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arXiv:2102.04607 · Physical Review Research

Control of superexchange interactions with DC electric fields

Shunsuke C. Furuya, Kazuaki Takasan, Masahiro Sato

Published Jul 19, 2021• 8 citations
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Abstract

We discuss DC electric-field controls of superexchange interactions. We first present generic results about antiferromagnetic and ferromagnetic superexchange interactions valid in a broad class of Mott insulators, where we also estimate typical field strength to observe DC electric-field effects: $\ensuremath{\sim}1\phantom{\rule{3.33333pt}{0ex}}\mathrm{MV}/\mathrm{cm}$ for inorganic Mott insulators such as transition-metal oxides and $\ensuremath{\sim}0.1\phantom{\rule{3.33333pt}{0ex}}\mathrm{MV}/\mathrm{cm}$ for organic ones. Next, we apply these results to geometrically frustrated quantum spin systems. Our theory widely applies to (quasi-)two-dimensional and thin-film systems and one-dimensional quantum spin systems on various lattices such as square, honeycomb, triangular, and kagome ones. In this paper, we give our attention to those on the square lattice and on the chain. For the square lattice, we show that DC electric fields can control a ratio of the nearest-neighbor and next-nearest-neighbor exchange interactions. In some realistic cases, DC electric fields make the two next-nearest-neighbor interactions nonequivalent and eventually turns the square-lattice quantum spin system into a deformed triangular-lattice one. For the chain, DC electric fields can induce singlet-dimer and Haldane-dimer orders. We show that the DC electric-field-induced spin gap $\ensuremath{\propto}{|\mathbit{E}|}^{2/3}$ in the Heisenberg antiferromagnetic chain will reach $\ensuremath{\sim}10%$ of the dominant superexchange interaction in the case of a spin-chain compound ${\mathrm{KCuMoO}}_{4}(\mathrm{OH})$ when the DC electric field of $\ensuremath{\sim}1\phantom{\rule{3.33333pt}{0ex}}\mathrm{MV}/\mathrm{cm}$ is applied.

DOI
10.1103/physrevresearch.3.033066

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Bulletin of the American Physical Society•Mar 18, 2021•0 citations
We discuss DC electric-field controls of superexchange interactions. We first present generic results about antiferromagnetic and ferromagnetic superexchange interactions valid in a broad class of Mott insulators, where we also estimate typical field strength to observe DC electric-field effects: \ensuremath∼1MV/cm\ensuremath{\sim}1\phantom{\rule{3.33333pt}{0ex}}\mathrm{MV}/\mathrm{cm}\ensuremath∼1MV/cm for inorganic Mott insulators such as transition-metal oxides and \ensuremath∼0.1MV/cm\ensuremath{\sim}0.1\phantom{\rule{3.33333pt}{0ex}}\mathrm{MV}/\mathrm{cm}\ensuremath∼0.1MV/cm for organic ones. Next, we apply these results to geometrically frustrated quantum spin systems. Our theory widely applies to (quasi-)two-dimensional and thin-film systems and one-dimensional quantum spin systems on various lattices such as square, honeycomb, triangular, and kagome ones. In this paper, we give our attention to those on the square lattice and on the chain. For the square lattice, we show that DC electric fields can control a ratio of the nearest-neighbor and next-nearest-neighbor exchange interactions. In some realistic cases, DC electric fields make the two next-nearest-neighbor interactions nonequivalent and eventually turns the square-lattice quantum spin system into a deformed triangular-lattice one. For the chain, DC electric fields can induce singlet-dimer and Haldane-dimer orders. We show that the DC electric-field-induced spin gap \ensuremath∝∣\mathbitE∣2/3\ensuremath{\propto}{|\mathbit{E}|}^{2/3}\ensuremath∝∣\mathbitE∣2/3 in the Heisenberg antiferromagnetic chain will reach \ensuremath∼10\ensuremath{\sim}10%\ensuremath∼10 of the dominant superexchange interaction in the case of a spin-chain compound KCuMoO4(OH){\mathrm{KCuMoO}}_{4}(\mathrm{OH})KCuMoO4​(OH) when the DC electric field of \ensuremath∼1MV/cm\ensuremath{\sim}1\phantom{\rule{3.33333pt}{0ex}}\mathrm{MV}/\mathrm{cm}\ensuremath∼1MV/cm is applied.
We theoretically propose a route to control magnetic and topological orders in a broad class of insulating magnets with a DC electric field. We show from the strong-coupling expansion that magnetic exchange interactions along the electric field direction are generally enhanced in Mott insulators. Employing this DC field effect, we demonstrate that several magnetic or topological ordered phases such as quantum spin liquids and Haldane-gap states can be induced if we apply a strong enough DC electric field to typical frustrated or low-dimensional magnets. Our proposal is effective especially for magnets in the vicinity of magnetic phase transition points, and would also be applicable for magnets under low-frequency AC electric fields such as terahertz laser pulses. A similar strategy of controlling exchange interactions can also be utilized in cold atomic systems.
The triangular lattice Hubbard model at strong coupling, whose effective spin model contains both Heisenberg and ring exchange interactions, exhibits a rich phase diagram as the ratio of the hopping ttt to on-site Coulomb repulsion UUU is tuned. This includes a chiral spin liquid (CSL) phase. Nevertheless, this exotic phase remains challenging to realize experimentally because a given material has a fixed value of t/Ut/Ut/U, which is difficult to tune with external stimuli. One approach to address this problem is applying a dc electric field, which renormalizes the exchange interactions as electrons undergo virtual hopping processes; in addition to creating virtual doubly occupied sites, electrons must overcome electric potential energy differences. Performing a small t/Ut/Ut/U expansion to fourth order, we derive the ring exchange model in the presence of an electric field and find that it not only introduces spatial anisotropy but also tends to enhance the ring exchange term compared to the dominant nearest-neighbor Heisenberg interaction. Thus, increasing the electric field serves as a way to increase the importance of the ring exchange at constant t/Ut/Ut/U. Through density matrix renormalization group calculations, we compute the ground-state phase diagram of the ring exchange model for two different electric field directions. In both cases, we find that the electric field shifts the phase boundary of the CSL towards a smaller ratio of t/Ut/Ut/U. Therefore, the electric field can drive a magnetically ordered state into the CSL. This explicit demonstration opens the door to tuning other quantum spin systems into spin liquid phases via the application of an electric field.
In this dissertation we present the results of a theoretical investigation of spin models on two-dimensional and quasi one-dimensional lattices, all unified under the concept of quantum frustrated antiferromagnetism, and all discussing various aspects of the antiferromagnetic Heisenberg model on the kagomé lattice. In the Introduction (Chapter 1), we discuss at some length such concepts as frustration and superexchange, among others, which are of common relevance in the rest of the chapters. In Chapter 2, we study the effect of Dzyaloshinskii--Moriya (DM) interactions on the zero-temperature magnetic susceptibility of systems whose low energy can be described by short-range valence bond states. Our work shows that this treatment is consistent with the experimentally observed non-vanishing susceptibility -- in the specified temperature limit -- of the spin-1/2 kagomé antiferromagnetic compound ZnCu3(OH)6Cl2, also known as herbertsmithite. Although the objective of this work is explaining the aforementioned characteristic of the experimental system, our methods are more general and we apply them to the checkerboard and Shastry-Sutherland lattices as well. In Chapter 3, we discuss our findings in the study of ghost-mediated domain wall interactions in the diamondback ladder. These domain walls are the the spin excitations -- the kinks and the antikinks -- separating the ground states along one chain of the ladder. While as individual entities an antikink is energy costly and a kink energy free, our study finds that both interact via the ghosts that they produce in the opposite side of the ladder from where they are located. Through the study of these ghosts, we find that domain walls proliferate in the system above a critical value of the system's coupling constants. It is this proliferation that makes their treatment as free, non-interacting particles impossible, so we study here their interactions both quantitatively and qualitatively, in a region where the latter are yet not very strong, namely below the critical point. Based on the calculated two-body interaction potential, domain walls interact attractively (repulsively) when separated at even (odd) distances, with a strength that decays as 1/sp, where s is their separation and p<1. We also consider higher-order interactions. In the last chapter, Chapter 4, we present our study of the spin-1 kagomé Heisenberg antiferromagnet. Our approach is to first consider an SU(2)-symmetric parent Hamiltonian with known ground states on the S=1 kagomé lattice, in which nearest-neighbor Heisenberg interactions are already present. We then enhance these interactions by an additional Heisenberg term added perturbatively in order to move the system closer to a pure Heisenberg antiferromagnet. The results of this enhancement is obtaining a description of the system in terms of an effective Hamiltonian, namely a transverse field Ising AF on the triangular lattice. Based on the particular values of this effective Hamiltonian, our system is found to be in the order-by-disorder phase.
The interplay between the Kondo effect, indirect magnetic interaction, and geometrical frustration is studied in the Kondo lattice on the one-dimensional zigzag ladder. Using the density-matrix renormalization group, the ground-state and various short- and long-range spin- and density-correlation functions are calculated for the model at half filling as a function of the antiferromagnetic Kondo interaction down to J=0.3tJ=0.3tJ=0.3t, where ttt is the nearest-neighbor hopping on the zigzag ladder. Geometrical frustration is shown to lead to at least two critical points: Starting from the strong-JJJ limit, where almost local Kondo screening dominates and where the system is a nonmagnetic Kondo insulator, antiferromagnetic correlations between nearest-neighbor and next-nearest-neighbor local spins become stronger and stronger, until at ${J}_{\mathrm{c}}^{\mathrm{dim}}\ensuremath{\approx}0.89t$ frustration is alleviated by a spontaneous breaking of translational symmetry and a corresponding transition to a dimerized state. This is characterized by antiferromagnetic correlations along the legs and by alternating antiferro- and ferromagnetic correlations on the rungs of the ladder. A mechanism of partial Kondo screening that has been suggested for the Kondo lattice on the two-dimensional triangular lattice is not realized in the one-dimensional case. Furthermore, within the symmetry-broken dimerized state, there is a magnetic transition to a ${90}^{\ensuremath{\circ}}$ quantum spin spiral with quasi-long-range order at ${J}_{\mathrm{c}}^{\mathrm{mag}}\ensuremath{\approx}0.84t$. The quantum-critical point is characterized by a closure of the spin gap (with decreasing JJJ) and a divergence of the spin-correlation length and of the spin-structure factor S(q)S(q)S(q) at wave vector $q=\ensuremath{\pi}/2$. This is opposed to the model on the one-dimensional bipartite chain, which is known to have a finite spin gap for all J>0J>0J>0 at half filling.
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 δ−J1−J2 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 fluctuating 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.