ARPES/Spin-PES Systems

We present angle-resolved photoemission data from Cu(111). Using a focused 6 eV continuous-wave laser for photoexcitation, we achieve a high effective momentum resolution, enabling detection of the Rashba spin splitting in the Shockley surface state on Cu(111). The magnitude of the spin splitting of $\Delta k\sim 0.006$ Å${}^{}$ is surprisingly large and exceeds values predicted for the analogous surface state on Ag(111), but is reproduced by first-principles calculations. We further resolve a kink in the dispersion, which we attribute to electron-phonon coupling.

A. Tamai, W. Meevasana, P. D. C. King, C. W. Nicholson, A. de la Torre, E. Rozbicki, and F. Baumberger
Phys. Rev. B 87, 075113

We report a Rashba spin splitting of a two-dimensional electron gas in the topological insulator ${\mathrm{Bi}}_2{\mathrm{Se}}_3$ from angle-resolved photoemission spectroscopy. We further demonstrate its electrostatic control, and show that spin splittings can be achieved which are at least an order-of-magnitude larger than in other semiconductors. Together these results show promise for the miniaturization of spintronic devices to the nanoscale and their operation at room temperature.

P. D. C. King, R. C. Hatch, M. Bianchi, R. Ovsyannikov, C. Lupulescu, G. Landolt, B. Slomski, J. H. Dil, D. Guan, J. L. Mi, E. D. L. Rienks, J. Fink, A. Lindblad, S. Svensson, S. Bao, G. Balakrishnan, B. B. Iversen, J. Osterwalder, W. Eberhardt, F. Baumbe
Phys. Rev. Lett. 107, 096802

We investigate the excited state electronic structure of the model phase transition system In/Si(111) using femtosecond time- and angle-resolved photoemission spectroscopy (trARPES). An extreme ultraviolet 500 kHz laser source at 21.7 eV is utilized both to map the energy of excited states above the Fermi level and follow the momentum-resolved population dynamics on a femtosecond timescale. Excited-state band mapping is used to characterize the normally unoccupied electronic structure above the Fermi level in both structural phases of In/Si(111): the metallic (4 x 1) and the gapped (8 x 2) phases. The extracted band positions are compared withband-structure calculations utilizing density functional theory within both the local density approximation and GW approximations (single-particle Green's function (G) + screened Coulomb interaction (W)). While good overall agreement is found between the GW-calculated band structure and experiment, deviations in specific momentum regions may indicate the importance of excitonic effects not accounted for at this level of approximation. To probe the dynamics of these excited states, their momentum-resolved transient population dynamics are extracted with trARPES. The transient intensities are compared to a simulated spectral function modeled by a state population employing a transient elevated electronic temperature as determined experimentally. This allows the momentum-resolved population dynamics to be quantitatively reproduced, revealing important insights into the transfer of energy from the electronic system to the lattice. In particular, a comparison between the magnitude and relaxation time of the transient electronic temperature observed by trARPES with those of the lattice as probed in previous ultrafast electron diffraction studies implies a highly nonthermal phonon distribution at the surface following photo-excitation. This suggests that the energy from the initially excited electronic system is initially transferred to high-energy optical phonon modes followed by cooling and thermalization of the photo-excited system by much slower phonon-phonon coupling

C. W. Nicholson, M. Puppin, A. Lücke, U. Gerstmann, M. Krenz, W. G. Schmidt, L. Rettig, R. Ernstorfer, and M. Wolf
Phys. Rev. B 99, 155107

Interlayer excitons (ILXs) — electron–hole pairs bound across two atomically thin layered semiconductors — have emerged as attractive platforms to study exciton condensation, single-photon emission and other quantum information applications. Yet, despite extensive optical spectroscopic investigations, critical information about their size, valley configuration and the influence of the moiré potential remains unknown. Here, in a WSe₂/MoS₂ heterostructure, we captured images of the time-resolved and momentum-resolved distribution of both of the particles that bind to form the ILX: the electron and the hole. We thereby obtain a direct measurement of both the ILX diameter of around 5.2 nm, comparable with the moiré-unit-cell length of 6.1 nm, and the localization of its centre of mass. Surprisingly, this large ILX is found pinned to a region of only 1.8 nm diameter within the moiré cell, smaller than the size of the exciton itself. This high degree of localization of the ILX is backed by Bethe–Salpeter equation calculations and demonstrates that the ILX can be localized within small moiré unit cells. Unlike large moiré cells, these are uniform over large regions, allowing the formation of extended arrays of localized excitations for quantum technology.

Ouri Karni, Elyse Barré, Vivek Pareek, Johnathan D. Georgaras, Michael K. L. Man, Chakradhar Sahoo, David R. Bacon, Xing Zhu, Henrique B. Ribeiro, Aidan L. O’Beirne, Jenny Hu, Abdullah Al-Mahboob, Mohamed M. M. Abdelrasoul, Nicholas S. Chan, Arka Karmakar
Nature 603, pages 247–252 (2022)

Resolving momentum degrees of freedom of excitons, which are electron-hole pairs bound by the Coulomb attraction in a photoexcited semiconductor, has remained an elusive goal for decades. In atomically thin semiconductors, such a capability could probe the momentum-forbidden dark excitons, which critically affect proposed opto-electronic technologies but are not directly accessible using optical techniques. Here, we probed the momentum state of excitons in a tungsten diselenide monolayer by photoemitting their constituent electrons and resolving them in time, momentum, and energy. We obtained a direct visual of the momentum-forbidden dark excitons and studied their properties, including their near degeneracy with bright excitons and their formation pathways in the energy-momentum landscape. These dark excitons dominated the excited-state distribution, a surprising finding that highlights their importance in atomically thin semiconductors.

Julien Madéo, Michael K. L. Man, Chakradhar Sahoo, Marshall Campbell, Vivek Pareek, E. Laine Wong, Abdullah Al-Mahboob, Nicholas S. Chan, Arka Karmakar, Bala Murali Krishna Mariserla, Xiaoqin Li, Tony F. Heinz, Ting Cao, Keshav M. Dani
Science 370, 1199–1204 (2020)

Kagome metals $A{V}_3{\mathrm{Sb}}_5$ ($A=K$, Rb, and Cs) exhibit a characteristic superconducting ground state coexisting with a charge density wave (CDW), whereas the mechanisms of the superconductivity and CDW have yet to be clarified. Here we report a systematic angle-resolved photoemission spectroscopy (ARPES) study of $\mathrm{Cs}(V_{1-x}{\mathrm{Nb}}_x{)}_3{\mathrm{Sb}}_5$ as a function of Nb content $x$, where isovalent Nb substitution causes an enhancement of superconducting transition temperature ($T_c$) and the reduction of CDW temperature ($T_{\mathrm{CDW}}$). We found that the Nb substitution shifts the Sb-derived electron band at the $\Gamma$ point downward and simultaneously moves the V-derived band around the $M$ point upward to lift up the saddle point (SP) away from the Fermi level, leading to the reduction of the CDW-gap magnitude and $T_{\mathrm{CDW}}$. This indicates a primary role of the SP density of states to stabilize the CDW. The present result also suggests that the enhancement of superconductivity by Nb substitution is caused by the cooperation between the expansion of the Sb-derived electron pocket and the recovery of the V-derived density of states at the Fermi level.

Takemi Kato, Yongkai Li, Kosuke Nakayama, Zhiwei Wang, Seigo Souma, Fumihiko Matsui, Miho Kitamura, Koji Horiba, Hiroshi Kumigashira, Takashi Takahashi, Yugui Yao and Takafumi Sato
PHYSICAL REVIEW LETTERS 129, 206402 (2022)

The 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.

Stefano Ponzoni, Felix Paßlack, Matija Stupar, David Maximilian Janas, Giovanni Zamborlini, Mirko Cinchetti
Adv. Physics Res.2023, 2200016

The exciton, a bound state of an electron and a hole, is a fundamental quasiparticle induced by coherent light–matter interactions in semiconductors. When the electrons and holes are in distinct spatial locations, spatially indirect excitons are formed with a much longer lifetime and a higher condensation temperature. One of the ultimate frontiers in this field is to create long-lived excitonic topological quasiparticles by driving exciton states with topological properties, to simultaneously leverage both topological effects and correlation. Here we reveal the existence of a transient excitonic topological surface state (TSS) in a topological insulator, Bi₂Te₃. By using time-, spin- and angle-resolved photoemission spectroscopy, we directly follow the formation of a long-lived exciton state as revealed by an intensity buildup below the bulk-TSS mixing point and an anomalous band renormalization of the continuously connected TSS in the momentum space. Such a state inherits the spin-polarization of the TSS and is spatially indirect along the z axis, as it couples photoinduced surface electrons and bulk holes in the same momentum range, which ultimately leads to an excitonic state of the TSS. These results establish Bi₂Te₃ as a possible candidate for the excitonic condensation of TSSs and, in general, opens up a new paradigm for exploring the momentum space emergence of other spatially indirect excitons, such as moiré and quantum well excitons, and for the study of non-equilibrium many-body topological physics.

Ryo Mori, Samuel Ciocys, Kazuaki Takasan, Ping Ai, Kayla Currier,
Takahiro Morimoto, Joel E. Moore, Alessandra Lanzara
Nature 614, 249–255 (2023)

Singlet fission may boost photovoltaic efficiency by transforming a singlet exciton into two triplet excitons and thereby doubling the number of excited charge carriers. The primary step of singlet fission is the ultrafast creation of the correlated triplet pair. Whereas several mechanisms have been proposed to explain this step, none has emerged as a consensus. The challenge lies in tracking the transient excitonic states. Here we use time- and angle-resolved photoemission spectroscopy to observe the primary step of singlet fission in crystalline pentacene. Our results indicate a charge-transfer mediated mechanism with a hybridization of Frenkel and charge-transfer states in the lowest bright singlet exciton. We gained intimate knowledge about the localization and the orbital character of the exciton wave functions recorded in momentum maps. This allowed us to directly compare the localization of singlet and bitriplet excitons and decompose energetically overlapping states on the basis of their orbital character. Orbital- and localization-resolved many-body dynamics promise deep insights into the mechanics governing molecular systems and topological materials.

Alexander Neef, Samuel Beaulieu, Sebastian Hammer, Shuo Dong, Julian Maklar,
Tommaso Pincelli, R. Patrick Xian, Martin Wolf, Laurenz Rettig, Jens Pflaum,
Ralph Ernstorfer
Nature 616, 275–279 (2023). https://doi.org/10.1038/s41586-023-05814-1

The electronic structure of heterointerfaces is a pivotal factor for their device functionality. We use soft x-ray angle-resolved photoelectron spectroscopy to directly measure the momentum-resolved electronic band structures on both sides of the Schottky heterointerface formed by epitaxial films of the superconducting NbN on semiconducting GaN, and determine their momentum-dependent interfacial band offset as well as the band-bending profile. We find, in particular, that the Fermi states in NbN are well separated in energy and momentum from the states in GaN, excluding any notable electronic cross-talk of the superconducting states in NbN to GaN. We support the experimental findings with first-principles calculations for bulk NbN and GaN. The Schottky barrier height obtained from photoemission is corroborated by electronic transport and optical measurements. The momentum-resolved understanding of electronic properties of interfaces elucidated in our work opens up new frontiers for the quantum materials where interfacial states play a defining role.

Tianlun Yu, John Wright, Guru Khalsa, Betül Pamuk, Celesta S. Chang, Yury Matveyev,
Xiaoqiang Wang, Thorsten Schmitt, Donglai Feng, David A. Muller, Huili Grace Xing, Debdeep Jena, Vladimir N. Strocov
Sci. Adv. 7, eabi5833 (2021)

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 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 femtosecond light pulses requiring exploration of the possible control of ferroelectricity on this timescale. Here, we probe the room temperature transient dynamics of the electronic band structure of α-GeTe(111) using time and angle-resolved photoemission spectroscopy. Our experiments reveal an ultrafast modulation of the Rashba coupling mediated on the fs timescale by a surface photovoltage, namely an increase corresponding to a 13% enhancement of the lattice distortion. This opens the route for the control of the ferroelectric polarization in α-GeTe(111) and ferroelectric semiconducting materials in quantum heterostructures.

Geoffroy Kremer, Julian Maklar, Laurent Nicolaï, Christopher W. Nicholson, Changming Yue, Caio Silva, PhilippWerner, J. Hugo Dil, Juraj Krempaský, Gunther Springholz, Ralph Ernstorfer,
Jan Minár, Laurenz Rettig, Claude Monney
Nat Commun 13, 6396 (2022)

Fermi surface is at the heart of our understanding of metals and strongly correlated many-body systems. An abrupt change in the Fermi surface topology, also called Lifshitz transition, can lead to the emergence of fascinating phenomena like colossal magnetoresistance and superconductivity. While Lifshitz transitions have been demonstrated for a broad range of materials by equilibrium tuning of macroscopic parameters such as strain, doping, pressure, and temperature, a nonequilibrium dynamical route toward ultrafast modification of the Fermi surface topology has not been experimentally demonstrated. Combining time-resolved multidimensional photoemission spectroscopy with state-of-the-art TDDFT+U simulations, we introduce a scheme for driving an ultrafast Lifshitz transition in the correlated type-II Weyl semimetal T_d-MoTe₂. We demonstrate that this nonequilibrium topological electronic transition finds its microscopic origin in the dynamical modification of the effective electronic correlations. These results shed light on a previously unexplored ultrafast scheme for controlling the Fermi surface topology in correlated quantum materials.

Samuel Beaulieu, Shuo Dong, Nicolas Tancogne-Dejean, Maciej Dendzik, Tommaso Pincelli, Julian Maklar, R. Patrick Xian, Michael A. Sentef, Martin Wolf, Angel Rubio, Laurenz Rettig, Ralph Ernstorfer
Sci. Adv. 2021; 7 : eabd9275

An experimental setup for time- and angle-resolved photoemission spectroscopy using a femtosecond 1 kHz high harmonic light source and a two-dimensional electron analyzer for parallel energy and momentum detection is presented. A selection of the 27th harmonic (41.85 eV) from the harmonic spectrum of the light source is achieved with a multilayer Mo∕Si double mirror monochromator. The extinction efficiency of the monochromator in selecting this harmonic is shown to be better than 7:1, while the transmitted bandwidth of the selected harmonic is capable of supporting temporal pulse widths as short as 3fs. The recorded E(k) photoelectron spectrum from a Cu(111) surface demonstrates an angular resolution of better than 0.6° (=0.03 Å−1 at Ekin,e=36 eV). Used in a pump-probe configuration, the described experimental setup represents a powerful experimental tool for studying the femtosecond dynamics of ultrafast surface processes in real time.

S. Mathias, L. Miaja-Avila, M. M. Murnane, H. Kapteyn, M. Aeschlimann, M. Bauer
Review of Scientific Instruments 78, 083105

We performed a full mapping of the bulk electronic structure including the Fermi surface and Fermi-velocity distribution vF(kF) of tungsten. The 4D spectral function ρ(EB; k) in the entire bulk Brillouin zone and 6 eV binding-energy (EB) interval was acquired in ∼3 h thanks to a new multidimensional photoemission data-recording technique (combining full-field k-microscopy with time-of-flight parallel energy recording) and the high brilliance of the soft X-rays used. A direct comparison of bulk and surface spectral functions (taken at low photon energies) reveals a time-reversal-invariant surface state in a local bandgap in the (110)-projected bulk band structure. The surface state connects hole and electron pockets that would otherwise be separated by an indirect local bandgap. We confirmed its Dirac-like spin texture by spin-filtered momentum imaging. The measured 4D data array enables extraction of the 3D dispersion of all bands, all energy isosurfaces, electron velocities, hole or electron conductivity, effective mass and inner potential by simple algorithms without approximations. The high-Z bcc metals with large spin–orbit-induced bandgaps are discussed as candidates for topologically non-trivial surface states.

K. Medjanik, O. Fedchenko, S. Chernov, D. Kutnyakhov, M. Ellguth, A. Oelsner, B. Schönhense, T. R. F. Peixoto, P. Lutz, C.-H. Min, F. Reinert, S. Däster, Y. Acremann, J. Viefhaus, W. Wurth, H. J. Elmers, G. Schönhense
Nature Materials 16, pp. 615–621

We present a versatile apparatus for the study of ferromagnetic surfaces, which combines spin-polarized photoemission and inverse photoemission spectroscopies. Samples can be grown by molecular beam epitaxy and analyzed in situ. Spin-resolved photoemission spectroscopy analysis is done with a hemispherical electron analyzer coupled to a 25 kV-Mott detector. Inverse photoemission spectroscopy experiments are performed with GaAs crystals as spin-polarized electron sources and a UV bandpass photon detector. As an example, measurements on the oxygen passivated Fe(100)-p(1×1)O surface are presented.

G. Berti, A. Calloni, A. Brambilla, G. Bussetti, L. Duò, F. Ciccacci
Review of Scientific Instruments 85, 073901

Two-dimensional quantum well states in ultrathin metal films generally exhibit a dispersion relation of s-p-derived states that can be described through an effective mass of the corresponding bulk band. By contrast, the effective masses in Pb quantum well states on Si(111), measured through angle-resolved photoemission, are up to an order of magnitude larger than those from the bulk states or predicted by slab calculations, while similar anomalies are not observed in the related In∕Si(111) system. We interpret these data in terms of an enhanced electron localization, and use them to interpret recent scanning tunneling microscopy results.

J. H. Dil, J. W. Kim, Th. Kampen, K. Horn, A. R. H. F. Ettema
Physical Review B 73, 161308 (R)

The spin-resolved electronic structure of thin Cr overlayers on top of the Fe(110) surface was investigated by means of spin- and angle-resolved photoelectron spectroscopy. The initial fast drop of photoelectron spin-polarization at the Fermi level, followed by weak oscillatory behavior with the period of about 2 ML, can give an evidence for the first time spectroscopic observation of the short period oscillations in (110)-oriented thin Cr films.

Yu. S. Dedkov
Eur. Phys. J. B 57, pp. 15-19

We report on a magnetic analysis by means of spin-resolved photoelectron spectroscopy of an atomically flat heteromagnetic rare-earth interface of 1 ML Eu∕Gd(0001). The measurements reveal a high net Eu magnetization at low temperatures reflected by a spin polarization ∼15% of the Eu 4f state. This magnetic Eu configuration is due to a strong ferromagnetic interlayer exchange coupling across the Eu∕Gd interface which overcomes a weak negative intralayer coupling between Eu spins in the hexagonal two-dimensional lattice.

Yu. S. Dedkov, Th. Kleissner, E. N. Voloshina, S. Danzenbächer, S. L. Molodtsov, C. Laubschat
Physical Review B 73, 012402

We report on angle-resolved photoemission studies of the electronic π states of high-quality epitaxial graphene layers on a Ni(111) surface. In this system the electron binding energy of the π states shows a strong dependence on the magnetization reversal of the Ni film. The observed extraordinarily large energy shift up to 225 meV of the graphene-derived π band peak position for opposite magnetization directions is attributed to a manifestation of the Rashba interaction between spin-polarized electrons in the π band and the large effective electric field at the graphene/Ni interface. Our findings show that an electron spin in the graphene layer can be manipulated in a controlled way and have important implications for graphene-based spintronic devices.

Yu. S. Dedkov, M. Fonin, U. Rüdiger, C. Laubschat
Phys. Rev. Lett. 100, 107602

The implementation of graphene in semiconducting technology requires precise knowledge about the graphene–semiconductor interface. In our work the structure and electronic properties of the graphene/n-Ge(110) interface are investigated on the local (nm) and macro (from μm to mm) scales via a combination of different microscopic and spectroscopic surface science techniques accompanied by density functional theory calculations. The electronic structure of freestanding graphene remains almost completely intact in this system, with only a moderate n-doping indicating weak interaction between graphene and the Ge substrate. With regard to the optimisation of graphene growth it is found that the substrate temperature is a crucial factor, which determines the graphene layer alignment on the Ge(110) substrate during its growth from the atomic carbon source. Moreover, our results demonstrate that the preparation route for graphene on the doped semiconducting material (n-Ge) leads to the effective segregation of dopants at the interface between graphene and Ge(110). Furthermore, it is shown that these dopant atoms might form regular structures at the graphene/Ge interface and induce the doping of graphene. Our findings help to understand the interface properties of the graphene–semiconductor interfaces and the effect of dopants on the electronic structure of graphene in such systems.

J. Tesch, F. Paschke, M. Fonin, M. Wietstruk, S. Böttcher, R. J. Koch, A. Bostwick, C. Jozwiak, E. Rotenberg, A. Makarova, B. Paulus, E. Voloshina, Y. Dedkov
Nanoscale, 10, pp. 6088-6098

Excitons, electron–hole pairs bound by the Coulomb potential, are the fundamental quasiparticles of coherent light–matter interaction relevant for processes such as photosynthesis and optoelectronics. The existence of excitons in semiconductors is well established. For metals, however, although implied by the quantum theory of the optical response, experimental manifestations of excitons are tenuous owing to screening of the Coulomb interaction taking place on timescales of a few femtoseconds. Here we present direct evidence for the dominant transient excitonic response at a Ag(111) surface, which precedes the full onset of screening of the Coulomb interaction, in the course of a three-photon photoemission process with 15 fs laser pulses. During this transient regime, electron–hole pair Coulomb interactions introduce coherent quasiparticle correlations beyond the single-particle description of the optics of metals that dominate the multi-photon photoemission process on the timescale of screening at a Ag(111) surface.

X. Cui, C. Wang, A. Argondizzo, S. Garrett-Roe, B. Gumhalter, H. Petek
Nature Physics 10, pp. 505–509

The electronic band structure and crystal structure are the two complementary identifiers of solid-state materials. Although convenient instruments and reconstruction algorithms have made large, empirical, crystal structure databases possible, extracting the quasiparticle dispersion (closely related to band structure) from photoemission band mapping data is currently limited by the available computational methods. To cope with the growing size and scale of photoemission data, here we develop a pipeline including probabilistic machine learning and the associated data processing, optimization and evaluation methods for band-structure reconstruction, leveraging theoretical calculations. The pipeline reconstructs all 14 valence bands of a semiconductor and shows excellent performance on benchmarks and other materials datasets. The reconstruction uncovers previously inaccessible momentum-space structural information on both global and local scales, while realizing a path towards integration with materials science databases. Our approach illustrates the potential of combining machine learning and domain knowledge for scalable feature extraction in multidimensional data.

R. Patrick Xian, Vincent Stimper, Marios Zacharias, Maciej Dendzik, Shuo Dong, Samuel Beaulieu, Bernhard Schölkopf, Martin Wolf, Laurenz Rettig, Christian Carbogno, Stefan Bauer, Ralph Ernstorfer
Nat Comput Sci (2022) https://doi.org/10.1038/s43588-022-00382-2

Hybrid plasmonic devices involve a nanostructured metal supporting localized surface plasmons to amplify light–matter interaction, and a non-plasmonic material to functionalize charge excitations. Application-relevant epitaxial heterostructures, however, give rise to ballistic ultrafast dynamics that challenge the conventional semiclassical understanding of unidirectional nanometal-to-substrate energy transfer. Epitaxial Au nanoislands are studied on WSe₂ with time- and angle-resolved photoemission spectroscopy and femtosecond electron diffraction: this combination of techniques resolves material, energy, and momentum of charge-carriers and phonons excited in the heterostructure. A strong non-linear plasmon–exciton interaction that transfers the energy of sub-bandgap photons very efficiently to the semiconductor is observed, leaving the metal cold until non-radiative exciton recombination heats the nanoparticles on hundreds of femtoseconds timescales. The results resolve a multi-directional energy exchange on timescales shorter than the electronic thermalization of the nanometal. Electron–phonon coupling and diffusive charge-transfer determine the subsequent energy flow. This complex dynamics opens perspectives for optoelectronic and photocatalytic applications, while providing a constraining experimental testbed for state-of-the-art modelling.

Tommaso Pincelli, Thomas Vasileiadis, Shuo Dong, Samuel Beaulieu, Maciej Dendzik,
Daniela Zahn, Sang-Eun Lee, Hélène Seiler, Yingpeng Qi, R. Patrick Xian, Julian Maklar,
Emerson Coy, Niclas S. Mueller, Yu Okamura, Stephanie Reich, Martin Wolf,
Laurenz
Advanced Materials 2023, 2209100

Excitons, Coulomb-bound electron–hole pairs, are the fundamental excitations governing the optoelectronic properties of semiconductors. Although optical signatures of excitons have been studied extensively, experimental access to the excitonic wave function itself has been elusive. Using multidimensional photoemission spectroscopy, we present a momentum-, energy-, and time-resolved perspective on excitons in the layered semiconductor WSe₂. By tuning the excitation wavelength, we determine the energy–momentum signature of bright exciton formation and its difference from conventional single-particle excited states. The multidimensional data allow to retrieve fundamental exciton properties like the binding energy and the exciton–lattice coupling and to reconstruct the real-space excitonic distribution function via Fourier transform. All quantities are in excellent agreement with microscopic calculations. Our approach provides a full characterization of the exciton properties and is applicable to bright and dark excitons in semiconducting materials, heterostructures, and devices.

Shuo Dong, Michele Puppin, Tommaso Pincelli, Samuel Beaulieu, Dominik Christiansen, Hannes Hübener, Christopher W. Nicholson, Rui Patrick Xian, Maciej Dendzik, YunpeiDeng, Yoav William Windsor, Malte Selig, Ermin Malic, Angel Rubio, Andreas Knorr, Martin
NatSci. 2021;1:e10010

Angle-resolved photoelectron spectroscopy is an extremely powerful probe of materials to access the occupied electronic structure with energy and momentum resolution. However, it remains blind to those dynamic states above the Fermi level that determine technologically relevant transport properties. In this work we extend band structure mapping into the unoccupied states and across the entire Brillouin zone by using a state-of-the-art high repetition rate, extreme ultraviolet femtosecond light source to probe optically excited samples. The wide-ranging applicability and power of this approach are demonstrated by measurements on the two-dimensional semiconductor ${\mathrm{WSe}}_2$, where the energy-momentum dispersion of valence and conduction bands are observed in a single experiment. This provides a direct momentum-resolved view, not only on the complete out-of-equilibrium band gap but also on its renormalization induced by electronic screening. Our work establishes a benchmark for measuring the band structure of materials, with direct access to the energy-momentum dispersion of the excited-state spectral function.

M. Puppin, C. W. Nicholson, C. Monney, Y. Deng, R. P. Xian, J. Feldl, S. Dong, A. Dominguez, H. Hübener, A. Rubio, M. Wolf, L. Rettig, and R. Ernstorfer
Phys. Rev. B 105, 075417

Angle-resolved photoemission spectroscopy (ARPES) is the most powerful technique to investigate the electronic band structure of crystalline solids. To completely characterize the electronic structure of topological materials, one needs to go beyond band structure mapping and access information about the momentum-resolved Bloch wave function, namely, orbitals, Berry curvature, and topological invariants. However, because phase information is lost in the process of measuring photoemission intensities, retrieving the complex-valued Bloch wave function from photoemission data has yet remained elusive. We introduce a novel measurement methodology and associated observable in extreme ultraviolet angle-resolved photoemission spectroscopy, based on continuous modulation of the ionizing radiation polarization axis. Tracking the energy- and momentum-resolved amplitude and phase of the photoemission intensity modulation upon polarization axis rotation allows us to retrieve the circular dichroism in photoelectron angular distributions (CDAD) without using circular photons, providing direct insights into the phase of photoemission matrix elements. In the case of two relevant bands, it is possible to reconstruct the orbital pseudospin (and thus the Bloch wave function) with moderate theory input, as demonstrated for the prototypical, layered, semiconducting, transition metal dichalcogenide $2H\text{−}{\mathrm{WSe}}_2$. This novel measurement methodology in ARPES, which is articulated around the manipulation of the photoionization transition dipole matrix element, in combination with a simple tight-binding theory, is general and adds a new dimension to obtaining insights into the orbital pseudospin, Berry curvature, and Bloch wave functions of many relevant crystalline solids.

Michael Schüler, Tommaso Pincelli, Shuo Dong, Thomas P. Devereaux, Martin Wolf, Laurenz Rettig, Ralph Ernstorfer, and Samuel Beaulieu
Phys. Rev. X 12, 011019

Strong light fields have created opportunities to tailor novel functionalities of solids. Floquet–Bloch states can form under periodic driving of electrons and enable exotic quantum phases. On subcycle timescales, lightwaves can simultaneously drive intraband currents and interband transitions, which enable high-harmonic generation and pave the way towards ultrafast electronics. Yet, the interplay of intraband and interband excitations and their relation to Floquet physics have been key open questions as dynamical aspects of Floquet states have remained elusive. Here we provide this link by visualizing the ultrafast build-up of Floquet–Bloch bands with time-resolved and angle-resolved photoemission spectroscopy. We drive surface states on a topological insulator with mid-infrared fields—strong enough for high-harmonic generation—and directly monitor the transient band structure with subcycle time resolution. Starting with strong intraband currents, we observe how Floquet sidebands emerge within a single optical cycle; intraband acceleration simultaneously proceeds in multiple sidebands until high-energy electrons scatter into bulk states and dissipation destroys the Floquet bands. Quantum non-equilibrium calculations explain the simultaneous occurrence of Floquet states with intraband and interband dynamics. Our joint experiment and theory study provides a direct time-domain view of Floquet physics and explores the fundamental frontiers of ultrafast band-structure engineering.

S. Ito, M. Schüler, M. Meierhofer, S. Schlauderer, J. Freudenstein, J. Reimann, D. Afanasiev, K. A. Kokh, O. E. Tereshchenko, J. Güdde, M. A. Sentef, U. Höfer, R. Huber
Nature (2023). https://doi.org/10.1038/s41586-023-05850-x