arXiv subjects

S. Kaiser

Publications and source records attributed to S. Kaiser.

At least 19 recordsLinked to original sources

arXiv2024

THz Second and Third Harmonic Generation in PdCoO$_2$ Thin Films

Terahertz high harmonic generation (THz HHG) is a common property of nonlinear systems. Recently it has been used to investigate fundamental principles that govern transport and nonlinear dynamics in novel quantum materials like graphene, Dirac semimetals or high-temperature superconductors. Here, we report on the observation of exceptionally large THz second harmonic and third harmonic generation in thin films of the highly conducting delafossite PdCoO$_2$ down to low temperatures. The growth of this material on offcut substrate allows for a significant enhancement of the third harmonic intensity compared to ordinary $c$-axis grown thin films. Furthermore, it appears to be a necessity for the observation of THz second harmonic generation. We model the temperature dependence of the third harmonic generation by means of Boltzmann transport theory and provide an explanation for the second harmonic generation by comparing the system to the electric field induced second harmonic generation. The present investigation thus provides an important contribution to the ongoing discussion of low temperature origins of THz HHG and might serve as a new platform for THz high harmonic applications.

cond-mat.mtrl-sci↗

arXiv2021

All-Optical and Microwave-Free Detection of Meissner Screening using Nitrogen-Vacancy Centers in Diamond

Microscopic studies on thin film superconductors play an important role for probing non-equilibrium phase transitions and revealing dynamics at the nanoscale. However, magnetic sensors with nanometer scale spatial and picosecond temporal resolution are essential for exploring these. Here, we present an all-optical, microwave-free method, that utilizes the negatively charged nitrogen-vacancy (NV) center in diamond as a non-invasive quantum sensor and enables the spatial detection of the Meissner state in a superconducting thin film. We place an NV implanted diamond membrane on a superconducting LSCO thin film. The strong B-field dependence of the NV photoluminescence (PL) allows us to investigate the Meissner screening in LSCO under an externally applied magnetic field in a non-resonant manner.

cond-mat.supr-con↗

arXiv2017

Classification and characterization of nonequilibrium Higgs modes in unconventional superconductors

Recent findings of new Higgs modes in unconventional superconductors require a classification and characterization of the modes allowed by nontrivial gap symmetry. Here we develop a theory for a tailored nonequilibrium quantum quench to excite all possible oscillation symmetries of a superconducting condensate. We show that both a finite momentum transfer and quench symmetry allow for an identification of the resulting Higgs oscillations. These serve as a fingerprint for the ground state gap symmetry. We provide a classification scheme of these oscillations and the quench symmetry based on group theory for the underlying lattice point group. For characterization, analytic calculations as well as full scale numeric simulations of the transient optical response resulting from an excitation by a realistic laser pulse are performed. Our classification of Higgs oscillations allows us to distinguish between different symmetries of the superconducting condensate.

cond-mat.str-el↗

arXiv2016

Dynamical decoherence of the light induced interlayer coupling in YBa$_{2}$Cu$_{3}$O$_{6+δ}$

Optical excitation of apical oxygen vibrations in YBa$_{2}$Cu$_{3}$O$_{6+δ}$ has been shown to enhance its c-axis superconducting-phase rigidity, as evidenced by a transient blue shift of the equilibrium inter-bilayer Josephson plasma resonance. Surprisingly, a transient c-axis plasma mode could also be induced above T$_{c}$ by the same apical oxygen excitation, suggesting light activated superfluid tunneling throughout the pseudogap phase of YBa$_{2}$Cu$_{3}$O$_{6+δ}$. However, despite the similarities between the above T$_{c}$ transient plasma mode and the equilibrium Josephson plasmon, alternative explanations involving high mobility quasiparticle transport should be considered. Here, we report an extensive study of the relaxation of the light-induced plasmon into the equilibrium incoherent phase. These new experiments allow for a critical assessment of the nature of this mode. We determine that the transient plasma relaxes through a collapse of its coherence length rather than its carrier (or superfluid) density. These observations are not easily reconciled with quasiparticle interlayer transport, and rather support transient superfluid tunneling as the origin of the light-induced interlayer coupling in YBa$_{2}$Cu$_{3}$O$_{6+δ}$.

cond-mat.supr-con↗

arXiv2015

THz-Frequency Modulation of the Hubbard U in an Organic Mott Insulator

We use midinfrared pulses with stable carrier-envelope phase offset to drive molecular vibrations in the charge transfer salt ET-F2TCNQ, a prototypical one-dimensional Mott insulator. We find that the Mott gap, which is probed resonantly with 10 fs laser pulses, oscillates with the pump field. This observation reveals that molecular excitations can coherently perturb the electronic on-site interactions (Hubbard U) by changing the local orbital wave function. The gap oscillates at twice the frequency of the vibrational mode, indicating that the molecular distortions couple quadratically to the local charge density.

cond-mat.str-el↗

arXiv2015

An optically stimulated superconducting-like phase in K3C60 far above equilibrium Tc

The control of non-equilibrium phenomena in complex solids is an important research frontier, encompassing new effects like light induced superconductivity. Here, we show that coherent optical excitation of molecular vibrations in the organic conductor K3C60 can induce a non-equilibrium state with the optical properties of a superconductor. A transient gap in the real part of the optical conductivity and a low-frequency divergence of the imaginary part are measured for base temperatures far above equilibrium Tc=20 K. These findings underscore the role of coherent light fields in inducing emergent order.

cond-mat.supr-con↗

arXiv2015

Two distinct kinetic regimes for the relaxation of light-induced superconductivity in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_{4}$

We address the kinetic competition between charge striped order and superconductivity in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_{4}$. Ultrafast optical excitation is tuned to a mid-infrared vibrational resonance that destroys charge order and promptly establishes transient coherent interlayer coupling in this material. This effect is evidenced by the appearance of a longitudinal plasma mode reminiscent of a Josephson plasma resonance. We find that coherent interlayer coupling can be generated up to the charge order transition $T_{CO} \approx$ 80 K, far above the equilibrium superconducting transition temperature of any lanthanide cuprate. Two key observations are extracted from the relaxation kinetics of the interlayer coupling. Firstly, the plasma mode relaxes through a collapse of its coherence length and not its density. Secondly, two distinct kinetic regimes are observed for this relaxation, above and below spin order transition $T_{SO} =$ 25 K. Especially, the temperature independent relaxation rate observed below $T_{SO}$ is anomalous and suggests coexistence of superconductivity and stripes rather than competition. Both observations support arguments that a low temperature coherent stripe (or pair density wave) phase suppresses c-axis tunnelling by disruptive interference rather than by depleting the condensate.

cond-mat.supr-con↗

arXiv2015

Pressure dependent relaxation in the photo-excited Mott insulator ETF2TCNQ: Influence of hopping and correlations on quasiparticle recombination rates

Femtosecond relaxation of photo-excited quasiparticles in the one dimensional Mott insulator ET-F2TCNQ are measured as a function of external pressure, which is used to tune the electronic structure. By fitting the static optical properties and measuring femtosecond decay times at each pressure value, we correlate the relaxation rates with the electronic bandwidth t and on the intersite correlation energy V. The scaling of relaxation times with microscopic parameters is different than for metals and semiconductors. The competition between localization and delocalization of the Mott-Hubbard exciton dictates the efficiency of the decay, as exposed by a fit based on the solution of the time-dependent extended Hubbard Hamiltonian.

cond-mat.str-el↗

arXiv2015

Femtosecond x rays link melting of charge-density wave correlations and light-enhanced coherent transport in YBa2Cu3O6.6

We use femtosecond resonant soft x-ray diffraction to measure the optically stimulated ultrafast changes of charge density wave correlations in underdoped YBa2Cu3O6.6. We find that when coherent interlayer transport is enhanced by optical excitation of the apical oxygen distortions, at least 50% of the in-plane charge density wave order is melted. These results indicate that charge ordering and superconductivity may be competing up to the charge ordering transition temperature, with the latter becoming a hidden phase that is accessible only by nonlinear phonon excitation.

cond-mat.supr-con↗

arXiv2014

Optically induced superconductivity in striped La2-xBaxCuO4 by polarization-selective excitation in the near infrared

We show that superconducting interlayer coupling, which coexists with and is depressed by stripe order in La1.885Ba0.115CuO4, can be enhanced by excitation with near-infrared laser pulses. For temperatures lower than Tc = 13 K, we observe a blue-shift of the equilibrium Josephson plasma resonance, detected by terahertz-frequency reflectivity measurements. Key to this measurement is the ability to probe the optical properties at frequencies as low as 150 GHz, detecting the weak interlayer coupling strengths. For T > Tc a similar plasma resonance, absent at equilibrium, is induced up to the spin-ordering temperature TSO = 40 K. These effects are reminiscent but qualitatively different from the light-induced superconductivity observed by resonant phonon excitation in La1.675Eu0.2Sr0.125CuO6.5. Importantly, enhancement of the below-Tc interlayer coupling and its appearance above Tc are preferentially achieved when the near-infrared pump light is polarized perpendicular to the superconducting planes, likely due to more effective melting of stripe order and the less effective excitation of quasiparticles from the Cooper pair condensate when compared to in-plane excitation.

cond-mat.supr-con↗

arXiv2014

Optically enhanced coherent transport in YBa2Cu3O6.5 by ultrafast redistribution of interlayer coupling

Nonlinear optical excitation of infrared active lattice vibrations has been shown to melt magnetic or orbital orders and to transform insulators into metals. In cuprates, this technique has been used to remove charge stripes and promote superconductivity, acting in a way opposite to static magnetic fields. Here, we show that excitation of large-amplitude apical oxygen distortions in the cuprate superconductor YBa2Cu3O6.5 promotes highly unconventional electronic properties. Below the superconducting transition temperature (Tc = 50 K), interbilayer coherence is transiently enhanced at the expense of intra-bilayer coupling. Strikingly, even above Tc a qualitatively similar effect is observed up to room temperature, with transient inter-bilayer coherence emerging from the incoherent ground state and similar transfer of spectral weight from high to low frequency. These observations are compatible with previous reports of an inhomogeneous normal state that retains important properties of a superconductor, in which light may be melting competing orders or dynamically synchronizing the interlayer phase. The transient redistribution of coherence discussed here could lead to new strategies to enhance superconductivity in steady state.

cond-mat.supr-con↗

arXiv2014

Optically induced coherent transport far above Tc in underdoped YBa2Cu3O6+x

We report on a photo-induced transient state of YBa2Cu2O6+x in which transport perpendicular to the Cu-O planes becomes highly coherent. This effect is achieved by excitation with mid-infrared optical pulses, tuned to the resonant frequency of apical oxygen vibrations, which modulate both lattice and electronic properties. Below the superconducting transition temperature Tc, the equilibrium signatures of superconducting interlayer coupling are enhanced. Most strikingly, the optical excitation induces a new reflectivity edge at higher frequency than the equilibrium Josephson plasma resonance, with a concomitant enhancement of the low frequency imaginary conductivity. Above Tc, the incoherent equilibrium conductivity becomes highly coherent, with the appearance of a reflectivity edge and a positive imaginary conductivity that increases with decreasing frequency. These features are observed up to room temperature in YBa2Cu2O6.45 and YBa2Cu2O6.5. The data above Tc can be fitted by hypothesizing that the light re-establishes a transient superconducting state over only a fraction of the solid, with a lifetime of a few picoseconds. Non-superconducting transport could also explain these observations, although one would have to assume transient carrier mobilities near 10^4 cm^2/(V.sec) at 100 K, with a density of charge carriers similar to the below Tc superfluid density. Our results are indicative of highly unconventional non-equilibrium physics and open new prospects for optical control of complex solids.

cond-mat.supr-con↗

arXiv2013

Possible observation of parametrically amplified coherent phasons in K0.3MoO3 using time-resolved extreme-ultraviolet ARPES

We use time- and angle-resolved photoemission spectroscopy (tr-ARPES) in the Extreme Ultraviolet (EUV) to measure the time- and momentum-dependent electronic structure of photo-excited K0.3MoO3. Prompt depletion of the Charge Density Wave (CDW) condensate launches coherent oscillations of the amplitude mode, observed as a 1.7-THz-frequency modulation of the bonding band position. In contrast, the anti-bonding band oscillates at about half this frequency. We attribute these oscillations to coherent excitation of phasons via parametric amplification of phase fluctuations.

cond-mat.str-el↗

arXiv2012

Deconstructing the Hubbard Hamiltonian by Ultrafast Quantum Modulation Spectroscopy in Solid-state Mott Insulators

Most available theories for correlated electron transport are based on the Hubbard Hamiltonian. In this effective theory, renormalized hopping and interaction parameters only implicitly incorporate the coupling of correlated charge carriers to microscopic degrees of freedom. Unfortunately, no spectroscopy can individually probe such renormalizations, limiting the applicability of Hubbard models. We show here that the role of each individual degree of freedom can be made explicit by using a new experimental technique, which we term 'quantum modulation spectroscopy' and we demonstrate here in the one-dimensional Mott insulator ET-F2TCNQ. We explore the role on the charge hopping of two localized molecular modes, which we drive with a mid infrared optical pulse. Sidebands appear in the modulated optical spectrum, and their linshape is fitted with a model based on the dynamic Hubbard Hamiltonian. A striking asymmetry between the renormalization of doublons and holons is revealed. The concept of quantum modulation spectroscopy can be used to systematically deconstruct Hubbard Hamiltonians in many materials, exposing the role of any mode, electronic or magnetic, that can be driven to large amplitude with a light field.

cond-mat.str-el↗

arXiv2011

Ultrafast strain engineering in complex oxide heterostructures

We report on ultrafast optical experiments in which femtosecond mid-infrared radiation is used to excite the lattice of complex oxide heterostructures. By tuning the excitation energy to a vibrational mode of the substrate, a long-lived five-order-of-magnitude increase of the electrical conductivity of NdNiO3 epitaxial thin films is observed as a structural distortion propagates across the interface. Vibrational excitation, extended here to a wide class of heterostructures and interfaces, may be conducive to new strategies for electronic phase control at THz repetition rates.

cond-mat.str-el↗

arXiv2011

Spin excitations of the correlated semiconductor FeSi probed by THz radiation

By direct measurements of the complex optical conductivity $σ(ν)$ of FeSi we have discovered a broad absorption peak centered at frequency $ν_{0}(4.2 K) \approx 32 cm^{-1}$ that develops at temperatures below 20 K. This feature is caused by spin-polaronic states formed in the middle of the gap in the electronic density of states. We observe the spin excitations between the electronic levels split by the exchange field of $H_{e}=34\pm 6 T$. Spin fluctuations are identified as the main factor determining the formation of the spin polarons and the rich magnetic phase diagram of FeSi.

cond-mat.str-el↗

arXiv2010

Bandwidth tuning triggers interplay of charge order and superconductivity in two-dimensional organic materials

We observe charge-order fluctuations in the quasi-two-dimensional organic superconductor $β^{\prime\prime}$-(BEDT-TTF)2 SF5 CH2 CF2 SO3 both by means of vibrational spectroscopy, locally probing the fluctuating charge order, and investigating the in-plane dynamical response by infrared reflectance spectroscopy. The decrease of effective electronic interaction in an isostructural metal suppresses both charge-order fluctuations and superconductivity, pointing on their interplay. We compare the results of our experiments with calculations on the extended Hubbard model.

cond-mat.str-el↗

arXiv2009

Effects of the magnetic orderings on the dynamical conductivity: optical investigations of EuFe$_2$As$_2$ single crystals

The magnetic, transport and optical properties of EuFe$_2$As$_2$ single crystals have been investigated parallel and perpendicular to the $ab$-plane. The anisotropy $ρ_c/ρ_{ab}\approx 8$ depends only slightly on temperature. In both orientations, the spin-density wave transition at $T_{\rm SDW}=189$ K shows up as a considerable increase in the dc resistivity. Susceptibility measurements evidence the magnetic order of the Eu$^{2+}$ moments at $T_N=19$ K with little influence on the electronic transport taking place in the FeAs layers. Polarization-dependent infrared spectroscopy reveals strongly anisotropic optical properties and yields a carrier density of only $4.2\times 10^{21} {\rm cm}^{-3}$ and a bandmass of $m_b=2m_0$. A sizeable Drude contribution is present at all temperatures and narrows upon cooling. Below $T_{\rm SDW}$, the spin-density-wave gap develops in the in-plane optical conductivity; no appreciable change is detected for the perpendicular polarization. Modifications in the phonon features are associated with changes of the electronic properties at $T_{\rm SDW}$. The extended Drude analysis yields a linear behavior of the frequency-dependent scattering rate below $T_{\rm SDW}$, indicating an interaction between the charge carriers and spin fluctuations in the spin-density-wave state.

cond-mat.supr-con↗