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Optical Spectroscopy of Spin Ladders

Marco Windt

Published Jan 1, 2002• 0 citations
OpenAlex

Abstract

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.

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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.

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Properties of undoped and doped spin-1/2 ladders at finite temperature

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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.

•Jan 18, 2011•1 citation

Cyclic spin exchange in cuprate spin ladders

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We investigate the influence of a cyclic spin exchange ${J}_{\mathrm{cyc}}$ on the one- and two-triplet excitations of an undoped two-leg $S=1/2$ ladder, using the density-matrix renormalization group (DMRG). The dispersion of the $S=0$ two-triplet bound state is dramatically reduced by ${J}_{\mathrm{cyc}}$ due to a repulsion between triplets on neighboring rungs. In $(\mathrm{La},\mathrm{Ca}{)}_{14}{\mathrm{Cu}}_{24}{\mathrm{O}}_{41}$ a consistent description of both the spin gap and the $S$=0 bound state requires ${J}_{\mathrm{cyc}}{/J}_{\ensuremath{\perp}}\ensuremath{\approx}0.20--0.27$ and ${J/J}_{\ensuremath{\perp}}\ensuremath{\approx}1.25--1.35.$ With these coupling ratios the recently developed dynamical DMRG yields an excellent description of the entire $S=0$ excitation spectrum observed in the optical conductivity, including the continuum contribution.

arXiv:cond-mat/0203472•Physical review. B, Condensed matter•Nov 27, 2002•63 citations

Magnetic Susceptibilities of Spin-1/2 Antiferromagnetic Heisenberg Ladders and Applications to Ladder Oxide Compounds

D. C. Johnston, Matthias Troyer, S. Miyahara +11 more

A comprehensive theoretical and experimental study is presented of the magnetic susceptibility versus temperature χ(T) of spin S = 1/2 two- and three-leg Heisenberg ladders and ladder oxide compounds. Extensive quantum Monte Carlo simulations of χ(T) were carried out for both isolated and coupled two-leg ladders with spatially anisotropic intraladder exchange. Accurate fits to these and related literature QMC data were obtained. We have also calculated the one- and two-magnon dispersion relations and the dynamical spin structure factor for anisotropic isolated 2 x 12 ladders. The exchange constants in the two-leg ladder compound SrCu2O3 are estimated from LDA+U calculations. We report the detailed crystal structure of SrCu2O3 and of the three-leg ladder compound Sr2Cu3O5. New experimental χ(T) data are reported for the two-leg ladder cuprates SrCu2O3 and LaCuO_{2.5}, and for the (nominally) two-leg ladder vanadates CaV2O5 and MgV2O5. The new and literature χ(T) data for these compounds and for Sr2Cu3O5 are modeled using our QMC χ(T) simulation fits, and the exchange coupling constants between the spins-1/2 are thereby estimated for each material. The surpisingly strong spatial anisotropy of the bilinear intraladder exchange constants in the cuprate compounds is discussed together with the results of other experiments sensitive to this anisotropy. Recent theoretical predictions are discussed including those which indicate that a four-spin cyclic exchange interaction within a Cu4 plaquette is important to determining the magnetic properties and which can significantly influence the exchange interactions estimated from χ(T) data assuming the presence of only bilinear exchange.

arXiv:cond-mat/0001147•Jan 11, 2000•12 citations

Numerical Study of Magnetic Raman Scattering Spectra in Ladder Antiferromagnets –Exchange Scatterings from the Singlet Ground State–

Shinichiro Tada, Yuhei Natsume, Toshihiko Suzuki

The exchange-scattering spectra are reproduced by the numerical calculation for the finite Heisenberg ladder, in which two-legs with antiferromagnetic bond J c is connected by rungs with antiferromagnetic bond J r . The numerical calculation is made for the system of 12 ×2 sites by Lanczos method. The ratio of J c / J r is considered to be 0.6–1.0 in order to discuss the experimental work for ladders of Cu 2+ ions in oxide compounds Sr 14- x Ca x Cu 24 O 41 . In addition to the Raman edge about J r corresponding twice the singlet-triplet spin gap, the characteristic structure appears around 2 or 3 times of J r i.e. 3 or 5 times the spin-gap. We concentrate our attention on characteristic features of excited levels, transitions to which are Raman-active. In particular, the relationship between correlations for spins in those states and corresponding Raman intensities is discussed in the picture of triplet pairs excited from singlet dimers. By the perturbation theory, the essential dependence of those intensities on distances between triplet dimers is investigated.

Journal of the Physical Society of Japan•Aug 15, 2001•1 citation

Pseudogap in the c -axis (along the ladder) optical conductivity of t − J ladders and its quasiparticle interpretation

Paulína Karlubíková, Hana Růžičková, Jiří Chaloupka +1 more

Motivated by similarities between cuprate superconductors and two-leg ladder copper-oxide compounds and in order to obtain a better understanding of optical properties of cuprate superconductors we have studied the c-axis (along the ladder) optical conductivity [Formula: see text] of a doped [Formula: see text] two-leg ladder. Using exact diagonalization, we have calculated the conductivity and related quantities for cyclic ladders of up to 13 rungs. In agreement with results of an early study by Hayward and coworkers (Hayward et al 1996 Phys. Rev. B 53 8863) we find that [Formula: see text] consists of a Drude peak at zero frequency and an absorption band in the infrared region that is separated from the former by a pseudogap. The width of the pseudogap [Formula: see text] increases with increasing J/t, in parallel with an increase of the magnitude [Formula: see text] of the gap in the quasiparticle excitation spectra. Our central finding is that [Formula: see text], where [Formula: see text] is the magnitude of the gap in the spin excitation spectra. We demonstrate that this approximate relation can be understood in terms of a phenomenological model involving a superconducting ladder and a coupling between charged quasiparticles and spin excitations. The relation is remarkably similar to the one between experimental values of the energy scale of a dip in the in-plane optical conductivity, the superconducting gap [Formula: see text] and the energy of the spin-resonance in cuprate superconductors (for a recent discussion of the optical data, see Šopík et al 2015 New J. Phys. 17 053022). Our findings support the point of view that low energy infrared active excited states of cuprate superconductors can be viewed as consisting of two charged quasiparticles connected with pair-breaking and a spin excitation.

Journal of Physics Condensed Matter•Jan 9, 2019•1 citation
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.
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.
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.
We investigate the influence of a cyclic spin exchange Jcyc{J}_{\mathrm{cyc}}Jcyc​ on the one- and two-triplet excitations of an undoped two-leg S=1/2S=1/2S=1/2 ladder, using the density-matrix renormalization group (DMRG). The dispersion of the S=0S=0S=0 two-triplet bound state is dramatically reduced by Jcyc{J}_{\mathrm{cyc}}Jcyc​ due to a repulsion between triplets on neighboring rungs. In (La,Ca)14Cu24O41(\mathrm{La},\mathrm{Ca}{)}_{14}{\mathrm{Cu}}_{24}{\mathrm{O}}_{41}(La,Ca)14​Cu24​O41​ a consistent description of both the spin gap and the SSS=0 bound state requires ${J}_{\mathrm{cyc}}{/J}_{\ensuremath{\perp}}\ensuremath{\approx}0.20--0.27$ and ${J/J}_{\ensuremath{\perp}}\ensuremath{\approx}1.25--1.35.$ With these coupling ratios the recently developed dynamical DMRG yields an excellent description of the entire S=0S=0S=0 excitation spectrum observed in the optical conductivity, including the continuum contribution.
A comprehensive theoretical and experimental study is presented of the magnetic susceptibility versus temperature χ(T) of spin S = 1/2 two- and three-leg Heisenberg ladders and ladder oxide compounds. Extensive quantum Monte Carlo simulations of χ(T) were carried out for both isolated and coupled two-leg ladders with spatially anisotropic intraladder exchange. Accurate fits to these and related literature QMC data were obtained. We have also calculated the one- and two-magnon dispersion relations and the dynamical spin structure factor for anisotropic isolated 2 x 12 ladders. The exchange constants in the two-leg ladder compound SrCu2O3 are estimated from LDA+U calculations. We report the detailed crystal structure of SrCu2O3 and of the three-leg ladder compound Sr2Cu3O5. New experimental χ(T) data are reported for the two-leg ladder cuprates SrCu2O3 and LaCuO_{2.5}, and for the (nominally) two-leg ladder vanadates CaV2O5 and MgV2O5. The new and literature χ(T) data for these compounds and for Sr2Cu3O5 are modeled using our QMC χ(T) simulation fits, and the exchange coupling constants between the spins-1/2 are thereby estimated for each material. The surpisingly strong spatial anisotropy of the bilinear intraladder exchange constants in the cuprate compounds is discussed together with the results of other experiments sensitive to this anisotropy. Recent theoretical predictions are discussed including those which indicate that a four-spin cyclic exchange interaction within a Cu4 plaquette is important to determining the magnetic properties and which can significantly influence the exchange interactions estimated from χ(T) data assuming the presence of only bilinear exchange.
The exchange-scattering spectra are reproduced by the numerical calculation for the finite Heisenberg ladder, in which two-legs with antiferromagnetic bond J c is connected by rungs with antiferromagnetic bond J r . The numerical calculation is made for the system of 12 ×2 sites by Lanczos method. The ratio of J c / J r is considered to be 0.6–1.0 in order to discuss the experimental work for ladders of Cu 2+ ions in oxide compounds Sr 14- x Ca x Cu 24 O 41 . In addition to the Raman edge about J r corresponding twice the singlet-triplet spin gap, the characteristic structure appears around 2 or 3 times of J r i.e. 3 or 5 times the spin-gap. We concentrate our attention on characteristic features of excited levels, transitions to which are Raman-active. In particular, the relationship between correlations for spins in those states and corresponding Raman intensities is discussed in the picture of triplet pairs excited from singlet dimers. By the perturbation theory, the essential dependence of those intensities on distances between triplet dimers is investigated.
Motivated by similarities between cuprate superconductors and two-leg ladder copper-oxide compounds and in order to obtain a better understanding of optical properties of cuprate superconductors we have studied the c-axis (along the ladder) optical conductivity [Formula: see text] of a doped [Formula: see text] two-leg ladder. Using exact diagonalization, we have calculated the conductivity and related quantities for cyclic ladders of up to 13 rungs. In agreement with results of an early study by Hayward and coworkers (Hayward et al 1996 Phys. Rev. B 53 8863) we find that [Formula: see text] consists of a Drude peak at zero frequency and an absorption band in the infrared region that is separated from the former by a pseudogap. The width of the pseudogap [Formula: see text] increases with increasing J/t, in parallel with an increase of the magnitude [Formula: see text] of the gap in the quasiparticle excitation spectra. Our central finding is that [Formula: see text], where [Formula: see text] is the magnitude of the gap in the spin excitation spectra. We demonstrate that this approximate relation can be understood in terms of a phenomenological model involving a superconducting ladder and a coupling between charged quasiparticles and spin excitations. The relation is remarkably similar to the one between experimental values of the energy scale of a dip in the in-plane optical conductivity, the superconducting gap [Formula: see text] and the energy of the spin-resonance in cuprate superconductors (for a recent discussion of the optical data, see Šopík et al 2015 New J. Phys. 17 053022). Our findings support the point of view that low energy infrared active excited states of cuprate superconductors can be viewed as consisting of two charged quasiparticles connected with pair-breaking and a spin excitation.