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My thesis chiefly aims to shed light on the favourable properties of LHP semiconductors from the point of view of their electronic structure.
Currently, various hypotheses are circulating to explain the exceptionally favourable transport properties of LHPs. Seeking an explanation for the low non-radiative recombination rates and long carrier lifetimes is particularly interesting to the halide perovskites research community.
The first part of this work investigates the two main hypotheses that are believed to play a significant role: the existence of a giant Rashba effect and large polarons. The experimental method of ARPES is mainly applied to verify their credibility.
The first hypothesis presumes that a giant Rashba effect restricts the recombination losses of the charge carriers by making the band gap slightly indirect. The Rashba effect is based on a strong SOC that could appear in LHPs thanks to incorporating the heavy element Pb in their structure. Earlier experimental work had pointed out this effect at the VBM of a hybrid LHP as a viable explanation for the long lifetimes of the charge carriers.
My systematic ARPES studies on hybrid MAPbBr3 and spin-resolved ARPES studies on the inorganic CsPbBr3 disprove the presence of any Rashba effect in the VBM of the reported order of magnitude. Therefore, neither the spin texture nor an indirect band gap character at the VBM in the bulk or at the surface can explain the high efficiency of LHP. In case of existence, this effect is in terms of the Rashba parameter at least a factor of a hundred smaller than previously assumed.
The second hypothesis proposes large polaron formation in the electronic structure of LHPs and attributes it to their high defect tolerance and low non-radiative recombination rate. Because the perovskite structure consists of negative and positive ions, polarons of this kind can be expected due to the Coulomb interaction between carriers and the polar lattice at intermediate electron-phonon coupling strength. Their existence is proposed to screen the carriers and defects to avoid recombination and trapping, thus leading to long carrier lifetimes. ARPES results by one group supported this assumption, reporting a 50% effective mass enhancement over the theoretical effective mass for CsPbBr3 in the orthorhombic structure.
The current thesis examines this hypothesis experimentally by photon-energy-dependent ARPES spectra and theoretically by GW band calculations of CsPbBr3 perovskites. The investigation is based on the fact that a polaron contribution in charge transport can become evident by an increase of the effective mass as measured by ARPES over the calculated one without polaron effects. However, my experiments on crystalline CsPbBr3 did not imply a larger effective mass for which one could postulate large polarons. In fact, the effective masses determined from ARPES agree with that of theoretical predictions.
The second part of my thesis thoroughly investigates the possibility of spontaneously magnetizing LHPs by introducing Mn2+ ions. Mn doping was reported to cause ferromagnetism in one of the most common LHPs, MAPbI3, mediated by super-exchange. The current work investigates the magnetic properties of a wide concentration range of Mn-doped MAPbI3 and triple-cation films by XAS, XMCD, and SQUID measurements. Based on the XAS line shape and a sum-rule analysis of the XMCD spectra, a pure Mn2+ configuration has been confirmed. Negative Curie temperatures are extracted from fitting the magnetization with a Curie-Weiss law. However, a remanent magnetization, which would be an indication of the absence of ferromagnetism down to 2K. As far as the double exchange is concerned, the element-specific XAS excludes a sufficient amount of Mn3+ as a prerequisite for this mechanism. All the findings show no evidence of significant double exchange or ferromagnetism in Mn-doped LHPs. The magnetic behavior is paramagnetic rather than ferromagnetic.
In the dissertation's last chapter, orthorhombic features of CsPbBr3 are revealed by ARPES, including an extra VBM at the Γ-point. The VBM of CsPbBr3 shows a temperature-dependent splitting, which decreases by 190 meV between 38K and 300K and tracks a shift of a saddle point at the cubic M-point. It is possible to reproduce the energy shift using an atomic model with a larger unit cell for room temperature, allowing local inversion symmetry breaking. This indicates the importance of electric dipoles for the inorganic LHPs, which may contribute to their high efficiency by breaking inversion symmetry and a Berry-phase effect.
The first part of the thesis studies the properties of fast mode in magneto hydro-dynamic (MHD) turbulence. 1D and 3D numerical simulations are carried out to generate decaying fast mode MHD turbulence. The injection of waves are carried out in a collinear and isotropic fashion to generate fast mode turbulence. The properties of fast mode turbulence are analyzed by studying their energy spectral density, 2D structure functions and energy decay/cascade time. The injection wave vector is varied to study the dependence of the above properties on the injection wave vectors. The 1D energy spectrum obtained for the velocity and magnetic fields has 𝐸 (𝑘) ∝ 𝑘−2. The 2D energy spectrum and 2D structure functions in parallel and perpendicular directions shows that fast mode turbulence generated is isotropic in nature. The cascade/decay rate of fast mode MHD turbulence is proportional to 𝑘−0.5 for different kinds of wave vector injection. Simulations are also carried out in 1D and 3D to compare balanced and imbalanced turbulence. The results obtained shows that while 1D imbalanced turbulence decays faster than 1D balanced turbulence, there is no difference in the decay of 3D balanced and imbalanced turbulence for the current resolution of 512 grid points.
"The second part of the thesis studies cosmic ray (CR) transport in driven MHD turbulence and is strongly dependent on it’s properties. Test particle simulations are carried out to study CR interaction with both total MHD turbulence and decomposed MHD modes. The spatial diffusion coefficients and the pitch angle scattering diffusion coefficients are calculated from the test particle trajectories in turbulence. The results confirms that the fast modes dominate the CR propagation, whereas Alfvén, slow modes are much less efficient with similar pitch angle scattering rates. The cross field transport on large and small scales are investigated next. On large/global scales, normal diffusion is observed and the diffusion coefficient is suppressed by 𝑀𝜁𝐴 compared to the parallel diffusion coefficients, with 𝜁 closer to 4 in Alfvén modes than that in total turbulence as theoretically expected. For the CR transport on scales smaller than the turbulence injection scale 𝐿, both the local and global magnetic reference frames are adopted. Super diffusion is observed on such small scales in all the cases. Particularly, CR transport in Alfvén modes show clear Richardson diffusion in the local reference frame. The diffusion transition smoothly from the Richardson’s one with index 1.5 to normal diffusion as particle’s mean free path decreases from 𝜆∥ ≫ 𝐿 to 𝜆∥ ≪ 𝐿. These results have broad applications to CRs in various astrophysical environments".
Pranav, Manasi ; Hultzsch, Thomas ; Musiienko, Artem ; Sun, Bowen ; Shukla, Atul ; Jaiser, Frank ; Shoaee, Safa ; Neher, Dieter
Understanding the origin of inefficient photocurrent generation in organic solar cells with low energy offset remains key to realizing high-performance donor-acceptor systems. Here, we probe the origin of field-dependent free-charge generation and photoluminescence in wnon-fullereneacceptor (NFA)-based organic solar cells using the polymer PM6 and the NFA Y5-a non-halogenated sibling to Y6, with a smaller energetic offset to PM6. By performing time-delayed collection field (TDCF) measurements on a variety of samples with different electron transport layers and active layer thickness, we show that the fill factor and photocurrent are limited by field-dependent free charge generation in the bulk of the blend. We also introduce a new method of TDCF called m-TDCF to prove the absence of artifacts from non-geminate recombination of photogenerated and dark charge carriers near the electrodes. We then correlate free charge generation with steady-state photoluminescence intensity and find perfect anticorrelation between these two properties. Through this, we conclude that photocurrent generation in this low-offset system is entirely controlled by the field-dependent dissociation of local excitons into charge-transfer states. (c) 2023 Author(s).
When two initially thermal many-body systems start to interact strongly, their transient states quickly become non-Gibbsian, even if the systems eventually equilibrate. To see beyond this apparent lack of structure during the transient regime, we use a refined notion of thermality, which we call g-local. A system is g-locally thermal if the states of all its small subsystems are marginals of global thermal states. We numerically demonstrate for two harmonic lattices that whenever the total system equilibrates in the long run, each lattice remains g-locally thermal at all times, including the transient regime. This is true even when the lattices have long-range interactions within them. In all cases, we find that the equilibrium is described by the generalized Gibbs ensemble, with three-dimensional lattices requiring special treatment due to their extended set of conserved charges. We compare our findings with the well-known two-temperature model. While its standard form is not valid beyond weak coupling, we show that at strong coupling it can be partially salvaged by adopting the concept of a g-local temperature.
The evolution of a galaxy is pivotally governed by its pattern of star formation over a given period of time. The star formation rate at any given time is strongly dependent on the amount of cold gas available in the galaxy. Accretion of pristine gas from the Intergalactic medium (IGM) is thought to be one of the primary sources for star-forming gas. This gas first passes through the virial regions of the galaxy before reaching the Interstellar medium (ISM), the hub of star formation. On the other hand, owing to the evolutionary course of young and massive stars, energetic winds are ejected from the ISM to the virial regions of the galaxy. A bunch of interlinked, complex astrophysical processes, arising from the concurrent presence of both infalling as well as outbound gas, play out over a range of timescales in the halo region or the Circumgalactic medium (CGM) of a galaxy. It would not be incorrect to say that the CGM has a stronghold over the gas reserves of a galaxy and thus, plays a backhand, yet, rather pivotal role in shaping many galactic properties, some of which are also readily observable. Observing the multi-phase CGM (via spectral-line ion measurements), however, remains a non-trivial effort even today. Low particle densities as well as the CGM’s vast spatial extent, coupled with likely deviations from a spherical distribution, marr the possibility of obtaining complete, unbiased, high-quality spectral information tracing the full extent of the gaseous halo. This often incomplete information leads to multiple inferences about the CGM properties that give rise to multiple contradicting models. In this regard, computer simulations offer a neat solution towards testing and, subsequently, falsifying many of these existing CGM models. Thanks to their controlled environments, simulations are able to not only effortlessly transcend several orders of magnitude in time and space, but also get around many of the observational limitations and provide some unique views on many CGM properties. In this thesis, I focus on effectively using different computer simulations to understand the role of CGM in various astrophysical contexts, namely, the effect of Local Group (LG) environment, major merger events and satellite galaxies. In Chapter 2, I discuss the approach used for modeling various phases of the simulated z = 0 LG CGM in Hestia constrained simulations. Each of the three realizations contain a Milky Way (MW)–Andromeda (M31) galaxy pair, along with their corresponding sets of satellite galaxies, all embedded within the larger cosmological context. For characterizing the different temperature–density phases within the CGM, I model five tracer ions with cloudy ionization modeling. The cold and cool–ionized CGM (H i and Si iii respectively) in Hestia is very clumpy and distributed close to the galactic centers, while the warm-hot and hot CGM (O vi, O vii and O viii) is tenuous and volume-filling. On comparing the H i and Si iii column densities for the simulated M31 with observational measurements from Project AMIGA survey and other low-z galaxies, I found that Hestia galaxies produced less gas in the outer CGM, unlike observations. My carefully designed observational bias model subsequently revealed the possibility that some MW gas clouds might be incorrectly associated with the M31 CGM in observations, and hence, may be partly responsible for giving rise to the detected mismatch between simulated data and observations. In Chapter 3, I present results from four zoom–in, major merger, gas–rich simulations and the subsequent role of the gas, originally situated in the CGM, in influencing some of the galactic observables. The progenitor parameters are selected such that the post–merger remnants are MW–mass galaxies. We generally see a very clear gas bridge joining the merging galaxies in case of multiple passage mergers while such a bridge is mostly absent when a direct collision occurs. On the basis of particle–to–galaxy distance computations and tracer particle analysis, I found that about 33–48 percent of the cold gas contributing to the merger–induced star formation in the bridge originated from the CGM regions. In Chapter 4, I used a sample of 234 MW-mass, L* galaxies from the TNG50 cosmological simulations, with an aim of characterizing the impact of their global satellite populations on the extended cold CGM properties of their host L* halos. On the basis of halo mass and number of satellite galaxies (N_sats ), I categorized the sample into low and high mass bins, and subsequently into bottom, inter and top quartiles respectively. After confirming that satellites indeed influence the extended cold halo gas density profiles of the host galaxies, I investigated the effects of different satellite population parameters on the host halo cold CGMs. My analysis showed that there is hardly any cold gas associated with the satellite population of the lowest mass halos. The stellar mass of the most massive satellite (M_*mms ) impacted the cold gas in low mass bin halos the most, while N_sats (followed by M_*mms ) was the most influential factor for the high mass halos. In any case, how easily cold gas was stripped off the most massive satellite did not play much role. The number of massive (Stellar mass, M* > 10^8 M_solar) satellites as well as the M_*mms associated with a galaxy are two of the most crucial parameters determining how much cold gas ultimately finds its way from the satellites to the host halo. Low mass galaxies are found rather lacking on both these fronts unlike their high mass counterparts. This work highlights some aspects of the complex gas physics that constitute the basic essence of a low-z CGM. My analysis proved the importance of a cosmological environment, local surroundings and merger history in defining some key observable properties of a galactic CGM. Furthermore, I found that different satellite properties were responsible for affecting the cold–dense CGM of the low and high-mass parent galaxies. Finally, the LG emerged as an exciting prospect for testing and pinning down several intricate details about the CGM.
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 𝐶𝑝 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 𝑚𝑒𝑉) 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 𝐶𝑝 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 𝑛𝑚 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.
The study addresses the question, if observed changes in terms of Arctic-midlatitude linkages during winter are driven by Arctic Sea ice decline alone or if the increase of global sea surface temperatures plays an additional role. We compare atmosphere-only model experiments with ECHAM6 to ERA-Interim Reanalysis data. The model sensitivity experiment is implemented as a set of four combinations of sea ice and sea surface temperature boundary conditions. Atmospheric circulation regimes are determined and evaluated in terms of their cyclone and blocking characteristics and changes in frequency during winter. As a prerequisite, ECHAM6 reproduces general features of circulation regimes very well. Tropospheric changes induced by the change of boundary conditions are revealed and further impacts on the large-scale circulation up into the stratosphere are investigated. In early winter, the observed increase of atmospheric blocking in the region between Scandinavia and the Urals are primarily related to the changes in sea surface temperatures. During late winter, we f nd a weakened polar stratospheric vortex in the reanalysis that further impacts the troposphere. In the model sensitivity study a climatologically weakened polar vortex occurs only if sea ice is reduced and sea surface temperatures are increased together. This response is delayed compared to the reanalysis. The tropospheric response during late winter is inconclusive in the model, which is potentially related to the weak and delayed response in the stratosphere. The model experiments do not reproduce the connection between early and late winter as interpreted from the reanalysis. Potentially explaining this mismatch, we identify a discrepancy of ECHAM6 to reproduce the weakening of the stratospheric polar vortex through blocking induced upward propagation of planetary waves.
Mattern, Maximilian ; Pudell, Jan-Etienne ; Dumesnil, Karine ; Reppert, Alexander von ; Bargheer, Matias
Using time-resolved x-ray diffraction, we demonstrate the manipulation of the picosecond strain response of a metallic heterostructure consisting of a dysprosium (Dy) transducer and a niobium (Nb) detection layer by an external magnetic field. We utilize the first-order ferromagnetic–antiferromagnetic phase transition of the Dy layer, which provides an additional large contractive stress upon laser excitation compared to its zerofield response. This enhances the laser-induced contraction of the transducer and changes the shape of the picosecond strain pulses driven in Dy and detected within the buried Nb layer. Based on our experiment with rare-earth metals we discuss required properties for functional transducers, which may allow for novel field-control of the emitted picosecond strain pulses.
Mattern, Maximilian ; Pudell, Jan-Etienne ; Dumesnil, Karine ; Reppert, Alexander von ; Bargheer, Matias
Using time-resolved x-ray diffraction, we demonstrate the manipulation of the picosecond strain response of a metallic heterostructure consisting of a dysprosium (Dy) transducer and a niobium (Nb) detection layer by an external magnetic field. We utilize the first-order ferromagnetic–antiferromagnetic phase transition of the Dy layer, which provides an additional large contractive stress upon laser excitation compared to its zerofield response. This enhances the laser-induced contraction of the transducer and changes the shape of the picosecond strain pulses driven in Dy and detected within the buried Nb layer. Based on our experiment with rare-earth metals we discuss required properties for functional transducers, which may allow for novel field-control of the emitted picosecond strain pulses.
Di Bello, Costantino ; Hartmann, Alexander K. ; Majumdar, Satya N. ; Mori, Francesco ; Rosso, Alberto ; Schehr, Gregory
We consider a system of noninteracting particles on a line with initial positions distributed uniformly with density ? on the negative half-line. We consider two different models: (i) Each particle performs independent Brownian motion with stochastic resetting to its initial position with rate r and (ii) each particle performs run -and-tumble motion, and with rate r its position gets reset to its initial value and simultaneously its velocity gets randomized. We study the effects of resetting on the distribution P(Q, t) of the integrated particle current Q up to time t through the origin (from left to right). We study both the annealed and the quenched current distributions and in both cases, we find that resetting induces a stationary limiting distribution of the current at long times. However, we show that the approach to the stationary state of the current distribution in the annealed and the quenched cases are drastically different for both models. In the annealed case, the whole distribution P-an(Q, t) approaches its stationary limit uniformly for all Q. In contrast, the quenched distribution P-qu(Q, t) attains its stationary form for Q < Q(crit)(t), while it remains time dependent for Q > Q(crit)(t). We show that Q(crit)(t) increases linearly with t for large t. On the scale where Q <; Q(crit)(t), we show that P-qu(Q, t) has an unusual large deviation form with a rate function that has a third-order phase transition at the critical point. We have computed the associated rate functions analytically for both models. Using an importance sampling method that allows to probe probabilities as tiny as 10-14000, we were able to compute numerically this nonanalytic rate function for the resetting Brownian dynamics and found excellent agreement with our analytical prediction.