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Phys. Status Solidi B, 13 (2010) / DOI 10.1002/pssb.200983028

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Coupled spinphonon excitations in helical multiferroics

Chenglong Jia* and Jamal Berakdar

basic solid state physics

Institut fur Physik, Martin Luther Universitat Halle-Wittenberg, Heinrich-Damerow-Strae 4, 06120 Halle, Germany Received 23 June 2009, revised 24 September 2009, accepted 24 September 2009 Published online 9 February 2010 PACS 71.70.Ej, 71.70.Gm, 75.85.t, 77.80.e
* Corresponding

author: e-mail cheng-long.jia@physik.uni-halle.de, Phone: 49 345 5528528, Fax: 49 345 5527393

Both the DzyaloshiskiiMoriya interaction and the exchange striction are shown to affect dynamically the magnetoelectric excitations in the helical multiferroics. The exchange striction results in a biquadratic interaction between the spins and the transverse phonons, giving rise to quantum uctuations of the ferroelectric polarization P. This leads to low-lying phonon modes that are perpendicular to P and to the helical spins at

small wave vector but are parallel to P at a wave vector close to the magnetic modulation vector. For spin-1/2 helimagnet, the local polarization can be completely reversed by the spin uctuation, and so does the direction of the on-site spin chirality, which allows for a nite differential scattering intensity of polarized neutrons from a cycloidal magnet.

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1 Introduction Details of the coupling mechanisms of the magnetic and the ferroelectric (FE) order in multiferroics is currently under active research. This is due to the fundamental physics involved and to promising technological applications [1]. Our focus here is the helical multiferroics such as perovskite RMnO3 with R Tb, Dy, Gd, and Eu1xYx [2]. The experimental nding is that RMnO3 has an incommensurate spiral magnetic order and a nite FE polarization. The driving mechanisms of this ordering is an interplay between the exchange interaction and the DzyaloshiskiiMoriya (DM) interaction. Specically, the spinorbit coupling with a strength a related to the d(p)orbitals of the magnetic (oxygen) ions results in the FE ^ polarization [3, 4] P a^ij Si Sj . eij is a unit vector e connecting the sites i and j. Generally, it is to be expected that the magnetoelectric coupling will affect not only the material static properties but also the dynamical response. Based on the above spin-current model, the dynamical properties of DM interaction were studied in Refs. [57]. A novel magnonphonon excitation so-called electromagnon, was theoretically predicted. When the spiral plane rotates with respected to the axis of the helical wave vector, so does the induced electric polarization, which couples the magnetic excitation to the electric eld E of the radiation in the direction perpendicular to the spin spiral plane [5]. Experimental observations in RMnO3 [8] and

Eu0.75Y0.25MnO3 [9] seem to be consistent with this nding. However, a detailed study of the terahertz spectrum of Eu1xYxMnO3 [10] revealed that infrared absorption along the spontaneous polarization direction is also possible, which is not explained by the theory mentioned above. This violation suggests that the static and the dynamic magnetoelectric coupling may be different [11]. We carried out a detailed investigations of the dynamical properties of the multiferroics and nd that both, the DM interaction and the (super-)exchange striction play an essential role and need to be taken into account. 2 Theoretical model We consider a one-dimensional spin chain along the z-axis with a frustrated spin interaction. An effective model that captures the spin phonon coupling [5, 12] corresponds to the Hamiltonian H Hs HDM Hp P J1 ri rj Si Sj
hijinn

Hs

J2 rl rm Sl Sm P

hlminnn

(1)

HDM l ui ^z Si Si1 e i P P k 1 Hp 2 u2 2M P2 i i
i i

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C. Jia and J. Berakdar: Coupled spinphonon excitations in helical multiferroics

where the notation hijinn indicates that i and j are nearestneighbors (nn), and hlminnn corresponds to l and m being next-nearest-neighboring (nnn). The competition between the nn ferromagnetic interaction (J1 < 0) and the nnn antiferromagnetic interaction (J2 > 0) leads to magnetic frustration and realizes a spiral spin ordering with the wave vector cos Q J1 =4J2 [1315]. Hp describes optical phonons. The spinphonon interaction HDM originates from a spinorbital coupling and breaks the inversion symmetry along the chain. Minimizing the energy yields the condition of the atomic displacement and the local spin conguration l ^ ui ez Si Si1 : k (2)

Particularly, if the zx helical spins are aligned along the chain, i.e., Si Ssin iQ; 0; cos iQ, a uniform electric polarization P along the x direction is induced by the condensation of the transverse optical phonons, P e u0 e e lS2 =ksin Q^x with a Born charge e. Generally, ux cannot be softened through the hybridization between the transverse optical phonons and the magnons because of k=M ) JS. The spontaneous FE polarization Px is frozen at e ux in the FE phase. However, after accounting for the 0 super-exchange striction, we have transverse acoustic phonons, which induces the uctuation of the polarization hybridized with the spin bosons and soften thus the transverse phonon behavior. Considering small atomic displacements perpendicular ^ to the chain, u? ez 0, the exchange energy J falls off as a i power law with the separation of the magnetic ions h i g 1;2 ? J1;2 jri rj j % J1;2 1 ui u? 2 (3) j 2 where g is in the range of 614 [16]. The emerging transverse acoustic phonon mode is coupled to the spins with the bi-quadratic interaction $ u? u? 2 Si Sj . i j This dynamical coupling does not contribute any additional static electric polarization but induces the uctuation of the electric dipole moment due to the low-frequency excitation modes of transverse acoustic phonon. We write explicitly the atomic displacements into two parts: (i) the statical part ui ux ; 0; 0 and (ii) the dynamical part 0 dui dux ; duy ; 0. Retaining terms up to the second order i i in the quantum uctuation, the spin-current model delivers the following coupling terms: P ~ ~ ~ HDM lS cos Q dux Sx Sx i i1 i i P y y (4) ~ cos Qi1 Sy cos Qi ~ lS dui Si i1
i

spin chirality as the average of the outer product of two ^ adjacent spins ci si si1 =jsi si1 j, in accord with the spin current model the direction of local FE polarization is determined by the on-site spin chirality [14]. The dynamical DM interaction in Eq. (4) yields the coupling term between the spin and the spin chirality in the spin-1/2 multiferroics, P x x P x x ^x ^ s sx s c i ci ^i1 ^i i ^i ^i1 ci , which indicates that ^ s when the spin at site i is ipped, si ! ^i , the direction of ^ ^ spin-chirality ci and ci1 are also reversed. Assuming all spins point along their corresponding classical directions in the ground state of the spin-1/2 helical magnet as in NaCu2O2, where the J1 J2 spin model provides a good description of the helix state [15]. So the spin interaction can s ^ be ferromagnetically given as Js Q^i sj where Q is taken as the pitch angle along the chain. An effective model that describes the interplay between the helical spin and spinchirality has the form P ^ ^ Hsc Js ^i ^j Jc ci cj s s i;j P x x (5) ^i ^ c g si ^i1 cx :
i

The Hilbert space can be considered as the tensor product space jii ! jsz is  jcz ic : Now if the spin at site i is ipped, i i the spin and spin-chirality excitations are mixed due to the spinphonon coupling. The expected value of spin-chirality is given by h^i 1 h^i; c s (6)

which is less than one. The experimental data for a nite differential scattering intensity of polarized neutrons from LiCu2O2 [14] suggests h^i % 0:3 which is consistent with c the estimated value h^i 0:44 based on the ordered c moment, 0.56mB per magnetic copper site [15]. For RMnO3, the helical spin ordering occurs, corresponding to the condensation of the spin bosons. By using the standard linear-spin-wave approximation, a dynamical magnonphonon interaction reads ~ HDM lS cos Q lS P
q

~ dux Sx cos q 1 q q (7) : 2

~ X duy Sy eiQ eiqQ q qQ

q

duy is hybridized with the spin at q Q (optical magnons), q ~ but dux is coupled to Sx at q (acoustical magnons). The q polarization correlation functions are given as ( dux jdux ) q q v2 v2 s ; v2 v2 v2 v2 s p s sp 1 #; ( duy jduy ) " q q P 2 2 v 2 l S3 0 Gs q M v p 2M Mv4 v2 v2 p
q0 qQ

~ ~ in the rotated spin frame: Sx Sx cos iQ Sz sin iQ, i i i ~ ~ ~ Sy Sy , and Sz Sx sin iQ Sz cos iQ. i i i i i 3 Results and analysis In spin-1/2 helical multiferroics, such as LiCu2O2 [14], the spin uctuations may spontaneously reverse the local spin. Dening the vector of
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Original Paper
Phys. Status Solidi B (2010) 3

where vp is the frequency for the transverse phonon, vs(q) is the energy dispersion of the spin excitation, v0sp q 2Aq 2Bql2 S3 cos2 Q1 cos q=k1=2 , and Gs q Q Aq Q2BqQ1 cosq 2Q= v2 vs q Q with   1 Aq J2 cos 2Q 1 cos 2Qcos 2q 2   1 (9) J2 cos 2Q 1 cos 2Qcos 2q 2 l2 S2 sin2 Q 2 cos q; 2k Bq J1 J2 1 cos Qcos q 1 cos 2Qcos 2q 4 4 l2 S2 sin2 Q cos q: 4k

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(10) p At small wave vectors, q $ 0 and vp % k=M , the TA phonon is decoupled from the spins. The antisymmetric DM interaction dominates over the spinphonon coupling. duy is 0 ~ ~ coupled via Sy Sy to the rotation of the spin plane and Q Q the direction of the polarization along the chain. However, at a wave vector close to the magnetic modulation vector, i.e., q $ Q, both the symmetric and antisymmetric magnetoelectric interaction respond to the uctuations of the polarization. Especially, in the direction parallel to the FE polarization P, there is a low-frequency range around vx vs Q where ux couples resonantly to light. Introdu cing an easy-plane spin anisotropy DSy 2 into the spin system, we observe nearly the same low-frequency behavior p of the polarization correlation functions vx % JSD % vy . These conclusions are also qualitatively consistent with experiment observations for Eu1xYxMnO3 [10]. 4 Summary In conclusion, we studied the origin of the magnetoelectric dynamics in the helical multiferroics. At a small wave vector, the DM interaction determines the lowfrequency behavior of the phonons. For a wave vector close to that of the magnetically modulated structure, the exchange striction induces uctuations in the FE polarization, and additional low-lying mode parallel to the FE polarization emerges. Due to the dynamical DM interaction, the spinchirality is strongly coupled to the spin uctuation which implies a large quantum uctuation of the spin-chirality in the ordered spin-1/2 system and results in a nite scattering intensity of polarized neutrons from a cycloidal helimagnet.
Acknowledgements This work is supported by the German Science Foundation DFG through SFB762-B7-functionality of oxide interfaces.

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