The photoexcited state in a correlated electron system with a spin-state degree of freedom is studied. We start from the two-orbital extended Hubbard model where the energy difference between the two orbitals is intro...
The photoexcited state in a correlated electron system with a spin-state degree of freedom is studied. We start from the two-orbital extended Hubbard model where the energy difference between the two orbitals is introduced. The photoexcited metastable state is examined based on the effective model Hamiltonian derived using the two-orbital Hubbard model. Spin-state change is induced by photoirradiation in the low-spin band insulator near the phase boundary, and it is found that a high-spin state is stabilized by creating a ferromagnetic bound state with photodoped hole carriers. An optical absorption occurs between the bonding and antibonding orbitals inside the bound state. The time evolution of photoexcited states is simulated in the time-dependent mean-field scheme. It is found that pair annihilations of photodoped electrons and holes generate the high-spin state in a low-spin band insulator. We propose that this process is directly observed by the time-resolved photoemission experiments.
We performed a laser angle-resolved photoemission spectroscopy (ARPES) study on a wide doping range of Ba1−xKxFe2As2 (BaK) and precisely determined the doping evolution of the superconducting gaps in this compound. Th...
We performed a laser angle-resolved photoemission spectroscopy (ARPES) study on a wide doping range of Ba1−xKxFe2As2 (BaK) and precisely determined the doping evolution of the superconducting gaps in this compound. The gap size of the outer hole Fermi-surface (FS) sheet around the Brillouin zone (BZ) center shows an abrupt drop with overdoping (for x≳ 0.6) while the inner and middle FS gaps roughly scale with Tc. This is accompanied by the simultaneous disappearance of the electron FS sheet with similar orbital character at the BZ corner. These results indicate the different contributions of X2−Y2 and XZ/YZ orbitals to superconductivity in BaK and can hardly be completely reproduced by the available theories on iron-based superconductors.
We report that the ionic-liquid gating of bulk single crystals of a topological insulator can control the type of the surface carriers and even results in ambipolar transport. This was made possible by the use of a hi...
We report that the ionic-liquid gating of bulk single crystals of a topological insulator can control the type of the surface carriers and even results in ambipolar transport. This was made possible by the use of a highly bulk-insulating BiSbTeSe2 system where the chemical potential is located close to both the surface Dirac point and the middle of the bulk band gap. Thanks to the use of ionic liquid, the control of the surface chemical potential by gating was possible on the whole surface of a bulk three-dimensional sample, opening new experimental opportunities for topological insulators. In addition, our data suggest the existence of a nearly reversible electrochemical reaction that causes bulk carrier doping into the crystal during the ionic-liquid gating process.
Polymer-protected metal nanoparticles (NPs) are recognized as a type of complex between a polymer and metal NPs, since the metal NPs are stabilized by coordination to the polymer. Thus, they can work as an effective c...
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Polymer-protected metal nanoparticles (NPs) are recognized as a type of complex between a polymer and metal NPs, since the metal NPs are stabilized by coordination to the polymer. Thus, they can work as an effective catalyst in a dispersed state due to their high surface area-to-volume ratio and high stability by protection with poly(N-vinyl-2-pyrrolidone) (PVP). In this study, colloidal dispersions of PVP-protected and Au-containing bi- and trimetallic NPs were prepared and applied to the catalyst for the aerobic oxidation of glucose into gluconic acid in an alkaline solution. The AuAg and AuPt bimetallic NPs were more active than the Au NPs although the Ag and Pt NPs were less active than the Au NPs. The AuAgPt (Au/Ag/Pt = 7/2/1) trimetallic NPs were the most active catalyst for the same reaction. The high activity can be explained by electronic charge transfer from the Ag or Pt to the Au.
A photoinduced spin-state change in the itinerant correlated electron system is studied. A photon introduced in the low-spin band insulator induces a bound state of the high-spin state and a photoexcited hole. This bo...
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A photoinduced spin-state change in the itinerant correlated electron system is studied. A photon introduced in the low-spin band insulator induces a bound state of the high-spin state and a photoexcited hole. This bound state brings a characteristic peak in the pump-probe optical absorption spectra which are completely different from the spectra in thermal-excited states. The present results well explain the recent experiments of the ultrafast optical spectroscopy in perovskite cobaltites.
We have studied the conditions for the THz radiation in many systems with different shapes and dimensions such as rectangles, squares, cylinders and (equilateral and isosceles including right-angled isosceles) triangl...
We have studied the conditions for the THz radiation in many systems with different shapes and dimensions such as rectangles, squares, cylinders and (equilateral and isosceles including right-angled isosceles) triangles and rectangles with non-uniform width (asymmetric rectangles) fabricated from single crystals of Bi2Sr2CaCu2O8+δ, which are known as a typical intrinsic Josephson junction system. As a result two conditions have been deduced to be fulfilled: one is the ac-Josephson effect always working at each intrinsic Josephson junction. Another one is the standing wave formation of the THz waves excited inside the mesa due to the cavity resonance for the radiation. The former condition is always necessary for the radiation but the latter may have only the secondary role for the radiation because the Q-value of the resonance cavity in some cases seems to be quite low and of order of unity. Therefore, the radiation frequency can be controlled by the voltage effectively and widely varied by the ac-Josephson effect only. In addition, we show a new phenomenon observed at high current region and a comprehensive physical picture for the extraordinary THz radiation phenomenon is given.
The generation and recombination dynamics of photocarriers (polarons) in poly(3-hexylthiophene) and [6,6]-phenyl-C61-butyric acid methyl ester blended thin films have been investigated by means of continuous-wave phot...
The generation and recombination dynamics of photocarriers (polarons) in poly(3-hexylthiophene) and [6,6]-phenyl-C61-butyric acid methyl ester blended thin films have been investigated by means of continuous-wave photoinduced absorption spectroscopy. Continuous-wave photoinduced absorption spectroscopy has the advantage of being used to investigate long-lived excited species with lifetimes that range from microseconds to milliseconds. In this time range, three kinds of excited species are recognized in the blends: trapped, mobile, and delocalized polarons. From the modulation-frequency dependence, the mean lifetimes of the three types of polarons at low temperature were estimated. It is known that polarons are not generated directly by the pump beam but rather through Coulombically bound radical pairs. We have found that this two-step model for polaron generation can be recognized on a microsecond time scale by continuous-wave photoinduced absorption measurements.
Ultrafast time-resolved PYP was studied by pump-probe spectroscopy using a sub-8 fs pulse laser with a central wavelength at 400 nm[1].The broadband spectrum of the UV pulse allowed us to detect the pump-probe signal ...
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Ultrafast time-resolved PYP was studied by pump-probe spectroscopy using a sub-8 fs pulse laser with a central wavelength at 400 nm[1].The broadband spectrum of the UV pulse allowed us to detect the pump-probe signal over a broad spectral range in UV covering 360-440nm.A 128-channel detector array was used to simultaneously obtain the
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