In this thesis we investigate dynamical correlations of spin systems at finite temperature. Especially we focus on the anomalous decoherence effects found previously in experiments of several quantum magnets. We develop and apply a diagrammatic perturbative approach, which incorporates the hard-core bosonic nature of spin excitations. This allows for a computation of the leading low-temperature contributions to the spectral function. The Jordan-Wigner transformation is used to benchmark the approach against exact results of the XX-chain in a strong transverse field. To tackle also more complex problems and vertex corrections we combine the approach with effective models derived by continuous unitary transformations. We perform an in-depth analysis of the approach to assess its properties in the context of conserving approximations in the sense of Baym and Kadanoff. The key result of this thesis is the investigation of two quantum magnets: BaCu2V2O8 and Cu(NO3)2·2.5D2O. We show that the anomalous decoherence observed can be traced back to non-trivial scattering processes of the hard-core bosonic excitations. This indicates, that quantum coherence plays a significant rolein describing dynamical correlations, even at finite temperature. Finally we show, how additional interactions can be taken into account in the full diagrammatic approach, going beyond a mean-field decoupling.
In this thesis we investigate dynamical correlations of spin systems at finite temperature. Especially we focus on the anomalous decoherence effects found previously in experiments of several quantum magnets. We develop and apply a diagrammatic perturbative approach, which incorporates the hard-core bosonic nature of spin excitations. This allows for a computation of the leading low-temperature contributions to the spectral function. The Jordan-Wigner transformation is used to benchmark the approach against exact results of the XX-chain in a strong transverse field. To tackle also more complex problems and vertex corrections we combine the approach with effective models derived by continuous unitary transformations. We perform an in-depth analysis of the approach to assess its properties in the context of conserving approximations in the sense of Baym and Kadanoff. The key result of this thesis is the investigation of two quantum magnets: BaCu2V2O8 and Cu(NO3)2·2.5D2O. We show that the anomalous decoherence observed can be traced back to non-trivial scattering processes of the hard-core bosonic excitations. This indicates, that quantum coherence plays a significant rolein describing dynamical correlations, even at finite temperature. Finally we show, how additional interactions can be taken into account in the full diagrammatic approach, going beyond a mean-field decoupling.
Complex interactions in quantum magnets lead to a variety of phases with manifold correlations, which are measurable at temperatures very low compared to the energy scale of the system. The common expectation is that quantum effects are just suppressed upon increasing temperature due to the additional thermal fluctuations. However, recent inelastic neutron scattering investigations in one- and three-dimensional compounds indicate that interplay between quantum and thermal effects is much more complicated. By combining high-resolution neutron resonance spin-echo measurements with diagrammatic perturbation theory, the authors show that anomalous decoherence effects can also be observed in the time domain, the natural domain for decaying correlations. This offers a complementary view on this phenomenon, allowing for a direct comparison between experimental data and theoretical prediction without the need for intensive data analysis. The specific form of the echo amplitude, in combination with the temperature dependence of the spectral weight, provides a smoking gun signature for nontrivial scattering processes of hard-core bosonic excitations.
The dynamics in quantum magnets can often be described by effective models with bosonic excitations obeying a hard-core constraint. Such models can be systematically derived by renormalization schemes such as continuous unitary transformations or by variational approaches. Even in the absence of further interactions the hard-core constraint makes the dynamics of the hard-core bosons nontrivial. Here, we develop a systematic diagrammatic approach to the spectral properties of hard-core bosons at finite temperature. Starting from an expansion in the density of thermally excited bosons in a system with an energy gap, our approach leads to a summation of ladder diagrams. Conceptually, the approach is not restricted to one dimension, but the one-dimensional case offers the opportunity to gauge the method by comparison to exact results obtained via a mapping to Jordan-Wigner fermions. In particular, we present results for the thermal broadening of single-particle spectral functions at finite temperature. The line shape is found to be asymmetric at elevated temperatures and the bandwidth of the dispersion narrows with increasing temperature. Additionally, the total number of thermally excited bosons is calculated and compared to various approximations and analytic results. Thereby, a flexible approach is introduced that can also be applied to more sophisticated and higher dimensional models.
This thesis is concerned with the numerical study of one-dimensional (1D) spin-1/2 quantum magnets and related method development. Its focus is on the calculation of dynamical spin correlation functions both at zero and finite temperature. This is motivated by the accessibility of dynamical quantities in experiments such as inelastic neutron scattering (INS) and electron spin resonance (ESR). The numerical methods used in this thesis are based on extensions of the density-matrix renormalization group (DMRG) and are formulated in the framework of matrix product states (MPS). While zero-temperature dynamical correlation functions are computed with existing MPS frequency-domain methods, an MPS frequency-domain approach for their calculation at finite temperature is developed in this thesis. The new method combines the Liouville-space formulation of the dynamics with a moment expansion of the dynamical correlation function. The majority of the results are obtained via MPS-based Chebyshev expansions. These numerical techniques are applied to two different model systems describing real materials. The first one is the material copper pyrimidine dinitrate (Cu-PM) which is modeled by a 1D spin-1/2 Heisenberg antiferromagnet with Dzyaloshinskii-Moriya interactions. The spin dynamics of this model is studied in an applied magnetic field and compared to ESR experiments. Zero-temperature calculations for momentum- and frequency-resolved dynamical quantities give direct access to the intensity of the elementary excitations and go beyond the low-energy description by the quantum sine-Gordon model. Thus, a deviation from the Lorentz invariant dispersion for the single-soliton resonance is found. The presence of the strongest boundary bound state previously predicted from a boundary sine-Gordon field theory is confirmed, while composite boundary-bulk excitations have too low intensities to be found in the numerical results. At finite temperature, there is a temperature-induced crossover of the soliton. Moreover, additional temperature effects such as interbreather transitions emerge, which is confirmed by accompanying ESR experiments on Cu-PM over a wide range of the applied field strength. The second system studied in this thesis is the compound BaCu2V2O8. It is shown that the magnetic properties of this quasi-1D material can be described by a strongly alternating antiferromagnetic-ferromagnetic spin-1/2 Heisenberg chain. As found for other dimerized systems, the strong correlations in BaCu2V2O8 persist even at elevated temperatures. Moreover, these correlations lead to an asymmetric lineshape broadening of the magnetic excitations at finite temperature. Upon raising the temperature, an increasingly asymmetric lineshape is observed in high-resolution INS experiments for BaCu2V2O8. In this thesis, the lineshape is calculated by the MPS finite-temperature method developed as a part of this work. Comparing these results to the INS data and the lineshape obtained by a diagrammatic approach, excellent agreement is found over a broad temperature range. This demonstrates that coherent quantum behavior persists at elevated temperatures in BaCu2V2O8 and that it can be predicted quantitatively.
We investigate how dynamic correlations of hard-core bosonic excitation at finite temperature are affected by additional interactions besides the hard-core repulsion which prevents them from occupying the same site. We focus especially on dimerized spin systems, where these additional interactions between the elementary excitations, triplons, lead to the formation of bound states, relevant for the correct description of scattering processes. In order to include these effects quantitatively, we extend the previously developed Br\"uckner approach to include also nearest-neighbor (NN) and next-nearest neighbor (NNN) interactions correctly in a low-temperature expansion. This leads to the extension of the scalar Bethe-Salpeter equation to a matrix-valued equation. As an example, we consider the Heisenberg spin ladder to illustrate the significance of the additional interactions on the spectral functions at finite temperature, which are proportional to inelastic neutron scattering rates.
This thesis is devoted to diagrammatic frameworks for computing the dynamic structure factor (DSF) and the static susceptibility of spin systems at finite temperature in the thermodynamic limit. We consider two complementary diagrammatic frameworks. First, we study functional renormalization group (FRG) approaches based on pseudo-fermion (pf-FRG) and pseudo-Majorana (pm-FRG) representations. Second, we develop high-order strong-coupling and high-temperature expansions (HTE) using free and restricted-graph techniques. To enable finite-temperature calculations in pf-FRG, we eliminate unphysical states by incorporating the Popov–Fedotov trick. Within pm-FRG, we introduce a temperature-flow scheme that significantly improves the efficiency and accuracy of finite-size scaling analyses of thermal phase transitions. We further extend pm-FRG to include external magnetic fields, allowing treatment of XXZ models with a field along the z direction. While the pseudo-Majorana representation maps local spin-1/2 operators to free Majorana fermions, higher spin values S>1/2 can instead be represented as strongly interacting real bosons, an idea underlying the recently proposed spin-FRG. Rather than implementing the spin-FRG itself, we analyze its perturbation series using a strong-coupling expansion. To evaluate the high-dimensional imaginary-time integrals arising in this expansion analytically with efficient bookkeeping, we introduce the kernel trick, which rewrites any Matsubara diagram in terms of the partial spectral functions of its constituent Green’s functions. The resulting fourth-order strong-coupling expansion for general spin S provides systematic beyond-mean-field corrections to critical temperatures and fields in both 1/d and large-interaction-range expansions. More importantly, it provides an analytic explanation of the long-standing quantum-to-classical correspondence observed in diagrammatic Monte Carlo simulations: the normalized static susceptibilities of quantum and classical Heisenberg models coincide after a simple temperature rescaling. Our analysis shows that this arises from the fact that the static susceptibility is well approximated by a simple functional form akin to a mean-field susceptibility, which we call the renormalized-mean-field form. To reach higher orders, we generalize the HTE to Matsubara-frequency-resolved Green’s functions (Dyn-HTE). This includes the static susceptibility (at zero Matsubara frequency) as a special case and validates the renormalized-mean-field form up to 12th order in perturbation theory. By analytically continuing the frequency dependence obtained from Dyn-HTE using a continued-fraction expansion, we compute DSFs for one-parameter Heisenberg models on arbitrary lattices, which can be directly compared with experimental inelastic neutron-scattering spectra. All Dyn-HTE calculations are implemented in a publicly available, well-documented open-source code. Finally, we clarify the relation between pseudo-Majorana and spin-based diagrammatic approaches by deriving the exact pseudo-Majorana action directly from the spin Hamiltonian, without invoking any parton representation. This derivation paves the way for extending Majorana-based methods to higher-spin systems.
This thesis is dedicated to a theoretical study of the 1-band Hubbard model in the strong coupling limit. The investigation is based on the Dynamical Cluster Approximation (DCA) which systematically restores non-local corrections to the Dynamical Mean Field approximation (DMFA). The DCA is formulated in momentum space and is characterised by a patching of the Brillouin zone where momentum conservation is only recovered between two patches. The approximation works well if k-space correlation functions show a weak momentum dependence. In order to study the temperature and doping dependence of the spin- and charge excitation spectra, we explicitly extend the Dynamical Cluster Approximation to two-particle response functions. The full irreducible two-particle vertex with three momenta and frequencies is approximated by an effective vertex dependent on the momentum and frequency of the spin and/or charge excitations. The effective vertex is calculated by using the Quantum Monte Carlo method on the finite cluster whereas the analytical continuation of dynamical quantities is performed by a stochastic version of the maximum entropy method. A comparison with high temperature auxiliary field quantum Monte Carlo data serves as a benchmark for our approach to two-particle correlation functions. Our method can reproduce basic characteristics of the spin- and charge excitation spectrum. Near and beyond optimal doping, our results provide a consistent overall picture of the interplay between charge, spin and single-particle excitations: a collective spin mode emerges at optimal doping and sufficiently low temperatures in the spin response spectrum and exhibits the energy scale of the magnetic exchange interaction J. Simultaneously, the low energy single-particle excitations are characterised by a coherent quasiparticle with bandwidth J. The origin of the quasiparticle can be quite well understood in a picture of a more or less antiferromagnetic ordered background in which holes are dressed by spin-excitations to allow for a coherent motion. By increasing doping, all features which are linked to the spin-polaron vanish in the single-particle as well as two-particle spin response spectrum. In the second part of the thesis an analysis of superconductivity in the Hubbard model is presented. The superconducting instability is implemented within the Dynamical Cluster Approximation by essentially allowing U(1) symmetry breaking baths in the QMC calculations for the cluster. The superconducting transition temperature T_c is derived from the d-wave order parameter which is directly estimated on the Monte Carlo cluster. The critical temperature T_c is in astonishing agreement with the temperature scale estimated by the divergence of the pair-field susceptibility in the paramagnetic phase. A detailed study of the pseudo and superconducting gap is continued by the investigation of the local and angle-resolved spectral function.