Antiferromagnetic spin-1/2 ladders have been studied in theoretical and experimental physics for several years. The spin ladder is a good model to bridge between theory and experiment, because it is realized in the copper oxide family Sr14-x(La,Ca)xCu24O41. These copper oxides consist of alternating layers of edge-sharing chains and ladders. The insulating mother compound Sr14Cu24O41 is hole doped in the chains as well as slightly in the ladders. The hole content in the Sr14Cu24O41 ladders is reduced, if La3+ is substituted for Sr2+ resulting in a pure antiferromagnetic spin ladder given by La4Sr10Cu24O41. In this thesis such spin ladders are studied by an amalgamated approach of theoretical work and experiments. For the La4Sr10Cu24O41 ladder the temperature development is investigated using scattering techniques as well as computer modelling. At zero temperature the spin ladder has already been well described by effective models computed via perturbative continuous unitary transformations (PCUTs). These PCUT results are now combined with a mean field approach allowing for incorporation of temperature induced conditional excitations via vertex corrections. The vertex correction results in a decreasing one-triplon spectral weight upon increasing temperature. This effect is studied by inelastic neutron scattering (INS) on La4Sr10Cu24O41 crystals by measuring the scattering amplitude at various temperatures. Convincing agreement is found within the experimental and theoretical error bars. Additionally the coupling constants found in Ref. [1] could be confirmed. The importance of an inter-ladder coupling Jinter between isolated ladders in the plane is investigated by combination of the PCUT with a mean field approach. This calculation is undertaken for the square and the trellis lattice. The difference to the existing calculations [2], [3] and [4] is the partial inclusion of the hardcore interaction for neighbouring ladders. At zero temperature we reveal the effect of quantum fluctuations on the spin gap. In the case of the square lattice we find the closure of the spin gap at a critical inter-ladder coupling enlarged by 3 - 4%. In the case of the trellis lattice, the spin gap decreases also as a function of inter-ladder coupling. In this case we find an enlarged critical inter-ladder coupling up to 21%. In additon, the theoretically predicted shift of the spectral weight by Uhrig and Schmidt could experimentally be confirmed. Substituting Ca2+ for Sr2+ results in hole doped ladders, such as Sr2.5Ca11.5Cu24O41 and Sr8Ca6Cu24O41, where the hole doping depends on the substituted Ca2+ content. The magnetic spectra of these two doped ladders are measured by INS and compared with the undoped ladder La4Sr10Cu24O41. The comparison reveals new features tracing back to the presence of holes. At low temperature in both compounds scattering below the gap of the undoped ladder is found resulting in a subgap1 state at about 8meV. The subgap broadens at high temperature so much that the closing of the subgap results. Additionally for both dopings and at low and high temperature a hole-pair captured by triplons is found with a fixed energy gap at 23meV. The new features are qualitatively explained in terms of resonant valence bond theory (RVB) as well as stripe ordering theory.
Antiferromagnetic spin-1/2 ladders have been studied in theoretical and experimental physics for several years. The spin ladder is a good model to bridge between theory and experiment, because it is realized in the copper oxide family Sr14-x(La,Ca)xCu24O41. These copper oxides consist of alternating layers of edge-sharing chains and ladders. The insulating mother compound Sr14Cu24O41 is hole doped in the chains as well as slightly in the ladders. The hole content in the Sr14Cu24O41 ladders is reduced, if La3+ is substituted for Sr2+ resulting in a pure antiferromagnetic spin ladder given by La4Sr10Cu24O41. In this thesis such spin ladders are studied by an amalgamated approach of theoretical work and experiments. For the La4Sr10Cu24O41 ladder the temperature development is investigated using scattering techniques as well as computer modelling. At zero temperature the spin ladder has already been well described by effective models computed via perturbative continuous unitary transformations (PCUTs). These PCUT results are now combined with a mean field approach allowing for incorporation of temperature induced conditional excitations via vertex corrections. The vertex correction results in a decreasing one-triplon spectral weight upon increasing temperature. This effect is studied by inelastic neutron scattering (INS) on La4Sr10Cu24O41 crystals by measuring the scattering amplitude at various temperatures. Convincing agreement is found within the experimental and theoretical error bars. Additionally the coupling constants found in Ref. [1] could be confirmed. The importance of an inter-ladder coupling Jinter between isolated ladders in the plane is investigated by combination of the PCUT with a mean field approach. This calculation is undertaken for the square and the trellis lattice. The difference to the existing calculations [2], [3] and [4] is the partial inclusion of the hardcore interaction for neighbouring ladders. At zero temperature we reveal the effect of quantum fluctuations on the spin gap. In the case of the square lattice we find the closure of the spin gap at a critical inter-ladder coupling enlarged by 3 - 4%. In the case of the trellis lattice, the spin gap decreases also as a function of inter-ladder coupling. In this case we find an enlarged critical inter-ladder coupling up to 21%. In additon, the theoretically predicted shift of the spectral weight by Uhrig and Schmidt could experimentally be confirmed. Substituting Ca2+ for Sr2+ results in hole doped ladders, such as Sr2.5Ca11.5Cu24O41 and Sr8Ca6Cu24O41, where the hole doping depends on the substituted Ca2+ content. The magnetic spectra of these two doped ladders are measured by INS and compared with the undoped ladder La4Sr10Cu24O41. The comparison reveals new features tracing back to the presence of holes. At low temperature in both compounds scattering below the gap of the undoped ladder is found resulting in a subgap1 state at about 8meV. The subgap broadens at high temperature so much that the closing of the subgap results. Additionally for both dopings and at low and high temperature a hole-pair captured by triplons is found with a fixed energy gap at 23meV. The new features are qualitatively explained in terms of resonant valence bond theory (RVB) as well as stripe ordering theory.
This thesis describes the neutron scattering measurements of magnetic excitations in \nspin-chains and ladders. The first part discusses an experimental investigation of the copper oxide family Srâ â Cuâ â Oâ â composed of edge-sharing chains and spin-ladders. \nThe study of Laâ Srâ â Cuâ â Oâ â comprises a slightly hole-doped chain and an undoped ladder structure where the chain can be modeled by a ferromagnetic nearest and an \nantiferromagnetic next-nearest neighbor coupling. The hole effects are apparent in gaps in the dispersion relation and can be described by a charge-density wave agreeing with the commensuration of the dispersion. Investigating the undoped ladder establishes \nthe exchange constants including a cyclic exchange manifested by the two-magnon \ncontinuum and the suppression of the S = 1 bound mode. An orbital consideration \nprovides an explanation for the exchanges including the different sizes of rung and \nleg coupling. The excitation spectrum of the doped ladder in Caâ .â Srâ â .â Cuâ â Oâ â can be \ndescribed by a direct comparison with the undoped ladder and the differences consisting \nof a higher energy mode and subgap scattering can be successfully modeled by the charge spectrum of the ladder calculated from the free electron model. The second part of the thesis investigates the alternating chain material Cu(NOâ )â · 2.5D2O and establishes the gapped one-magnon dispersion, the two-magnon continuum and for the first time the S =1 bound mode. Applying magnetic field drives the system through two critical field transitions, condensation of magnons into the ground state and saturation. The modes beyond saturation can be modeled by spin wave theory and the excitations at the first critical field follow Luttinger Liquid behavior. Additionally investigated are the temperature effects with the excitations being of a different nature but containing the signature of a strong correlated system. For an outlook the measurements including temperature and field are provided with further theoretical descriptions necessary.
In the framework of this thesis the infrared spectra of two-leg spin ladders were measured. This study presents the first determination of the magnetic contribution to the optical conductivity of spin ladders. A comparison between experiment and new theoretical calculations provided a comprehensive understanding of the magnetic spectrum of the undoped telephone-number compounds La(y)Ca(14-y)Cu(24)O(41). To be able to study the weak magnetic contribution to the spectra, it was necessary to measure not only the reflectance but in particular the transmittance of thin single crystals. When both quantities are known, one can directly calculate the optical conductivity. The low-temperature spectra were compared with results of three different theoretical approaches in close collaboration with the theory groups of Uhrig et al. from the University of Cologne and of Kopp et al. from the University of Augsburg. The excellent agreement between theory and experiment allowed us to identify the two sharp peaks in the mid-infrared range unambiguously as the signature of a true bound state of two triplets. The occurrence of bound states in spin ladders had been predicted already by several groups, but we provided the first experimental verification. Further spectral weight at higher frequencies was attributed to the multi-triplet continuum. The exchange couplings were derived, and the importance of the four-spin cyclic exchange was demonstrated. With increasing temperature especially the line shape for polarization along the legs changes considerably. The spectral weight of the continuum strongly grows, whereas the bound-state peaks lose weight. The resemblance between the measured room-temperature data of the S=1/2 ladder and theoretical results for the S=1 Haldane chain was discussed. The corresponding calculations were performed by Nunner et al. in Augsburg. Another main part of this thesis was to examine the influence of doping on the infrared spectra. We observed the same bound-state features in Sr(14)Cu(24)O(41) as in the undoped compounds, but we found additional structure in the spectra. Several scenarios were discussed in order to explain the new features, including the modulation of the exchange coupling along the legs due to the incommensurate structure and due to the charge order in the chains.
A proper theoretical description of doped antiferromagnets is until now an unresolved issue. In this work we study chain and ladder systems, and in particularly we focus on the physically most interesting two leg ladder. Our starting point is the Spin Fermion model in which an antiferromagnetic background of localized spins interacts with mobile holes via a rotation invariant Kondo-like term. The interesting region of the phase diagram is that close to the Mott-insulator transition where the doping delta is zero. At zero doping in fact the system is an insulator and the spins organize themselves in a spin liquid, a rotational invariant state characterized by a finite correlation length and an energy gap (a spin gap) above the ground state. Such a state is also the ground state of a field theory, the non linear sigma model (NLsigmaM) which is recognized as the low energy effective theory for antiferromagnetic spin ladder. The first question we answer is how such a spin state evolves as one moves off from the Mott phase by increasing the doping. Integrating out the fermions in our model we obtain an effective theory for the spins which we are able to evaluate in the continuum limit. The effective theory is again a NLsigmaM with coupling constants which depend on the concentration of dopant holes. In contrast to existing mean field calculation our theory predicts a lowering of the spin gap with doping and a consequent increase in the correlation length. Indeed a lowering of the spin gap due to doping is also observed in numerical simulation and on NMR experiments on $Sr14-xCaxCu24O41 with which we obtain very good agreement. Secondly we concentrated on the behavior of the fermions. The general paradigm of interacting fermions in one dimension is that of the Luttinger Liquid characterized by bosonic excitations and spin charge separation. By generalizing our approach we are able to access the one particle fermion propagator as a quantity averaged over the NLsigmaM which controls the spin background. We see that in the limit of zero doping the quasiparticle weight Z is non-zero in a neighborhood of the Fermi energy. This in turn implies that the Luttinger liquid parameter Krho goes to one as the doping delta goes to zero as was first argued by Schulz. Our stronger result allows us to assert that in the very low doping regime the fermions constitute a Fermi liquid.
We report comprehensive Cu NMR studies on single crystals of ${\mathrm{Sr}}_{14\ensuremath{-}x}{\mathrm{Ca}}_{x}{\mathrm{Cu}}_{24}{\mathrm{O}}_{41},$ which contain simple CuO2 chains and two-leg Cu2O3 ladders. From measurements of the 63Cu NMR shift, it is clear that the spin gap in the ladders decreases with isovalent Ca substitution from $\ensuremath{\Delta}=550\ifmmode\pm\else\textpm\fi{}30$ K for Sr14Cu24O41 (Sr14) to $350\ifmmode\pm\else\textpm\fi{}30$ K, $280\ifmmode\pm\else\textpm\fi{}30$ K, and $270\ifmmode\pm\else\textpm\fi{}30$ K for x=6 (Ca6), x=9 (Ca9), and x=11.5 (Ca11.5), respectively. The exponential decrease of the nuclear spin-lattice relaxation rate 1/T1 below \ensuremath{\sim}130 K is consistent with the presence of the spin gap in the spin excitation spectrum. In the T range higher than $\ensuremath{\sim}200$ K, we observed the following dependences: 1/T1=const and the square of Gaussian spin-echo decay time, ${T}_{2G}^{2}\ensuremath{\propto}T$ which are consistent with the scaling theory for the S=1/2 one-dimensional (1D) Heisenberg model. The value of T2G/T1T is compatible with the theoretical prediction of an exchange constant along the leg ${J}_{\ensuremath{\parallel}}\ensuremath{\sim}1800$ K for Ca6 and ${J}_{\ensuremath{\parallel}}\ensuremath{\sim}1500$ K for Ca9 and Ca11.5. A notable finding is that the magnitude of the spin gap remains nearly constant and characteristics of novel 1D-like spin dynamics are maintained in the content varying from Ca9 to Ca11.5. On the other hand, the charge transport changes with increasing Ca content so that the more conductive Ca11.5 exhibits pressure-induced superconductivity exceeding 3.5 GPa. We have found that T2G2, which is proportional to the inverse spin correlation length ${\ensuremath{\xi}}^{\ensuremath{-}1}$, deviates from a linear T dependence upon cooling and is described by $A+BT\mathrm{exp}(\ensuremath{-}\ensuremath{\Delta}/T)$, regardless of the Ca substitution. We point out that the value of T2G2(T=0)=A is proportional to the finite value of ${\ensuremath{\xi}}_{0}^{\ensuremath{-}1}=\ensuremath{\Delta}{/c}_{1D},$ where ${c}_{1D}=(\ensuremath{\pi}{/2)J}_{\ensuremath{\parallel}}$ is the spin-wave velocity. From the result that the values of ${A}^{\ensuremath{-}1}\ensuremath{\sim}{\ensuremath{\xi}}_{\mathrm{eff}}$ for Ca6, Ca9, and Ca11.5 are significantly reduced compared to that for Sr14, it is suggested that ${\ensuremath{\xi}}_{\mathrm{eff}}$ is dominated at low T by an average distance d among mobile holes obeying the relation ${\ensuremath{\xi}}_{\mathrm{eff}}\ensuremath{\sim}d={\ensuremath{\xi}}_{h}.$ From an estimate of ${\ensuremath{\xi}}_{0}/a\ensuremath{\sim}$ 5.2 for Sr14, where a is the Cu-Cu distance along the leg, ${\ensuremath{\xi}}_{h}/a$ is obtained as $\ensuremath{\sim}3.5$, 2.3, and 2.0, and hole content x as $\ensuremath{\sim}0.14$, 0.22, and 0.25 per Cu2O3 ladder for Ca6, Ca9, and Ca11.5, respectively. These values were consistent with x= 0.14, 0.2, and 0.22 for Ca6, Ca9, and Ca11 estimated from the optical conductivity experiment by Osafune et al. [Phys. Rev. Lett. 78, 1980 (1997)]. The ${\mathrm{Sr}}_{14\ensuremath{-}x}{\mathrm{Ca}}_{x}{\mathrm{Cu}}_{24}{\mathrm{O}}_{41}$ compounds are thus hole-doped two-leg spin-ladder systems which reveal the metallic behavior dominated by the 1D-like spin dynamics at high T and accompanied by the spin gap formation at low T. For Ca11.5, as the spin gap is formed upon cooling below $\ensuremath{\sim}180$ K, the resistivity increases in the direction perpendicular to the ladder, whereas the conductivity along the ladder remains metallic, followed by the localization of mobile holes in both directions below ${T}_{L}\ensuremath{\sim}60$ K. We point out that preformed pairs are confined in each ladder and localized below $\ensuremath{\sim}60$ K at an ambient pressure.
We investigate weakly coupled spin-1/2 ladders in a magnetic field. The work is motivated by recent experiments on the compound (C5H12N)2CuBr4 (BPCB). We use a combination of numerical and analytical methods, in particular the density matrix renormalization group (DMRG) technique, to explore the phase diagram and the excitation spectra of such a system. We give detailed results on the temperature dependence of the magnetization and the specific heat, and the magnetic field dependence of the nuclear magnetic resonance (NMR) relaxation rate of single ladders. For coupled ladders, treating the weak interladder coupling within a mean field approach, we compute the transition temperature of triplet condensation and its corresponding antiferromagnetic order parameter. Existing experimental measurements are discussed and compared to our theoretical results. Furthermore we compute, using time dependent DMRG, the dynamical correlations of a single spin ladder. Our results allow to directly describe the inelastic neutron scattering cross section up to high energies. We focus on the evolution of the spectra with the magnetic field and compare their behavior for different couplings. The characteristic features of the spectra are interpreted using different analytical approaches such as the mapping onto a spin chain, a Luttinger liquid (LL) or onto a t-J model. For values of parameters for which such measurements exist, we compare our results to inelastic neutron scattering experiments on the compound BPCB and find excellent agreement. We make additional predictions for the high energy part of the spectrum that are potentially testable in future experiments.
Various forms of antiferromagnetic exchange interaction among quantized spins in one-dimensional and quasi-one-dimensional lattices are examined. Primary results are reported in two real compounds, the sodium vanadate NaV2O5 and the copper germanate CuGeO3, and in a class of compounds of real materials modeled as dimerized antiferromagnetically coupled spin-1/2 chains susceptible to spin-1 impurity doping and that include such examples as the strontium cuprate Sr14Cu24O41 and vanadium pyrophosphate (VO)2P2O7. Sodium vanadate, NaV2O5, a quarter-filled two-leg ladder compound that was originally thought to be composed of magnetic legs and nonmagnetic legs was subsequently shown to be a charge ordered system below room temperature. Initial models of the material as isolated antiferromagnetically coupled spin-1/2 chains can be mapped to the subsequently resolved magnetic system of the charge ordered state with the spins on molecular orbitals of V-O-V rungs antiferromagentically coupled between neighboring rungs either on the same ladder or on neighboring ladders. Comparing the model's dynamic structure factor to inelastic neutron scattering data could distinguish between the proposed spin coupling schemes and consequently reveal the details of the interaction between the lattice and the "zig-zag" charge density as well as the magnetic stabilization of the low temperature phase. Copper germanate, the first and only known inorganic spin-Peierls compound, exhibits a strong temperature dependent exchange coupling pattern among the spin-1/2 Cu2+ chains. Above the spin-Peierls transition temperature an unmodulated antiferromagnetic nearest neighbor exchange interaction J1 competes with an antiferromagnetic next nearest neighbor interaction J2. The next nearest neighbor exchange represents an effective coupling equivalent to the net effect of all longer range exchange interactions. This frustration to the nearest neighbor spin exchange produces a distinctive magnetic susceptibility χ (T) much different from the Bonner-Fisher susceptibility of the spin-1/2 Heisenberg chain with nearest neighbor antiferromagnetic exchange only. The ratio of the second to first nearest neighbor couplings α = J2/J1 ≈ 0.36 is sufficient to open a spontaneous gap in the spin-wave excitation spectrum at low temperatures. Below TSP = 14K, the dynamical structure factor is used to fit the dimerization δ and the exchange interactions J1 and J2 to the inelastic neutron scattering data of CuGeO3 at T = 10K. It is found that both δ and α increase significantly at lower temperatures, relative to the values obtained in the high temperature phase and at the onset of dimeration at 14 K. Static structure factor calculations how Scattering inconsistent with the δâJ1âJ2 model and can be attributed primarily to the phonon degrees of freedom but possibly also to the couplings between chains in the b and a directions of the crystal lattice. Structurally dimerized compounds of antiferromagnetic spin-1/2 chains possess dynamic structure factor and magnetic susceptibility features that are very sensitive to doping with magnetic and nonmagnetic impurities. It is shown that the effects of spin-1 impurities are very similar to those of nonmagnetic (S = 0) impurities if the coupling between impurity and native spin is about the same magnitude as or larger than between native S = 1/2 spins. The microscopic origins of the similarity can be appreciated with the consideration that neighboring spins to the impurity find it more energetically favorable to couple to the impurity than the other spins of the lattice. Thus the spin-1 impurity and its neighboring S = 1/2 spins decouple from the lattice, creating a nonmagnetic break in the chain. The spins that now observe a nonmagnetic cluster on one side can couple to the S = 1/2 spins on the other side with a higher AF correlation than in the pure compound since they do not have to have a ï¬uctuating dimer resonating between two neighbors. Such enhancements to the local correlations can stabilize the global AF order in one dimensional compounds as shown in theoretical and experimental studies of CuGeO3. ED calculations of the dynamic structure factor show that S(q, ω) developes states with ω = 0 in the gap at q = π. Magnetic susceptibilites in the presense of spin-1 impurities were obtained for 80 site chains by QMC simulations and for 16 site chains by ED calculations. An impurity concentration-dependent second peak in the low temperature region reveals an increasing second maximum with T as observed in doped copper germanates and suggests that the results of the study are applicable even to phonon mediated dimerization. This is not immediately apparent because spin-phonon coupling could distort the dimerization patterns. However, experimental and theoretical results show that elastic coupling between chains can stabilize the dimerization pattern due to the impurities and the results will still apply.