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U. Bovensiepen

Publications and source records attributed to U. Bovensiepen.

At least 19 recordsLinked to original sources
arXiv2024

Resonant molecular transitions in second harmonic generation spectroscopy of Fe-octaethylporphyrin adsorbed on Cu(001)

Metal-organic molecular adsorbates on metallic surfaces offer the potential to both generate materials for future (spin-)electronics applications as well as a better fundamental understanding of molecule-substrate interaction, provided that the electronic properties of such interfaces can be analyzed and/or manipulated in a targeted manner. To investigate electronic interactions at such interfaces, we measure optical second harmonic generation (SHG) from iron-octaethylporphyrin (FeOEP) adsorbed on Cu(001), and perform electronic structure calculations using coupled cluster methods including optical excitations. We find that the SHG response of FeOEP/Cu(001) is modified at 2.15-2.35 eV fundamental photon energy compared to the bare Cu(001) surface. Our polarization-dependent analysis shows that the $χ_{zzz}^{(2)}$ non-linear susceptibility tensor element dominates this modification. The first-principles calculations confirm this effect and conclude a resonantly enhanced SHG by molecular transitions at $\hbarω\geq 2$ eV. We show that the enhancement of $χ^{(2)}_{zzz}$ results from a strong charge-transfer character of the molecule-substrate interaction. Our findings demonstrate the suitability of surface SHG for the characterization of such interfaces and the potential to employ it for time-resolved SHG experiments on optically induced electronic dynamics.

cond-mat.mtrl-sci↗
arXiv2024

Table-top soft x-ray source for XAS experiments with photon energies up to 350 eV

We present a table-top setup for femtosecond x-ray absorption spectroscopy based on high harmonic generation (HHG) in noble gases. Using sub-millijoule pump pulses at a central wavelength of 1550 nm broadband HHG in the range 70 to 350 eV was demonstrated. The HHG coherence lengths of several millimeters were achieved by reaching the nonadiabatic regime of harmonic generation. NEXAFS experiments on the boron K edge of a boron foil and a hexagonal BN (hBN) 2D material demonstrate the capabilities of the setup.

physics.optics↗
arXiv2023

Electron phonon coupling in ultrathin Pb films on Si(111): Where the heck is the energy?

In this work, we study the heat transfer from electron to phonon system within a five monolayer thin epitaxial Pb film on Si(111) upon fs-laser excitation. The response of the electron system is determined using time-resolved photoelectron spectroscopy while the lattice excitation is measured by means of the Debye-Waller effect in time-resolved reflection high-energy electron diffraction. The electrons lose their heat within 0.5 ps while the lattice temperature rises slowly in 3.5 to 8 ps, leaving a gap of 3-7 ps. We propose that the hidden energy is transiently stored in high-frequency phonon modes for which diffraction is insensitive and which are excited in 0.5 ps. Within a three-temperature model we use three heat baths, namely electrons, high-frequency and low-frequency phonon modes to simulate the observations. The excitation of low-frequency acoustic phonons, i.e., thermalization of the lattice is facilitated through anharmonic phonon-phonon interaction.

cond-mat.mes-hall↗
arXiv2022

Transient spin injection efficiencies at ferromagnet/metal interfaces

Spin injection across interfaces driven by ultrashort optical pulses on femtosecond timescales constitutes a new way to design spintronics applications. Targeted utilization of this phenomenon requires knowledge of the efficiency of non-equilibrium spin injection. From a quantitative comparison of ab-initio time-dependent density functional theory and interface-sensitive, time-resolved non-linear optical experiment, we determine the spin injection efficiencies (SIE) across ferromagnetic/metal interfaces and discuss their microscopic origin, i.e. the influence of spin-orbit coupling and the interface electronic structure. Moreover, we find that the SIE can be optimized through laser pulse and materials parameters, namely the fluence, pulse duration, and substrate material.

cond-mat.mtrl-sci↗
arXiv2021

The ambivalent competition of Coulomb and van-der-Waals interactions in Xe-Cs+ aggregates on Cu(111) surfaces

Microscopic insight into interactions is a key for understanding the properties of heterogenous interfaces. We analyze local attraction in non-covalently bonded Xe{Cs+ aggregates and monolayers on Cu(111) as well as repulsion upon electron transfer. Using two-photon photoemission spectroscopy, scanning tunneling microscopy, and coupled cluster calculations combined with an image-charge model we explain the intricate impact Xe has on Cs+/Cu(111). We find that attraction between Cs+ and Xe counterbalances the screened Coulomb repulsion between Cs+ ions on Cu(111). Furthermore, we observe that the Cs 6s electron is repelled from Cu(111) due to xenon's electron density. Together, this yields a dual, i.e., attractive or repulsive, response of Xe depending on the positive or negative charge of the respective counterparticle, which emphasizes the importance of the Coulomb interaction in these systems.

cond-mat.mes-hall↗
arXiv2021

Effect of lattice excitations on transient near edge X-ray absorption spectroscopy

Time-dependent and constituent-specific spectral changes in soft near edge X-ray spectroscopy (XAS) of an [Fe/MgO]$_8$ metal/insulator heterostructure upon laser excitation are analyzed at the O K-edge with picosecond time resolution. The oxygen absorption edge of the insulator features a uniform intensity decrease of the fine structure at elevated phononic temperatures, which can be quantified by a simple simulation and fitting procedure presented here. Combining X-ray absorption spectroscopy with ultrafast electron diffraction measurements and ab initio calculations demonstrate that the transient intensity changes in XAS can be assigned to a transient lattice temperature. Thus, the sensitivity of transient near edge XAS to phonons is demonstrated.

cond-mat.mtrl-sci↗
arXiv2019

Microscopic non-equilibrium energy transfer dynamics in a photoexcited metal/insulator heterostructure

The element specificity of soft X-ray spectroscopy makes it an ideal tool for analyzing the microscopic origin of ultrafast dynamics induced by localized optical excitation in metal-insulator heterostructures. Using [Fe/MgO]$_n$ as a model system, we perform ultraviolet pump/soft X-ray probe experiments, which are sensitive to all constituents of these heterostructures, to probe both electronic and lattice excitations. Complementary ultrafast electron diffraction experiments independently analyze the lattice dynamics of the Fe constituent, and together with ab initio calculations yield comprehensive insight into the microscopic processes leading to local relaxation within a single constituent or non-local relaxation between two constituents. Besides electronic excitations in Fe, which are monitored at the Fe L$_3$ absorption edge and relax within 1 ps by electron-phonon coupling, soft X-ray analysis identifies a change at the oxygen K absorption edge of the MgO layers which occurs within 0.5 ps. This ultrafast energy transfer across the Fe-MgO interface is mediated by high-frequency, interface vibrational modes, which are excited by hot electrons in Fe and couple to vibrations in MgO in a mode-selective, non-thermal manner. A second, slower timescale is identified at the oxygen K pre-edge and the Fe L$_3$ edge. The slower process represents energy transfer by acoustic phonons and contributes to thermalization of the entire heterostructure. We thus find that the interfacial energy transfer is associated with non-equilibrium behavior in the phonon system. Because our experiments lack signatures of charge transfer across the interface, we conclude that phonon-mediated processes dominate the competition of electronic and lattice excitations in these non-local, non-equilibrium dynamics.

cond-mat.mtrl-sci↗
arXiv2019

Towards attosecond pulse synthesis from solids: spectral shaping, field autocorrelation, and two-color harmonic generation

Harmonic generation from solid surfaces is a promising tool for producing high energy attosecond pulses. We report shaping of the harmonic spectrum to achieve the bandwidth necessary for attosecond pulse generation. The shaping is demonstrated for lower as well as for higher harmonics using single and two-pulse pumping. The measured harmonic field autocorrelation function exhibits attosecond spikes in good agreement with the harmonic spectrum. Double slit experiments reveal a high spatial coherence of the harmonic beam.

physics.plasm-ph↗
arXiv2018

Competing spin transfer and dissipation at Co/Cu(001) interfaces on femtosecond timescales

By combining interface-sensitive non-linear magneto-optical experiments with femtosecond time resolution and ab-initio time-dependent density functional theory, we show that optically excited spin dynamics at Co/Cu(001) interfaces proceeds via spin-dependent charge transfer and backtransfer between Co and Cu. This ultrafast spin transfer competes with dissipation of spin angular momentum mediated by spin-orbit coupling already on sub 100 fs timescales. We thereby identify the fundamental microscopic processes during laser-induced spin transfer at a model interface for technologically relevant ferromagnetic heterostructures.

cond-mat.mtrl-sci↗
arXiv2018

Magneto-optical properties of Au upon the injection of hot spin-polarized electrons across Fe/Au(001) interfaces

We demonstrate a novel method for the excitation of sizable magneto-optical effects in Au by means of the laser-induced injection of hot spin-polarized electrons in Au/Fe/MgO(001) heterostructures. It is based on the energy- and spin-dependent electron transmittance of Fe/Au interface which acts as a spin filter for non-thermalized electrons optically excited in Fe. We show that after crossing the interface, majority electrons propagate through the Au layer with the velocity on the order of 1 nm/fs (close to the Fermi velocity) and the decay length on the order of 100 nm. Featuring ultrafast functionality and requiring no strong external magnetic fields, spin injection results in a distinct magneto-optical response of Au. We develop a formalism based on the phase of the transient complex MOKE response and demonstrate its robustness in a plethora of experimental and theoretical MOKE studies on Au, including our ab initio calculations. Our work introduces a flexible tool to manipulate magneto-optical properties of metals on the femtosecond timescale that holds high potential for active magneto-photonics, plasmonics, and spintronics.

cond-mat.mes-hall↗
arXiv2016

Doping dependence and electron-boson coupling in the ultrafast relaxation of hot electron populations in Ba(Fe_{1-x}Co_x)_2As_2

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 fluence dependent step in the relaxation time at E-E_F = 200meV which we explain by coupling of the excited electronic system to a boson of this energy. We compare our results with static ARPES and transport measurements and find disagreement and agreement concerning the doping-dependence, respectively. We discuss the effect of the electron-boson coupling on the energy-dependent relaxation and assign the origin of the boson to a magnetic excitation.

cond-mat.supr-con↗
arXiv2016

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↗
arXiv2015

Separation of ultrafast spin currents and spin-flip scattering in Co/Cu(001) driven by femtosecond laser excitation via the complex MOKE

Ultrafast magnetization dynamics in metallic heterostructures consists of a combination of local demagnetization in the ferromagnetic constituent and spin-dependent transport contributions within and in between the constituents. Separation of these local and non-local contributions is essential to obtain microscopic understanding and for potential applications of the underlying microscopic processes. By comparing the ultrafast changes of the polarization rotation and ellipticity in the magneto-optical Kerr effect (MOKE) we observe a time-dependent magnetization profile M(z,t) in Co/Cu(001) films by exploiting the effective depth sensitivity of the method. By analyzing the spatio-temporal correlation of these profiles we find that on time scales before hot electron thermalization (<100 fs) the transient magnetization of Co films is governed by spin-dependent transport effects, while after hot electron thermalization (>200 fs) local spin-flip processes dominate.

cond-mat.mtrl-sci↗
arXiv2015

Non-Fermi-liquid scattering rates and anomalous band dispersion in ferropnictides

Angle-resolved photoemission spectroscopy (ARPES) is used to study the band dispersion and the quasiparticle scattering rates in two ferropnictides systems. Our ARPES results show linear-in-energy dependent scattering rates which are constant in a wide range of control parameter and which depend on the orbital character of the bands. We demonstrate that the linear energy dependence gives rise to weakly dispersing band with a strong mass enhancement when the band maximum crosses the chemical potential. In the superconducting phase the related small effective Fermi energy favors a Bardeen-Cooper-Schrieffer (BCS)\,\cite{Bardeen1957}-Bose-Einstein (BE)\,\cite{Bose1924} crossover state.

cond-mat.supr-con↗
arXiv2013

Ultrafast modulation of the chemical potential in BaFe$_2$As$_2$ by coherent phonons

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 results establish a novel way to tune the electronic properties of iron pnictides: coherent control of the effective chemical potential. The results further suggest that the equilibration time for the effective chemical potential needs to be considered in the ultrafast electronic structure dynamics of materials with weak interlayer coupling.

cond-mat.supr-con↗
arXiv2013

Electronic structure and quantum criticality in Ba(Fe$_{1-x-y}$Co$_{x}$Mn$_{y}$)$_{2}$As$_{2}$, an ARPES study

We used angle-resolved photoemission spectroscopy (ARPES) and density functional theory calculations to study the electronic structure of Ba(Fe1-x-yCoxMny)2As2 for x=0.06 and 0<=y <=0.07. From ARPES we derive that the substitution of Fe by Mn does not lead to hole doping, indicating a localization of the induced holes. An evaluation of the measured spectral function does not indicate a diverging effective mass or scattering rate near optimal doping. Thus the present ARPES results indicate a continuous evolution of the quasiparticle interaction and therefore question previous quantum critical scenarios.

cond-mat.supr-con↗