-
Variation of strong correlation effects in A-site ordered perovskites CaCu3Ti4-xRuxO12: Photoemission and inverse photoemission studies
Authors:
H. J. Im,
M. Iwataki,
M. Tsunekawa,
T. Watanabe,
H. Sato,
M. Nakatake,
S. Kimura
Abstract:
We have systematically studied the strong correlation effects in A-site ordered perovskites CaCu3Ti4-xRuxO12 (x = 0, 1, 3.5, and 4) by using photoemission and inverse photoemission spectroscopies. In x = 0, 1, 3.5, the peak positions of the strongly correlated Cu 3d states around -3.8 eV and Ti 3d states around 3.6 eV little change. On the other hand, in x = 4, the Cu 3d states split into two peak…
▽ More
We have systematically studied the strong correlation effects in A-site ordered perovskites CaCu3Ti4-xRuxO12 (x = 0, 1, 3.5, and 4) by using photoemission and inverse photoemission spectroscopies. In x = 0, 1, 3.5, the peak positions of the strongly correlated Cu 3d states around -3.8 eV and Ti 3d states around 3.6 eV little change. On the other hand, in x = 4, the Cu 3d states split into two peaks around -2.5 and -4 eV. These indicate that Ti plays an important role to retain the strong correlation effects. In addition, the multiplet structures of Cu 3d final states from -8 to -14 eV become weak as Ru increases, indicating the reduction of the localized characters of Cu 3d states. At the Fermi level, we observe the absence of spectral weight in x = 0, 1 and the development of Ru 4d in-gap states in x = 3.5, 4, which give rise to the metal-insulator transition between x = 1 and x = 3.5.
△ Less
Submitted 8 March, 2023; v1 submitted 20 July, 2020;
originally announced July 2020.
-
Temperature dependence of the electronic structure of A-site ordered perovskite CaCu$_3$Ti$_4$O$_{12}$: Angle-integrated and -resolved photoemission studies
Authors:
H. J. Im,
T. Sakurada,
M. Tsunekawa,
T. Watanabe,
H. Miyazaki,
S. Kimura
Abstract:
We have investigated the electronic structure of A-site ordered CaCu$_3$Ti$_4$O$_{12}$ as a function of temperature by using angle-integrated and -resolved photoemission spectroscopies. Intrinsic changes of the electronic structure have been successfully observed in the valence band region by the careful consideration of charging effects. The obtained photoemission results have revealed that the i…
▽ More
We have investigated the electronic structure of A-site ordered CaCu$_3$Ti$_4$O$_{12}$ as a function of temperature by using angle-integrated and -resolved photoemission spectroscopies. Intrinsic changes of the electronic structure have been successfully observed in the valence band region by the careful consideration of charging effects. The obtained photoemission results have revealed that the intensity of the nearly non-dispersive Cu 3$d$-O 2$p$ hybridized bands at the binding energy of $\sim$2 eV increases with decreasing temperature from 300 to 120 K. This suggests that the density of the localized states, caused by the strong correlation effects, enhances as temperature decreases.
△ Less
Submitted 23 March, 2019;
originally announced March 2019.
-
Growth and Raman spectroscopy of thickness-controlled rotationally faulted multilayer graphene
Authors:
H. Kato,
N. Itagaki,
H. J. Im
Abstract:
We report the growth of thickness-controlled rotationally faulted multilayer graphene (rf-MLG) on Ni foils by low-pressure chemical vapor deposition and their characterization by micro-Raman spectroscopy. The surface morphology and thickness were investigated by scanning electron microscope, X-ray diffraction, and transmittance measurements. These results have revealed that the thickness of rf-MLG…
▽ More
We report the growth of thickness-controlled rotationally faulted multilayer graphene (rf-MLG) on Ni foils by low-pressure chemical vapor deposition and their characterization by micro-Raman spectroscopy. The surface morphology and thickness were investigated by scanning electron microscope, X-ray diffraction, and transmittance measurements. These results have revealed that the thickness of rf-MLG can be effectively controlled by the thickness of the Ni foil rather than the flow rate of CH$_4$, H$_2$, Ar. In the Raman spectroscopy measurements, we observed most Raman peaks of the graphitic materials. Raman spectra can be categorized into four patterns and show systematic behaviors. Especially, the in-plane (~1880 cm$^{-1}$, ~2035 cm$^{-1}$) and out-of-plane (~1750 cm$^{-1}$) modes are successfully analyzed to explain the dimensionality of rf-MLG as in the twisted (or rotated) bilayer graphene. In addition, it is found that the two peaks at ~1230 cm$^{-1}$ and ~2220 cm$^{-1}$ well reflect the properties of the in-plane mode. The peak intensities of the above four in-plane modes are proportional to that of 2D band, indicating that they share the common Raman resonance process.
△ Less
Submitted 8 September, 2018;
originally announced September 2018.
-
Electronic structure of Mott-insulator CaCu3Ti4O12: Photoemission and inverse photoemission study
Authors:
H. J. Im,
M. Iwataki,
S. Yamazaki,
T. Usui,
S. Adachi,
M. Tsunekawa,
T. Watanabe,
K. Takegahara,
S. Kimura,
M. Matsunami,
H. Sato,
H. Namatame,
M. Taniguchi
Abstract:
We have performed the photoemission and inverse photoemission experiments to elucidate the origin of Mott insulating states in A-site ordered perovskite CaCu$_3$Ti$_4$O$_{12}$ (CCTO). Experimental results have revealed that Cu 3$d$-O 2$p$ hybridized bands, which are located around the Fermi level in the prediction of the local-density approximation (LDA) band calculations, are actually separated i…
▽ More
We have performed the photoemission and inverse photoemission experiments to elucidate the origin of Mott insulating states in A-site ordered perovskite CaCu$_3$Ti$_4$O$_{12}$ (CCTO). Experimental results have revealed that Cu 3$d$-O 2$p$ hybridized bands, which are located around the Fermi level in the prediction of the local-density approximation (LDA) band calculations, are actually separated into the upper Hubbard band at $\sim$ 1.5 eV and the lower Hubbard band at $\sim$ $-$1.7 eV with a band gap of $\sim$ 1.5-1.8 eV. We also observed that Cu 3$d$ peak at $\sim$ $-$3.8 eV and Ti 3$d$ peak at $\sim$ 3.8 eV are further away from each other than as indicated in the LDA calculations. In addition, it is found that the multiplet strucutre around $-$9 eV includes a considerable number of O 2$p$ states. These observations indicate that the Cu 3$d$ and Ti 3$d$ electrons hybridized with the O 2$p$ states are strongly correlated, which originates in the Mott-insulating states of CCTO.
△ Less
Submitted 17 May, 2015; v1 submitted 15 April, 2015;
originally announced April 2015.
-
Strong Correlation Effects of A-site Ordered Perovskite CaCu3Ti4O12 revealed by Angle-Resolved Photoemission Spectroscopy
Authors:
H. J. Im,
M. Tsunekawa,
T. Sakurada,
M. Iwataki,
K. Kawata,
T. Watanabe,
K. Takegahara,
H. Miyazaki,
M. Matsunami,
T. Hajiri,
S. Kimura
Abstract:
We report angle-resolved photoemission spectroscopy (ARPES) results of A-site ordered perovskite CaCu$_3$Ti$_4$O$_{12}$. We have observed the clear band dispersions, which are shifted to the higher energy by 1.7 eV and show the band narrowing around 2 eV in comparison with the local density approximation calculations. In addition, the high energy multiplet structures of Cu 3$d^8$ final-states have…
▽ More
We report angle-resolved photoemission spectroscopy (ARPES) results of A-site ordered perovskite CaCu$_3$Ti$_4$O$_{12}$. We have observed the clear band dispersions, which are shifted to the higher energy by 1.7 eV and show the band narrowing around 2 eV in comparison with the local density approximation calculations. In addition, the high energy multiplet structures of Cu 3$d^8$ final-states have been found around 8 - 13 eV. These results reveal that CaCu$_3$Ti$_4$O$_{12}$ is a Mott-type insulator caused by the strong correlation effects of the Cu 3$d$ electrons well hybridized with O 2$p$ states. Unexpectedly, there exist a very small spectral weight at the Fermi level in the insulator phase, indicating the existence of isolated metallic states.
△ Less
Submitted 25 June, 2013; v1 submitted 19 March, 2013;
originally announced March 2013.
-
Crystalline electric field effects in Ce 3$d$ core-level spectra of heavy-fermion systems: Hard X-ray photoemission spectroscopy on CeNi$_{1-x}$Co$_x$Ge$_2$
Authors:
H. J. Im,
T. Ito,
S. Kimura,
H. -D. Kim,
J. B. Hong,
Y. S. Kwon
Abstract:
High-resolution hard X-ray photoemission measurements have been performed to clarify the electronic structure originating from the strong correlation between electrons in bulk Ce 3$d$ core-level spectra of CeNi$_{1-x}$Co$_x$Ge$_2$ (0 $\leq$ $x$ $\leq$ 1). In the Ce 3$d_{5/2}$ core-level spectra, the variation of satellite structures ($f^2$ peaks) shows that the hybridization strength between Ce…
▽ More
High-resolution hard X-ray photoemission measurements have been performed to clarify the electronic structure originating from the strong correlation between electrons in bulk Ce 3$d$ core-level spectra of CeNi$_{1-x}$Co$_x$Ge$_2$ (0 $\leq$ $x$ $\leq$ 1). In the Ce 3$d_{5/2}$ core-level spectra, the variation of satellite structures ($f^2$ peaks) shows that the hybridization strength between Ce 4$f$- and conduction electrons gradually increases with Co concentration in good agreement with the results of Ce 3$d-4f$ and 4$d-4f$ resonant photoemission spectroscopies. Particularly, in Ce 3$d_{3/2}$ core-level spectra, the multiplet structures of $f^1$ peaks systematically change with the degeneracy of $f$-states which originates from crystalline electric field effects.
△ Less
Submitted 6 May, 2009;
originally announced May 2009.
-
Fermi Surface Variation of Ce 4f-electrons in Hybridization Controlled Heavy-Fermion Systems
Authors:
H. J. Im,
T. Ito,
H. Miyazaki,
S. Kimura,
Y. S. Kwon,
Y. Saitoh,
S. -I. Fujimori,
A. Yasui,
H. Yamagami
Abstract:
Ce 3d-4f resonant angle-resolved photoemission measurements on CeCoGe$_{1.2}$Si$_{0.8}$ and CeCoSi$_{2}$ have been performed to understand the Fermi surface topology as a function of hybridization strength between Ce 4$f$- and conduction electrons in heavy-fermion systems. We directly observe that the hole-like Ce 4$f$-Fermi surfaces of CeCoSi$_{2}$ is smaller than that of CeCoGe$_{1.2}$Si…
▽ More
Ce 3d-4f resonant angle-resolved photoemission measurements on CeCoGe$_{1.2}$Si$_{0.8}$ and CeCoSi$_{2}$ have been performed to understand the Fermi surface topology as a function of hybridization strength between Ce 4$f$- and conduction electrons in heavy-fermion systems. We directly observe that the hole-like Ce 4$f$-Fermi surfaces of CeCoSi$_{2}$ is smaller than that of CeCoGe$_{1.2}$Si$_{0.8}$, indicating the evolution of the Ce 4$f$-Fermi surface with the increase of the hybridization strength. In comparision with LDA calculation, the Fermi surface variation cannot be understood even though the overall electronic structure are roughly explained, indicating the importance of strong correlation effects. We also discuss the relation between the Ce 4$f$-Fermi surface variation and the Kondo peaks.
△ Less
Submitted 14 October, 2014; v1 submitted 7 April, 2009;
originally announced April 2009.
-
Infrared spectroscopy under multi-extreme conditions: Direct observation of pseudo gap formation and collapse in CeSb
Authors:
T. Nishi,
S. Kimura,
T. Takahashi,
Y. Mori,
Y. S. Kwon,
H. J. Im,
H. Kitazawa
Abstract:
Infrared reflectivity measurements of CeSb under multi-extreme conditions (low temperatures, high pressures and high magnetic fields) were performed. A pseudo gap structure, which originates from the magnetic band folding effect, responsible for the large enhancement in the electrical resistivity in the single-layered antiferromagnetic structure (AF-1 phase) was found at a pressure of 4 GPa and…
▽ More
Infrared reflectivity measurements of CeSb under multi-extreme conditions (low temperatures, high pressures and high magnetic fields) were performed. A pseudo gap structure, which originates from the magnetic band folding effect, responsible for the large enhancement in the electrical resistivity in the single-layered antiferromagnetic structure (AF-1 phase) was found at a pressure of 4 GPa and at temperatures of 35 - 50 K. The optical spectrum of the pseudo gap changes to that of a metallic structure with increasing magnetic field strength and increasing temperature. This change is the result of the magnetic phase transition from the AF-1 phase to other phases as a function of the magnetic field strength and temperature. This result is the first optical observation of the formation and collapse of a pseudo gap under multi-extreme conditions.
△ Less
Submitted 18 April, 2005;
originally announced April 2005.
-
The origin of the phase separation in partially deuterated $κ$-(ET)$_2$Cu[N(CN)$_2$]Br studied by infrared magneto-optical imaging spectroscopy
Authors:
T. Nishi,
S. Kimura,
T. Takahashi,
T. Ito,
H. J. Im,
Y. S. Kwon,
K. Miyagawa,
H. Taniguchi,
A. Kawamoto,
K. Kanoda
Abstract:
The direct observation of the phase separation between the metallic and insulating states of 75 %-deuterated $κ$-(ET)$_2$Cu[N(CN)$_2$]Br ($d33$) using infrared magneto-optical imaging spectroscopy is reported, as well as the associated temperature, cooling rate, and magnetic field dependencies of the separation. The distribution of the center of spectral weight ($< ω>$) of $d33$ did not change u…
▽ More
The direct observation of the phase separation between the metallic and insulating states of 75 %-deuterated $κ$-(ET)$_2$Cu[N(CN)$_2$]Br ($d33$) using infrared magneto-optical imaging spectroscopy is reported, as well as the associated temperature, cooling rate, and magnetic field dependencies of the separation. The distribution of the center of spectral weight ($< ω>$) of $d33$ did not change under any of the conditions in which data were taken and was wider than that of the non-deuterated material. This result indicates that the inhomogenity of the sample itself is important as part of the origin of the metal - insulator phase separation.
△ Less
Submitted 10 January, 2005;
originally announced January 2005.
-
Electrical and magnetic properties of the new Kondo-lattice compound Ce3Pd4Ge4
Authors:
H. J. Im,
Y. S. Kwon,
M. H. Jung
Abstract:
We have measured the electric resistivity, magnetoresistance, magnetic susceptibility and magnetization of the new Kondo-lattice compound Ce3Pd4Ge4. The electrical resistivity exhibits a rapid drop at temperatures below 6 K, while the magnetic susceptibility does not show any corresponding anomaly at that temperature. This phenomenon is similar to that of Ce3Pd20Ge6 which shows quadrupolar inter…
▽ More
We have measured the electric resistivity, magnetoresistance, magnetic susceptibility and magnetization of the new Kondo-lattice compound Ce3Pd4Ge4. The electrical resistivity exhibits a rapid drop at temperatures below 6 K, while the magnetic susceptibility does not show any corresponding anomaly at that temperature. This phenomenon is similar to that of Ce3Pd20Ge6 which shows quadrupolar interation. We suggest that there is the possibility of quadrupolar interaction in the orthorhombic 4f-electron system Ce3Pd4Ge4. In addition, it is realized that the spin-dependent scattering effect is responsible for the magnetotransport.
△ Less
Submitted 25 February, 2002;
originally announced February 2002.