1,525 research outputs found

    Rotational Dynamics of Organic Cations in CH3NH3PbI3 Perovskite

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    Methylammonium lead iodide (CH3NH3PbI3) based solar cells have shown impressive power conversion efficiencies of above 20%. However, the microscopic mechanism of the high photovoltaic performance is yet to be fully understood. Particularly, the dynamics of CH3NH3+ cations and their impact on relevant processes such as charge recombination and exciton dissociation are still poorly understood. Here, using elastic and quasi-elastic neutron scattering techniques and group theoretical analysis, we studied rotational modes of the CH3NH3+ cation in CH3NH3PbI3. Our results show that, in the cubic (T > 327K) and tetragonal (165K < T < 327K) phases, the CH3NH3+ ions exhibit four-fold rotational symmetry of the C-N axis (C4) along with three-fold rotation around the C-N axis (C3), while in orthorhombic phase (T < 165K) only C3 rotation is present. Around room temperature, the characteristic relaxation times for the C4 rotation is found to be ps while for the C3 rotation ps. The -dependent rotational relaxation times were fitted with Arrhenius equations to obtain activation energies. Our data show a close correlation between the C4 rotational mode and the temperature dependent dielectric permittivity. Our findings on the rotational dynamics of CH3NH3+ and the associated dipole have important implications on understanding the low exciton binding energy and slow charge recombination rate in CH3NH3PbI3 which are directly relevant for the high solar cell performance

    Towards a Microscopic Model of Magnetoelectric Interactions in Ni3V2O8

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    We develop a microscopic magnetoelectric coupling in Ni3_3V2_2O8_8 (NVO) which gives rise to the trilinear phenomenological coupling used previously to explain the phase transition in which magnetic and ferroelectric order parameters appear simultaneously. Using combined neutron scattering measurements and first-principles calculations of the phonons in NVO, we determine eleven phonons which can induce the observed spontaneous polarization. Among these eleven phonons, we find that a few of them can actually induce a significant dipole moment. Using the calculated atomic charges, we find that the required distortion to induce the observed dipole moment is very small (~0.001 \AA) and therefore it would be very difficult to observe the distortion by neutron-powder diffraction. Finally, we identify the derivatives of the exchange tensor with respect to atomic displacements which are needed for a microscopic model of a spin-phonon coupling in NVO and which we hope will be obtained from a fundamental quantum calculation such as LDA+U. We also analyze two toy models to illustrate that the Dzyaloskinskii-Moriya interaction is very important for coexisting of magnetic and ferroelectric order but it is not the only mechanism when the local site symmetry of the system is low enough.Comment: 20 pages, 10 figure

    A Neutron Elastic Diffuse Scattering Study of PMN

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    We have performed elastic diffuse neutron scattering studies on the relaxor Pb(Mg1/3_{1/3}Nb2/3_{2/3})O3_3 (PMN). The measured intensity distribution near a (100) Bragg peak in the (hk0) scattering plane assumes the shape of a butterfly with extended intensity in the (110) and (11ˉ\bar{1}0) directions. The temperature dependence of the diffuse scattering shows that both the size of the polar nanoregions (PNR) and the integrated diffuse intensity increase with cooling even for temperatures below the Curie temperature TC213T_C \sim 213 K.Comment: Submitted to PR

    High Resolution Study of Spin Excitations in the Shastry-Sutherland Singlet Ground State of SrCu2(BO3)2

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    High resolution, inelastic neutron scattering measurements on SrCu2(BO3)2 reveal the dispersion of the three single triplet excitations continuously across the (H,0) direction within its tetragonal basal plane. These measurements also show distinct Q dependencies for the single and multiple triplet excitations, and that these excitations are largely dispersionless perpendicular to this plane. The temperature dependence of the intensities of these excitations is well described as the complement of the dc-susceptibility of SrCu2(BO3)2.Comment: 4 pages, 4 figures. Submitted to PR

    Revisiting Static and Dynamic Spin Ice Correlations in Ho2Ti2O7

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    Elastic and inelastic neutron scattering studies have been carried out on the pyrochlore magnet Ho2Ti2O7. Measurements in zero applied magnetic field show that the disordered spin ice ground state of Ho2Ti2O7 is characterized by a pattern of rectangular diffuse elastic scattering within the [HHL] plane of reciprocal space, which closely resembles the zone boundary scattering seen in its sister compound Dy2Ti2O7. Well-defined peaks in the zone boundary scattering develop only within the spin ice ground state below ~ 2 K. In contrast, the overall diffuse scattering pattern evolves on a much higher temperature scale of ~ 17 K. The diffuse scattering at small wavevectors below [001] is found to vanish on going to Q=0, an explicit signature of expectations for dipolar spin ice. Very high energy-resolution inelastic measurements reveal that the spin ice ground state below ~ 2 K is also characterized by a transition from dynamic to static spin correlations on the time scale of 10^{-9} seconds. Measurements in a magnetic field applied along the [11ˉ{\bar1}0] direction in zero-field cooled conditions show that the system can be broken up into orthogonal sets of polarized alpha chains along [11ˉ{\bar1}0] and quasi-one-dimensional beta chains along [110]. Three dimensional correlations between beta chains are shown to be very sensitive to the precise alignment of the [11ˉ{\bar1}0] externally applied magnetic field.Comment: 11 pages, 10 figures. Submitted for publicatio
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