We present Raman scattering studies of the structural and magnetic phases that accompany temperature- and field-dependent melting of charge- and orbital-order (COO) in La0.5Ca0.5MnO3 and La0.25Pr0.375Ca0.375MnO3. Our results show that thermal and field-induced COO melting in La0.5Ca0.5MnO3 exhibits three stages in a heterogeneous melting process associated with a structural change: a long-range, strongly JT distorted/COO regime; a coexistence regime; and weakly JT distorted/PM or FM phase. We provide a complete structural phase diagram of La0.5Ca0.5MnO3 for the temperature and field ranges 6<=T<=170 K and 0<=H<=9 T. We also investigate thermal and field-induced melting in La0.25Pr0.375Ca0.375MnO3 to elucidate the role of disorder in melting of COO. We find that while thermal melting of COO in La0.25Pr0.375Ca0.375MnO3 is quite similar to that in La0.5Ca0.5MnO3, the field-induced transition from the COO phase to the weakly JT-distorted/FM phase in La0.25Pr0.375Ca0.375MnO3 is very abrupt, and occurs at significantly lower fields (H~2 T at T~0 K) than in La0.5Ca0.5MnO3 (H~30 T at T=0 K). Moreover, the critical field H_c increases with increasing temperature in La0.25Pr0.375Ca0.375MnO3 in contrast to La0.5Ca0.5MnO3. To explain these differences, we propose that field-induced melting of COO in La0.25Pr0.375Ca0.375MnO3 is best described as the field-induced percolation of FM domains, and we suggest that Griffiths phase physics may be an appropriate theoretical model for describing the unusual temperature- and field- dependent transitions observed in La0.25Pr0.375Ca0.375MnO3.
The magnetic correlations in the charge- and orbital-ordered manganite La(0.5)Sr(1.5)MnO(4) have been studied by elastic and inelastic neutron scattering techniques. Out of the well-defined CE-type magnetic structure with the corresponding magnons a competition between CE-type and ferromagnetic fluctuations develops. Whereas ferromagnetic correlations are fully suppressed by the static CE-type order at low temperature, elastic and inelastic CE-type correlations disappear with the melting of the charge-orbital order at high temperature. In its charge-orbital disordered phase, La(0.5)Sr(1.5)MnO(…
Dc magnetic measurements across the charge ordering (CO) transition temperature (T$_{CO}$) in polycrystalline Pr$_{0.5}$Ca$_{0.5}$Mn$_{0.975}$Al$_{0.025}$O$_3$ have been performed under simultaneous influence of external hydrostatic pressure (P) and magnetic field (H). We show the first experimental evidence that the melting of charge order instability obey an interesting scaling function, $δ$T$_{CO}$/P$^α$ = $f$(H/P$^β$) in H-P-T landscape, where $δ$T$_{CO}$ is the suppression of T$_{CO}$ by P and H. Corresponding values of the exponents, $α$ = 1.63 and $β$ = 0.33 have been extracted from dat…
We report the evolution of the Raman active A_g phonon modes in the charge-ordered manganite Pr_{0.63}Ca_{0.37}MnO_{3} as a function of temperature from 300K to 25K. Our studies reveal that the linewidths of A_g(2) and A_g(4) phonons increase as temperature decreases. This anomalous temperature dependence of phonon lineshapes, seen for the first time in charge ordered manganites, can be quantitatively understood in terms of strong spin-phonon coupling involving t_{2g} spins and A_g phonons.
We report on a high-pressure Raman study on two members of the La$_{1-x}$Ca$_x$MnO$_{3-δ}$ manganite family ($x=0.20$, $δ=0$ and $δ=0.08$). The results obtained for the $δ=0$ sample show a different behavior in the low and high pressure regimes ascribed to the onset of a new pressure-activated interaction previously invoked in other manganite compounds. The comparison of our results with literature data gives further support to the identification of the Jahn-Teller active stretching mode and shows that pressure-induced octahedral symmetrization is more effective in systems exhibiting a lower m…
We report an inelastic light scattering study of the effects of charge-ordering on the spin-, charge-, and lattice-dynamics in ${\rm Bi}_{1-x}{\rm Ca}_{x}{\rm MnO}_3$ $(x>0.5)$. We find that charge-ordering results in anomalous phonon behavior, such as the appearance of `activated' modes. More significantly, however, the transition to the CO phase results in the appearance of a quasielastic scattering response with the symmetry of the spin chirality operator ($T_{1g}$); this scattering response is thus indicative of magnetic or chiral spin fluctuations in the AFM charge-ordered phase.
We investigated the temperature ($T=$ 15 $\sim $ 290 K) and the magnetic field ($H=$ 0 $\sim $ 17 T) dependent optical conductivity spectra of a charge/orbital ordered manganite, Nd$_{1/2}$Sr$_{1/2}$MnO$_3$. With variation of $T$ and $H$, large spectral weight changes were observed up to 4.0 eV. These spectral weight changes could be explained using the polaron picture. Interestingly, our results suggested that some local ordered state might remain above the charge ordering temperature, and that the charge/orbital melted state at a high magnetic field (i.e. at $H=$ 17 T and $% T=$ 4.2 K) shoul…
We report on Raman scattering measurements of single crystalline La$_{1-x}$Sr$_x$MnO$_3$ ($x$=0, 0.06, 0.09 and 0.125), focusing on the high frequency regime. We observe multi-phonon scattering processes up to fourth-order which show distinct features: (i) anomalies in peak energy and its relative intensity and (ii) a pronounced temperature-, polarization-, and doping-dependence. These features suggest a mixed orbiton-phonon nature of the observed multi-phonon Raman spectra.
We observe a disappearance of electron-hole asymmetry in hole and electron doped manganites of composition Pr(1-x)Ca(x)MnO3 (x=0.36, 0.64), as reflected in the g-parameter values. The bulk property of opposite g-shifts in room temperature seems to have disappeared in nanoparticles. We analyze the results in the light of ferromagnetic fluctuations and melting of charge order in nanoparticles.
Nanowires of Pr_0.57 Ca_0.41 Ba_0.02 MnO_3 (PCBM) (diameter ~ 80-90 nm and length ~ 3.5 mm) were synthesized by a low reaction temperature hydrothermal method. Single-phase nature of the sample was confirmed by XRD experiments. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) were used to characterize the morphology and microstructures of the nanowires. While the bulk PCBM is known to exhibit charge order (CO) below 230 K along with a ferromagnetic transition at 110 K, SQUID measurements on the nanowires of PCBM show that the charge order is completely absent and a…
We report low temperature specific heat measurements of Pr$_{1-x}$Ca$_{x}$MnO$_{3}$ ($0.3\leq x \leq 0.5$) and La$_{0.5}$Ca$_{0.5}$MnO$_{3}$ with and without applied magnetic field. An excess specific heat, $C^{\prime}(T)$, of non-magnetic origin associated with charge ordering is found for all the samples. A magnetic field sufficient to induce the transition from the charge-ordered state to the ferromagnetic metallic state does not completely remove the $C^{\prime}$ contribution. This suggests that the charge ordering is not completely destroyed by a "melting" magnetic field. In addition, the…
We report on the pressure effects on the orbital polaron lattice in the lightly doped manganites $\mathrm{La_{1-x}Sr_xMnO_{3}}$, with $x\sim 1/8$. The dependence of the orbital polaron lattice on $negative$ chemical pressure is studied by substituting Pr for La in $\mathrm{(La_{1-y}Pr_y)_{7/8}Sr_{1/8}MnO_{3}}$. In addition, we have studied its hydrostatic pressure dependence in $\mathrm{(La_{0.9}Pr_{0.1})_{7/8}Sr_{1/8}MnO_{3}}$. Our results strongly indicate that the hopping $t$ significantly contributes to the stabilization of the orbital polaron lattice and that the orbital polarons are ferr…
We present magnetization studies in a series of phase separated La$_{0.5}$Ca$%_{0.5}$MnO$_{3}$ samples, with different low temperature fractions of the ferromagnetic (FM) and charge ordered-antiferromagnetic (CO-AFM) phases. A particular experimental procedure probes the effect of the magnetic field applied while cooling the samples, which promotes FM fraction enlargement and enhances the melting of the CO phase. The response of the system depending on its magnetic field history indicates the existence of three different regimes in the phase separated state which develops below T$_{C}$. Our da…
We report a Raman scattering study of low-temperature, pressure-induced melting of the CDW phase of 1T-TiSe2. Our Raman scattering measurements reveal that the collapse of the CDW state occurs in three stages: (i) For P<5 kbar, the pressure dependence of the CDW amplitude mode energies and intensities are indicative of a ``crystalline'' CDW regime; (ii) for 5 < P < 25 kbar, there is a decrease in the CDW amplitude mode energies and intensities with increasing pressure that suggests a regime in which the CDW softens, and may decouple from the lattice; and (iii) for P>25 kbar, the absence of amp…
We calculated the polarization-dependent Raman scattering cross section spectra of LaMnO3 below the A-type magnetic ordering temperature. Two strong peaks appear around the MnO6 octahedra stretching phonon frequency. One mode shows Ag symmetry, while the other mode shows Bg symmetry. We found that the Ag symmetry peak is a Jahn-Teller phonon coupled to the orbital wave and the Bg symmetry peak is an orbital wave coupled to a Q2 phonon mode via the Jahn-Teller electron phonon coupling.
Raman spectra of LCMO films grown on LAO (001), STO (001), and MgO (001) substrates were studied at different temperatures. The effect of temperature, doping level and strain on Raman spectra are discussed in detail. With decreasing temperature, the changes of Raman spectra are correlated with the disorder-order transition, shuch as: paramagnetism to ferromagnetism, and charge-ordering. The strain induced by lattice-substrate mismatch affects the Raman spectra strongly. The mode induced by disorder of oxygen defects is apparently observed in $La_{0.67}Ca_{0.33}MnO_3$ film on STO due to the lar…
We present a rationalization of the Raman spectra of orthorhombic and rhombohedral, stoichiometric and doped, manganese perovskites. In particular we study RMnO3 (R= La, Pr, Nd, Tb, Ho, Er, Y and Ca) and the different phases of Ca or Sr doped RMnO3 compounds as well as cation deficient RMnO3. The spectra of manganites can be understood as combinations of two kinds of spectra corresponding to two structural configurations of MnO6 octahedra and independently of the average structure obtained by diffraction techniques. The main peaks of compounds with regular MnO6 octahedra, as CaMnO3, highly Ca …
The Mn spin correlations were studied near the O'-O phase transition at T{JT} = 750 K, up to 950 K with 17O and 139La NMR in a stoichiometric LaMnO3 crystalline sample. The measured local hyperfine fields originate from the electron density transfered from the eg- and t2g-orbitals to the 2s(O) and 6s(La) orbits, respectively. By probing the oxygen nuclei, we show that the correlations of the Mn spins are ferromagnetic in the ab-plane and robust up to T{JT} whereas along the c-axis, they are antiferromagnetic and start to melt below T{JT}, at about 550 K. Above T{JT} the ferromagnetic Mn-Mn exc…
We report temperature-dependent surface x-ray scattering studies of the orbital ordered surface in La$_{0.5}$Sr$_{1.5}$MnO$_4$. We find that the interfacial width of the electronic order grows as the bulk ordering temperature is approached from below, though the bulk correlation length remains unchanged. Close to the transition, the surface is so rough that there is no well-defined electronic surface, despite the presence of bulk electronic order, that is the electronic surface has melted. Above the bulk transition, finite-sized isotropic fluctuations of orbital order are observed, with a corr…
Collapse of Jahn-Teller Phonons in La$_{1-x}$Sr$_{x}$MnO$_3$ with Weak Magnetoresistance
University of Colorado Boulder（科罗拉多大学博尔德分校）；Oak Ridge National Laboratory（橡树岭国家实验室）；Japan Atomic Energy Agency（日本原子能机构）；High Energy Accelerator Research Organization (KEK)（高能加速器研究机构）；Comprehensive Research Organization for Science and Society（综合科学研究组织）；Karlsruhe Institute of Technology（卡尔斯鲁厄理工学院）
The dynamics of electrons, spins and phonons induced by optical femtosecond pulses has been simulated for the polaronic crystal $\rm{Pr_{1/2}Ca_{1/2}MnO_3}$. The model used for the simulation has been derived from first-principles calculations. The simulations reproduce the experimentally observed melting of charge/orbital order with increasing fluence. The loss of charge order in the high-fluence regime induces a transition to a ferromagnetic metal. At low fluence, the dynamics is deterministic and coherent phonons are created by the repopulation of electronic orbitals, which are strongly cou…
We report observation of substantial thermal relaxation in single crystal of charge ordered system Pr$_{0.63}$Ca$_{0.37}$MnO$_3$ in an applied magnetic field of H = 8T. The relaxation is observed when the temperature is scanned in presence of a magnetic field in the temperature interval $T_{MH}<T<T_{CO}$ where $T_{CO}$ is the charge ordering temperature and $T_{MH}$ is charge melting temperature in a field. In this temperature range the system has coexisting charged ordered insulator (COI) and ferromagnetic metallic (FMM) phases. No such relaxation is observed in the COI state in H = 0T or in …
The local structure about the Mn site in the half doped system La0.5Ca0.5MnO3 was measured in magnetic fields up 10 T to probe the melting of the charge ordered state. Examination of the Mn-O and Mn-Mn correlations reveal three distinct regions in the structure-field diagram. A broad region with weak field dependence (mainly antiferromatnetic phase below 7.5 T), a narrow-mixed phase region near ~ 8.5 T followed by a ferromagnetic phase region with strong field-structure coupling. At high field the Mn-O radial distribution becomes Gaussian and the Mn-Mn correlations are enhanced - consistent wi…
We present a systematic study of the structure and lattice dynamics at room temperature, and the phonon behavior at low temperatures in orthorhombic Gd$_{1-x}$Y$_{x}$MnO$_{3}$ manganites, with 0 $\leq$ x $\leq$ 0.4, using powder x-ray diffraction and Raman scattering. A thorough analysis towards the correlation between both structural and Raman modes parameters was undertaken. The data obtained at room temperature reveal structural distortions arising from the Jahn-Teller distortion and octahedra tilting. The Jahn-Teller distortion is apparently x-independent, while an increase of Mn-O1-Mn bon…
Strong electronic interactions can drive a system into a state with a symmetry breaking. Lattice frustration or competing interactions tend to prevent a symmetry breaking, leading to quantum disordered phases. In spin systems frustration can produce a spin liquid state. Frustration of a charge degree of freedom also can result in various exotic states, however, experimental data on these effects is scarce. In this work we demonstrate how a charge ordered ferroelectric looses the order on cooling to low temperatures using an example of a Mott insulator on a weakly anisotropic triangular lattice…
The polarized Raman spectra of orthorhombic RMnO3 series (R=La,Pr,Nd,Sm,Eu,Gd,Tb,Dy,Ho,Y) were studied at room temperature. The variation of phonon frequencies with R ionic radius rR as a whole confirms the commonly accepted Raman line assignments with two noticeable exceptions: (1) with decreasing rR the stretching Ag(1) and bending Ag(3) modes strongly mix for R=Sm to Tb, while for further decrease or rR (R=Dy,Ho,Y) the Ag(3) mode is observed at higher frequency than Ag(1) mode; (2) similar distortion-dependent mode mixing takes place for the rotational Ag(2) and O1(x) [Ag(7)] modes. The mod…
The ferrimagnetic spinel Mn3O4 exhibits large and anisotropic changes in electronic and structural properties in response to an applied magnetic field. These changes are thought to result from the field-dependent tuning---via strong spin-lattice coupling---between two nearly degenerate magnetostructural phases. Recent variable-magnetic-field studies of Mn3O4 have been performed on melt-grown crystals, which can exhibit twin domains due to a Jahn-Teller structural transition below the melting temperature. Because of the near degeneracy of the magnetostructural phases, however, strain associated…
We employ time-resolved resonant x-ray diffraction to study the melting of charge order and the associated insulator-metal transition in the doped manganite Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ after resonant excitation of a high-frequency infrared-active lattice mode. We find that the charge order reduces promptly and highly nonlinearly as function of excitation fluence. Density functional theory calculations suggest that direct anharmonic coupling between the excited lattice mode and the electronic structure drive these dynamics, highlighting a new avenue of nonlinear phonon control.
The transport and noise properties of Pr_{0.7}Ca_{0.3}MnO_{3} epitaxial thin films in the temperature range from room temperature to 160 K are reported. It is shown that both the broadband 1/f noise properties and the dependence of resistance on electric field are consistent with the idea of a collective electrical transport, as in the classical model of sliding charge density waves. On the other hand, the observations cannot be reconciled with standard models of charge ordering and charge melting. Methodologically, it is proposed to consider noise-spectra analysis as a unique tool for the ide…
The Shastry-Sutherland compound SrCu$_2$(BO$_3$)$_2$ constituting orthogonally coupled dimers harbors a $S=0$ singlet ground state. The confluence of strong interdimer interaction and frustration engenders a spectrum of low-energy excitations including localized triplons as well as singlet and triplet bound states. Their dynamics are controlled by an external magnetic field and temperature. Here, we employ high-field Raman spectroscopy to map the field and temperature evolution of such bosonic composite quasiparticles on approaching the 1/8 magnetization plateau. Our study unveils that the mag…
