Based on first-principles calculations, we study the origin of the large thermopower in Ni-doped LaRhO3 and Mg-doped CuRhO2. We calculate the band structure and construct the maximally localized Wannier functions from which a tight binding Hamiltonian is obtained. The Seebeck coefficient is calculated within the Boltzmann's equation approach using this effective Hamiltonian. For LaRhO3, we find that the Seebeck coefficient remains nearly constant within a large hole concentration range, which is consistent with the experimental observation. For CuRhO2, the overall temperature dependence of the calculated Seebeck coefficient is in excellent agreement with the experiment. The origin of the large thermopower is discussed.
Diamond is one of the most studied materials because of its unique combination of remarkable electrical, mechanical, thermal and optical properties. Using a fully self-consistent ab initio theory of coupled electron-phonon transport, we reveal another striking behavior: a huge drag enhancement of the thermopower of lightly doped diamond. Thermopower values of around 100,000 microvolts per Kelvin are found at 100 K, significantly exceeding the highest previously measured value in the correlated metal FeSb2, and occurring at much higher temperatures. The enormous thermopower in diamond arises pr…
The origin of the recently discovered large thermopower in hole-doped PtSb$_2$ is theoretically analyzed based on a model constructed from first principles band calculation. It is found that the valence band dispersion has an overall flatness combined with some local ups and downs, which gives small Fermi surfaces scattered over the entire Brillouin zone. The Seebeck coefficient is calculated using this model, which gives good agreement with the experiment. We conclude that the good thermoelectric property originates from this "corrugated flat band", where the coexistence of large Seebeck coef…
In this paper we explore the different mechanisms that affect the thermopower of a band insulating perovskite (in this case, SrTiO$_3$) when subject to strain (both compressive or tensile). We analyze the high temperature, entropy dominated limit and the lower temperature, energy-transport regime. We observe that the effect of strain in the high-temperature Seebeck coefficient is small at the concentration levels of interest for thermoelectric applications. However, the effective mass changes substantially with strain, which produces an opposite effect to that of the degeneracy-breakups produc…
Quantized spin-wave known as magnon, a bosonic quasiparticle, can drag electrons or holes via sd exchange interaction and boost the thermopower over the conventional diffusive thermopower. P-type magnon-drag thermopower has been observed in both ferromagnetic and antiferromagnetic metallic and degenerate semiconductors. However, it has been less reported for intrinsic or n-type magnetic semiconductors; therefore, the impact of magnon-bipolar carrier drag on thermopower has remained unexplored. Here, a theoretical model for magnon-bipolar carrier drag thermopower is derived based on the magnon-…
This paper has been withdrawn by the authors because the results were incorrect due to the use of an impurity solver that fails at large interaction strength and above half-filling. This led, first, to the development of a new impurity solver (arXiv:1202.5814 or Phys.Rev. B 86, 085133 (2012)) and, second, to a complete revision of the thermopower results with different conclusions. Therefore a new paper on thermopower was submitted (arXiv:1209.4349) and the present one withdrawn.
Using advanced ab-initio calculations, we describe the formation and confinement of a two-dimensional electron gas in short-period ($\simeq$4 nm) Nb-doped SrTiO$_3$ superlattices as function of Nb doping. We predict complete two-dimensional confinement for doping concentrations higher than 70%. In agreement with previous observations, we find a large thermopower enhancement at room temperature. However, this effect is primarily determined by dilution of the mobile charge over a multitude of weakly occupied bands. As a general rule, we conclude that thermopower in similar heterostructures will …
Both the semi-classical and quantum transport properties of F-doped SnO$_2$ thick films ($\sim$1\,$μ$m) were investigated experimentally. It is found that the resistivity caused by the thermal phonons obeys Bloch-Grüneisen law from $\sim$90 to 300\,K, while only the diffusive thermopower, which varies linearly with temperature from 300 down to 10\,K, can be observed.The phonon-drag thermopower is completely suppressed due to the long electron-phonon relaxation time in the compound. These observations, together with the temperature independent characteristic of carrier concentration, indicate t…
High thermoelectric performance in oxides requires stable conductive materials that have suitable band structures. Here we show based on an analysis of the thermopower and related properties using first-principles calculations and Boltzmann transport theory that hole doped Cu2O may be such a material. We find that hole-doped Cu2O has a high thermopower of above 200 microV/K even with doping levels as high as 5.5x10 20 cm-3 at 500 K, mainly attributed to the heavy valence bands of Cu2O. This is reminiscent of the cobaltate family of high performance oxide thermoelectrics and implies that hole-d…
We present a systematic investigation of the effect of H, B, C, and N interstitials on the electronic, lattice and magnetic properties of La(Fe,Si)$_{13}$ using density functional theory. The parent LaSiFe$_{12}$ alloy has a shallow, double-well free energy function that is the basis of itinerant metamagnetism. On increasing the dopant concentration, the resulting lattice expansion causes an initial increase in magnetisation for all interstitials that is only maintained at higher levels of doping in the case of hydrogen. Strong s-p band hybridisation occurs at high B,C and N concentrations. We…
Upon chemical substitution of oxygen with fluor, LaMnAsO has been electron-doped in experiments, resulting in samples with remarkably high Seebeck coefficients of around -300$μVK^{-1}$ at room temperature and 3% doping. Within the framework of density functional theory plus dynamical mean-field theory we are not only able to reproduce these experimental observations, but can also provide a thorough investigation of the underlying mechanisms. By considering electronic correlations in the half-filled Mn-3d shells, we trace the high Seebeck coefficient back to an asymmetry in the spectral functio…
In doped semiconductors and metals, the thermopower decreases with increasing carrier concentration, in agreement with the Pisarenko relation. Here, we demonstrate a new strain engineering approach to increase the thermopower of [001] Si/Ge superlattices (SLs) beyond this relation. Using two independent theoretical modeling approaches, we show that new bands form due to the structural symmetry, and, the SL bands are highly tunable with epitaxial substrate strain. The band shifts lead to a modulated thermopower, with a peak $\sim$5-fold enhancement in strained Si/Ge SLs in the high doping regim…
We analyze the cross-plane miniband transport in n-doped [001] silicon (Si)/germanium (Ge) superlattices using an effective mass approximation (EMA) approach that correctly accounts for the indirect nature of the Si and Ge band gaps. Direct-gap based EMA has been employed so far to investigate the electronic properties of these superlattices, that does not accurately predict transport properties. We use the Boltzmann transport equation framework in combination with the EMA band analysis, and predict that significant improvement of the thermopower of n-doped Si/Ge superlattices can be achieved …
We have investigated two-dimensional thermoelectric properties in transition metal oxide heterostructures. In particular, we adopted an unprecedented approach to direct tuning of the 2D carrier density using fractionally δ-doped oxide superlattices. By artificially controlling the carrier density in the 2D electron gas that emerges at a LaxSr1-xTiO3 δ-doped layer, we demonstrate that a thermopower as large as 408 μV K-1 can be reached. This approach also yielded a power factor of the 2D carriers 117 μWcm-1K-2, which is one of the largest reported values from transition metal oxide based materi…
We have measured the electrical resistivity and the thermopower of the electron-doped perovskite cobaltites LaCo$_{1-y}$Te$_y$O$_3$. In contrast to the hole-doped systems such as metallic ferromagnets La$_{1-x}M_x$CoO$_3$ ($M$ = Ca, Sr, Ba), the electron-doped samples show an insulating behavior even in a heavily doped range due to a spin-state blockade mechanism that an electron hopping from high-spin Co$^{2+}$ to low-spin Co$^{3+}$ site is energetically suppressed. We find that, despite the electron doping, the thermopower shows relatively large positive values above $y=0.05$, strikingly dis…
We study the origin of the large thermopower in quasi-two-dimensional a $τ$-type organic conductor, $τ-(EDO-S,S-DMEDT-TTF)_2(AuBr_2)_{1+y}$ ($y \le 0.875$), from the view point of a "pudding mold"-type band structure. We calculate the electronic band structure using an \textit{ab initio} band calculation package, and obtain a tight binding model fit to the \textit{ab initio} band structure. Using the model and the Boltzmann's equation approach, we calculate the temperature dependence of the Seebeck coefficient. We conclude that the peculiar band structure is the origin of the large Seebeck coe…
Temperature dependent electrical resistivity and thermopower measurements were carried out on Gd1-xCaxBaCo2O5.53 with x varying between 0 and 0.25. Ca subsitution leads to the incorporation of holes (Co4+) into the system that leads to a reduction in resistivity and a stabilisation of the ferromagnetic phase at low temperatures. The temperature dependence of resistivity and thermopower are markedly different in the Ca doped sample, with a dramatic reduction in the resistivity, as compared to that in the pristine sample. The variation in both the resistivity and thermopower with temperature is …
Here we investigate LaAlO_3-SrTiO_3 heterostructure withδ-doping of the interface by LaMnO_3 at less than one monolayer. This doping strongly inhibits the formation of mobile electron layer at the interface. This results in giant increase of the resistance and the thermopower of the heterostructure. Several aspects of this phenomena are investigated. A model to calculate the carrier concentration is presented and effect of doping and detailed temperature dependence is analyzed in terms of model parameters and the weak-scattering theory. The large enhancement of thermopower is attributed to the…
Thermoelectric properties of the system La$_2$NiO$_{4+δ}$ have been studied ab initio. Large Seebeck coefficient values are predicted for the parent compound, and to some extent remain in the hole-doped metallic phase, accompanied of an increase in the conductivity. This system, due to its layered structure would be a suitable candidate for an improvement of its thermoelectric figure of merit by nanostructurization in thin films, that has already been shown to increase the electrical conductivity ($σ$). Our calculations show that in the region around La$_2$NiO$_{4.05}$ the system has a large t…
The negative sign of the anomalous Nernst thermopower ($S_\text{ANE}$) observed in Mn-Ga ordered alloys is an attractive property for thermoelectric applications exploiting the anomalous Nernst effect (ANE); however, its origin has not been clarified. In this study, to gain insight into the negative $S_\text{ANE}$, we prepared epitaxial thin films of Mn$_{x}$Ga$_{100-x}$ with $x$ ranging from 56.2 to 71.7, and systematically investigated the structural, magnetic, and transport properties including the anomalous Hall effect (AHE) and the ANE. The measured $S_\text{ANE}$ is negative for all samp…
Measurements of magneto-thermopower (S(H, T)) of interfacial delta doped LaTiO$_3$/SrTiO$_3$ (LTO/STO) heterostructure by an iso-structural antiferromagnetic perovskite LaCrO$_3$ are reported. The thermoelectric power of the pure LTO/STO interface at 300 K is $\approx$ 118 $μ$V/K, but increases dramatically on $δ$-doping. The observed linear temperature dependence of S(T) over the temperature range 100 K to 300 K is in agreement with the theory of diffusion thermopower of a two-dimensional electron gas. The S(T) displays a distinct enhancement in the temperature range (T $<$ 100 K) where the s…
Motivated by the newly synthesized mixed-valent spinel LiRh$_2$O$_4$ for which a large thermopower is observed in the metallic cubic phase above 230K [Okamoto {\it et al.} (arXiv:0806.2504)], we calculate the Seebeck coefficient by the combination of local density approximation and dynamical mean field theory (LDA+DMFT). The experimental values are well reproduced not only by LDA+DMFT but also by the less involved Boltzmann equation approach. A careful analysis of the latter shows unexpectedly that the origin of the large thermopower shares a common root with a very different oxide: Na$_x$CoO$…
Thermoelectric properties of the system La$_2$NiO$_{4+δ}$ have been recently discussed [Phys. Rev. B 86, 165114 (2012)] via ab initio calculations. An optimum hole-doping value was obtained with reasonable thermopower and thermoelectric figure of merit being calculated. Here, a large increase in the thermoelectric performance through lattice strain and the corresponding atomic relaxations is predicted. This increase would be experimentally attainable via growth in thin films of the material on top of different substrates. A small tensile strain would produce large thermoelectric figures of mer…
In the present study, we pin down the origin of the coexistence of the large thermopower and the large conductivity in Na$_x$CoO$_2$. It is revealed that not just the density of states (DOS), the effective mass, nor the band width, but the peculiar {\it shape} of the $a_{1g}$ band referred to as the "pudding mold" type, which consists of a dispersive portion and a somewhat flat portion, is playing an important role in this phenomenon. The present study provides a new guiding principle for designing good thermoelectric materials.
We study the origin of the large Seebeck coefficient despite the metallic conductivity in the La-doped SrTiO$_3$ and Ba-doped KTaO$_3$. We calculate the band structure of SrTiO$_3$ and KTaO$_3$, from which the Seebeck coefficient is obtained using the Boltzmann's equation. We conclude that the multiplicity of the $t_{2g}$ bands in these materials is one major origin of the good thermoelectric property in that when compared at a fixed total number of doped electrons, the Seebeck coefficient and thus the power factor are larger in multiple band systems than in single band ones because the number…
Graphene halfly doped with H or F possesses local magnetization at the undoped C sites. Thus the Seebeck coefficient is different for each spin channel and its sign also changes depending on the spin polarization. Deposition of doped graphene on the C-face 4H-SiC(0001) with two buffer layers substantially varies the electronic and thermoelectric properties. These properties are efficiently calculated from the semiclassical Boltzmann equations, using the maximally-localized Wannier-functions interpolation of the band structures obtained with the density-functional theory. Our results indicate l…
Magnon-drag is shown to dominate the thermopower of elemental Fe from 2 to 80 K and of elemental Co from 150 to 600 K; it is also shown to contribute to the thermopower of elemental Ni from 50 to 500 K. Two theoretical models are presented for magnon-drag thermopower. One is a hydrodynamic theory based purely on non-relativistic, Galilean, spin-preserving electron-magnon scattering. The second is based on spin-motive forces, where the thermopower results from the electric current pumped by the dynamic magnetization associated with a magnon heat flux. In spite of their very different microscopi…
The electrical resistivity, Hall coefficient, and thermopower as functions of temperature are reported for lightly electron-doped Ca(1-x)La(x)MnO(3)(0 <= x <= 0.10). Unlike the case of hole-doped ferromagnetic manganites, the magnitude and temperature dependence of the Hall mobility for these compounds is found to be inconsistent with small-polaron theory. The transport data are better described by the Feynman polaron theory and imply intermediate coupling (alpha \~ 5.4) with a band effective mass, m*~4.3 m_0, and a polaron mass, m_p ~ 10 m_0.
Two extreme members of the cobaltite series, LaCoO3 and DyCoO3, were investigated by the electrical resistivity and thermopower measurements up to 800-1000 K. Special attention was given to effects of extra holes or electrons, introduced by light doping of Co sites by Mg2+ or Ti4+ ions. The experiments on the La based compounds were complemented with magnetic measurements. The study shows that both kinds of charge carriers induce magnetic states on surrounding CoIII sites and form thus thermally stable polarons of large total spin. Their itinerancy is characterized by low temperature resistivi…
The sodium cobaltate system Na$_{x}$CoO$_2$ is a prominent representant of strongly correlated materials with promising thermoelectric response. In a combined theoretical and experimental study we show that by doping the Co site of the compound at $x$=0.7 with iron, a further increase of the Seebeck coefficient is achieved. The Fe defects give rise to effective hole doping in the high-thermopower region of larger sodium content $x$. Originally filled hole pockets in the angular-resolved spectral function of the Fe-free material shift to low energy when introducing Fe, leading to a multi-sheet …
The pentatellurides, ZrTe5 and HfTe5 are layered compounds with one dimensional transition-metal chains that show a never understood temperature dependent transition in transport properties as well as recently discovered properties suggesting topological semimetallic behavior. Here we show that these materials are semiconductors and that the electronic transition is due to a combination of bipolar effects and different anisotropies for electrons and holes. We report magneto-transport properties for two kinds of ZrTe5 single crystals grown with the chemical vapor transport (S1) and the flux met…
The near infrared (NIR) photoluminescence (PL) in Bismuth-doped aluminosilicate glasses was reported about of 16 years ago. Although it has since been developed various kinds of fiber lasers and amplifiers based on the Bismuth-doped silica glasses, the main problem, namely the nature of NIR PL, remains unsolved. Here we show that this famous NIR PL in Bismuth-doped aluminosilicate glass originates from the defect, most probably positively charged oxygen vacancy V$_{O}^{2+}$ in the glass network. This defect interacts with Bi$^+$ ion in its environment via the energy transfer.
Dirac/Weyl semimetals hosting linearly-dispersing bands have received recent attention for potential thermoelectric applications, since their ultrahigh-mobility carriers could generate large thermoelectric and Nernst power factors. To optimize these efficiencies, the Fermi energy needs to be chemically controlled in a wide range, which is generally difficult in bulk materials because of disorder effects from the substituted ions. Here it is shown that the Fermi energy is tunable across the Dirac point for layered magnet EuMnBi$_2$ by partially substituting Gd$^{3+}$ for Eu$^{2+}$ in the insula…
A possible origin of unusual temperature behavior of transport coefficients observed in densely packed polycrystalline CaAl_{2} compound [M. Ausloos et al., J. Appl. Phys. 96, 7338 (2004)] is discussed, including a power-like dependence of resistivity with $ρ\propto T^{-3/4}$ and N-like form of the thermopower. All these features are found to be in good agreement with the Shklovskii-Efros localization scenario assuming polaron-mediated hopping processes controlled by the Debye energy.
The ternary semiconductors NiZrSn and CoZrBi with C1_b crystal structure are introduced by calculating their basic structural, electronic and phononic properties using density functional theory. Both the gradient-corrected PBE functional and the hybrid functional HSE06 are employed. While NiZrSn is found to be a small-band-gap semiconductor (E_g = 0.46 eV in PBE and 0.60 eV in HSE06), CoZrBi has a band gap of 1.01 eV in PBE (1.34 eV in HSE06). Moreover, effective masses and deformation potentials are reported. In both materials ABC, the intrinsic point defects introduced by species A (Ni or Co…
On the basis of detailed first-principles calculations the anisotropic thermoelectric transport properties of biaxially strained silicon were studied with focus on a possible enhancement of the powerfactor. Electron as well as hole doping were examined in a broad doping and temperature range. In the low-temperature and low-doping regime an enhancement of the powerfactor was obtained for compressive and tensile strain in the electron-doped case and for compressive strain in the hole-doped case. In the thermoelectrically more important high-temperature and high- doping regime a slight enhancemen…
The electronic properties of pentavalent-ion (Nb$^{5+}$, Ta$^{5+}$, and I$^{5+}$) doped anatase and rutile TiO$_2$ are studied using spin-polarized GGA+\emph{U} calculations. Our calculated results indicate that these two phases of TiO$_2$ exhibit different conductive behavior upon doping. For doped anatase TiO$_2$, some up-spin-polarized Ti 3\emph{d} states lie near the conduction band bottom and cross the Fermi level, showing an \emph{n}-type half-metallic character. For doped rutile TiO$_2$, the Fermi level is pinned between two up-spin-polarized Ti 3\emph{d} gap states, showing an insulati…
We report an observation of room temperature magnetodielectric (RTMD) effect in Mn doped LaGaO3. Results of frequency dependent magnetoresistance (FDMR) measurements discards the possibility of any magnetoresistive contribution in the observed MD effect. The intrinsic nature of MD coupling has been validated/evidenced by means of magnetic field dependent Raman spectroscopy and explained in terms of modified volume strain governed by magnetic field induced rerotation of spin coupled Mn-orbitals. Ultimately, present RTMD effect is attributed to magneto-compression/magnetostriction associated wit…
We uncover the origin of blue luminescence (BL) peak in Mg doped GaN thin film using a combination of experimental X-ray absorption near edge spectroscopy (XANES), first-principles calculations based on density functional theory and full multiple scattering theoretical analysis of various possible defect complexes and their XANES signatures. We demonstrate that a defect complex composed of Mg substituted at Ga site (MgGa) and Mg at interstitial site (Mgi) is primarily responsible for the observed BL by Donor-Acceptor Pair transition (DAP) associated with a deep donor state in the gap. It corre…
Nanolaminated materials exhibit characteristic magnetic, mechanical, and thermoelectric properties, with large contemporary scientific and technological interest. Here, we report on the anisotropic Seebeck coefficient in nanolaminated Ti3SiC2 single-crystal thin films and trace the origin to anisotropies in element-specific electronic states. In bulk polycrystalline form, Ti3SiC2 has a virtually zero Seebeck coefficient over a wide temperature range. In contrast, we find that the in-plane (basal ab) Seebeck coefficient of Ti3SiC2, measured on single-crystal films has a substantial and positive…
Optically-detected magnetic resonance (ODMR) and positron annihilation spectroscopy (PAS) experiments have been employed to study magnesium-doped GaN layers grown by metal-organic vapor phase epitaxy. As the Mg doping level is changed, the combined experiments reveal a strong correlation between the vacancy concentrations and the intensity of the red photoluminescence band at 1.8 eV. The analysis provides strong evidence that the emission is due to recombination in which electrons both from effective mass donors and from deeper donors recombine with deep centers, the deep centers being vacancy…
p x n-type materials refer to materials with a p-type Seebeck coefficient in one direction and a n-type coefficient in the orthogonal direction. This type of materials allows for a transverse thermoelectric response, which is highly desirable for energy applications. Here, we report the observation of p x n-type behavior in TaIrTe4, a type-II Weyl semimetal, with an in-plane thermopower anisotropy S$_{xx}$-S$_{yy}$ reaches a maximum value 40$μ$V/K at 200K. Intriguingly. we found that such a p x n-type behavior is absent in the similar compound NbIrTe4. The presence and absence of p x n-type be…
Currently, Fe doping in the ~10^18 cm-3 range is the most widely-available method for producing semi-insulating single crystalline beta-Ga2O3 substrates. Red luminescence features have been reported from multiple types of Ga2O3 samples including Fe-doped -Ga2O3, and attributed to Fe or N at O. Herein, however, we demonstrate that the high-intensity red luminescence from Fe-doped beta-Ga2O3 commercial substrates consisting of two sharp peaks at 689 nm and 697 nm superimposed on a broader peak centered at 710 nm originates from Cr impurities present at a concentration near 2 ppm. The red emissio…
P mono-doped and (P, N) co-doped ZnO are investigated by the first-principles calculations. It is found that substitutive P defect forms a deep acceptor level at O site (PO) and it behaves as a donor at Zn site (PZn), while interstitial P (Pi) is amphoteric. Under equilibrium conditions, these defects contribute little to the p-type conductivity of ZnO samples since the formation energy of PZn is much lower than that of Pi or PO when EF is below mid-gap (a prerequisite p-type condition). Zinc vacancies (VZn) and PZn-2VZn complex are demonstrated to be shallow acceptors with ionization energies…
Magnetocrystalline anisotropy (MCA) in doped Ce$_{2}$Co$_{17}$ and other competing structures was investigated using density functional theory. We confirmed that the MCA contribution from dumbbell Co sites is very negative. Replacing Co dumbbell atoms with a pair of Fe or Mn atoms greatly enhance the uniaxial anisotropy, which agrees quantitatively with experiment, and this enhancement arises from electronic-structure features near the Fermi level, mostly associated with dumbbell sites. With Co dumbbell atoms replaced by other elements, the variation of anisotropy is generally a collective eff…
Excellent thermoelectric performance in the out-of-layer n-doped SnSe has been observed experimentally (Chang et al., Science 360, 778-783 (2018)). However, a first-principles investigation of the dominant scattering mechanisms governing all thermoelectric transport properties is lacking. In the present work, by applying extensive first-principles calculations of electron-phonon coupling associated with the calculation of the scattering by ionized impurities, we investigate the reasons behind the superior figure of merit as well as the enhancement of zT above 600 K in n-doped out-of-layer SnSe…
We have applied extended X-ray absorption fine structure (EXAFS) analyses and ab-initio molecular dynamics (AIMD) simulations to study the atomic structure of Ag-doped (up to 42%) Ge1Sb2Te4 alloys. Analysis of the models that are consistent with the EXAFS experiment reveals that the Ge environment is significantly modified by Ag doping whereas those of Sb and Te are barely affected (except for high Ag concentrations), and suggests that Ag prefers bonding with Te to Ge or Sb. Doping with Ag promotes the conversion of tetrahedral Ge sites to octahedral Ge sites and enhances the speed of crystall…
Isotopic substitution of boron and carbon is applied for the identification of the vibrational modes of heavily boron-doped diamond synthesized by high-pressure high-temperature technique. None of the bands in the Raman spectra are shifting upon ^{10}B-substitution, whereas shifts to lower frequency are observed for all bands upon ^{13}C-substitution as compared to a sample with natural isotope abundancies. These isotopic substitution experiments exclude the hypothesis of boron dimer related normal modes and strongly support the assignment of the previously studied "500 cm^{-1}" and "1230 cm^{…
Enhanced visible light photocatalytic activity of transition metal-doped ceria (CeO2) nanomaterials have experimentally been demonstrated, whereas there are very few reports mentioning the mechanism of this behavior. Here we use first-principles calculations to explore the origin of enhanced photocatalytic performance of CeO2 doped with transition metal impurities (Fe, Cr and Co). When a transition metal atom substitutes a Ce atom into CeO2, t2g and eg levels of 3d orbits appear in the middle of band gap owing to the effect of cubic ligand field, and the former is higher than latter. Interesti…
Detailed Raman spectroscopy studies on polycrystalline Sr1-xPrxTiO3 (x=0.01, 0.025, 0.05, 0.075, 0.09, 0.13, 0.15, 0.17) samples are reported elucidating the microscopic mechanism of relaxor ferroelectrics. The polar mode was observed upto very high temperature ~1000 K suggesting that the dipoles exists at temperatures well above the characteristic relaxor temperatures and they develop a short range correlation at 505 K leading to formation of PNRs. The TO2 polar mode showed anomalous softening in cooling below T~505 K supporting the growth of PNRs. Fano resonance is reported in the Pr doped c…
Origin of anomalous p-type conductivity in monolayer Fe-doped MoS2
Electron Microscopy Centre of Lanzhou University, Lanzhou University（兰州大学电子显微镜中心）；Information Materials and Intelligent Sensing Laboratory of Anhui Province, Center of Free Electron Laser and High Magnetic Field, Institutes of Physical Science and Information Technology, Anhui University（安徽大学物理科学与信息技术学院）；School of Physical Science and Technology, Lanzhou University（兰州大学物理科学与技术学院）；School of Chemistry, Faculty of Science, The University of Sydney（悉尼大学理学院化学系）；Yunnan Key Laboratory of Electromagnetic Materials and Devices, School of Materials and Energy, Yunnan University（云南大学材料能源学院）；Electron Microscopy Center, Yunnan University（云南大学电子显微镜中心）；State Key Laboratory of Solid Lubrication, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences（中国科学院兰州化学物理研究所）
The environmental aging effect of doped graphene is investigated as a function of the organic doping species, humidity, and the number of graphene layers adjacent to the dopant by studies of the Raman spectroscopy, x-ray and ultraviolet photoelectron spectroscopy, scanning electron microscopy, infrared spectroscopy, and electrical transport measurements. It is found that higher humidity and structural defects induce faster degradation in doped graphene. Detailed analysis of the spectroscopic data suggest that the physical origin of the aging effect is associated with the continuing reaction of…
We calculate the photoemission spectra of suspended and epitaxial doped graphene using an ab initio cumulant expansion of the Green's function based on the GW self-energy. Our results are compared to experiment and to standard GW calculations. For doped graphene on a silicon carbide substrate, we find, in contrast to earlier calculations, that the spectral function from GW only does not reproduce experimental satellite properties. However, ab initio GW plus cumulant theory combined with an accurate description of the substrate screening results in good agreement with experiment, but gives no p…
Combining LSDA+$U$ and an analysis of superexchange interactions beyond DFT, we describe the magnetic ground states in rutile and anatase Cr-doped TiO$_2$. In parallel, we correct our LSDA+$U$ ground state through GW corrections ($GW$@LSDA+$U$) that reproduce the position of impurity states and the band gaps in satisfying agreement with experiments. Because of the different topological coordinations of Cr-Cr bonds in the ground states of rutile and anatase, superexchange interactions induce either ferromagnetic or antiferromagnetic couplings of Cr ions. In Cr-doped anatase, this interaction le…
