Momentum Microscopy Research Articles

Excited State Band Mapping and Ultrafast Nonequilibrium Dynamics in Topological Dirac Semimetal 1T-ZrTe2.

We performed time- and polarization-resolved extreme ultraviolet momentum microscopy on the topological Dirac semimetal candidate 1T-ZrTe2. Excited state band mapping uncovers the previously inaccessible linear dispersion of the Dirac cone above the Fermi level. We study the orbital texture of bands using linear dichroism in photoelectron angular distributions. These observations provide hints about the topological character of 1T-ZrTe2. Time-, energy-, and momentum-resolved nonequilibrium carrier dynamics reveal that intra- and interband scattering processes play a major role in the relaxation mechanism, leading to multivalley electron-hole accumulation near the Fermi level. We also show that electrons' inverse lifetime has a linear dependence as a function of their excess energy. Our time- and polarization-resolved XUV photoemission results shed light on the excited state electronic structure of 1T-ZrTe2 and provide valuable insights into the relatively unexplored field of quantum-state-resolved ultrafast dynamics in 3D topological Dirac semimetals.

Momentum-Space Observation of Optically Excited Nonthermal Electrons in Graphene with Persistent Pseudospin Polarization.

The unique optical properties of graphene, with broadband absorption and ultrafast response, make it a critical component of optoelectronic and spintronic devices. Using time-resolved momentum microscopy with high data rate and high dynamic range, we report momentum-space measurements of electrons promoted to the graphene conduction band with visible light and their subsequent relaxation. We observe a pronounced nonthermal distribution of nascent photoexcited electrons with lattice pseudospin polarization in remarkable agreement with results of simple tight-binding theory. By varying the excitation fluence, we vary the relative importance of electron-electron vs electron-phonon scattering in the relaxation of the initial distribution. Increasing the excitation fluence results in increased noncollinear electron-electron scattering and reduced pseudospin polarization, although up-scattered electrons retain a degree of polarization. These detailed momentum-resolved electron dynamics in graphene demonstrate the capabilities of high-performance time-resolved momentum microscopy in the study of 2D materials and can inform the design of graphene devices.

Asymmetric electrostatic dodecapole: compact bandpass filter with low aberrations for momentum microscopy.

Imaging energy filters in photoelectron microscopes and momentum microscopes use spherical fields with deflection angles of 90°, 180° and even 2 × 180°. These instruments are optimized for high energy resolution, and exhibit image aberrations when operated in high transmission mode at medium energy resolution. Here, a new approach is presented for bandpass-filtered imaging in real or reciprocal space using an electrostatic dodecapole with an asymmetric electrode array. In addition to energy-dispersive beam deflection, this multipole allows aberration correction up to the third order. Here, its use is described as a bandpass prefilter in a time-of-flight momentum microscope at the hard X-ray beamline P22 of PETRA III. The entire instrument is housed in a straight vacuum tube because the deflection angle is only 4° and the beam displacement in the filter is only ∼8 mm. The multipole is framed by transfer lenses in the entrance and exit branches. Two sets of 16 different-sized entrance and exit apertures on piezomotor-driven mounts allow selection of the desired bandpass. For pass energies between 100 and 1400 eV and slit widths between 0.5 and 4 mm, the transmitted kinetic energy intervals are between 10 eV and a few hundred electronvolts (full width at half-maximum). The filter eliminates all higher or lower energy signals outside the selected bandpass, significantly improving the signal-to-background ratio in the time-of-flight analyzer.

Development of dual-beamline photoelectron momentum microscopy for valence orbital analysis.

The soft X-ray photoelectron momentum microscopy (PMM) experimental station at the UVSOR Synchrotron Facility has been recently upgraded by additionally guiding vacuum ultraviolet (VUV) light in a normal-incidence configuration. PMM offers a very powerful tool for comprehensive electronic structure analyses in real and momentum spaces. In this work, a VUV beam with variable polarization in the normal-incidence geometry was obtained at the same sample position as the soft X-ray beam from BL6U by branching the VUV beamline BL7U. The valence electronic structure of the Au(111) surface was measured using horizontal and vertical linearly polarized (s-polarized) light excitations from BL7U in addition to horizontal linearly polarized (p-polarized) light excitations from BL6U. Such highly symmetric photoemission geometry with normal incidence offers direct access to atomic orbital information via photon polarization-dependent transition-matrix-element analysis.

Disentangling the multiorbital contributions of excitons by photoemission exciton tomography

Excitons are realizations of a correlated many-particle wave function, specifically consisting of electrons and holes in an entangled state. Excitons occur widely in semiconductors and are dominant excitations in semiconducting organic and low-dimensional quantum materials. To efficiently harness the strong optical response and high tuneability of excitons in optoelectronics and in energy-transformation processes, access to the full wavefunction of the entangled state is critical, but has so far not been feasible. Here, we show how time-resolved photoemission momentum microscopy can be used to gain access to the entangled wavefunction and to unravel the exciton’s multiorbital electron and hole contributions. For the prototypical organic semiconductor buckminsterfullerene (C60), we exemplify the capabilities of exciton tomography and achieve unprecedented access to key properties of the entangled exciton state including localization, charge-transfer character, and ultrafast exciton formation and relaxation dynamics.

Performance of a photoelectron momentum microscope in direct- and momentum-space imaging with ultraviolet photon sources.

The Photoelectron-Related Image and Nano-Spectroscopy (PRINS) endstation located at the Taiwan Photon Source beamline 27A2 houses a photoelectron momentum microscope capable of performing direct-space imaging, momentum-space imaging and photoemission spectroscopy with position sensitivity. Here, the performance of this microscope is demonstrated using two in-house photon sources - an Hg lamp and He(I) radiation - on a standard checkerboard-patterned specimen and an Au(111) single crystal, respectively. By analyzing the intensity profile of the edge of the Au patterns, the Rashba-splitting of the Au(111) Shockley surface state at 300 K, and the photoelectron intensity across the Fermi edge at 80 K, the spatial, momentum and energy resolution were estimated to be 50 nm, 0.0172 Å-1 and 26 meV, respectively. Additionally, it is shown that the band structures acquired in either constant energy contour mode or momentum-resolved photoemission spectroscopy mode were in close agreement.

Soft x-ray photoelectron momentum microscope for multimodal valence band stereography

The photoelectron momentum microscope (PMM) in operation at BL6U, an undulator-based soft x-ray beamline at the UVSOR Synchrotron Facility, offers a new approach for μm-scale momentum-resolved photoelectron spectroscopy (MRPES). A key feature of the PMM is that it can very effectively reduce radiation-induced damage by directly projecting a single photoelectron constant energy contour in reciprocal space with a radius of a few Å−1 or real space with a radius of a few 100 μm onto a two-dimensional detector. This approach was applied to three-dimensional valence band structure E(k) and E(r) measurements (“stereography”) as functions of photon energy (hν), its polarization (e), detection position (r), and temperature (T). In this study, we described some examples of possible measurement techniques using a soft x-ray PMM. We successfully applied this stereography technique to μm-scale MRPES to selectively visualize the single-domain band structure of twinned face-centered-cubic Ir thin films grown on Al2O3(0001) substrates. The photon energy dependence of the photoelectron intensity on the Au(111) surface state was measured in detail within the bulk Fermi surface. By changing the temperature of 1T-TaS2, we clarified the variations in the valence band dispersion associated with chiral charge-density-wave phase transitions. Finally, PMMs for valence band stereography with various electron analyzers were compared, and the advantages of each were discussed.

Soft X-ray Fermi surface tomography of palladium and rhodium via momentum microscopy

Fermi surfaces of transition metals, which describe all thermodynamical and transport quantities of solids, often fail to be modeled by one-electron mean-field theory due to strong correlations among the valence electrons. In addition, relativistic spin–orbit coupling pronounced in heavier elements lifts the degeneracy of the energy bands and further modifies the Fermi surface. Palladium and rhodium, two 4d metals attributed to show significant spin–orbit coupling and electron correlations, are ideal for a systematic and fundamental study of the two fundamental physical phenomena and their interplay in the electronic structure. In this study, we explored the Fermi surface of the 4d noble metals palladium and rhodium obtained via high-resolution constant initial state momentum microscopy. The complete 3D-Fermi surfaces of palladium and rhodium were tomographically mapped using soft X-ray photon energies from 34 eV up to 660 eV. To fully capture the orbital angular momentum of states across the Fermi surface, the Fermi surface tomography was performed using p- and s- polarized light. Applicability and limitations of the nearly-free electron final state model in photoemission are discussed using a complex band structure model supported by experimental evidence. The significance of spin–orbit coupling and electron correlations across the Fermi surfaces will be discussed within the context of the photoemission results. State-of-the-art fully relativistic Korringa–Kohn–Rostoker (KKR) calculations within the one-step model of photoemission are used to support the experimental results.

Ultrafast dynamics of bright and dark excitons in monolayer WSe2 and heterobilayer WSe2/MoS2

The energy landscape of optical excitations in mono- and few-layer transition metal dichalcogenides (TMDs) is dominated by optically bright and dark excitons. These excitons can be fully localized within a single TMD layer, or the electron- and the hole-component of the exciton can be charge-separated over multiple TMD layers. Such intra- or interlayer excitons have been characterized in detail using all-optical spectroscopies, and, more recently, photoemission spectroscopy. In addition, there are so-called hybrid excitons whose electron- and/or hole-component are delocalized over two or more TMD layers, and therefore provide a promising pathway to mediate charge-transfer processes across the TMD interface. Hence, an in-situ characterization of their energy landscape and dynamics is of vital interest. In this work, using femtosecond momentum microscopy combined with many-particle modeling, we quantitatively compare the dynamics of momentum-indirect intralayer excitons in monolayer WSe2 with the dynamics of momentum-indirect hybrid excitons in heterobilayer WSe2/MoS2, and draw three key conclusions: First, we find that the energy of hybrid excitons is reduced when compared to excitons with pure intralayer character. Second, we show that the momentum-indirect intralayer and hybrid excitons are formed via exciton-phonon scattering from optically excited bright excitons. And third, we demonstrate that the efficiency for phonon absorption and emission processes in the mono- and the heterobilayer is strongly dependent on the energy alignment of the intralayer and hybrid excitons with respect to the optically excited bright exciton. Overall, our work provides microscopic insights into exciton dynamics in TMD mono- and bilayers.

Circular dichroism in hard X-ray photoelectron diffraction observed by time-of-flight momentum microscopy

X-ray photoelectron diffraction (XPD) is a powerful technique that yields detailed structural information of solids and thin films that complements electronic structure measurements. Among the strongholds of XPD we can identify dopant sites, track structural phase transitions, and perform holographic reconstruction. High-resolution imaging of kll-distributions (momentum microscopy) presents a new approach to core-level photoemission. It yields full-field kx-ky XPD patterns with unprecedented acquisition speed and richness in details. Here, we show that beyond the pure diffraction information, XPD patterns exhibit pronounced circular dichroism in the angular distribution (CDAD) with asymmetries up to 80%, alongside with rapid variations on a small kll-scale (0.1 Å−1). Measurements with circularly-polarized hard X-rays (hν = 6 keV) for a number of core levels, including Si, Ge, Mo and W, prove that core-level CDAD is a general phenomenon that is independent of atomic number. The fine structure in CDAD is more pronounced compared to the corresponding intensity patterns. Additionally, they obey the same symmetry rules as found for atomic and molecular species, and valence bands. The CD is antisymmetric with respect to the mirror planes of the crystal, whose signatures are sharp zero lines. Calculations using both the Bloch-wave approach and one-step photoemission reveal the origin of the fine structure that represents the signature of Kikuchi diffraction. To disentangle the roles of photoexcitation and diffraction, XPD has been implemented into the Munich SPRKKR package to unify the one-step model of photoemission and multiple scattering theory.

Critical behavior and exchange splitting in the two-dimensional antiferromagnet Mn on Re(0001)

We investigated the temperature-dependent electronic structure of the antiferromagnetic fcc-monolayer Mn on Re(0001) using vacuum-ultraviolet momentum microscopy. At $T=25$ K the collinear, row-wise antiferromagnetic phase of the Mn monolayer results in a spin splitting of states. Density-functional theory, being in good agreement with the experimental results, reveals the spin and orbital projection of the observed electronic bands. The exchange split bands shift in opposite directions with increasing temperature, decreasing the exchange splitting of a pair of itinerant bands from $280\ifmmode\pm\else\textpm\fi{}10$ meV at 25 K down to $185\ifmmode\pm\else\textpm\fi{}10$ meV at the N\'eel temperature ${T}_{\text{N}}=75\ifmmode\pm\else\textpm\fi{}5$ K. The exchange splitting remains constant for $T>{T}_{\text{N}}$. The persisting exchange splitting is attributed to a remaining short-range, fluctuating antiferromagnetic order far above ${T}_{\text{N}}$.

Hole Doping to Perylene on Au(110): Photoelectron Momentum Microscopy

Photoemission spectroscopy of the perylene layers on the Au(110) surface was performed using a momentum microscope. The two-dimensional momentum maps of the perylene monolayer exhibit a “binary star” pattern with two asymmetric bright spots for the electrons from the highest occupied molecular orbital of perylene, reflecting the tilted molecular orientation. This pattern was absent for the perylene multilayer and the Br-doped monolayer because of the random orientation of the molecules in these layers. Br doped to the perylene monolayer facilitated hole injection in perylene, and the electrons attributable to the singly occupied molecular orbital were observed at binding energies of 1.0—1.5 eV.

Attosecond imaging of photoinduced dynamics in molecules using time-resolved photoelectron momentum microscopy

We explore the novel capabilities offered by attosecond extreme ultraviolet and x-ray pulses that can be now generated by free-electron lasers and high-harmonics generation sources for probing photon-induced electron dynamics in molecules. We theoretically analyze how spatial and temporal dependence of charge migration in a pentacene molecule can be followed by means of time-resolved photoelectron microscopy on the attosecond time scale. Performing the analysis, we accurately take into account that an attosecond probe pulse leads to considerable spectral broadening. We demonstrate that the excited-state dynamics of a neutral pentacene molecule in the real space map onto unique features of photoelectron momentum maps.

Dirac Bands in the Topological Insulator Bi2Se3 Mapped by Time‐Resolved Momentum Microscopy

AbstractThe energy dispersion of the unoccupied Dirac bands of the topological insulator Bi2Se3 has been studied up to large parallel momenta and intermediate state energies using a setup for laser‐based time‐resolved momentum microscopy with 6 eV probe‐photons. A strongly momentum‐dependent evolution of the topologically protected Dirac states into a conduction band resonance is observed, highlighting the anisotropy dictated by the symmetry of the surface. The results are in remarkable agreement with the theoretical surface spectrum obtained from a GW‐corrected tight‐binding model, suggesting the validity of the approach in the prediction of the quasiparticle excitation spectrum of large systems with non‐trivial topology. After photoexcitation with 0.97 eV photons, assigned to a bulk valence band‐conduction band transition, the out‐of‐equilibrium population of the surface state evolves on a multi‐picosecond time scale, in agreement with a simple thermodynamical model with a fixed number of particles, suggesting a significant decoupling between bulk and surface states.

Test signal generator for simulating electron events from a momentum microscope

Preparing experiments that utilize free electron lasers is challenging because obtaining access to the facility is difficult. The integration of detectors into the data acquisition system needs to be tested before the beamtime starts. In this study, we develop a test signal generator that simulates the signals from a delay-line detector used in a time-of-flight electron spectrometer. The output signals of the simulator are connected to the time-to-digital converter electronics and simulate a realistic energy spectrum of a real spectrometer. Through this method, the detector electronics can be tested and integrated into the data acquisition system at the free electron laser before the actual instrument is available on site. In addition, the saturation behavior of the signal processing chain can be tested by changing the number of simulated electrons per pulse.

Time- and angle-resolved photoemission spectroscopy (TR-ARPES) of TMDC monolayers and bilayers.

Many unique properties in two-dimensional (2D) materials and their heterostructures rely on charge excitation, scattering, transfer, and relaxation dynamics across different points in the momentum space. Understanding these dynamics is crucial in both the fundamental study of 2D physics and their incorporation in optoelectronic and quantum devices. A direct method to probe charge carrier dynamics with momentum resolution is time- and angle-resolved photoemission spectroscopy (TR-ARPES). Such measurements have been challenging, since photoexcited carriers in many 2D monolayers reside at high crystal momenta, requiring probe photon energies in the extreme UV (EUV) regime. These challenges have been recently addressed by development of table-top pulsed EUV sources based on high harmonic generation, and the successful integration into a TR-ARPES and/or time-resolved momentum microscope. Such experiments will allow direct imaging of photoelectrons with superior time, energy, and crystal momentum resolution, with unique advantage over traditional optical measurements. Recently, TR-ARPES experiments of 2D transition metal dichalcogenide (TMDC) monolayers and bilayers have created unprecedented opportunities to reveal many intrinsic dynamics of 2D materials, such as bandgap renormalization, charge carrier scattering, relaxation, and wavefunction localization in moiré patterns. This perspective aims to give a short review of recent discoveries and discuss the challenges and opportunities of such techniques in the future.

The SXP instrument at the European XFEL

The successful implementation of the baseline instruments at the European XFEL has triggered a second phase of instrument developments aiming to extend the portfolio of available techniques. At the soft X-ray undulator (SASE 3), the Soft X-ray Port (SXP) instrument is currently under construction. Conceived as an open port, it focuses primarily on femtosecond time-resolved X-ray photoelectron spectroscopy (TR-XPES), which has proven to be a powerful tool to understand the properties of materials and the interaction between their internal degrees of freedom. The extension of this technique to the soft X-ray energy range is only possible at MHz free electron lasers (FELs) due to space-charge effects which limit the maximum photon flux per pulse on the sample. In this contribution, the SXP instrument at the European XFEL and the implementation of TR-XPES using a momentum microscope are presented. The photon energy range available at SASE 3, 0.25 keV to 3.5 keV, and the variable polarization will allow for the simultaneous characterization of the electronic, magnetic, chemical and structural properties of materials with femtosecond time resolution. To this end, a wide range of laser excitation wavelengths, ranging from the XUV to the THz region, will be available.

UVSOR Synchrotron Facility Update

UVSOR is a Japanese low-energy synchrotron light source that has been operational since 1983. It has 750 MeV electron beam energy and a circumference of 53 m. The machine has undergone two major upgrades and is now called UVSOR-III, with a moderately small emittance of 17 nm·rad and is operated in the top-up mode at 300 mA. It has six undulators. Three in-vacuum undulators provide high-brightness VUV-SX light to the beamlines BL3U, BL4U, and BL6U. BL3U and BL4U are actively used for chemistry and life sciences using in situ and operando measurements, such as soft X-ray absorption and photoelectron spectroscopy. Since 2020, a unique photoelectron analyzer called the Momentum Microscope has been in operation in BL6U. Two variable polarization undulators provide high-brightness VUV light to the beamlines, BL5U and BL7U, which are used for solid-state physics through angle- and spin-resolved photoelectron spectroscopy. BL1U is equipped with two APPLE-II undulators in tandem and is used for various research purposes, including laser Compton scattering gamma rays. In addition to these beamlines, eight beamlines are operational which use bending magnet radiation, ranging from THz to tender X-rays. In 38 years of operation, we have dealt with and properly resolved machine problems, such as water leakage from magnet coils and cooling water flow paths in ultrahigh vacuum. Considering the machine’s declining competitiveness as a light source due to its aging and emerging demands in the low-energy area, we have started a design study on the future plan, as well as discussing it closely with the user community.

Through the Lens of a Momentum Microscope: Viewing Light-Induced Quantum Phenomena in 2D Materials.

Van der Waals (vdW) materials at their 2D limit are diverse, flexible, and unique laboratories to study fundamental quantum phenomena and their future applications. Their novel properties rely on their pronounced Coulomb interactions, variety of crystal symmetries and spin-physics, and the ease of incorporation of different vdW materials to form sophisticated heterostructures. In particular, the excited state properties of many 2D semiconductors and semi-metals are relevant for their technological applications, particularly those that can be induced by light. In this paper, the recent advances made in studying out-of-equilibrium, light-induced, phenomena in these materials are reviewed using powerful, surface-sensitive, time-resolved photoemission-based techniques, with a particular emphasis on the emerging multi-dimensional photoemission spectroscopy technique of time-resolved momentum microscopy. The advances this technique has enabled in studying the nature and dynamics of occupied excited states in these materials are discussed. Then, the future research directions opened by these scientific and instrumental advancements are projected for studying the physics of 2D materials and the opportunities to engineer their band-structure and band-topology by laser fields.

Enhancing Electron Correlation at a 3d Ferromagnetic Surface.

Spin-resolved momentum microscopy and theoretical calculations are combined beyond the one-electron approximation to unveil the spin-dependent electronic structure of the interface formed between iron (Fe) and an ordered oxygen (O) atomic layer, and an adsorbate-induced enhancement of electronic correlations is found. It is demonstrated that this enhancement is responsible for a drastic narrowing of the Fe d-bands close to the Fermi energy (EF ) and a reduction of the exchange splitting, which is not accounted for in the Stoner picture of ferromagnetism. In addition, correlation leads to a significant spin-dependent broadening of the electronic bands at higher binding energies and their merging with satellite features, which are manifestations of a pure many-electron behavior. Overall, adatom adsorption can be used to vary the material parameters of transition metal surfaces to access different intermediate electronic correlated regimes, which will otherwise not be accessible. The results show that the concepts developed to understand the physics and chemistry of adsorbate-metal interfaces, relevant for a variety of research areas, from spintronics to catalysis, need to be reconsidered with many-particle effects being of utmost importance. These may affect chemisorption energy, spin transport, magnetic order, and even play a key role in the emergence of ferromagnetism at interfaces between non-magnetic systems.