@phdthesis{Haseeb2023, author = {Haseeb, Haider}, title = {Charge and heat transport across interfaces in nanostructured porous silicon}, doi = {10.25932/publishup-61122}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-611224}, school = {Universit{\"a}t Potsdam}, pages = {84}, year = {2023}, abstract = {This thesis discusses heat and charge transport phenomena in single-crystalline Silicon penetrated by nanometer-sized pores, known as mesoporous Silicon (pSi). Despite the extensive attention given to it as a thermoelectric material of interest, studies on microscopic thermal and electronic transport beyond its macroscopic characterizations are rarely reported. In contrast, this work reports the interplay of both. PSi samples synthesized by electrochemical anodization display a temperature dependence of specific heat 𝐢𝑝 that deviates from the characteristic 𝑇^3 behaviour (at 𝑇<50𝐾). A thorough analysis reveals that both 3D and 2D Einstein and Debye modes contribute to this specific heat. Additional 2D Einstein modes (~3 π‘šπ‘’π‘‰) agree reasonably well with the boson peak of SiO2 in pSi pore walls. 2D Debye modes are proposed to account for surface acoustic modes causing a significant deviation from the well-known 𝑇^3 dependence of 𝐢𝑝 at 𝑇<50𝐾. A novel theoretical model gives insights into the thermal conductivity of pSi in terms of porosity and phonon scattering on the nanoscale. The thermal conductivity analysis utilizes the peculiarities of the pSi phonon dispersion probed by the inelastic neutron scattering experiments. A phonon mean-free path of around 10 π‘›π‘š extracted from the presented model is proposed to cause the reduced thermal conductivity of pSi by two orders of magnitude compared to p-doped bulk Silicon. Detailed analysis indicates that compound averaging may cause a further 10-50\% reduction. The percolation threshold of 65\% for thermal conductivity of pSi samples is subsequently determined by employing theoretical effective medium models. Temperature-dependent electrical conductivity measurements reveal a thermally activated transport process. A detailed analysis of the activation energy 𝐸𝐴𝜎 in the thermally activated transport exhibits a Meyer Neldel compensation rule between different samples that originates in multi-phonon absorption upon carrier transport. Activation energies 𝐸𝐴𝑆 obtained from temperature-dependent thermopower measurements provide further evidence for multi-phonon assisted hopping between localized states as a dominant charge transport mechanism in pSi, as they systematically differ from the determined 𝐸𝐴𝜎 values.}, language = {en} } @article{DebPopovaHehnetal.2019, author = {Deb, Marwan and Popova, Elena and Hehn, Michel and Keller, Niels and Petit-Watelot, Sebastien and Bargheer, Matias and Mangin, Stephane and Malinowski, Gregory}, title = {Femtosecond Laser-Excitation-Driven High Frequency Standing Spin Waves in Nanoscale Dielectric Thin Films of Iron Garnets}, series = {Physical review letters}, volume = {123}, journal = {Physical review letters}, number = {2}, publisher = {American Physical Society}, address = {College Park}, issn = {0031-9007}, doi = {10.1103/PhysRevLett.123.027202}, pages = {6}, year = {2019}, abstract = {We demonstrate that femtosecond laser pulses allow triggering high-frequency standing spin-wave modes in nanoscale thin films of a bismuth-substituted yttrium iron garnet. By varying the strength of the external magnetic field, we prove that two distinct branches of the dispersion relation are excited for all the modes. This is reflected in particular at a very weak magnetic field (similar to 33 mT) by a spin dynamics with a frequency up to 15 GHz, which is 15 times higher than the one associated with the ferromagnetic resonance mode. We argue that this phenomenon is triggered by ultrafast changes of the magnetic anisotropy via laser excitation of incoherent and coherent phonons. These findings open exciting prospects for ultrafast photo magnonics.}, language = {en} } @article{SarhanKoopmanSchuetzetal.2019, author = {Sarhan, Radwan Mohamed and Koopman, Wouter-Willem Adriaan and Schuetz, Roman and Schmid, Thomas and Liebig, Ferenc and Koetz, Joachim and Bargheer, Matias}, title = {The importance of plasmonic heating for the plasmondriven photodimerization of 4-nitrothiophenol}, series = {Scientific Reports}, volume = {9}, journal = {Scientific Reports}, publisher = {Macmillan Publishers Limited}, address = {London}, issn = {2045-2322}, doi = {10.1038/s41598-019-38627-2}, pages = {8}, year = {2019}, abstract = {Metal nanoparticles form potent nanoreactors, driven by the optical generation of energetic electrons and nanoscale heat. The relative influence of these two factors on nanoscale chemistry is strongly debated. This article discusses the temperature dependence of the dimerization of 4-nitrothiophenol (4-NTP) into 4,4β€²-dimercaptoazobenzene (DMAB) adsorbed on gold nanoflowers by Surface-Enhanced Raman Scattering (SERS). Raman thermometry shows a significant optical heating of the particles. The ratio of the Stokes and the anti-Stokes Raman signal moreover demonstrates that the molecular temperature during the reaction rises beyond the average crystal lattice temperature of the plasmonic particles. The product bands have an even higher temperature than reactant bands, which suggests that the reaction proceeds preferentially at thermal hot spots. In addition, kinetic measurements of the reaction during external heating of the reaction environment yield a considerable rise of the reaction rate with temperature. Despite this significant heating effects, a comparison of SERS spectra recorded after heating the sample by an external heater to spectra recorded after prolonged illumination shows that the reaction is strictly photo-driven. While in both cases the temperature increase is comparable, the dimerization occurs only in the presence of light. Intensity dependent measurements at fixed temperatures confirm this finding.}, language = {en} } @article{IurchukSchickBranetal.2016, author = {Iurchuk, V. and Schick, D. and Bran, J. and Colson, D. and Forget, A. and Halley, D. and Koc, Azize and Reinhardt, Mathias and Kwamen, C. and Morley, N. A. and Bargheer, Matias and Viret, M. and Gumeniuk, R. and Schmerber, G. and Doudin, B. and Kundys, B.}, title = {Optical Writing of Magnetic Properties by Remanent Photostriction}, series = {Physical review letters}, volume = {117}, journal = {Physical review letters}, publisher = {American Physical Society}, address = {College Park}, issn = {0031-9007}, doi = {10.1103/PhysRevLett.117.107403}, pages = {5}, year = {2016}, abstract = {We present an optically induced remanent photostriction in BiFeO3, resulting from the photovoltaic effect, which is used to modify the ferromagnetism of Ni film in a hybrid BiFeO3/Ni structure. The 75\% change in coercivity in the Ni film is achieved via optical and nonvolatile control. This photoferromagnetic effect can be reversed by static or ac electric depolarization of BiFeO3. Hence, the strain dependent changes in magnetic properties are written optically, and erased electrically. Light-mediated straintronics is therefore a possible approach for low-power multistate control of magnetic elements relevant for memory and spintronic applications.}, language = {en} } @article{ShaydukHerzogBojahretal.2013, author = {Shayduk, Roman and Herzog, Marc and Bojahr, Andre and Schick, Daniel and Gaal, Peter and Leitenberger, Wolfram and Navirian, Hengameh and Sander, Mathias and Goldshteyn, Jevgenij and Vrejoiu, Ionela and Bargheer, Matias}, title = {Direct time-domain sampling of subterahertz coherent acoustic phonon spectra in SrTiO3 using ultrafast x-ray diffraction}, series = {Physical review : B, Condensed matter and materials physics}, volume = {87}, journal = {Physical review : B, Condensed matter and materials physics}, number = {18}, publisher = {American Physical Society}, address = {College Park}, issn = {1098-0121}, doi = {10.1103/PhysRevB.87.184301}, pages = {7}, year = {2013}, abstract = {We synthesize sub-THz longitudinal quasimonochromatic acoustic phonons in a SrTiO3 single crystal using a SrRuO3/SrTiO3 superlattice as an optical-acoustic transducer. The generated acoustic phonon spectrum is determined using ultrafast x-ray diffraction. The analysis of the generated phonon spectrum in the time domain reveals a k-vector dependent phonon lifetime. It is observed that even at sub-THz frequencies the phonon lifetime agrees with the 1/omega(2) power law known from Akhiezer's model for hyper sound attenuation. The observed shift of the synthesized spectrum to the higher q is discussed in the framework of nonlinear effects appearing due to the high amplitude of the synthesized phonons.}, language = {en} } @article{ReinhardtKocLeitenbergeretal.2016, author = {Reinhardt, Matthias and Koc, Azize and Leitenberger, Wolfram and Gaal, Peter and Bargheer, Matias}, title = {Optimized spatial overlap in optical pump-X-ray probe experiments with high repetition rate using laser-induced surface distortions}, series = {Journal of synchrotron radiation}, volume = {23}, journal = {Journal of synchrotron radiation}, publisher = {International Union of Crystallography}, address = {Chester}, issn = {1600-5775}, doi = {10.1107/S1600577515024443}, pages = {474 -- 479}, year = {2016}, abstract = {Ultrafast X-ray diffraction experiments require careful adjustment of the spatial overlap between the optical excitation and the X-ray probe pulse. This is especially challenging at high laser repetition rates. Sample distortions caused by the large heat load on the sample and the relatively low optical energy per pulse lead to only tiny signal changes. In consequence, this results in small footprints of the optical excitation on the sample, which turns the adjustment of the overlap difficult. Here a method for reliable overlap adjustment based on reciprocal space mapping of a laser excited thin film is presented.}, language = {en} } @phdthesis{TchoumbaKwamen2018, author = {Tchoumba Kwamen, Christelle Larodia}, title = {Investigating the dynamics of polarization reversal in ferroelectric thin films by time-resolved X-ray diffraction}, doi = {10.25932/publishup-42781}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-427815}, school = {Universit{\"a}t Potsdam}, pages = {xvii, 126, xxiii}, year = {2018}, abstract = {Ferroic materials have attracted a lot of attention over the years due to their wide range of applications in sensors, actuators, and memory devices. Their technological applications originate from their unique properties such as ferroelectricity and piezoelectricity. In order to optimize these materials, it is necessary to understand the coupling between their nanoscale structure and transient response, which are related to the atomic structure of the unit cell. In this thesis, synchrotron X-ray diffraction is used to investigate the structure of ferroelectric thin film capacitors during application of a periodic electric field. Combining electrical measurements with time-resolved X-ray diffraction on a working device allows for visualization of the interplay between charge flow and structural motion. This constitutes the core of this work. The first part of this thesis discusses the electrical and structural dynamics of a ferroelectric Pt/Pb(Zr0.2,Ti0.8)O3/SrRuO3 heterostructure during charging, discharging, and polarization reversal. After polarization reversal a non-linear piezoelectric response develops on a much longer time scale than the RC time constant of the device. The reversal process is inhomogeneous and induces a transient disordered domain state. The structural dynamics under sub-coercive field conditions show that this disordered domain state can be remanent and can be erased with an appropriate voltage pulse sequence. The frequency-dependent dynamic characterization of a Pb(Zr0.52,Ti0.48)O3 layer, at the morphotropic phase boundary, shows that at high frequency, the limited domain wall velocity causes a phase lag between the applied field and both the structural and electrical responses. An external modification of the RC time constant of the measurement delays the switching current and widens the electromechanical hysteresis loop while achieving a higher compressive piezoelectric strain within the crystal. In the second part of this thesis, time-resolved reciprocal space maps of multiferroic BiFeO3 thin films were measured to identify the domain structure and investigate the development of an inhomogeneous piezoelectric response during the polarization reversal. The presence of 109Β° domains is evidenced by the splitting of the Bragg peak. The last part of this work investigates the effect of an optically excited ultrafast strain or heat pulse propagating through a ferroelectric BaTiO3 layer, where we observed an additional current response due to the laser pulse excitation of the metallic bottom electrode of the heterostructure.}, language = {en} } @article{DebPopovaHehnetal.2019, author = {Deb, Marwan and Popova, Elena and Hehn, Michel and Keller, Niels and Petit-Watelot, Sebastien and Bargheer, Matias and Mangin, Stephane and Malinowski, Gregory}, title = {Damping of Standing Spin Waves in Bismuth-Substituted Yttrium Iron Garnet as Seen via the Time-Resolved Magneto-Optical Kerr Effect}, series = {Physical review applied}, volume = {12}, journal = {Physical review applied}, number = {4}, publisher = {American Physical Society}, address = {College Park}, issn = {2331-7019}, doi = {10.1103/PhysRevApplied.12.044006}, pages = {7}, year = {2019}, abstract = {We investigate spin-wave resonance modes and their damping in insulating thin films of bismuth-substituted yttrium iron garnet by performing femtosecond magneto-optical pump-probe experiments. For large magnetic fields in the range below the magnetization saturation, we find that the damping of high-order standing spin-wave (SSW) modes is about 40 times lower than that for the fundamental one. The observed phenomenon can be explained by considering different features of magnetic anisotropy and exchange fields that, respectively, define the precession frequency for fundamental and high-order SSWs. These results provide further insight into SSWs in iron garnets and may be exploited in many new photomagnonic devices.}, language = {en} } @phdthesis{Jay2020, author = {Jay, Raphael Martin}, title = {Principles of charge distribution and separation}, school = {Universit{\"a}t Potsdam}, pages = {xi, 162}, year = {2020}, abstract = {The electronic charge distributions of transition metal complexes fundamentally determine their chemical reactivity. Experimental access to the local valence electronic structure is therefore crucial in order to determine how frontier orbitals are delocalized between different atomic sites and electronic charge is spread throughout the transition metal complex. To that end, X-ray spectroscopies are employed in this thesis to study a series of solution-phase iron complexes with respect to the response of their local electronic charge distributions to different external influences. Using resonant inelastic X-ray scattering (RIXS) and X-ray absorption spectroscopy (XAS) at the iron L-edge, changes in local charge densities are investigated at the iron center depending on different ligand cages as well as solvent environments. A varying degree of charge delocalization from the metal center onto the ligands is observed, which is governed by the capabilities of the ligands to accept charge density into their unoccupied orbitals. Specific solvents are furthermore shown to amplify this process. Solvent molecules of strong Lewis-acids withdraw charge from the ligand allowing in turn for more metal charge to be delocalized onto the ligand. The resulting local charge deficiencies at the metal center are, however, counteracted by competing electron-donation channels from the ligand towards the iron, which are additionally revealed. This is interpreted as a compensating effect which strives to maintain local charge densities at the iron center. This mechanism of charge density preservation is found to be of general nature. Using time-resolved RIXS and XAS at the iron L-edge, an analogous interplay of electron donation and back-donation channels is also revealed for the case of charge-transfer excited states. In such transient configurations, the electronic occupation of iron-centered frontier orbitals has been altered by an optical excitation. Changes in local charge densities that are expected to follow an increased or decreased population of iron-centered orbitals are, however, again counteracted. By scaling the degree of electron donation from the ligand onto the metal, local charge densities at the iron center can be efficiently maintained. Since charge-transfer excitations, however, often constitute the initial step in many electron transfer processes, these findings challenge common notions of charge-separation in transition metal dyes.}, language = {en} } @article{BojahrHerzogSchicketal.2012, author = {Bojahr, Andre and Herzog, Marc and Schick, Daniel and Vrejoiu, Ionela and Bargheer, Matias}, title = {Calibrated real-time detection of nonlinearly propagating strain waves}, series = {Physical review : B, Condensed matter and materials physics}, volume = {86}, journal = {Physical review : B, Condensed matter and materials physics}, number = {14}, publisher = {American Physical Society}, address = {College Park}, issn = {1098-0121}, doi = {10.1103/PhysRevB.86.144306}, pages = {5}, year = {2012}, abstract = {Epitaxially grown metallic oxide transducers support the generation of ultrashort strain pulses in SrTiO3 (STO) with high amplitudes up to 0.5\%. The strain amplitudes are calibrated by real-time measurements of the lattice deformation using ultrafast x-ray diffraction. We determine the speed at which the strain fronts propagate by broadband picosecond ultrasonics and conclude that, above a strain level of approx. 0.2\%, the compressive and tensile strain components travel at considerably different sound velocities, indicating nonlinear wave behavior. Simulations based on an anharmonic linear-chain model are in excellent accord with the experimental findings and show how the spectrum of coherent phonon modes changes with time.}, language = {en} }