Elastic and structural instability of cubic Sn3N4 and C3N4 under pressure

We use in-situ high pressure angle dispersive x-ray diffraction measurements to determine the equation of state of cubic tin nitride Sn3N4 under pressure up to about 26 GPa. While we find no evidence for any structural phase transition, our estimate of the bulk modulus (B) is 145 GPa, much lower than the earlier theoretical estimates and that of other group IV-nitrides. We corroborate and understand these results with complementary first-principles analysis of structural, elastic and vibrational properties of group IV-nitrides, and predict a structural transition of Sn3N4 at a higher pressure of 88 GPa compared to earlier predictions of 40 GPa. Our comparative analysis of cubic nitrides shows that bulk modulus of cubic C3N4 is the highest (379 GPa) while it is structurally unstable and should not exist at ambient conditions.Comment: 5 pages, 4 figure

Brillouin Scattering Studies of La_{0.77}Ca_{0.23}MnO_3 Across Metal-Insulator Transition

Temperature-dependent Brillouin scattering studies have been carried out on La_{0.77}Ca_{0.23}MnO_3 across the paramagnetic insulator - ferromagnetic metal (I-M) transition. The spectra show a surface Rayleigh wave (SRW) and a high velocity pseudo surface acoustic wave (HVPSAW) besides bulk acoustic waves (BAW). The Brillouin shifts associated with SRW and HVPSAW show blue-shifts, where as the frequencies of the BAW decrease below the I-M transition temperature (T_C) of 230 K. These results can be understood based on the temperature dependence of the elastic constants. We also observe a central peak whose width is maximum at T_C.Comment: 7 pages, 8 figure

Griffiths phase-like behaviour and spin-phonon coupling in double perovskite Tb2_{2}NiMnO6_{6}

The Griffiths phase-like features and the spin-phonon coupling effects observed in Tb$_2$NiMnO$_6$ are reported. The double perovskite compound crystallizes in monoclinic $P2_1/n$ space group and exhibits a magnetic phase transition at $T_c \sim$ 111 K as an abrupt change in magnetization. A negative deviation from ideal Curie-Weiss law exhibited by 1/$\chi(T)$ curves and less-than-unity susceptibility exponents from the power-law analysis of inverse susceptibility are reminiscent of Griffiths phase-like features. Arrott plots derived from magnetization isotherms support the inhomogeneous nature of magnetism in this material. The observed effects originate from antiferromagnetic interactions which arise from inherent disorder in the system. Raman scattering experiments display no magnetic-order-induced phonon renormalization below $T_c$ in Tb$_2$NiMnO$_6$ which is different from the results observed in other double perovskites and is correlated to the smaller size of the rare earth. The temperature evolution of full-width-at-half-maximum for the {\it stretching} mode at 645 cm$^{-1}$ presents an anomaly which coincides with the magnetic transition temperature and signals a close connection between magnetism and lattice in this material.Comment: 17 pages, 8 figures; accepted in J. Appl. Phy

Switching of the topologically trivial and non-trivial quantum phase transitions in compressed 1T-TiTe2: Experiments and Theory

We report the structural, vibrational and electrical transport properties up to 16 GPa of the 1T-TiTe2, a prominent layered 2D system, which is predicted to show a series of topologically trivial - nontrivial transitions under hydrostatic compression. We clearly show signatures of two iso-structural transition at 2 GPa and 4 GPa obtained from the minima in c/a ratio concomitant with the phonon linewidth anomalies of Eg and A1g modes at around the same pressures, providing strong indication of unusual electron-phonon coupling associated to these transitions. Resistivity presents nonlinear behavior over similar pressure ranges providing a strong indication of the electronic origin of these pressure driven isostructural transitions. Our data thus provide clear evidences of topological changes at A and L point of the Brillouin zone predicted to be present in the compressed 1T-TiTe2. Between 4 GPa and 8 GPa, the c/a ratio shows a plateau suggesting a transformation from an anisotropic 2D layer to a quasi 3D crystal network. First principles calculations suggest that the 2D to quasi 3D evolution without any structural phase transitions is mainly due to the increased interlayer Te-Te interactions (bridging) via the charge density overlap. In addition to the pressure dependent isostructural phase transitions, our data also evidences the occurrence of a first order structural phase transition from the trigonal (P-3m1) phase at higher pressures. We estimate the start of this structural phase transition to be 8 GPa and the symmetric of the new high-pressure phase to be monoclinic (C2/m).Comment: 22 pages, 11 Figures, 2 Table

Influence of lattice distortion on the Curie temperature and spin-phonon coupling in LaMn0.5_{0.5}Co0.5_{0.5}O3_{3}

Two distinct ferromagnetic phases of LaMn$_{0.5}$Co$_{0.5}$O$_{3}$ having monoclinic structure with distinct physical properties have been studied. The ferromagnetic ordering temperature $\textit{T}_{c}$ is found to be different for both the phases. The origin of such contrasting characteristics is assigned to the changes in the distance(s) and angle(s) between Mn - O - Co resulting from distortions observed from neutron diffraction studies. Investigations on the temperature dependent Raman spectroscopy provide evidence for such structural characteristics, which affects the exchange interaction. The difference in B-site ordering which is evident from the neutron diffraction is also responsible for the difference in $\textit{T}_{c}$. Raman scattering suggests the presence of spin-phonon coupling for both the phases around the $\textit{T}_{c}$. Electrical transport properties of both the phases have been investigated based on the lattice distortion.Comment: 9 figure

Spin-phonon coupling in multiferroic RCrO3_3 (R-Y, Lu, Gd, Eu, Sm): A Raman study

Raman study on a select few orthochromites, RCrO$_3$ (R = Y, Lu, Gd, Eu and Sm) shows that the phonon behavior at TN in compounds with magnetic R-ion (Gd and Sm) is remarkably different from that of non-magnetic R-ion (Y, Lu and Eu). While anomalies in most of the observed phonon frequencies in all these compounds may result from the distortion of CrO$_6$ octahedra due to size effect and magnetostriction arising from Cr-ordering, the anomalous behavior of their linewidths observed at TN for the compounds with only magnetic R-ion suggests spin-phonon coupling. The presence of spin-phonon coupling and the anomalies in the low frequency modes related to R-ion motion in orthochromites (R = Gd and Sm) support the suggestion that the coupling between 4f-3d moments play important role in inducing switchable electric polarization.Comment: 6 pages (two column format), 7 figures; The updated version of the manuscript can be found at Euro. Phys. Lett. 101, 17008 (2013

Reversible Pressure-Induced Amorphization in Solid C70 : Raman and Photoluminescence Study

We have studied single crystals of $C_{70}$ by Raman scattering and photoluminescence in the pressure range from 0 to 31.1 GPa. The Raman spectrum at 31.1 GPa shows only a broad band similar to that of the amorphous carbon without any trace of the Raman lines of $C_{70}$. After releasing the pressure from 31.1 GPa, the Raman and the photoluminescence spectra of the recovered sample are that of the starting $C_{70}$ crystal. These results indicate that the $C_{70}$ molecules are stable upto 31.1 GPa and the amorphous carbon high pressure phase is reversible, in sharp contrast to the results on solid $C_{60}$. A qualitative explaination is suggested in terms of inter- versus intra-molecular interactions.Comment: To appear in Phys. Rev. Lett., 12 pages, RevTeX (preprint format), 3 figures available upon reques

Brillouin scattering studies on charge-ordered manganites

Brillouin scattering studies were carried out for the first time on charge-ordered manganites, namely, Nd0.5Ca0.5MnO3 and Pr0.63Ca0.37MnO3. We observe surface and bulk magnetic excitations (magnons) in the Brillouin spectra with the characteristics of ferromagnetic magnons. The frequency and intensity of these magnons in the temperature range 300 to 25 K, covering both charge-ordering and antiferromagnetic transition, follow exactly the temperature dependence of the DC magnetic susceptibility. The study strongly suggests the presence of ferromagnetic inhomogeneities in the charge-ordered as well as antiferromagnetic phases

Brillouin scattering studies in Fe3_3O4_4 across the Verwey transition

Brillouin scattering studies have been carried out on high quality single crystals of Fe$_3$O$_4$ with [100] and [110] faces in the temperature range of 300 to 30 K. The room temperature spectrum shows a surface Rayleigh wave (SRW) mode at 8 GHz and a longitudinal acoustic (LA) mode at 60 GHz. The SRW mode frequency shows a minimum at the Verwey transition temperature $T_V$ of 123 K. The softening of the SRW mode frequency from about 250 K to $T_V$ can be quantitatively understood as a result of a decrease in the shear elastic constant C$_{44}$, arising from the coupling of shear strain to charge fluctuations. On the other hand, the LA mode frequency does not show any significant change around $T_V$, but shows a large change in its intensity. The latter shows a maximum at around 120 K in the cooling run and at 165 K in the heating run, exhibiting a large hysteresis of 45 K. This significant change in intensity may be related to the presence of stress-induced ordering of Fe$^{3+}$ and Fe$^{2+}$ at the octahedral sites, as well as to stress-induced domain wall motion.Comment: 14 pages, 3 figures, accepted in Physical Review B 200