Characteristic properties of excited states in anitiferromagnetic ladder systems with spin-1/2 are investigated in relation with the theoretical analysis of the quite asymmetric shape of the peak for twice the spin gap Δg in magnetic Raman spectra. Here, the structure of exchange-scattering spectra are reproduced by the numerical calculation for the finite Heisenberg ladder, in which legs with antiferromagnetic bond Jc is connected by rungs with antiferromagnetic bond Jr. The singlet ground state in this system can be expressed as the ordering of singlet dimers on rungs in the ladder for Jc/Jr →+0. In fact, the value of 0.1 is adopted to be the ratio of Jc /Jr in order to discuss the experimental work of the magnetic Raman spectra for the ladder of V4+ ions in the oxide compound CaV2O5 reported in Konstantinović et al., Phys. Rev. B61 (2000), 15185. As for this peak of 2Δg , quite an asymmetric observed shape is explained by the present calculation. According to the analysis of spectra, we discuss the expression of excited states by triplet dimers on rungs: The dominant contribution of the pair of triplet dimers on adjacent rungs to the corresponding state for 2Δg peak is pointed out.
The frustrated ladder with alternate ferromagnetic exchange $\ensuremath{-}{J}_{F}$ and antiferromagnetic exchange
JA to first neighbors and ferromagnetic exchange $\ensuremath{-}{J}_{L}$ to second neighbors is studied by exact diagonalization and density matrix renormalization group calculations in systems of
2N spins-
21 with periodic boundary conditions. The ground state is a singlet
(S=0) and the singlet-triplet gap ${\ensuremath{\varepsilon}}_{T}$ is finite for the exchanges considered. Spin-
21 string correlation functions
g1(N) and
g2(N) are defined for an even number
N of consecutive spins in systems with two spins per unit cell; the ladder has string order ${g}_{2}(\ensuremath{\infty})>0$ and ${g}_{1}(\ensuremath{\infty})=0$. The minimum
N∗ of
g2(N) is related to the range of ground-state spin correlations. Convergence to ${g}_{2}(\ensuremath{\infty})$ is from below, and
g1(N) decreases exponentially for $N\ensuremath{\ge}{N}^{*}$. Singlet valence bond (VB) diagrams account for the size dependencies. The frustrated ladder at special values of
JF,JL, and
JA reduces to well-known models such as the spin-1 Heisenberg antiferromagnet and the ${J}_{1}\text{\ensuremath{-}}{J}_{2}$ model, among others. Numerical analysis of ladders matches previous results for spin-1 gaps or string correlation functions and extends them to spin-
21 systems. The nondegenerate singlet ground state of the ladder is a bond-order wave, a Kekul\'e VB diagram at ${J}_{L}={J}_{F}/2\ensuremath{\le}{J}_{A}$, that is reversed on interchanging $\ensuremath{-}{J}_{F}$ and
JA. Inversion symmetry is spontaneously broken in the dimer phase of the ${J}_{1}\text{\ensuremath{-}}{J}_{2}$ model where the Kekul\'e diagrams are the doubly degenerate ground states at
J2/J1=1/2.
The frustrated ladder with alternate ferromagnetic(F) exchange
−JF and AF exchange
JA to first neighbors and F exchange
−JL to second neighbors is studied by exact diagonalization (ED) and density matrix renormalization group (DMRG) calculations in systems of
2N spins-1/2 with periodic boundary conditions. The ground state is a singlet
(S=0) and the singlet-triplet gap
εT is finite for the exchanges considered. Spin-1/2 string correlation functions
g1(N) and
g2(N) are defined for an even number
N of consecutive spins in systems with two spins per unit cell; the ladder has string order
g2(∞)>0 and
g1(∞)=0. The minimum
N∗ of
g2(N) is related to the range of ground-state spin correlations. Convergence to
g2(∞) is from below, and
g1(N) decreases exponentially for
N≥N∗. Singlet valence bond (VB) diagrams account for the size dependencies. The frustrated ladder at special values of
JF,
JL and
JA reduces to well-known models such as the spin-1 Heisenberg antiferromagnet and the
J1−J2 model, among others. Numerical analysis of ladders matches previous results for spin-1 gaps or string correlation functions and extends them to spin-1/2 systems. The nondegenerate singlet ground state of ladder is a bond-order wave, a Kekulé VB diagrams at
JL=JF/2≤JA, that is reversed on interchanging
−JF and
JA. Inversion symmetry is spontaneously broken in the dimer phase of the
J1−J2 model where the Kekulé diagrams are the doubly degenerate ground states at
J2/J1=1/2.
The Raman response in the antiferromagnetic 2-leg S = 1/2 Heisenberg ladder is calculated for various couplings by continuous unitary transformations. For leg couplings above 80% of the rung coupling a characteristic 2-peak structure occurs with a point of zero intensity within the continuum. Experimental data for CaV 2 O 5 and La y Ca 14 − y Cu 24 O 41 are analyzed and the coupling constants are determined. Evidence is found that the Heisenberg model is not sufficient to describe cuprate ladders. We argue that a cyclic exchange term is the appropriate extension.
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.