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arXiv:1602.08223 · Physical review. B./Physical review. B

Anomalous thermal decoherence in a quantum magnet measured with neutron spin echo spectroscopy

Felix Groitl, T. Keller, Katharina Rolfs, D. M. Tennant, Klaus Habicht

Published Apr 4, 2016• 7 citations
arXivHTMLPDF

Abstract

The effect of temperature dependent asymmetric line broadening is investigated in $\mathrm{Cu}({\mathrm{NO}}_{3}{)}_{2}\ifmmode\cdot\else\textperiodcentered\fi{}2.5{\mathrm{D}}_{2}\mathrm{O}$, a model material for a one-dimensional bond alternating Heisenberg chain, using the high resolution neutron-resonance spin echo (NRSE) technique. Inelastic neutron scattering experiments on dispersive excitations including phase sensitive measurements demonstrate the potential of NRSE to resolve line shapes, which are non-Lorentzian, opening up a new and hitherto unexplored class of experiments for the NRSE method beyond standard linewidth measurements. The particular advantage of NRSE is its direct access to the correlations in the time domain without convolution with the resolution function of the background spectrometer. This application of NRSE is very promising and establishes a basis for further experiments on different systems, since the results for Cu(${\mathrm{NO}}_{3}$)${}_{2}\ifmmode\cdot\else\textperiodcentered\fi{}2.5{\mathrm{D}}_{2}\mathrm{O}$ are applicable to a broad range of quantum systems.

DOI
10.1103/physrevb.93.134404

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•Jan 1, 2014•0 citations
The effect of temperature dependent asymmetric line broadening is investigated in Cu(NO3)2\ifmmode⋅\else\textperiodcentered\fi2.5D2O\mathrm{Cu}({\mathrm{NO}}_{3}{)}_{2}\ifmmode\cdot\else\textperiodcentered\fi{}2.5{\mathrm{D}}_{2}\mathrm{O}Cu(NO3​)2​\ifmmode⋅\else\textperiodcentered\fi2.5D2​O, a model material for a one-dimensional bond alternating Heisenberg chain, using the high resolution neutron-resonance spin echo (NRSE) technique. Inelastic neutron scattering experiments on dispersive excitations including phase sensitive measurements demonstrate the potential of NRSE to resolve line shapes, which are non-Lorentzian, opening up a new and hitherto unexplored class of experiments for the NRSE method beyond standard linewidth measurements. The particular advantage of NRSE is its direct access to the correlations in the time domain without convolution with the resolution function of the background spectrometer. This application of NRSE is very promising and establishes a basis for further experiments on different systems, since the results for Cu(NO3{\mathrm{NO}}_{3}NO3​)2\ifmmode⋅\else\textperiodcentered\fi2.5D2O{}_{2}\ifmmode\cdot\else\textperiodcentered\fi{}2.5{\mathrm{D}}_{2}\mathrm{O}2​\ifmmode⋅\else\textperiodcentered\fi2.5D2​O are applicable to a broad range of quantum systems.
The effect of thermal fluctuations on the dynamics of a gapped quantum magnet is studied using inelastic neutron scattering on copper nitrate, a model material for the spin-1/2, one-dimensional (1D) bond alternating Heisenberg chain. A large, highly deuterated, single-crystal sample of copper nitrate is produced using a solution growth method and measurements are made using the high-resolution backscattering spectrometer OSIRIS at the ISIS Facility. Theoretical calculations and numerical analysis are combined to interpret the physical origin of the thermal effects observed in the magnetic spectra. The primary observations are (1) a thermally induced central peak due to intraband scattering, which is similar to Villain scattering familiar from soliton systems in 1D, and (2) the one-magnon quasiparticle pole is seen to develop with temperature into an asymmetric continuum of scattering. We relate this asymmetric line broadening to a thermal strongly correlated state caused by hard-core constraints and quasiparticle interactions. These findings are a counter example to recent assertions of the universality of line broadening in 1D systems and are applicable to a broad range of quantum systems.
The effect of thermal fluctuations on the dynamics of a gapped quantum magnet is studied using inelastic neutron scattering on copper nitrate, a model material for the one-dimensional (1D) bond alternating Heisenberg chain, combined with theoretical and numerical analysis. We observe and interpret the thermally induced central peak due to intraband scattering as well as the thermal development of an asymmetric continuum of scattering. We relate this asymmetric line broadening to hard core constraints and quasi-particle interactions. Our findings are a counter example to recent assertions of universality of line broadening in 1D systems and are to be considered as a new paradigm of behaviour, applicable to a broad range of quantum systems.
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.
Dimerized magnets forming alternating Heisenberg chains exhibit quantum coherence and entanglement and thus can find potential applications in quantum information and computation. However, magnetic systems typically undergo thermal decoherence at finite temperatures. Here, we show inelastic neutron scattering results on an alternating antiferromagnetic-ferromagnetic chain compound Na2Cu2TeO6{\mathrm{Na}}_{2}{\mathrm{Cu}}_{2}{\mathrm{TeO}}_{6}Na2​Cu2​TeO6​ that the excited quasiparticles can counter thermal decoherence and maintain strong correlations at elevated temperatures. At low temperatures, we observe clear dispersive singlet-triplet excitations arising from the dimers formed along the crystalline bbb axis. The excitation gap is of $\ensuremath{\sim}18\phantom{\rule{0.16em}{0ex}}\mathrm{meV}$ and the bandwidth is about half of the gap. The band top energy has a weak modulation along the [100] direction, indicative of a small interchain coupling. The gap increases while the bandwidth decreases with increasing temperature, leading to a strong reduction in the available phase space for the triplons. As a result, the Lorentzian-type energy broadening becomes highly asymmetric as the temperature is raised. These results are associated with a strongly correlated state resulting from hard-core constraint and quasiparticle interactions. We consider these results to be not only evidence for strong correlations at finite temperatures in Na2Cu2TeO6{\mathrm{Na}}_{2}{\mathrm{Cu}}_{2}{\mathrm{TeO}}_{6}Na2​Cu2​TeO6​, but also for the universality of the strongly correlated state in a broad range of quantum magnetic systems.
Unlike most quantum systems which rapidly become incoherent as temperature is raised, strong correlations persist at elevated temperatures in S=12S=\frac{1}{2}S=21​ dimer magnets, as revealed by the unusual asymmetric line shape of their excitations at finite temperatures. Here, we quantitatively explore and parametrize the strongly correlated magnetic excitations at finite temperatures using high-resolution inelastic neutron scattering of the model compound BaCu2V2O8{\mathrm{BaCu}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{8}BaCu2​V2​O8​ which we show to be an alternating antiferromagnetic-ferromagnetic $\mathrm{spin}\ensuremath{-}\frac{1}{2}$ chain. Comparison to state of the art computational techniques shows excellent agreement over a wide temperature range. Our findings hence demonstrate the possibility to quantitatively predict coherent behavior at elevated temperatures in quantum magnets.
Many phenomena in magnetism can be described using classical models, yet magnetism is a quantum mechanical effect. In addition to thermal fluctuations, quantum fluctuations arise due to the quantum uncertainty of the ground state. These fluctuations are enhanced by low dimensionality and low spin. Spin chains show interesting excitations associated with quasiparticles. Model materials for spin chains can be realized in compounds where the interchain interactions are weak enough. This thesis presents neutron scattering studies of two model materials for spin chains with different spin symmetry. The spin2 Heisenberg antiferromagnetic chain CuSO4*5D2O has a main exchange of J ∼ 3 K, which permits to study its excitation spectrum up to temperatures of ten times the exchange. The spin2 Heisenberg magnet has been studied widely both theoretically and experimentally. The excitation spectrum of the spin2 Heisenberg antiferromagnet consists of quasiparticles called spinons, and calculations for it exist for T = 0 and as a function of temperature. A quantitative comparison between experimental data and theoretical models across a range of temperatures is presented. The excitation spectrum of CuSO4*5D2O is excellently described by the excitation spectrum of a spin2 Heisenberg antiferromagnetic chain at finite temperatures. Energy-temperature scaling is observed at temperatures up to 2J . For these temperatures the Luttinger liquid description of the spin2 Heisenberg antiferromagnetic chain is valid. A spinon continuum is confirmed at all measured temperatures. Therefore, even at ten times the main exchange (T ≈ 10 J), CuSO4*5D2O shows the behavior of a quantum magnet, and not of a classical system at infinite temperatures, for which one would expect single spin flips. The Ising chain is one of the most studied models in magnetism, one model compound for it is RbCoCl3. Optical spectroscopy measurements suggest a lower gap than for similar compounds, which makes it better suited for high resolution neutron spectroscopy. Magnetic correlations along the chains arise in RbCoCl3 below 80 K. A gapped continuum is observed, which arises from isolated antiferromagnetic Ising chains. Below the first magnetic ordering temperature TN1 ≈ 28 K bound states are observed, which arise due to correlations which form between the chains. Strong diffuse scattering leads to the conclusion that disorder is still present. At the second magnetic ordering transition, at TN2 ≈ 14 K, the bound states split as the correlations between the chains change. Fits indicate that the correlations change continuously as a function of temperature. Above TN2 the excitation spectrum of RbCoCl3 can be described by a spin1 2 Ising chain with an XY-component which is treated as a perturbation. Below TN2 the main features are reproduced correctly, but deviations from the details indicate that additional terms in the Hamiltonian may be necessary. This thesis was carried out at the Institut Laue-Langevin, the Laboratory for Neutron Scattering and Imaging at the Paul Scherrer Institute and ETH Zurich.