the sample is pumped at 1030 nm, and magnetic domain images are acquired via MOKE microscopy at 515 nm (the second harmonic). We successfully observed the dynamics of the magnetic domain of the NCO thin film via laser irradiation, and obtained a demagnetization time constant of approximately 0.4 ps. …
Time-resolved photoemission with ultrafast pump and probe pulses is an emerging technique with wide application potential. Real-time recording of non-equilibrium electronic processes, transient states in chemical reactions or the interplay of electronic and structural dynamics offers fascinating opportunities for future research. Combining valence-band and core-level spectroscopy with photoelectron diffraction for electronic, chemical and structural analysis requires few 10 fs soft X-ray pulses with some 10 meV spectral resolution, which are currently available at high repetition rate free-ele…
There is still no general consensus on how one can describe the out-of-equilibrium phenomena in matter induced by an ultrashort light pulse. We investigate the pulse-induced dynamics in a layered Dirac semimetal SrMnBi2 by pump-and-probe photoemission spectroscopy. At ~<1 ps, the electronic recovery slowed upon increasing the pump power. Such a bottleneck-type slowing is expected in a two-temperature model (TTM) scheme, although opposite trends have been observed to date in graphite and in cuprates. Subsequently, an unconventional power-law cooling took place at ~100 ps, indicating that spatia…
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 c…
Ultrafast dynamics of excitons in black phosphorus
Université de Lorraine（洛林大学）；CNRS（法国国家科学研究中心）；IJL（界面与层状材料研究所）；University of Fribourg（弗里堡大学）；Paul Scherrer Institute（保罗谢勒研究所）；TU Wien（维也纳工业大学）；University of Geneva（日内瓦大学）
High-resolution time- and angle-resolved photoemission measurements were made on FeSe superconductors. With ultrafast photoexcitation, two critical excitation fluences that correspond to two ultrafast electronic phase transitions were found only in the $d_{yz}$-orbit-derived band near the Brillouin-zone center within our time and energy resolution. Upon comparison to the detailed temperature dependent measurements, we conclude that there are two equilibrium electronic phase transitions (at approximately 90 and 120 K) above the superconducting transition temperature, and an anomalous contributi…
Time-Resolved Photoemission Spectroscopy of Quantum Materials Using High Harmonic Generation: Probing Electron-Phonon Interactions and Non-Equilibrium Dynamics
Black phosphorus is a quasi-two-dimensional layered semiconductor with a narrow direct band gap of 0.3 eV. A giant surface Stark effect can be produced by the potassium doping of black phosphorus, leading to a semiconductor to semimetal phase transition originating from the creation of a strong surface dipole and associated band bending. By using time- and angle-resolved photoemission spectroscopy, we report the partial photoinduced screening of this band bending by the creation of a compensating surface photovoltage. We further resolve the detailed dynamics of this effect at the pertinent tim…
Using femtosecond time- and angle- resolved photoemission spectroscopy, we investigated the nonequilibrium dynamics of the topological insulator Bi2Se3. We studied p-type Bi2Se3, in which the metallic Dirac surface state and bulk conduction bands are unoccupied. Optical excitation leads to a meta-stable population at the bulk conduction band edge, which feeds a nonequilibrium population of the surface state persisting for >10ps. This unusually long-lived population of a metallic Dirac surface state with spin texture may present a channel in which to drive transient spin-polarized currents.
Rashba materials have appeared as an ideal playground for spin-to-charge conversion in prototype spintronics devices. Among them, $α$-GeTe(111) is a non-centrosymmetric ferroelectric (FE) semiconductor for which a strong spin-orbit interaction gives rise to giant Rashba coupling. Its room temperature ferroelectricity was recently demonstrated as a route towards a new type of highly energy-efficient non-volatile memory device based on switchable polarization. Currently based on the application of an electric field, the writing and reading processes could be outperformed by the use of femtosecon…
Spin-to-charge conversion (SCC) involving topological surface states (TSS) is one of the most promising routes for highly efficient spintronic devices for terahertz (THz) emission. Here, the THz generation generally occurs mainly via SCC consisting in efficient dynamical spin injection into spin-locked TSS. In this work, we demonstrate sizable THz emission from a nanometric thick topological insultator (TI)/ferromagnetic junction - SnBi$_2$Te$_4$/Co - specifically designed to avoid bulk band crossing with the TSS at the Fermi level, unlike its parent material Bi$_2$Te$_3$. THz emission time do…
An SDW antiferromagnetic (SDW-AF) low temperature phase transition is generally observe and the AF spin fluctuations are considered to play an important role for the superconductivity paring mechanism in FeAs superconductors. However, a similar magnetic phase transition is not observed in FeSe superconductors, which has caused considerable discussion. We report on the intrinsic electronic states of FeSe as elucidated by transport measurements under magnetic fields using a high quality single crystal. A mobility spectrum analysis, an ab initio method that does not make assumptions on the transp…
Calculations combining first-principles electron-phonon ($e$-ph) interactions with the Boltzmann equation enable studies of ultrafast carrier and phonon dynamics. However, in materials with weak Coulomb screening, electrons and holes form bound excitons and their scattering processes become correlated, posing additional challenges for modeling nonequilibrium physics. Here we show calculations of ultrafast exciton dynamics and related time-domain spectroscopies using $ab~initio$ exciton-phonon (ex-ph) interactions together with an excitonic Boltzmann equation. Starting from the nonequilibrium e…
Despite being the most studied nodal line semimetal, a clear understanding of the transient state relaxation dynamics and the underlying mechanism in ZrSiS is lacking. Using time and angle resolved photoemission spectroscopy, we study the ultrafast relaxation dynamics in ZrSiS and reveal a unique relaxation in the bulk nodal-line state which is well captured by a simple model based on optical and acoustic phonon cooling. We find linear decay processes for both optical and acoustic phonon relaxations with acoustic cooling suppressed at high temperatures. Our results reveal different decay mecha…
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）
The quasiparticle spectra of atomically thin semiconducting transition metal dichalcogenides (TMDCs) and their response to an ultrafast optical excitation critically depend on interactions with the underlying substrate. Here, we present a comparative time- and angle-resolved photoemission spectroscopy (TR-ARPES) study of the transient electronic structure and ultrafast carrier dynamics in the single- and bilayer TMDCs MoS$_2$ and WS$_2$ on three different substrates: Au(111), Ag(111) and graphene/SiC. The photoexcited quasiparticle bandgaps are observed to vary over the range of 1.9-2.3 eV bet…
We perform time- and angle-resolved photoemission spectroscopy of a prototypical topological insulator Bi$_2$Se$_3$ to study the ultrafast dynamics of surface and bulk electrons after photo-excitation. By analyzing the evolution of surface states and bulk band spectra, we obtain their electronic temperature and chemical potential relaxation dynamics separately. These dynamics reveal strong phonon-assisted surface-bulk coupling at high lattice temperature and total suppression of inelastic scattering between the surface and the bulk at low lattice temperature. In this low temperature regime, th…
Clustering-Enhanced Time- and Angle-Resolved Photoemission Study of LaTe$_3$: Absence of a Photoinduced Secondary CDW in the Electronic Structure
Aarhus University（奥胡斯大学）；CNR, Consiglio Nazionale delle Ricerche, Istituto officina dei materiali（意大利国家研究委员会材料研究所）；Central Laser Facility, STFC Rutherford Appleton Laboratory（STFC鲁瑟福阿普尔顿实验室中央激光设施）；SUPA, School of Physics and Astronomy, University of St Andrews（圣安德鲁斯大学物理与天文学学院）；Stanford University（斯坦福大学）；Diamond Light Source Ltd（钻石光源有限公司）；Princeton University（普林斯顿大学）；Department of Physics, Indian Institute of Technology Guwahati（印度理工学院古瓦哈提分校物理系）
We present a general formalism of ultrafast diffractive voltammetry approach as a contact-free tool to investigate the ultrafast surface charge dynamics in nanostructured interfaces. As case studies, the photoinduced surface charging processes in oxidized silicon surface and the hot electron dynamics in nanoparticle-decorated interface are examined based on the diffractive voltammetry framework. We identify that the charge redistribution processes appear on the surface, sub-surface, and vacuum levels when driven by intense femtosecond laser pulses. To elucidate the voltammetry contribution fro…
