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MAGNETIC SYSTEMS 2009Nd 3+ crystal-field studies of weakly doped Nd 1−x Ca x MnO 3Manganites RMnO 3 compounds based on lanthani<strong>des</strong> (R)are antiferromagnetic systems with important Jahn-Tellerdistortions. Substitution of lanthani<strong>des</strong> by Ba, Sr, or Caleads to appearance of double exchange interactions, reductionof Jahn-Teller-type distortions and simultaneous observationof metallic and ferromagnetic character with increasingmolar fraction x (R 1−x A x MnO 3 , A = Ba, Sr, orCa). In this work, Nd 3+ ions crystal field (CF) excitationsin Nd 1−x Ca x MnO 3 (x = 0.025, 0.05 and 0.1) singlecrystals have be<strong>en</strong> investigated using infrared transmissionspectroscopy at differ<strong>en</strong>t temperatures and external magneticfields and compared to undoped NdMnO 3 .Our study reveals the pres<strong>en</strong>ce of a magnetic phase separationin the doped samples. As a consequ<strong>en</strong>ce of dopingby calcium, we report the detection of two sets ofCF levels, as already observed in Nd 1−x Sr x MnO 3 [see S.Jandl et al., Phys. Rev. B 71, 024417 (2005) and S.Jandl et al., ibid 72, 024423 (2005)]. One is associatedwith unperturbed sites related to the NdMnO 3 antiferromagnetismwith its typical Zeeman splitting below Neeltemperature, and a second one is linked to perturbed sitesin the vicinity of the Ca 2+ cations where local A-typeantiferromagnetism is suppressed. While the <strong>en</strong>ergy differ<strong>en</strong>cesbetwe<strong>en</strong> the two sets are within the uncertaintyvalues of the CF parameters that <strong>des</strong>cribe the NdMnO 3CF Hamiltonian and predict the CF levels, their detectionstr<strong>en</strong>gth<strong>en</strong>s the role of local probe the rare-earth CF levelsplay in manganite compounds. Finally, under appliedexternal magnetic field, Zeeman splittings are observed inNdMnO 3 and Nd 0.975 Ca 0.025 MnO 3 , while they are maskedin Nd 0.95 Ca 0.05 MnO 3 and Nd 0.9 Ca 0.1 MnO 3 . The latter resultsare due to doping-induced band broad<strong>en</strong>ing and possibletwining.The Zeeman splitting well-resolved at lower doping d<strong>en</strong>sitiesis demonstrated in Fig. 104, where the middle-infraredtransmission spectra of investigated samples tak<strong>en</strong> withoutand with the externally applied magnetic field (parts A andB) are pres<strong>en</strong>ted. For details see, S. Jandl et al., J. Magn.Magn. Mater. 321, 3607 (2009).Figure 104: Transmission spectra showing 4 I 9/2 → 4 I 11/2 Nd 3+transitions in Nd 1−x Ca x MnO 3 at T = 1.8 K: x = 0 (a), x = 0.025(b), x = 0.05 (c) and x = 0.1 (d) measured at (A) B = 0 T andB = 12 T. ∗ indicates the new CF excitations that are due to thedoping. The Zeem<strong>en</strong> splitting is well-resolved at lower conc<strong>en</strong>trations(x = 0 and 0.025) but masked at higher doping d<strong>en</strong>sities.M. OrlitaS. Jandl (University of Sherbrooke, Canada), A. A. Mukhin, V. Yu. Ivanov (G<strong>en</strong>eral Physics Institute of the RussianAcademy of Sci<strong>en</strong>ces, Moscow, Russia), A. Balbashov (Moscow Power Engineering Institute, Moscow, Russia)78

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