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A. F. Kemper

Publications and source records attributed to A. F. Kemper.

At least 55 records · Page 3Linked to original sources

Review of the theoretical description of time-resolved angle-resolved photoemission spectroscopy in electron-phonon mediated superconductors

We review recent work on the theory for pump/probe photoemission spectroscopy of electron-phonon mediated superconductors in both the normal and the superconducting states. We describe the formal developments that allow one to solve the Migdal-Eliashberg theory in nonequilibrium for an ultrashort laser pumping field, and explore the solutions which illustrate the relaxation as energy is transferred from electrons to phonons. We focus on exact results emanating from sum rules and approximate numerical results which describe rules of thumb for relaxation processes. In addition, in the superconducting state, we describe how Higg's oscillations can be excited due to the nonlinear coupling with the electric field and how pumping the system can enhance superconductivity.

cond-mat.supr-con↗

Energy dissipation in the time domain governed by bosons in a correlated material

In complex materials various interactions play important roles in determining the material properties. Angle Resolved Photoelectron Spectroscopy (ARPES) has been used to study these processes by resolving the complex single particle self energy $Σ(E)$ and quantifying how quantum interactions modify bare electronic states. However, ambiguities in the measurement of the real part of the self energy and an intrinsic inability to disentangle various contributions to the imaginary part of the self energy often leave the implications of such measurements open to debate. Here we employ a combined theoretical and experimental treatment of femtosecond time-resolved ARPES (tr-ARPES) and show how measuring the population dynamics using tr-ARPES can be used to separate electron-boson interactions from electron-electron interactions. We demonstrate the analysis of a well-defined electron-boson interaction in the unoccupied spectrum of the cuprate Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+x}$ characterized by an excited population decay time constant $τ_{QP}$ that maps directly to a discrete component of the equilibrium self energy not readily isolated by static ARPES experiments.

cond-mat.str-el↗

Theory of light-enhanced phonon-mediated superconductivity

We investigate the dynamics of a phonon-mediated superconductor driven out of equilibrium. The electronic hopping amplitude is ramped down in time, resulting in an increased electronic density of states. The dynamics of the coupled electron-phonon model is investigated by solving Migdal-Eliashberg equations for the double-time Keldysh Green's functions. The increase of the density of states near the Fermi level leads to an enhancement of superconductivity when the system thermalizes to the new state at the same temperature. We provide a time- and momentum-resolved view on this thermalization process, and show that it involves fast processes associated with single-particle scattering and much slower dynamics associated with the superconducting order parameter. The importance of electron-phonon coupling for the rapid enhancement and the efficient thermalization of superconductivity is demonstrated, and the results are compared to a BCS time-dependent mean-field approximation.

cond-mat.supr-con↗

The rate of quasiparticle recombination probes the onset of coherence in cuprate superconductors

The condensation of an electron superfluid from a conventional metallic state at a critical temperature $T_c$ is described well by the BCS theory. In the underdoped copper-oxides, high-temperature superconductivity condenses instead from a nonconventional metallic "pseudogap" phase that exhibits a variety of non-Fermi liquid properties. Recently, it has become clear that a charge density wave (CDW) phase exists within the pseudogap regime, appearing at a temperature $T_{CDW}$ just above $T_c$. The near coincidence of $T_c$ and $T_{CDW}$, as well the coexistence and competition of CDW and superconducting order below $T_c$, suggests that they are intimately related. Here we show that the condensation of the superfluid from this unconventional precursor is reflected in deviations from the predictions of BSC theory regarding the recombination rate of quasiparticles. We report a detailed investigation of the quasiparticle (QP) recombination lifetime, $τ_{qp}$, as a function of temperature and magnetic field in underdoped HgBa$_{2}$CuO$_{4+δ}$ (Hg-1201) and YBa$_{2}$Cu$_{3}$O$_{6+x}$ (YBCO) single crystals by ultrafast time-resolved reflectivity. We find that $τ_{qp}(T)$ exhibits a local maximum in a small temperature window near $T_c$ that is prominent in underdoped samples with coexisting charge order and vanishes with application of a small magnetic field. We explain this unusual, non-BCS behavior by positing that $T_c$ marks a transition from phase-fluctuating SC/CDW composite order above to a SC/CDW condensate below. Our results suggest that the superfluid in underdoped cuprates is a condensate of coherently-mixed particle-particle and particle-hole pairs.

cond-mat.supr-con↗

Direct observation of Higgs mode oscillations in the pump-probe photoemission spectra of electron-phonon mediated superconductors

Using the non-equilibrium Keldysh formalism, we solve the equations of motion for electron-phonon superconductivity, including an ultrafast pump field. We present results for time-dependent photoemission spectra out of equilibrium which probes the dynamics of the superconducting gap edge. The partial melting of the order by the pump field leads to oscillations at twice the melted gap frequency, a hallmark of the Higgs or amplitude mode. Thus the Higgs mode can be directly excited through the nonlinear effects of an electromagnetic field and detected without any additional symmetry breaking.

cond-mat.supr-con↗

Bandwidth and Electron Correlation-Tuned Superconductivity in Rb$_{0.8}$Fe$_{2}$(Se$_{1-z}$S$_z$)$_2$

We present a systematic angle-resolved photoemission spectroscopy study of the substitution-dependence of the electronic structure of Rb$_{0.8}$Fe$_{2}$(Se$_{1-z}$S$_z$)$_2$ (z = 0, 0.5, 1), where superconductivity is continuously suppressed into a metallic phase. Going from the non-superconducting Rb$_{0.8}$Fe$_{2}$(Se$_{1-z}$S$_z$)$_2$ to superconducting Rb$_{0.8}$Fe$_{2}$Se$_2$, we observe little change of the Fermi surface topology, but a reduction of the overall bandwidth by a factor of 2 as well as an increase of the orbital-dependent renormalization in the $d_{xy}$ orbital. Hence for these heavily electron-doped iron chalcogenides, we have identified electron correlation as explicitly manifested in the quasiparticle bandwidth to be the important tuning parameter for superconductivity, and that moderate correlation is essential to achieving high $T_C$.

cond-mat.supr-con↗

Anomalous longitudinal relaxation of nuclear spins in CaF$_2$

We consider the effect of non-secular resonances for interacting nuclear spins in solids which were predicted theoretically to exist in the presence of strong static and strong radio-frequency magnetic fields. These resonances imply corrections to the standard secular approximation for the nuclear spin-spin interaction in solids, which, in turn, should lead to an anomalous longitudinal relaxation in nuclear magnetic resonance experiments. In this article, we investigate the feasibility of the experimental observation of this anomalous longitudinal relaxation in calcium fluoride (CaF$_2$) and conclude that such an observation is realistic.

cond-mat.mes-hall↗

Classification of Collective Modes in a Charge Density Wave by Momentum-Dependent Modulation of the Electronic Band Structure

We present time- and angle-resolved photoemission spectroscopy measurements on the charge density wave system CeTe$_{3}$. Optical excitation transiently populates the unoccupied band structure and reveals a gap size of 2$Δ$ = 0.59 eV. The occupied Te-5p band dispersion is coherently modified by three modes at $Ω_{1}$ = 2.2 THz, $Ω_{2}$ = 2.7 THz and $Ω_{3}$ = 3 THz. All three modes lead to small rigid energy shifts whereas $Δ$ is only affected by $Ω_{1}$ and $Ω_{2}$. Their spatial polarization is analyzed by fits of a transient model dispersion and DFT frozen phonon calculations. We conclude that the modes $Ω_{1}$ and $Ω_{2}$ result from in-plane ionic lattice motions, which modulate the charge order, and that $Ω_{3}$ originates from a generic out-of-plane $A_{1g}$ phonon. We thereby demonstrate how the rich information from trARPES allows identification of collective modes and their spatial polarization, which explains the mode-dependent coupling to charge order.

cond-mat.mtrl-sci↗

Direct characterization of photo-induced lattice dynamics in BaFe2As2

Ultrafast light pulses can modify the electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins, and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved x-ray scattering to measure the lattice dynamics of photo-excited BaFe2As2. Upon optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation of an A1g mode that modulates the Fe-As-Fe bond angle. We directly quantify the coherent lattice dynamics and show that even a small photo-induced lattice distortion can induce notable changes in the electronic and magnetic properties. Our analysis implies that transient structural modification can generally be an effective tool for manipulating the electronic properties of multi-orbital systems, where electronic instabilities are sensitive to the orbital character of bands near the Fermi level.

cond-mat.str-el↗

Theory of pump-probe photoemission in graphene: Ultrafast tuning of Floquet bands and local pseudospin textures

The control of physical properties of solids with short laser pulses is an intriguing prospect of ultrafast materials science. Continuous-wave high-frequency laser driving with circular polarization was predicted to induce a light-matter coupled new state possessing a quasi-static band structure with an energy gap and a quantum Hall effect, coined "Floquet topological insulator". Whereas the envisioned Floquet topological insulator requires well separated Floquet bands and therefore high-frequency pumping, a natural follow-up question regards the creation of Floquet-like states in graphene with realistic pump laser pulses. Here we predict that with short low-frequency laser pulses attainable in pump-probe experiments, states with local spectral gaps at the Dirac points and novel pseudospin textures can be achieved in graphene using circular light polarization. We demonstrate that time- and angle-resolved photoemission spectroscopy can track these states by measuring sizeable energy gaps and quasi-Floquet energy bands that form on femtosecond time scales. By analyzing Floquet energy level crossings and snapshots of pseudospin textures near the Dirac points, we identify transitions to new states with optically induced nontrivial changes of sublattice mixing that can lead to Berry curvature corrections of electrical transport and magnetization.

cond-mat.mes-hall↗

A balancing act: Evidence for a strong subdominant d-wave pairing channel in ${\rm Ba_{0.6}K_{0.4}Fe_2As_2}$

We present an analysis of the Raman spectra of optimally doped ${\rm Ba_{0.6}K_{0.4}Fe_2As_2}$ based on LDA band structure calculations and the subsequent estimation of effective Raman vertices. Experimentally a narrow, emergent mode appears in the $B_{1g}$ ($d_{x^2-y^2}$) Raman spectra only below $T_c$, well into the superconducting state and at an energy below twice the energy gap on the electron Fermi surface sheets. The Raman spectra can be reproduced quantitatively with estimates for the magnitude and momentum space structure of the s$_{+-}$ pairing gap on different Fermi surface sheets, as well as the identification of the emergent sharp feature as a Bardasis-Schrieffer exciton, formed as a Cooper pair bound state in a subdominant $d_{x^2-y^2}$ channel. The binding energy of the exciton relative to the gap edge shows that the coupling strength in this subdominant $d_{x^2-y^2}$ channel is as strong as 60% of that in the dominant $s_{+-}$ channel. This result suggests that $d_{x^2-y^2}$ may be the dominant pairing symmetry in Fe-based sperconductors which lack central hole bands.

cond-mat.str-el↗

Transient Exchange Interaction in a Helical Antiferromagnet

We have performed time-resolved resonant x-ray scattering studies in the Lanthanide metal Dy to reveal the dynamic response of the helical order exchange coupling to injection of unpolarized spins. The observed spin dynamics are significantly slower than that exhibited by the ferromagnetic phase in Lanthanide metals and are strongly dependent on temperature and excitation fluence. This unique behavior results from transient changes in the shape of the conduction electron Fermi surface and subsequent scattering events that transfer the excitation to the core spin.

cond-mat.str-el↗

Effect of dynamical spectral weight redistribution on effective interactions in time-resolved spectroscopy

The redistribution of electrons in an ultrafast pump-probe experiment causes significant changes to the effective interaction between electrons and bosonic modes. We study the influence of these changes on pump-probe photoemission spectroscopy for a model electron-phonon coupled system using the nonequilibrium Keldysh formalism. We show that spectral rearrangement due to the driving field preserves an overall sum rule for the electronic self-energy, but modifies the effective electron-phonon scattering as a function of energy. Experimentally, this pump-modified scattering can be tracked by analyzing the fluence or excitation energy dependence of population decay rates and transient changes in dispersion kinks.

cond-mat.mes-hall↗

Dynamic competition between spin density wave order and superconductivity in underdoped $Ba_{1-x}K_xFe_2As_2$

An intriguing aspect of unconventional superconductivity is that it always appears in the vicinity of other competing phases, whose suppression brings the full emergence of superconductivity. In the iron-pnictides, these competing phases are marked by a tetragonal-to-orthorhombic structural transition and a collinear spin-density-wave (SDW) transition. There has been macroscopic evidence for competition between these phases and superconductivity as the magnitude of both the orthorhombicity and magnetic moment are suppressed in the superconducting state. Here, using angle-resolved photoemission spectroscopy on detwinned underdoped $Ba_{1-x}K_xFe_2As_2$, we observe a coexistence of both the SDW gap and superconducting gap in the same electronic structure. Furthermore, our data reveal that following the onset of superconductivity, the SDW gap decreases in magnitude and shifts in a direction consistent with a reduction of the orbital anisotropy. This observation provides direct spectroscopic evidence for the dynamic competition between superconductivity and both SDW and electronic nematic orders in these materials.

cond-mat.supr-con↗

Nonequilibrium sum rules for the Holstein model

We derive frequency moment sum rules for the retarded electronic Green's function and self-energy of the Holstein model for both equilibrium and nonequilibrium cases. We also derive sum rules for the phonon propagator in equilibrium and nonequilibrium. These sum rules allow one to benchmark nonequilibrium calculations and help with interpreting the behavior of electrons driven out of equilibrium by an applied electric field. We exactly evaluate the sum rules when the system is in the atomic limit. We also discuss the application of these sum rules to pump/probe experiments like time-resolved angle-resolved photoemission spectroscopy.

cond-mat.str-el↗

Tunneling spectroscopy for probing orbital anisotropy in iron pnictides

Using realistic multi-orbital tight-binding Hamiltonians and the T-matrix formalism, we explore the effects of a non-magnetic impurity on the local density of states in Fe-based compounds. We show that scanning tunneling spectroscopy (STS) has very specific anisotropic signatures that track the evolution of orbital splitting (OS) and antiferromagnetic gaps. Both anisotropies exhibit two patterns that split in energy with decreasing temperature, but for OS these two patterns map onto each other under 90 degree rotation. STS experiments that observe these signatures should expose the underlying magnetic and orbital order as a function of temperature across various phase transitions.

cond-mat.supr-con↗

Time-Dependent Charge-Order and Spin-Order Recovery in Striped Systems

Using time-dependent Ginzburg-Landau theory, we study the role of amplitude and phase fluctuations in the recovery of charge and spin stripe phases in response to a pump pulse that melts the orders. For parameters relevant to the case where charge order precedes spin order thermodynamically, amplitude recovery governs the initial time scales, while phase recovery controls behavior at longer times. In addition to these intrinsic effects, there is a longer spin re-orientation time scale related to the scattering geometry that dominates the recovery of the spin phase. Coupling between the charge and spin orders locks the amplitude and similarly the phase recovery, reducing the number of distinct time scales. Our results well reproduce the major experimental features of pump-probe x-ray diffraction measurements on the striped nickelate La$_{1.75}$Sr$_{0.25}$NiO$_4$. They highlight the main idea of this work, which is the use of time-dependent Ginzburg-Landau theory to study systems with multiple coexisting order parameters.

cond-mat.str-el↗

Mapping of the unoccupied states and relevant bosonic modes via the time dependent momentum distribution

The unoccupied states of complex materials are difficult to measure, yet play a key role in determining their properties. We propose a technique that can measure the unoccupied states, called time-resolved Compton scattering, which measures the time-dependent momentum distribution (TDMD). Using a non-equilibrium Keldysh formalism, we study the TDMD for electrons coupled to a lattice in a pump-probe setup. We find a direct relation between temporal oscillations in the TDMD and the dispersion of the underlying unoccupied states, suggesting that both can be measured by time-resolved Compton scattering. We demonstrate the experimental feasibility by applying the method to a model of MgB$_2$ with realistic material parameters.

cond-mat.stat-mech↗