Prof. Dr. Ralf Röhlsberger
Abstract: The spontaneous crystal surface reconstruction of M-plane alpha-Al2O3 is employed for nanopatterning and nanofabrication in various fields of research including, among others, magnetism, superconductivity, and optoelectronics. In this reconstruction process the crystalline surface transforms from a planar morphology to one with a nanoscale ripple patterning. However, the high sample temperature required to induce surface reconstruction made in situ studies of the process seem unfeasible. The kinetics of ripple pattern formation therefore remained uncertain, and thus production of templates for nanofabrication could not advance beyond a trial-and-error stage. We present an approach combining in situ real-time grazing incidence small-angle X-ray scattering experiments (GISAXS) with model-based analysis and with ex situ atomic force microscopy (AFM) to observe this morphological transition in great detail. Our approach provides time-resolved information about all relevant morphological parameters required to trace the surface topography on the nanometer scale during reconstruction, i.e., the time dependence of the pattern wavelength, the ripple length, width, and height, and thus their facet angles. It offers a comprehensive picture of this process exemplified by a M-plane alpha-Al2O3 surface annealed at 1325 degrees C for 930 min. Fitting the model parameters to the experimental GISAXS data revealed a Johnson-Mehl-Avrami-Kolmogorov type of behavior for the pattern wavelength and a predominantly linear time dependence of the other parameters. In this case the reconstruction resulted in a crystalline surface fully patterned with asymmetric ripple-shaped nanostructures of 75 nm periodicity, 15 nm in height, and 630 nm in length. By elucidating the time dependence of these morphological parameters, this study shows a powerful way to significantly advance the predictability of annealing outcome and thus to efficiently customize nanopatterned alpha-Al2O3 templates for improved nanofabrication routines.
Abstract: Here, we use x-rays to create and probe quantum coherence in the photoionized amino acid glycine. The outgoing photoelectron leaves behind the cation in a coherent superposition of quantum mechanical eigenstates. Delayed x-ray pulses track the induced coherence through resonant x-ray absorption that induces Auger decay and by photoelectron emission from sequential double photoionization. Sinusoidal temporal modulation of the detected signal at early times (0 to 25 fs) is observed in both measurements. Advanced ab initio many-electron simulations allow us to explain the first 25 fs of the detected coherent quantum evolution in terms of the electronic coherence. In the kinematically complete x-ray absorption measurement, we monitor its dynamics for a period of 175 fs and observe an evolving modulation that may implicate the coupling of electronic to vibronic coherence at longer time scales. Our experiment provides a direct support for the existence of long-lived electronic coherence in photoionized biomolecules.
Abstract: In recent years, high-precision x-ray polarimeters have become a key method for the investigation of fundamental physical questions from solid-state physics to quantum optics. Here, we report on the verification of a polarization purity of better than 8×10−11 at an x-ray free-electron laser, which implies a suppression of the incoming photons to the noise level in the crossed polarizer setting. This purity provides exceptional sensitivity to tiny polarization changes and offers intriguing perspectives for fundamental tests of quantum electrodynamics.
Abstract: Controlling the magnetic properties of ultrathin films remains one of the main challenges to the further development of tunnel magnetoresistive (TMR) device applications. The magnetic response in such devices is mainly governed by extending the primary TMR trilayer with the use of suitable contact materials. The transfer of magnetic anisotropy to ferromagnetic electrodes consisting of CoFeB layers results in a field-dependent TMR response, which is determined by the magnetic properties of the CoFeB as well as the contact materials. We flexibly apply oblique-incidence deposition (OID) to introduce arbitrary intrinsic in-plane anisotropy profiles into the magnetic layers. The OID-induced anisotropy shapes the magnetic response and eliminates the requirement of additional magnetic contact materials. Functional control is achieved via an adjustable shape anisotropy that is selectively tailored for the ultrathin CoFeB layers. This approach circumvents previous limitations on TMR devices and allows for the design of new sensing functionalities, which can be precisely customized to a specific application, even in the high field regime. The resulting sensors maintain the typical TMR signal strength as well as a superb thermal stability of the tunnel junction, revealing a striking advantage in functional TMR design using anisotropic interfacial roughness.
Abstract: We show that Fano interference can be realized in a macroscopic microwave cavity coupled to a spin ensemble at room temperature. Via a formalism developed from the linearized Jaynes-Cummings model of cavity electromagnonics, we show that generalized Fano interference emerges from the photon–magnon interaction at low cooperativity. In this regime, the reflectivity approximates the scattering cross-section derived from the Fano-Anderson model. Although asymmetric lineshapes in this system are often associated with the Fano formalism, we show that whilst Fano interference is actually present, an exact Fano form cannot be achieved from the linear Jaynes-Cummings model. In the Fano model an additional contribution arises, which is attributed to decoherence in other systems, and in this case is due to the resonant nature of the photonic mode. The formalism is experimentally verified and accounts for the asymmetric lineshapes arising from the interaction between magnon and photon channels. As the magnon–photon coupling strength is increased, these channels merge into hybridized magnon–photon modes and the generalized Fano interference picture breaks down. Our results are universally applicable to systems underlying the linearized Jaynes-Cummings Hamiltonian at low cooperativity and connect the microscopic parameters of the quantum optical model to generalized Fano lineshapes.
Abstract: Phonon modes play a vital role in the cooperative phenomenon of light-induced spin transitions in spin crossover (SCO) molecular complexes. Although the cooperative vibrations, which occur over several hundreds of picoseconds to nanoseconds after photoexcitation, are understood to play a crucial role in this phase transition, they have not been precisely identified. Therefore, we have performed a novel optical laser pump-nuclear resonance probe experiment to identify the Fe-projected vibrational density of states (pDOS) during the first few nanoseconds after laser excitation of the mononuclear Fe(II) SCO complex [Fe(PM-BiA)(2)(NCS)(2)]. Evaluation of the so obtained nanosecond-resolved pDOS yields an excitation of similar to 8% of the total volume of the complex from the low-spin to high-spin state. Density functional theory calculations allow simulation of the observed changes in the pDOS and thus identification of the transient inter- and intramolecular vibrational modes at nanosecond time scales.
Abstract: The 35-fs-long pulses of a commercial Ti:sapphire amplifier are compressed to similar to 20 fs via self-phase modulation in bulk glass substrates. The cascading of both nonlinear broadening and dispersion compensation stages makes use of the increasing peak power in the successive nonlinear stages. As an application example, the compressed pulses are used for electro-optical sampling of terahertz waves created by optically pumped thin-film spin emitters. (C) 2021 Optical Society of America under the terms of the OSA Open Access Publishing Agreement
Abstract: Coherent control of quantum dynamics is key to a multitude of fundamental studies and applications1. In the visible or longer-wavelength domains, near-resonant light fields have become the primary tool with which to control electron dynamics2. Recently, coherent control in the extreme-ultraviolet range was demonstrated3, with a few-attosecond temporal resolution of the phase control. At hard-X-ray energies (above 5--10 kiloelectronvolts), Mössbauer nuclei feature narrow nuclear resonances due to their recoilless absorption and emission of light, and spectroscopy of these resonances is widely used to study the magnetic, structural and dynamical properties of matter4,5. It has been shown that the power and scope of Mössbauer spectroscopy can be greatly improved using various control techniques6--16. However, coherent control of atomic nuclei using suitably shaped near-resonant X-ray fields remains an open challenge. Here we demonstrate such control, and use the tunable phase between two X-ray pulses to switch the nuclear exciton dynamics between coherent enhanced excitation and coherent enhanced emission. We present a method of shaping single pulses delivered by state-of-the-art X-ray facilities into tunable double pulses, and demonstrate a temporal stability of the phase control on the few-zeptosecond timescale. Our results unlock coherent optical control for nuclei, and pave the way for nuclear Ramsey spectroscopy17 and spin-echo-like techniques, which should not only advance nuclear quantum optics18, but also help to realize X-ray clocks and frequency standards19. In the long term, we envision time-resolved studies of nuclear out-of-equilibrium dynamics, which is a long-standing challenge in Mössbauer science20.
Abstract: This work presents the improvements in the design and testing of polarimeters based on channel-cut crystals for nuclear resonant scattering experiments at the 14.4 keV resonance of Fe-57. By using four asymmetric reflections at asymmetry angles of alpha(1) = -28 degrees, alpha(2) = 28 degrees, alpha(3) = -28 degrees and alpha(4) = 28 degrees, the degree of polarization purity could be improved to 2.2 x 10(-9). For users, an advanced polarimeter without beam offset is now available at beamline P01 of the storage ring PETRA III.
Abstract: Dichroism is one of the most important optical effects in both the visible and the X-ray range. Besides absorption, scattering can also contribute to dichroism. This paper demonstrates that, based on the example of polyimide, materials can show tiny dichroism even far from electronic resonances due to scattering. Although the effect is small, it can lead to a measurable polarization change and might have influence on highly sensitive polarimetric experiments.
Abstract: High-brilliance synchrotron radiation sources have opened new avenues for x-ray polarization analysis that go far beyond conventional polarimetry in the optical domain. With linear x-ray polarizers in a crossed setting, polarization extinction ratios down to 10⁻¹⁰ can be achieved. This renders the method sensitive to probe the tiniest optical anisotropies that would occur, for example, in strong-field quantum electrodynamics due to vacuum birefringence and dichroism. Here we show that high-purity polarimetry can be employed to reveal electronic anisotropies in condensed matter systems with utmost sensitivity and spectral resolution. Taking CuO and La₂CuO₄ as benchmark systems, we present a full characterization of the polarization changes across the Cu K-absorption edge and their separation into dichroic and birefringent contributions. At diffraction-limited synchrotron radiation sources and x-ray lasers, where polarization extinction ratios of 10⁻¹² can be achieved, our method has the potential to assess birefringence and dichroism of the quantum vacuum in extreme electromagnetic fields.
Abstract: Ultrafast and precise control of quantum systems at x-ray energies involves photons with oscillation periods below 1 as. Coherent dynamic control of quantum systems at these energies is one of the major challenges in hard x-ray quantum optics. Here, we demonstrate that the phase of a quantum system embedded in a solid can be coherently controlled via a quasi-particle with subattosecond accuracy. In particular, we tune the quantum phase of a collectively excited nuclear state via transient magnons with a precision of 1 zs and a timing stability below 50 ys. These small temporal shifts are monitored interferometrically via quantum beats between different hyperfine-split levels.The experiment demonstrates zeptosecond interferometry and shows that transient quasi-particles enable accurate control of quantum systems embedded in condensed matter environments.