Modulating electron-phonon coupling offers a route to control structural displacements and tune material functionality. Valence-to-conduction band transitions, however, provide limited leverage over the driving force. Here, we demonstrate coherent lattice dynamics in trigonal tellurium using free-electron laser pulses tuned to the Te N4,5-edge. Over a broad fluence range, the oscillation amplitude obeys the displacive excitation of coherent phonons framework, extended to core resonance with twice the driving efficiency of a visible pump. Ab initio calculations decompose the force into competing multiband contributions, inaccessible to optical excitation, whose balance shifts as carriers relax. Tunable extreme-ultraviolet and X-ray pulses thus open a regime in which the displacive response is set by band-dependent coupling to the lattice, not by the number and temperature of the photocarriers alone.
The kagome lattice stands as a rich platform for hosting a wide array of correlated quantum phenomena, ranging from charge density waves and superconductivity to electron nematicity and loop current states. Direct detection of loop currents in kagome systems has remained a formidable challenge due to their intricate spatial arrangements and the weak magnetic field signatures they produce. This has left their existence and underlying mechanisms a topic of intense debate. In this work, we uncover a hallmark reconcilable with loop currents: spin handedness-selective signals that surpass conventional dichroic, spin, and spin-dichroic responses. We observe this phenomenon in the kagome metal CsTi_3Bi_5 and we call it the anomalous spin-optical helical effect. This effect arises from the coupling of light' s helicity with spin-orbital electron correlations, providing a groundbreaking method to visualize loop currents in quantum materials. Our discovery not only enriches the debate surrounding loop currents but also paves the way for new strategies to exploit the electronic phases of quantum materials via light-matter interaction.
To date, controlling the steady-state electronic band structure in high-Tc cuprate superconductors has been achieved primarily through chemical doping or magnetic fields. Here, we present that ultrafast optical excitation can instead drive the electronic band structure of Bi2Sr2CaCu2O8+δ into a photostationary, long-lived excited state. At sufficiently high pump fluences, this state undergoes a Lifshitz transition of the Fermi surface, characterized by a change in topology from hole-like to electron-like. Time- and angle-resolved photoemission spectroscopy, supported by single-band tight-binding calculations, reveals that 1.6 eV photoexcitation induces band-structure evolutions closely analogous to those produced by chemical doping. These results point to an efficient photodoping mechanism involving cooperative effects, including charge transfer, renormalization of effective electronic correlations, and defect-assisted charge trapping. Our findings raise fundamental questions regarding thermalization processes occurring on timescales comparable to the laser repetition period in cuprates. More broadly, ultrafast optical control enables access to otherwise inaccessible regions of the phase diagram by tuning the pump fluence.
Van der Waals layered materials offer unprecedented opportunities to tune electronic properties by controlling, for instance, the number of layers or their mutual twist angle. However, the translational degree of freedom has not been given proportionate attention. Within the wide family of transition metal dichalcogenides, the commensurate charge density wave (CCDW) phase of 1T-TaSe_{2} is predicted to host several quantum states ranging from 1D metal to 3D insulator depending on the lateral stacking. By means of angle-resolved photoemission spectroscopy with micrometer spatial resolution, we studied the charge-ordered 1T-TaSe_{2}, revealing the coexistence of metallic and insulating surface domains. Our investigation clarifies that metallicity is due to a specific lateral sliding of the CCDW layers, while insulating behavior is driven by surface interlayer dimerization. These results open intriguing potentialities in surface functionalization and control of electronic structure.
We developed a time-resolved high-order harmonic generation scheme for probing the ultrafast lattice and electron dynamics of Tellurium. The results show the high sensitivity of this technique.
The relation between crystal symmetries, electron correlations and electronic structure steers the formation of a large array of unconventional phases of matter, including magneto-electric loop currents and chiral magnetism 1 – 6 . The detection of such hidden orders is an important goal in condensed-matter physics. However, until now, non-standard forms of magnetism with chiral electronic ordering have been difficult to detect experimentally 7 . Here we develop a theory for symmetry-broken chiral ground states and propose a methodology based on circularly polarized, spin-selective, angular-resolved photoelectron spectroscopy to study them. We use the archetypal quantum material Sr 2 RuO 4 and reveal spectroscopic signatures that, despite being subtle, can be reconciled with the formation of spin–orbital chiral currents at the surface of the material 8 – 10 . As we shed light on these chiral regimes, our findings pave the way for a deeper understanding of ordering phenomena and unconventional magnetism.
Chirality in tellurium arises from a Peierls distortion driven by strong electron-phonon coupling, making this material a unique candidate for observing a light-induced topological phase transition. Using time- and angle- resolved photoelectron spectroscopy (trARPES), we reveal that, upon near-infrared photoexcitation, the Peierls gap is modulated by displacively excited coherent phonons with A 1g symmetry as well as chiral-symmetry- breaking ELO ' modes. By comparison with state-of-the-art TDDFT + U calculations, we reveal the microscopic origin of the in-phase oscillations of band edges, owing to phonon-induced modulation of the effective Hubbard U term.
We introduce a classification of the radial spin textures in momentum space that emerge at high-symmetry points in crystals characterized by non-polar chiral point groups ($D_2$, $D_3$, $D_4$, $D_6$, $T$, $O$). Based on the symmetry constraints imposed by these point groups in a vector field, we study the general expression for the radial spin textures up to third order in momentum. Furthermore, we determine the high-symmetry points of the 45 non-polar chiral space groups supporting a radial spin texture. These two principles are used to screen materials databases for archetypes that go beyond the basic hedgehog radial spin texture. Among the selected materials we highlight the axion insulator candidate $\mathrm{Ta}_2 \mathrm{Se}_8\mathrm{I}$, the material proposed for dark matter detection $\mathrm{Ag}_3\mathrm{Au}\mathrm{Te}_2$ and heazlewoodite $\mathrm{Ni}_3\mathrm{S}_2$, a conventional metal predicted to exhibit current-induced spin polarization. We point out that the symmetry analysis proposed in this Letter is more general and extends to studying other vector properties in momentum space.
When a semiconductor material called black phosphorus is hit with intense laser light, the behaviour of its electrons is found to change. The discovery opens a route to time-dependent engineering of exotic electronic phases in solids.
Describing the nanoscale charge carrier transport at surfaces and interfaces is fundamental for designing high-performance optoelectronic devices. To achieve this, we employ time- and angle-resolved photoelectron spectroscopy with ultraviolet pump and extreme ultraviolet probe pulses. The resulting high surface sensitivity reveals an ultrafast carrier population decay associated with surface-to-bulk transport, which was tracked with a sub-nanometer spatial resolution normal to the surface, and on a femtosecond time scale, in the case of the inorganic CsPbBr3 lead halide perovskite. The decay time exhibits a pronounced carrier density dependence, which is attributed via modeling to enhanced diffusive transport and concurrent recombination. The transport is found to approach an ordinary diffusive regime, limited by electron-hole scattering, at the highest excitation fluences. This approach constitutes an important milestone in our capability to probe hot-carrier transport at solid interfaces with sub-nanometer resolution in a theoretically and experimentally challenging, yet technologically relevant, high-carrier-density regime.
Collective modes are responsible for the emergence of novel quantum phases in topological materials. In the quasi-one dimensional (1D) Weyl semimetal (TaSe4)(2)I < i , a charge density wave (CDW) opens band gaps at the Weyl points, thus turning the system into an axionic insulator. Melting the CDW would restore the Weyl phase, but 1D fluctuations extend the gapped regime far above the 3D transition temperature (T CDW < i = 263 K), thus preventing the investigation of this topological phase transition with conventional spectroscopic methods. Here we use a non-equilibrium approach: we perturb the CDW phase by photoexcitation, and we monitor the dynamical evolution of the band structure by time- and angle-resolved photoelectron spectroscopy. We find that, upon optical excitation, electrons populate the linearly dispersing states at the Fermi level (E F < i ), and fill the CDW gap. The dynamics of both the charge carrier population and the band gap renormalization (BGR) show a fast component with a characteristic time scale of a few hundreds femtoseconds. However, the BGR also exhibits a second slow component on the mu s time scale. The combination of an ultrafast response and of persistent changes in the spectral weight at E F < i , and the resulting sensitivity of the linearly dispersing states to optical excitations, may explain the high performances of (TaSe4)(2)I < i as a material for broadband infrared photodetectors.
FeSexTe1−x compounds display a rich phase diagram, ranging from the nematicity of FeSe to the (π,π) magnetism of FeTe. We focus on FeSe0.4Te0.6, and exploit tr-ARPES to study its ultrafast electron dynamics following photoexcitation by near-infrared pump pulses. By exploiting probe-polarization-dependent matrix element effects, we reveal a photoinduced long-lived state, lasting for a few tens of picoseconds, showing features compatible with a nematic state. The possibility to induce a long-lived state in this compound by using ultra-short pulses might shed a new light on the driving force behind the nematic symmetry breaking in iron-based superconductors. With the aid of a phenomenological model, we illustrate how our results possibly question the common belief that a low-energy coupling with fluctuations is a necessary condition to stabilize the nematic order. On the contrary, the tendency towards orbital differentiation due to strong electronic correlations induced by the Hund’s coupling could be at the origin of the nematic order in iron-based superconductors.
In non-magnetic materials the combination of inversion symmetry breaking (ISB) and spin-orbit coupling (SOC) determines the spin polarization of the band structure. However, a local spin polarization can also arise in centrosymmetric crystals containing ISB subunits. This is namely the case for the nodal-line semimetal ZrSiTe where, by combining spin- and angle-resolved photoelectron spectroscopy with ab initio band structure calculations, we reveal a complex spin polarization. In the bulk, the valence and conduction bands exhibit opposite spin orientations in two spatially separated two-dimensional ZrTe sectors within the unit cell, yielding no net polarization. We also observe spin-polarized surface states that are well separated in energy and momentum from the bulk bands. A layer-by-layer analysis of the spin polarization allows us to unveil the complex evolution of the signal in the bulk states near the surface, thus bringing the intertwined nature of surface and bulk effects to the fore.
TaSe3 is a layered van der Waals semimetal with several inverted band gaps throughout the entire Brillouin zone and nontrivial Z(2) topological indices, which place it at the boundary between a strong and a weak topological phase. Our transport experiments reveal a quadratic nonsaturating magnetoresistance (MR) with values reaching 10(4)% at 1.8 K and 14 T, whose origins have to be searched in the material's band structure. Here we combine angle-resolved photoelectron spectroscopy experiments, also with spin resolution, with ab initio calculations based on density functional theory in order to draw a connection between the Fermi surface topology and the measured transport properties. Simulations based on the calculated Fermi surface clarify that electron-hole compensation plays an important role for the observed MR in the bulk material. At the surface, the position of Fermi level differs, and it can be controlled by alkali metal deposition which accounts not only for the energy shift of the bands but it slightly modifies the dispersion of the valence and conduction bands. We propose that the observed band-gap renormalization might offer a route for engineering the topological phase in TaSe3, alternative to strain.
Metal monochalcogenides (MX) have recently been rediscovered as two-dimensional materials with electronic properties highly dependent on the number of layers. Although some intriguing properties appear in the few-layer regime, the carrier mobility of MX compounds increases with the number of layers, motivating the interest in multilayered heterostructures or bulk materials. By means of angle-resolved photoemission spectroscopy (ARPES) measurements and density functional theory calculations, we compare the electronic band structure of bulk epsilon-GaSe and epsilon-InSe semiconductors. We focus our attention on the top valence band of the two compounds along main symmetry directions, discussing the effect of spin-orbit coupling and contributions from post-transition-metal (Ga or In) and Se atoms. Our results show that the top valence band at Gamma point is dominated by Se p(z) states, while the main effect of Ga or In appears more deeply in binding energy, at the Brillouin zone corners, and in the conduction band. These findings explain also the experimental observation of a hole effective mass rather insensitive to the post-transition metal. Finally, by means of spin-resolved ARPES and surface band structure calculations we describe Rashba-Bychkov spin splitting of surface states in epsilon-InSe.
In nodal-line semimetals linearly dispersing states form Dirac loops in the reciprocal space, with high degree of electron-hole symmetry and almost-vanishing density of states near the Fermi level. The result is reduced electronic screening and enhanced correlations between Dirac quasiparticles. Here we investigate the electronic structure of ZrSiSe, by combining time- and angle-resolved photoelectron spectroscopy with ab initio density functional theory (DFT) complemented by an extended Hubbard model (DFT +U +V). We show that electronic correlations are reduced on an ultrashort timescale by optical excitation of high-energy electrons-hole pairs, which transiently screen the Coulomb interaction. Our findings demonstrate an all-optical method for engineering the band structure of a quantum material.
Lead-halide perovskite (LHP) semiconductors are emergent optoelectronic materials with outstanding transport properties which are not yet fully understood. We find signatures of large polaron formation in the electronic structure of the inorganic LHP CsPbBr_{3} by means of angle-resolved photoelectron spectroscopy. The experimental valence band dispersion shows a hole effective mass of 0.26±0.02 m_{e}, 50% heavier than the bare mass m_{0}=0.17 m_{e} predicted by density functional theory. Calculations of the electron-phonon coupling indicate that phonon dressing of the carriers mainly occurs via distortions of the Pb-Br bond with a Fröhlich coupling parameter α=1.81. A good agreement with our experimental data is obtained within the Feynman polaron model, validating a viable theoretical method to predict the carrier effective mass of LHPs ab initio.
Trigonal tellurium, a small-gap semiconductor with pronounced magneto-electric and magneto-optical responses, is among the simplest realizations of a chiral crystal. We have studied by spin- and angle-resolved photoelectron spectroscopy its unconventional electronic structure and unique spin texture. We identify Kramers-Weyl, composite, and accordionlike Weyl fermions, so far only predicted by theory, and show that the spin polarization is parallel to the wave vector along the lines in k space connecting high-symmetry points. Our results clarify the symmetries that enforce such spin texture in a chiral crystal, thus bringing new insight in the formation of a spin vectorial field more complex than the previously proposed hedgehog configuration. Our findings thus pave the way to a classification scheme for these exotic spin textures and their search in chiral crystals.