The interactions that lead to the emergence of superconductivity in iron-based materials remain a subject of debate. It has been suggested that electron-electron correlations enhance electron-phonon ...coupling in iron selenide (FeSe) and related pnictides, but direct experimental verification has been lacking. Here we show that the electron-phonon coupling strength in FeSe can be quantified by combining two time-domain experiments into a “coherent lock-in” measurement in the terahertz regime. X-ray diffraction tracks the light-induced femtosecond coherent lattice motion at a single phonon frequency, and photoemission monitors the subsequent coherent changes in the electronic band structure.Comparison with theory reveals a strong enhancement of the coupling strength in FeSe owing to correlation effects. Given that the electron-phonon coupling affects superconductivity exponentially, this enhancement highlights the importance of the cooperative interplay between electron-electron and electron-phonon interactions.
Cuprate superconductors host a multitude of low-energy optical phonons. Using time- and angle-resolved photoemission spectroscopy, we study coherent phonons in ...Bi_{2}Sr_{2}Ca_{0.92}Y_{0.08}Cu_{2}O_{8+δ}. Sub-meV modulations of the electronic band structure are observed at frequencies of 3.94±0.01 and 5.59±0.06 THz. For the dominant mode at 3.94 THz, the amplitude of the band energy oscillation weakly increases as a function of momentum away from the node. Theoretical calculations allow identifying the observed modes as CuO_{2}-derived A_{1g} phonons. The Bi- and Sr-derived A_{1g} modes which dominate Raman spectra in the relevant frequency range are absent in our measurements. This highlights the mode selectivity for phonons coupled to the near-Fermi-level electrons, which originate from CuO_{2} planes and dictate thermodynamic properties.
Obtaining insight into microscopic cooperative effects is a fascinating topic in condensed matter research because, through self-coordination and collectivity, they can lead to instabilities with ...macroscopic impacts like phase transitions. We used femtosecond time- and angle-resolved photoelectron spectroscopy (trARPES) to optically pump and probe TbTe3, an excellent model system with which to study these effects. We drove a transient charge density wave melting, excited collective vibrations in TbTe3, and observed them through their time-, frequency-, and momentum-dependent influence on the electronic structure. We were able to identify the role of the observed collective vibration in the transition and to document the transition in real time. The information that we demonstrate as being accessible with trARPES will greatly enhance the understanding of all materials exhibiting collective phenomena.
We report time- and angle-resolved photoemission spectroscopy measurements on the topological insulator Bi2Se3. We observe oscillatory modulations of the electronic structure of both the bulk and ...surface states at a frequency of 2.23 THz due to coherent excitation of an A1g phonon mode. A distinct, additional frequency of 2.05 THz is observed in the surface state only. The lower phonon frequency at the surface is attributed to the termination of the crystal and thus reduction of interlayer van der Waals forces, which serve as restorative forces for out-of-plane lattice distortions. Density functional theory calculations quantitatively reproduce the magnitude of the surface phonon softening. These results represent the first band-resolved evidence of the A1g phonon mode coupling to the surface state in a topological insulator.
Using femtosecond time- and angle-resolved photoemission spectroscopy, we investigated the nonequilibrium dynamics of the topological insulator Bi2Se3. We studied p-type Bi2Se3, in which the metallic ...Dirac surface state and bulk conduction bands are unoccupied. Optical excitation leads to a metastable population at the bulk conduction band edge, which feeds a nonequilibrium population of the surface state persisting for >10 ps. This unusually long-lived population of a metallic Dirac surface state with spin texture may present a channel in which to drive transient spin-polarized currents.
We study optimally doped Bi-2212 (T(c)=96 K) using femtosecond time- and angle-resolved photoelectron spectroscopy. Energy-resolved population lifetimes are extracted and compared with ...single-particle lifetimes measured by equilibrium photoemission. The population lifetimes deviate from the single-particle lifetimes in the low excitation limit by 1-2 orders of magnitude. Fundamental considerations of electron scattering unveil that these two lifetimes are in general distinct, yet for systems with only electron-phonon scattering they should converge in the low-temperature, low-fluence limit. The qualitative disparity in our data, even in this limit, suggests that scattering channels beyond electron-phonon interactions play a significant role in the electron dynamics of cuprate superconductors.
We characterize the occupied and unoccupied electronic structure of the topological insulator Bi2Se3 by one-photon and two-photon angle-resolved photoemission spectroscopy and slab band structure ...calculations. We reveal a second, unoccupied Dirac surface state with similar electronic structure and physical origin to the well-known topological surface state. This state is energetically located 1.5 eV above the conduction band, which permits it to be directly excited by the output of a Ti:sapphire laser. This discovery demonstrates the feasibility of direct ultrafast optical coupling to a topologically protected, spin-textured surface state.
Non-equilibrium conditions may lead to novel properties of materials with broken symmetry ground states not accessible in equilibrium as vividly demonstrated by non-linearly driven mid-infrared ...active phonon excitation. Potential energy surfaces of electronically excited states also allow to direct nuclear motion, but relaxation of the excess energy typically excites fluctuations leading to a reduced or even vanishing order parameter as characterized by an electronic energy gap. Here, using femtosecond time- and angle-resolved photoemission spectroscopy, we demonstrate a tendency towards transient stabilization of a charge density wave after near-infrared excitation, counteracting the suppression of order in the non-equilibrium state. Analysis of the dynamic electronic structure reveals a remaining energy gap in a highly excited transient state. Our observation can be explained by a competition between fluctuations in the electronically excited state, which tend to reduce order, and transiently enhanced Fermi surface nesting stabilizing the order.
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