Time-resolved Angle-resolved Photoemission Spectroscopy Research Articles

Giant self-driven exciton-Floquet signatures in time-resolved photoemission spectroscopy of MoS2 from time-dependent GW approach

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 MoS2. We show that photoexcited excitons may be measured and quantified as satellite bands and lead 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 are orders of magnitude stronger than those of laser field-induced Floquet bands in low-dimensional semiconductors. Our findings imply a way to engineer Floquet matter through the coherent oscillation of excitons and open the new door for mechanisms for band structure engineering.

Enhance high harmonic generation (HHG) efficiency via compact multi-plate continuum post-compression for time-resolved angle-resolved photoemission spectroscopy.

Time-resolved angle-resolved photoemission spectroscopy (Tr-APRES) gives direct insight into electron dynamics by providing temporal-, energy-, and momentum-resolved information in one experiment. A major obstacle to using high harmonic generation (HHG) probe pulses for photoemission spectroscopy is the low conversion efficiency, that is, the low flux of probe photons. We use a Yb-KGW based duo-laser source with an oscillator to pump two separate amplifiers and generate two synchronized pulsed laser sources with average energies of 7.5 and 6W. By using the multiplate continuum method and chirped mirrors, the resulting flux of HHG photons at 33-70eV can be increased 50-fold (up to 1011 photons/s) by using post-compressed 30fs pulses compared with the photon flux generated by the fundamental 190fs pulses. Moreover, pulses from the 6W amplifier are used to pump an optical parametric amplifier that can vary the wavelengths for photoexcitation. The system performance is demonstrated by applying Tr-ARPES to single-crystal graphite. The front tilt broadening is significantly suppressed by the off-plane mounted conical grating, leading to a 184fs temporal resolution that is mainly limited by the pump pulse. The energy resolution is 176meV.

Quasi One-Dimensional Band Structure of Photoinduced Semimetal Phase of Ta2Ni1−xCoxSe5 (x = 0.0 and 0.1)

The photoinduced semimetal phase of Ta2Ni1−xCoxSe5 (x = 0.0 and 0.1) is studied by time-resolved angle-resolved photoemission spectroscopy. The observed band dispersions roughly agree with the generalized gradient approximation (GGA) calculation which fails to reproduce the band gap at the ambient condition. This suggests that the electron–hole interaction, which is not exactly included in GGA, is screened out by the photoexcited carriers. There is no indication of pseudogap. The conduction and valence bands provide quasi one-dimensional Fermi surfaces with similar momentum positions suggesting a quasi one-dimensional line-node semimetal.

Nonequilibrium spectral moment sum rules of the Holstein–Hubbard model

We derive a general procedure for evaluating the nth derivative of a time-dependent operator in the Heisenberg representation and employ this approach to calculate the zeroth to third spectral moment sum rules of the retarded electronic Green’s function and self-energy for a system described by the Holstein–Hubbard model allowing for arbitrary spatial and time variation of all parameters (including spatially homogeneous electric fields and parameter quenches). For a translationally invariant (but time-dependent) Hamiltonian, we also provide sum rules in momentum space. The sum rules can be applied to various different phenomena like time-resolved angle-resolved photoemission spectroscopy and benchmarking the accuracy of numerical many-body calculations. This work also corrects some errors found in earlier work on simpler models.

Few-cycle pulse compression and white light generation in cascaded multipass cells.

We report supercontinuum generation and pulse compression in two stacked multipass cells based on dielectric mirrors. The 230fs pulses at 1 MHz containing 12 µJ are compressed by a factor of 33 down to 7fs, corresponding to 1.0GW peak power and overall transmission of 84%. The source is particularly interesting for such applications as time-resolved angle-resolved photoemission spectroscopy (ARPES), photoemission electron microscopy, and nonlinear spectroscopy.

Exciton-driven renormalization of quasiparticle band structure in monolayer MoS2

Optical excitation serves as a powerful approach to control the electronic structure of layered Van der Waals materials via many-body screening effects, induced by photoexcited free carriers, or via light-driven coherence, such as optical Stark and Bloch-Siegert effects. Although theoretical work has also pointed to an exotic mechanism of renormalizing band structure via excitonic correlations in bound electron-hole pairs (excitons), experimental observation of such exciton-driven band renormalization and the full extent of their implications is still lacking, largely due to the limitations of optical probes and the impact of screening effects. Here, by using extreme-ultraviolet time-resolved angle-resolved photoemission spectroscopy together with excitonic many-body theoretical calculations, we directly unmask the band renormalization effects driven by excitonic correlations in a monolayer semiconductor. We revealed a surprising bandgap opening, increased by 40 meV, and a simultaneous enhancement of band effective mass. Our findings unmask the novel exciton-driven mechanism towards the band engineering in photoexcited semiconducting materials, opening a new playground to manipulate the transient energy states in layered quantum materials via optical controls of excitonic many-body correlations.

Ultraviolet photon source advances time-resolved angle-resolved photoemission spectroscopy

Study brings new “light” to technique examining the electronic structure of crystalline materials

An integrated quantum material testbed with multi-resolution photoemission spectroscopy

We present the development of a multi-resolution photoemission spectroscopy (MRPES) setup, which probes quantum materials in energy, momentum, space, and time. This versatile setup integrates three light sources in one photoemission setup and can conveniently switch between traditional angle-resolved photoemission spectroscopy (ARPES), time-resolved ARPES (trARPES), and micrometer-scale spatially resolved ARPES. It provides a first-time all-in-one solution to achieve an energy resolution of <4 meV, a time resolution of <35 fs, and a spatial resolution of ∼10 μm in photoemission spectroscopy. Remarkably, we obtain the shortest time resolution among the trARPES setups using solid-state nonlinear crystals for frequency upconversion. Furthermore, this MRPES setup is integrated with a shadow-mask assisted molecular beam epitaxy system, which transforms the traditional photoemission spectroscopy into a quantum device characterization instrument. We demonstrate the functionalities of this novel quantum material testbed using FeSe/SrTiO3 thin films and MnBi4Te7 magnetic topological insulators.

What do the two times in two-time correlation functions mean for interpreting tr-ARPES?

Time-resolved angle-resolved photoemission spectroscopy is one of the most powerful pump–probe measurements of materials driven far from equilibrium. Unlike the linear-response regime, where the frequency-dependent response function is independent of time, in a far-from-equilibrium experiment, the response function depends on two times in the time domain. In this work, we describe how one can use time-dependent frequency response functions and how they involve contributions from times that are near to each other. This implies that they should not be thought of as a frequency-dependent response at a single definite time. Instead, the Fourier uncertainty relations show that they involve contributions from ranges of times and must be interpreted in this light. We use this insight to help understand what time-resolved photoemission measurements actually measure.

Determination of the surface states from the ultrafast electronic states in a thermoelectric material

We reveal the electronic structure in YbCd2Sb2, a thermoelectric material, by angle-resolved photoemission spectroscopy (ARPES) and time-resolved ARPES (trARPES). Specifically, three bulk bands at the vicinity of the Fermi level are evidenced near the Brillouin zone center, consistent with the density functional theory (DFT) calculation. It is interesting that the spin-unpolarized bulk bands respond unexpectedly to right- and left-handed circularly polarized probe. In addition, a hole band of surface states, which is not sensitive to the polarization of the probe beam and is not expected from the DFT calculation, is identified. We find that the non-equilibrium quasiparticle recovery rate is much smaller in the surface states than that of the bulk states. Our results demonstrate that the surface states can be distinguished from the bulk ones from a view of time scale in the nonequilibrium physics.

Observing photo-induced chiral edge states of graphene nanoribbons in pump-probe spectroscopies

Photo-induced edge states in low-dimensional materials have attracted considerable attention due to the tunability of topological properties and dispersion. Specifically, graphene nanoribbons have been predicted to host chiral edge modes upon irradiation with circularly polarized light. Here, we present numerical calculations of time-resolved angle resolved photoemission spectroscopy and trRIXS of a graphene nanoribbon. We characterize pump-probe spectroscopic signatures of photo-induced edge states, illustrate the origin of distinct spectral features that arise from Floquet topological edge modes, and investigate the roles of incoming photon energies and finite core–hole lifetime in RIXS. With momentum, energy, and time resolution, pump-probe spectroscopies can play an important role in understanding the behavior of photo-induced topological states of matter.

Time-resolved photoemission of infinitely periodic atomic arrangements: correlation-dressed excited states of solids

A theory of the time-resolved photoemission spectroscopy (TRPES) is developed, which enables to explore the real-time electron dynamics of infinitely periodic crystalline solids. In the strongly correlated electron systems NiO and CuO, the early-stage dynamics of the valence band edge are found to be sharply contrasted between those in the spectra of TRPES. This provides a new dynamical insight to the Zaanen–Sawatzky–Allen (ZSA) classification scheme of correlated insulators and makes us assert that NiO dynamically behaves like the Mott–Hubbard insulator (MHI) and CuO like the charge transfer insulator (CTI). In the two-dimensional carbon layer graphene, the real-time electron dynamics of quantum-phase-dressed excited states, i.e., due to the Berry phase and the pseudospin correlation, are investigated in an unprecedented way through the time-resolved angle-resolved photoemission spectroscopy (TR-ARPES). In particular, the dephasing dynamics of optically doped electrons and holes in the massless Dirac band, accompanying a field-induced gliding of the Dirac cone, are discovered.

Attosecond light source in material science investigation

Since the dawn of the 21st century, attosecond (1 as =10–18 s) science has been explored and is now fast developing. It brought us the unprecedented time-resolved spectroscopy of quasiparticle dynamics in materials. To date, femtosecond (1 fs =10–15 s) time-resolved pump-probe technology is widely used to study the ultrafast quasiparticle dynamics of quantum materials, such as strong correlated quantum materials, topological materials, superconductors, and semiconductors. In a typical pump-probe experiment, the laser source will be divided into two beams, namely the pump and the probe beams. The pump beam excites the quasiparticles in target materials, and the time-delayed probe beam scans the ultrafast dynamics of the excited state carriers and the coherent lattice vibrations. By employing this method, we are able to observe the lifetimes due to various interactions, such as the electron-electron scattering, electron-phonon coupling, phonon-phonon scattering, etc. By manipulating the various laser pulse characteristic parameters, such as the photon energy, polarization, pulse duration and laser fluence, femtosecond ultrafast spectroscopy excels in investigating the physical properties of materials, which are largely determined by the outer electrons. To investigate the excited states of various materials, femtosecond pump-probe spectroscopy is often conducted under extreme conditions, such as low temperature, strong magnetic field, and high pressure. As a comparison, attosecond ultrafast spectroscopy can not only get access to exploring even faster ultrafast processes, but also probe the inner shell electrons of various types of materials. Attosecond pulses are usually prepared by high-order harmonic generation (HHG). The most common way of generating HHG is in an atomic gas. The excited unbound electrons are accelerated to the nuclei, and the electron-core collisions lead to multiple ionizations. The photons are emitted as trains of ultra-shot pulses. Recently, HHG has also been realized in liquids and solids. The separation of isolated attosecond pulses from trains of attosecond harmonics can be achieved by manipulating the polarization gating, the ultrashort few-cycle driving lasers, or both. Both attosecond pulse trains and isolated attosecond pulses can be applied to the investigation of quantum materials. With the aid of attosecond time-resolved ultrafast pump-probe spectroscopy, more and more fundamental physical properties and relevant applications will be revealed, which will greatly lead the development of condensed matter physics, material sciences, and their applications. Conversely, the attosecond science and technology can also benefit from the deeper understanding of the physical properties of solid state materials. In this article, we first introduce two types of attosecond time-resolved pump-probe experimental techniques, attosecond transient absorption spectrum (ATAS) and attosecond time-resolved angle-resolved photoemission spectroscopy (atto-ARPES). We review typical experiments carried out using such facilities in dielectrics, semiconductors, layered materials, transition metals, etc., and make an outlook for the potential applications of attosecond laser spectroscopy in this field of material science. Furthermore, as the attosecond pulses are often generated from the HHG of mid-infrared laser beams, the mid-infrared ultrafast spectroscopy itself can also be applied to material investigations. Moreover, we review the applications of mid-infrared ultrafast spectroscopy in condensed matter physics, with intriguing laser-induced novel phenomena.

Momentum-resolved analysis of condensate dynamic and Higgs oscillations in quenched superconductors with time-resolved ARPES

Higgs oscillations in nonequilibrium superconductors provide an unique tool to obtain information about the underlying order parameter. Several properties like the absolute value, existence of multiple gaps and the symmetry of the order parameter can be encoded in the Higgs oscillation spectrum. Studying Higgs oscillations with time-resolved angle-resolved photoemission spectroscopy (ARPES) has the advantage over optical measurements that a momentum-resolved analysis of the condensate dynamic is possible. In this paper, we investigate the time-resolved spectral function measured in ARPES for different quench protocols. We find that analyzing amplitude oscillations of the ARPES intensity in the whole Brillouin zone allows to understand how the condensate dynamic contributes to the emerging of collective Higgs oscillations. Furthermore, by evaluating the phase of these oscillations the symmetry deformation dynamic of the condensate can be revealed, which gives insight about the ground state symmetry of the system. With such an analysis, time-resolved ARPES experiments might be used in future as a powerful tool in the field of Higgs spectroscopy.

Tunable third harmonic generation in the vacuum ultraviolet region using dielectric nanomembranes

Tunable coherent light sources operating in the vacuum ultraviolet (VUV) region in the 100–200-nm (6–12 eV) wavelength range have important spectroscopic applications in many research fields, including time-resolved angle-resolved photoemission spectroscopy. Recent advances in laser technology have enabled the upconversion of visible femtosecond lasers to the vacuum and extreme ultraviolet regions. However, the complexity of their experimental setups and the scarcity of bulk nonlinear crystals for VUV generation have hampered its widespread use. Here, we propose the use of a free-standing dielectric nanomembrane as a simple and practical method for tunable VUV generation. We demonstrate that third harmonic VUV light is generated with sufficient intensity for spectroscopic applications from commercially available SiO2 nanomembranes of submicron thicknesses under excitation with visible femtosecond laser pulses. The submicron thickness of the nanomembranes is optimal for maximizing VUV generation efficiency and prevents self-phase modulation and spectral broadening of the fundamental beam. The observed VUV photons are up to 107 photons per pulse at 157 nm with a 1-kHz repetition rate, corresponding to a conversion efficiency of 10−6. Moreover, the central VUV wavelength can be tuned in the 146–190-nm wavelength range by changing the fundamental wavelength. We also explore material and thickness dependence with experiments and calculations. The presented results suggest that dielectric nanomembranes can be used as practical nonlinear media for VUV spectroscopic applications.

Manipulating long-lived topological surface photovoltage in bulk-insulating topological insulators Bi2Se3 and Bi2Te3

The appearance of topologically protected spin-momentum locked surface states in topological insulators gives rise to robust room temperature spin currents making them ideal candidates for the realization of spintronic devices. New methods are needed to access and manipulate such currents with timescales that are compatible with modern electronics. Here we reveal that an optically induced long-lived (~10 ns), spin-polarized surface state excitation in topological insulators can be easily tuned in both magnitude and duration. Time-resolved angle-resolved photoemission spectroscopy, together with a quantitative model, reveals the ideal conditions for a surface photovoltage in two different topological insulators. Our model predicts that the reported effects are an intrinsic property of topological insulators, as long as the chemical potential falls within the band gap. This work demonstrates that persistent excited topological surface states are photon-accessible and easily tuned in both magnitude and duration, merging photonics- and spintronics-based devices in the same material.

Angle-resolved photoemission spectroscopy and its application to topological materials

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 bulk and surface electronic structures that can be directly detected by ARPES. Over the past few years, ARPES has had a crucial role in several landmark discoveries in topological materials, including the identification of topological insulators and topological Dirac and Weyl semimetals. In this Technical Review , we assess the latest developments in different ARPES techniques and illustrate the capabilities of these techniques with applications in the study of topological materials.

Electronic band structure for occupied and unoccupied states of the natural topological superlattice phase Sb2Te

We present an experimental study describing the effects of surface termination on the electronic structure of the natural topological superlattice phase ${\mathrm{Sb}}_{2}\mathrm{Te}$. Using scanning angle-resolved photoemission microscopy, we consistently find various nonequivalent regions on the same surface after cleaving various ${\mathrm{Sb}}_{2}\mathrm{Te}$ single crystals. We were able to identify three distinct terminations characterized by different Sb/Te surface stoichiometric ratios and with clear differences in their band structure. For the dominating Te-rich termination, we also provide a direct observation of the excited electronic states and of their relaxation dynamics by means of time-resolved angle-resolved photoemission spectroscopy. Our results clearly indicate that the surface electronic structure is strongly affected by the bulk properties of the superlattice.

Constant Matrix Element Approximation to Time-Resolved Angle-Resolved Photoemission Spectroscopy

We discuss several issues associated with employing a constant matrix element approximation for the coupling of light to multiband electrons in the context of time-resolved angle-resolved photoemission spectroscopy (TR-ARPES). In particular, we demonstrate that the “constant matrix element approximation” —even when reasonable—only holds for specific choices of the one-electron basis, and changing to other bases, requires including nonconstant corrections to the matrix element. We also discuss some simplifying approximations, where a constant matrix element is employed in multiple bases, and the consequences of this further approximation (especially with respect to the calculated TR-ARPES signal becoming negative). We also discuss issues related to gauge invariance of the final spectra.

Quasiparticle dynamics across the full Brillouin zone of Bi2Sr2CaCu2O8+δ traced with ultrafast time and angle-resolved photoemission spectroscopy.

A hallmark in the cuprate family of high-temperature superconductors is the nodal-antinodal dichotomy. In this regard, angle-resolved photoemission spectroscopy (ARPES) has proven especially powerful, providing band structure information directly in energy-momentum space. Time-resolved ARPES (trARPES) holds great promise of adding ultrafast temporal information, in an attempt to identify different interaction channels in the time domain. Previous studies of the cuprates using trARPES were handicapped by the low probing energy, which significantly limits the accessible momentum space. Using 20.15 eV, 12 fs pulses, we show for the first time the evolution of quasiparticles in the antinodal region of Bi2Sr2CaCu2O8+δ and demonstrate that non-monotonic relaxation dynamics dominates above a certain fluence threshold. The dynamics is heavily influenced by transient modification of the electron-phonon interaction and phase space restrictions, in stark contrast to the monotonic relaxation in the nodal and off-nodal regions.