BaFe$_2$As$_2$ is the parent compound for a family of iron-based high-temperature superconductors as well as a prototypical example of the spin-density wave (SDW) system. In this study, we perform an optical pump-probe study of this compound to systematically investigate the SDW order across the pressure-temperature phase diagram. The suppression of the SDW order by pressure manifests itself by the increase of relaxation time together with the decrease of the pump-probe signal and the pump energy necessary for complete vaporization of the SDW condensate. We have found that the pressure-driven suppression of the SDW order at low temperature occurs gradually in contrast to the thermally-induced SDW transition. Our results suggest that the pressure-driven quantum phase transition in BaFe$_2$As$_2$ (and probably other iron pnictides) is continuous and it is caused by the gradual worsening of the Fermi-surface nesting conditions.
The interplay among charge, spin and lattice degrees of freedom in solids gives rise to intriguing macroscopic quantum phenomena such as colossal magnetoresistance, multiferroicity and high-temperature superconductivity. Strong coupling or competition between various orders in these systems presents the key to manipulate their functional properties by means of external perturbations such as electric and magnetic fields or pressure. Ultrashort and intense optical pulses have emerged as an interesting tool to investigate elementary dynamics and control material properties by melting an existing …
Using femtosecond time-resolved x-ray diffraction we investigate the structural dynamics of the coherently excited A1g phonon mode in the Fe-pnictide parent compound BaFe2As2. The fluence dependent intensity oscillations of two specific Bragg reflections with distinctly different sensitivity to the pnictogen height in the compound allow us to quantify the coherent modifications of the Fe-As tetrahedra, indicating a transient increase of the Fe magnetic moments. By a comparison with time-resolved photoemission data we derive the electron-phonon deformation potential for this particular mode. Th…
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 …
Time- and angle-resolved extreme ultraviolet photoemission spectroscopy is used to study the electronic structure dynamics in BaFe$_2$As$_2$ around the high-symmetry points $Γ$ and $M$. A global oscillation of the Fermi level at the frequency of the $A_{1g}$(As) phonon mode is observed. It is argued that this behavior reflects a modulation of the effective chemical potential in the photoexcited surface region that arises from the high sensitivity of the band structure near the Fermi level to the $A_{1g}$ phonon mode combined with a low electron diffusivity perpendicular to the layers. The resu…
Zero-field (ZF) muon spin relaxation ($μ$SR) measurements have revealed static commensurate magnetic order of Fe moments in NdOFeAs below $T_{N} \sim 135$ K, with the ordered moment size nearly equal to that in LaOFeAs, and confirmed similar behavior in BaFe$_{2}$As$_{2}$. In single crystals of superconducting (Ba$_{0.55}$K$_{0.45}$)Fe$_{2}$As$_{2}$, $μ$SR spectra indicate static magnetism with incommensurate or short-ranged spin structure in $\sim$ 70 % of volume below $T_{N} \sim$ 80 K, coexisting with remaining volume which exhibits superfluid-response consistent with nodeless gap below $T_…
Transient single-particle spectral function of BaFe$_{2}$As$_{2}$, a parent compound of iron-based superconductors, has been studied by time- and angle-resolved photoemission spectroscopy with an extreme-ultraviolet laser generated by higher harmonics from Ar gas, which enables us to investigate the dynamics in the entire Brillouin zone. We observed electronic modifications from the spin-density-wave (SDW) ordered state within $\sim$ 1 ps after the arrival of a 1.5 eV pump pulse. We observed optically excited electrons at the zone center above $E_{F}$ at 0.12 ps, and their rapid decay. After t…
We present the strain and temperature dependence of an anomalous nematic phase in optimally doped BaFe$_2$(As,P)$_2$. Polarized ultrafast optical measurements reveal broken 4-fold rotational symmetry in a temperature range above $T_c$ in which bulk probes do not detect a phase transition. Using ultrafast microscopy, we find that the magnitude and sign of this nematicity vary on a ${50{-}100}~μ$m length scale, and the temperature at which it onsets ranges from 40 K near a domain boundary to 60 K deep within a domain. Scanning Laue microdiffraction maps of local strain at room temperature indica…
We report 75As-NMR measurements of the ternary iron arsenide BaFe2As2. 75As-NMR spectra clearly revealed that magnetic transition occurs at around 131 K in our samples, which corresponds to the emergence of spin density wave. Temperature dependence of the internal magnetic field suggests that the transition is likely of the first order. The critical-slowing-down phenomenon in the spin-lattice relaxation rate 1/T1 is not pronounced in this material.
We study the vortex-dynamics of a BaFe{1.82}Ni_{0.18}As_2 crystal with Tc = 8 K, by measuring flux-creep over the second magnetisation (or fish-tail) peak for both H//c-axis and H//ab planes. Magnetic relaxation data show an anomalously long initial stage of relaxation, lasting approximately10 minutes for H//c-axis and 2-3 min for H//ab, resembling a transient effect with a lower relaxation rate, which is followed by the usual log(time) relaxation. Interestingly, study of the relaxation rate R vs H for both stages of relaxation and for both field directions, are featureless over the field rang…
We report on the nonequilibrium quasiparticle dynamics in BaFe$_2$As$_2$ on both the hole doped (Ba$_{1-x}$K$_x$Fe$_2$As$_2$) and electron doped (BaFe$_{2-y}$Co$_y$As$_2$) sides of the phase diagram using ultrafast pump-probe spectroscopy. Below $T_c$, measurements conducted at low photoinjected quasiparticle densities in the optimally and overdoped Ba$_{1-x}$K$_x$Fe$_2$As$_2$ samples reveal two distinct relaxation processes: a fast component whose decay rate increases linearly with excitation density and a slow component with an excitation density independent decay rate. We argue that these t…
To identify the key parameter for optimal superconductivity in iron pnictides, we measured the $^{31}$P-NMR relaxation rate on BaFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ ($x = 0.22$ and 0.28) under pressure and compared the effects of chemical substitution and physical pressure. For $x = 0.22$, structural and antiferromagnetic (AFM) transition temperatures both show minimal changes with pressure up to 2.4~GPa, whereas the superconducting transition temperature $T_{\rm c}$ increases to twice its former value. In contrast, for $x=0.28$ near the AFM quantum critical point (QCP), the structural phase tra…
Spin dynamics evolution of BaFe$_2$(As$_{1-x}$P$_x$)$_2$ was probed as a function of P concentration via $^{31}$P NMR. Our NMR study reveals that two-dimensional antiferromagnetic (AF) fluctuations are notably enhanced with little change in static susceptibility on approaching the AF phase from the superconducting dome. Moreover, magnetically ordered temperature $θ$ deduced from the relaxation rate vanishes at optimal doping. These results provide clear-cut evidence for a quantum-critical point (QCP), suggesting that the AF fluctuations associated with the QCP play a central role in the high-$…
We study the temperature and pressure dependence of the structural and electronic properties of the iron pnictide superconductor BaFe2As2. We use density functional theory based Born-Oppenheimer molecular dynamics simulations to investigate the system at temperatures from T=5 K to 150 K and pressures from P=0 GPa to 30 GPa. When increasing the pressure at low temperature, we find the two transitions from an orthorhombic to a tetragonal and to a collapsed tetragonal structure that are also observed in zero temperature structure relaxations and in experiment. However, these transitions are consi…
We report an $^{75}$As NMR study of BaFe$_2$As$_2$ in both single crystals and polycrystal forms. We find that Sn impurities in the single crystal dramatically alter the low energy spin fluctuations and suppress the ordering temperature from 138 K to 85 K. In contrast to Sn-free samples, we find that the temperature dependence of the $^{75}$As NMR spectra and spin lattice relaxation rates reveal a second order phase transition to a state of incommensurate magnetic order.
^{31}P and ^{75}As NMR measurements were performed in superconducting BaFe_2(As_{0.67}P_{0.33})_2 with T_c = 30 K. The nuclear-spin-lattice relaxation rate T_1^{-1} and the Knight shift in the normal state indicate the development of antiferromagnetic fluctuations, and T_1^{-1} in the superconducting (SC) state decreases without a coherence peak just below T_c, as observed in (Ba_{1-x}K_{x})Fe_2As_2. In contrast to other iron arsenide superconductors, the T_1^{-1} \propto T behavior is observed below 4K, indicating the presence of a residual density of states at zero energy. Our results sugges…
We have performed extensive ab initio calculations to investigate phonon dynamics and their possible role in superconductivity in BaFe2As2 and related systems. The calculations are compared to inelastic neutron scattering data that offer improved resolution over published data [Mittal et al., PRB 78 104514 (2008)], in particular at low frequencies. Effects of structural phase transition and full/partial structural relaxation, with and without magnetic ordering, on the calculated vibrational density of states are reported. Phonons are best reproduced using either the relaxed magnetic structures…
The NMR results in iron pnictides BaFe2(As1-xPx)2 and Ba(Fe1-xCox)2As2 are analyzed based on the self-consistent renormalization (SCR) spin fluctuation theory. The temperature dependence of the NMR relaxation rate (T_1)^{-1} as well as the electrical resistivity is well reproduced by a SCR model where two-dimensional antiferromagnetic (AF) spin fluctuations are dominant. The successful description of the crossover feature from non-Fermi liquid to Fermi liquid behavior strongly suggests that low-lying spin fluctuations in BaFe2(As1-xPx)2 and Ba(Fe1-xCox)2As2 possess an itinerant AF nature, and …
The majority of the iron-based superconductors (FeSCs) exhibit a two-dimensional square lattice structure. Recent reports of pressure-induced superconductivity in the spin-ladder system, BaFe$_2$X$_3$ (X =S,Se), introduce a quasi-one-dimensional prototype and an insulating parent compound to the FeSCs. Here we report X-ray, neutron diffraction and muon spin relaxation experiments on BaFe$_2$Se$_3$ under hydrostatic pressure to investigate its magnetic and structural properties across the pressure-temperature phase diagram. A structural phase transition was identified at a pressure of 3.7(3) GP…
We report experimental studies of a series of BaFe$_2$S$_{3-x}$Se$_x$ ($0\leq x\leq3$) single crystals and powder specimens using x-ray diffraction, neutron diffraction, muon spin relaxation, and electrical transport measurements. A structural transformation from Cmcm (BaFe$_2$S$_3$) to Pnma (BaFe$_2$Se$_3$) was identified around $x = 0.7\sim 1$. Neutron diffraction measurements on the samples with $x$ = 0.2, 0.4, and 0.7 reveal that the N$é$el temperature of the stripe antiferromagnetic order is gradually suppressed from $\sim$120 to 85 K, while the magnitude of the ordered Fe$^{2+}$ moments …
We use neutron diffraction and muon spin relaxation to study the effect of in-plane uniaxial pressure on the antiferromagnetic (AF) orthorhombic phase in BaFe$_2$As$_2$ and its Co- and Ni-substituted members near optimal superconductivity. In the low temperature AF ordered state, uniaxial pressure necessary to detwin the orthorhombic crystals also increases the magnetic ordered moment, reaching an 11$\%$ increase under 40 MPa for BaFe$_{1.9}$Co$_{0.1}$As$_2$, and a 15$\%$ increase for BaFe$_{1.915}$Ni$_{0.085}$As$_2$. We also observe an increase of the AF ordering temperature ($T_N$) of about …
Employing the momentum-sensitivity of time- and angle-resolved photoemission spectroscopy we demonstrate the analysis of ultrafast single- and many-particle dynamics in antiferromagnetic EuFe2As2. Their separation is based on a temperature-dependent difference of photo-excited hole and electron relaxation times probing the single particle band and the spin density wave gap, respectively. Reformation of the magnetic order occurs at 800 fs, which is four times slower compared to electron-phonon equilibration due to a smaller spin-dependent relaxation phase space.
A series of high quality BaFe$_{2-x}$Ni$_x$As$_2$ pnictide superconductors were studied using magnetic relaxation and isothermal magnetic measurements in order to study the second magnetization peak (SMP) and critical current behaviour in Ni-doped 122 family. The temperature dependence of the magnetic relaxation rate suggests a pinning crossover, whereas, it's magnetic field dependence hints a vortex-lattice structural phase-transition. The activation energy ($U$) estimated using the magnetic relaxation data was analyzed in detail for slightly-underdoped, slightly-overdoped and an overdoped sa…
We measure magnetization as a function of temperature, magnetic field and time in a BaFe$_2$(As$_{0.68}$P$_{0.32}$)$_2$ single crystal with $T_c$ = 27.6 K. The fish-tail observed on many $M$($H$) curves are used to construct isofield $M$($T$) curves which show an anomalous peak at some temperature $Tt$ suggesting a possible phase transition in the irreversible regime. A vortex dynamics study performed along the peaks evidences a minimum in the relaxation rate occurring at the same position $Tt$ of the minimum value of $M$ in these peaks. A vortex dynamics study performed on $M$($H$) curves sho…
We investigate carrier and collective mode dynamics in 2H-NbSe$_2$ using time-resolved optical pump-probe spectroscopy and compare the results with first-principle calculations. Broadband ultrafast reflectivity studies of 2H-NbSe$_2$ in a wide temperature interval covering the normal, charge density wave (CDW) and superconducting phase were performed. Spectral features observed in the transient reflectivity experiment were associated with specific optical transitions obtained from band structure calculations. Displacive excitation of coherent phonons showed CDW-associated coherent oscillations…
We report pressure-dependent neutron diffraction and muon spin relaxation/rotation measurements combined with first-principles calculations to investigate the structural, magnetic, and electronic properties of BaFe$_2$S$_3$ under pressure. The experimental results reveal a gradual enhancement of the stripe-type ordering temperature with increasing pressure up to 2.6 GPa and no observable change in the size of the ordered moment. The ab initio calculations suggest that the magnetism is highly sensitive to the Fe-S bond lengths and angles, clarifying discrepancies with previously published resul…
The temperature dependence of the relaxation dynamics in the bilayer thin film heterostructure composed of multiferroic BiFeO$_{3}$ (BFO) and superconducting YBa$_{2}$Cu$_{3}$O$_{7}$ (YBCO) grown on a (001) SrTiO$_{3}$ substrate is studied by a time-resolved pump-probe technique, and compared with that of pure YBCO thin film grown under the same growth conditions. The superconductivity of YBCO is found to be retained in the heterostructure. We observe a speeding up of the YBCO recombination dynamics in the superconducting state of the heterostructure, and attribute it to the presence of weak f…
We investigate the quasiparticle relaxation and low-energy electronic structure in undoped SrFe_2As_2 exhibiting spin-density wave (SDW) ordering using optical pump-probe femtosecond spectroscopy. A remarkable critical slowing down of the quasiparticle relaxation dynamics at the SDW transition temperature T_SDW = 200K is observed. From temperature dependence of the transient reflectivity amplitude we determine the SDW-state charge gap magnitude, 2Delta_SDW/k_BT_SDW=7.2+-1. The second moment of the Eliashberg function, lambda<(hbar omega)^2>=110+-10meV^2, determined from the relaxation time abo…
Using femtosecond time- and angle-resolved photoemission spectroscopy we investigate the effect of electron doping on the electron dynamics in Ba(Fe_{1-x}Co_x)_2As_2 in a range of 0 < x < 0.15 at temperatures slightly above the Néel temperature. By analyzing the time-dependent photoemission intensity of the pump laser excited population as a function of energy, we found that the relaxation times at 0 < E-E_F < 0.2 eV are doping dependent and about 100 fs shorter at optimal doping than for overdoped and parent compounds. Analysis of the relaxation rates also reveals the presence of a pump fluen…
Nonequilibrium quasiparticle relaxation dynamics is reported in superconducting CaFe1.89Co0.11As2 single crystal using femtosecond time-resolved pump-probe spectroscopy. The carrier dynamics reflects a three-channel decay of laser deposited energy with characteristic time scales varying from few hundreds of femtoseconds to order of few nanoseconds where the amplitudes and time-constants of the individual electronic relaxation components show significant changes in the vicinity of the spin density wave (T_SDW ~ 85 K) and superconducting (T_SC ~ 20 K) phase transition temperatures. The quasipart…
Ultrafast optical pump-probe spectroscopy is used to track carrier dynamics in the large magnetoresistance material WTe$_{2}$. Our experiments reveal a fast relaxation process occurring on a sub-picosecond time scale that is caused by electron-phonon thermalization, allowing us to extract the electron-phonon coupling constant. An additional slower relaxation process, occurring on a time scale of $\sim$5-15 picoseconds, is attributed to phonon-assisted electron-hole recombination. As the temperature decreases from 300 K, the timescale governing this process increases due to the reduction of the…
The non-equilibrium state of the high-Tc superconductor Bi2Sr2CaCu2O8+delta and its ultrafast dynamics have been investigated by femtosecond time- and angle-resolved photoemission spectroscopy well below the critical temperature. We probe optically excited quasiparticles at different electron momenta along the Fermi surface and detect metastable quasiparticles near the antinode. Their decay through e-e scattering is blocked by a phase space restricted to the nodal region. The lack of momentum dependence in the decay rates is in agreement with relaxation dominated by Cooper pair recombination i…
We review our recent experimental results on the electronic nematic phase in electron- and hole-doped BaFe$_2$As$_2$ and FeSe. The nematic susceptibility is extracted from shear-modulus data (obtained using a three-point-bending method in a capacitance dilatometer) using Landau theory and is compared to the nematic susceptibility obtained from elastoresistivity and Raman data. FeSe is particularly interesting in this context, because of a large nematic, i.e., a structurally distorted but paramagnetic, region in its phase diagram. Scaling of the nematic susceptibility with the spin lattice rela…
We used femtosecond optical pump-probe spectroscopy to study the photoinduced change in reflectivity of thin films of the electron-doped cuprate La$_{2-x}$Ce$_x$CuO$_4$ (LCCO) with dopings of x$=$0.08 (underdoped) and x$=$0.11 (optimally doped). Above T$_c$, we observe fluence-dependent relaxation rates which onset at a similar temperature that transport measurements first see signatures of antiferromagnetic correlations. Upon suppressing superconductivity with a magnetic field, it is found that the fluence and temperature dependence of relaxation rates is consistent with bimolecular recombina…
