The(electro)chemical stability and Li dendrite suppression capability of sulfide solid electrolytes(SEs)need further improvement for developing all-solid-state Li batteries(ASSLBs).Here,we report advanced halogen-rich...The(electro)chemical stability and Li dendrite suppression capability of sulfide solid electrolytes(SEs)need further improvement for developing all-solid-state Li batteries(ASSLBs).Here,we report advanced halogen-rich argyrodites via I and Cl co-occupation on the crystal lattice.Notably,a proper I content forms a single phase,whereas an excessive I causes precipitation of two argyrodite phases like a superlattice structure.The resultant synergistic effect of the optimized composition allows to gain high ionic conductivities at room temperature and-20℃,and enhances the(electro)chemical stability against Li and Li dendrite suppression capability.The Li|argyrodite interface is very sensitive to the ratio of I and Cl.A LiCl-and LiI-rich double-layer interface is observed from the cell using the SE with optimized composition,whereas too high I content forms only a single interface layer with a mixture of Lil and LiCl.This double-layer interface is found to effectively mitigate the Li/SE reaction.The proper designed argyrodite enables ASSLBs to achieve good electrochemical properties at a broad temperature range regardless of the electrode materials.This co-occupation strategy provides a novel exploration for advanced halogen-rich argyrodite system.展开更多
The mechanical behavior and microstructural evolution of an Fe-30Mn-3Al-3Si twinninginduced plasticity(TWIP)steel processed using warm forging was investigated.It is found that steel processed via warm forging improve...The mechanical behavior and microstructural evolution of an Fe-30Mn-3Al-3Si twinninginduced plasticity(TWIP)steel processed using warm forging was investigated.It is found that steel processed via warm forging improves comprehensive mechanical properties compared to the TWIP steel processed via cold rolling,with a high tensile strength(R_(m))of 793 MPa,a yield strength(R_(P))of 682 MPa,an extremely large R_(P)/R_(m)ratio as high as 0.86 as well as an excellent elongation rate of 46.8%.The microstructure observation demonstrates that steel processed by warm forging consists of large and elongated grains together with fine,equiaxed grains.Complicated micro-defect configurations were also observed within the steel,including dense dislocation networks and a few coarse deformation twins.As the plastic deformation proceeds,the densities of dislocations and deformation twins significantly increase.Moreover,a great number of slip lines could be observed in the elongated grains.These findings reveal that a much more dramatic interaction between microstructural defect and dislocations glide takes place in the forging sample,wherein the fine and equiaxed grains propagated dislocations more rapidly,together with initial defect configurations,are responsible for enhanced strength properties.Meanwhile,larger,elongated grains with more prevalently activated deformation twins result in high plasticity.展开更多
As a sister compound of PbTe, SnTe possesses the environmentally friendly elements. However, the pristine SnTe compounds suffer from the high carrier concentration, the large valence band offset between the L and Σpo...As a sister compound of PbTe, SnTe possesses the environmentally friendly elements. However, the pristine SnTe compounds suffer from the high carrier concentration, the large valence band offset between the L and Σpositions and high thermal conductivity. Using high-pressure and high-temperature technology, we synthesized the pristine SnTe samples at different pressures and systemically investigated their thermoelectric properties.High pressure induces rich microstructures, including the high-density dislocations and lattice distortions, which serve as the strong phonon scattering centers, thereby reducing the lattice thermal conductivity. For the electrical properties, pressure reduces the harmful high carrier concentration, due to the depression of Sn vacancies.Moreover, pressure induces the valence band convergence, reducing the energy separation between the L and Σpositions. The band convergence and suppressed carrier concentration increase the Seebeck coefficient. Thus, the power factors of pressure-sintered compounds do not deteriorate significantly under the condition of decreasing electrical conductivity. Ultimately, for a pristine SnTe compound synthesized at 5 GPa, a higher ZT value of 0.51 is achieved at 750 K, representing a 140% improvement compared to the value of 0.21 obtained using SPS. Therefore, the high-pressure and high-temperature technology is demonstrated as an effectively approach to optimize thermoelectric performance.展开更多
The composite internal friction peak(versus temperature)assumed to be consisted of a relaxation peak and a phase transformation peak previously observed in cold-worked Al-0.50wt%(0.21at%)Cu at temperatures below room ...The composite internal friction peak(versus temperature)assumed to be consisted of a relaxation peak and a phase transformation peak previously observed in cold-worked Al-0.50wt%(0.21at%)Cu at temperatures below room temperature are now resolved into two separate peaks.Internal friotion peaks as a function of strain amplitude(the amplitude peak)are observed around the temperature region of both peaks for he first time.展开更多
The need for reducing the wear in mechanical parts used in the industry makes self-lubricant films one of the sustainable solutions to achieve long-term protection under different environmental conditions.The purpose ...The need for reducing the wear in mechanical parts used in the industry makes self-lubricant films one of the sustainable solutions to achieve long-term protection under different environmental conditions.The purpose of this work is to study the influence of C additions on the tribological behavior of a magnetron-sputtered TiN film in air,water,and seawater.The results show that the addition of C into the TiN binary film induced a new amorphous phase,and the films exhibited a dual phase of fcc(face-centered cubic)-TiN and amorphous carbon.The antifriction and wear-resistance properties were enhanced in air and water by adding 19.1at%C.However,a further increase in the C concentration improved anti-frictional properties but also led to higher wear rates.Although the amorphous phase induced microbatteries and accelerated the corrosion of TiN phases in seawater,the negative abrasion state was detected for all Ti-C-N films due to the adhesion of the tribocorrosion debris on the wear track.展开更多
By employing a combined approach of density-functional theory(DFT) and dynamical mean-field theory(DMFT) calculations, we examine the structural, electronic, and magnetic characteristics of two distinct strontium ruth...By employing a combined approach of density-functional theory(DFT) and dynamical mean-field theory(DMFT) calculations, we examine the structural, electronic, and magnetic characteristics of two distinct strontium ruthenates: Sr2RuO4,an unconventional superconductor, and the correlated metal SrRuO3, both at 50% Fe-doping level. In both Sr2Fe0.5Ru0.5O4and SrFe0.5Ru0.5O3, the original ruthenium(Ru) and the dopant iron(Fe) atoms adopt 3-dimensional and 2-dimensional G-type structures, respectively. The hybridization between Fe-3d and Ru-4d is comparatively weaker than in other double perovskite systems. The interplay between strong correlations and reduced itinerancy results in significant spin splitting at Fe and Ru sites. Consequently, a charge transfer process, along with the super-exchange effect, leads to antiferromagnetically coupled Fe3+and Ru5+ions and establishes a semiconducting ferrimagnetic order. Subsequent DMFT calculations demonstrate the persistence of the ferrimagnetic order even at room temperature(300 K). These findings align with prior reports on Sr Fe0.5Ru0.5O3, thus reinforcing the notion that 3d–4d transition metal oxides hold considerable promise as candidates for high-performance spintronic devices, such as spin-valve sensors and spintronic giant magnetoresistance devices.展开更多
The activation and dissociation of hydrogen molecules(H_(2))on the Cu(001)surface are studied theoretically.Using first-principles calculations,the activation barrier for the dissociation of H_(2) on Cu(001)is determi...The activation and dissociation of hydrogen molecules(H_(2))on the Cu(001)surface are studied theoretically.Using first-principles calculations,the activation barrier for the dissociation of H_(2) on Cu(001)is determined to be~0.59 eV in height.It is found that the electron transfer from the copper substrate to H_(2) plays a key role in the activation and breaking of the H–H bond,and the formation of the Cu–H bonds.Two stationary states are identified at around the critical height of bond breaking,corresponding to the molecular and the dissociative states,respectively.Using the transfer matrix method,we also investigate the role of quantum tunneling in the dissociation process along the minimum energy pathway(MEP),which is found to be significant at or below room temperature.At a given temperature,the tunneling contributions due to the translational and the vibrational motions of H_(2) are quantified for the dissociation process.Within a wide range of temperature,the effects of quantum tunneling on the effective barriers of dissociation and the rate constants are observed.The deduced energetic parameters associated with the thermal equilibrium and non-equilibrium(molecular beam)conditions are comparable to experimental data.In the low-temperature region,the crossover from classical to quantum regime is identified.展开更多
The total ionizing dose(TID) effect is a key cause for the degradation/failure of semiconductor device performance under energetic-particle irradiation. We developed a dynamic model of mobile particles and defects by ...The total ionizing dose(TID) effect is a key cause for the degradation/failure of semiconductor device performance under energetic-particle irradiation. We developed a dynamic model of mobile particles and defects by solving the rate equations and Poisson's equation simultaneously, to understand threshold voltage shifts induced by TID in silicon-based metal–oxide–semiconductor(MOS) devices. The calculated charged defect distribution and corresponding electric field under different TIDs are consistent with experiments. TID changes the electric field at the Si/SiO_(2) interface by inducing the accumulation of oxide charged defects nearby, thus shifting the threshold voltage accordingly. With increasing TID, the oxide charged defects increase to saturation, and the electric field increases following the universal 2/3 power law. Through analyzing the influence of TID on the interfacial electric field by different factors, we recommend that the radiation-hardened performance of devices can be improved by choosing a thin oxide layer with high permittivity and under high gate voltages.展开更多
Graphene hosts intriguing photocarrier dynamics such as negative transient terahertz(THz) photoconductivity, high electron temperature, benefiting from the unique linear Dirac dispersion. In this work, the pressure ef...Graphene hosts intriguing photocarrier dynamics such as negative transient terahertz(THz) photoconductivity, high electron temperature, benefiting from the unique linear Dirac dispersion. In this work, the pressure effects of photocarrier dynamics of graphene have been investigated using in situ time-resolved THz spectroscopy in combination with diamond anvil cell exceeding 9 GPa. We find that the negative THz conductivity maintains in our studied pressure range both for monolayer and bilayer graphene. In particular, the amplitude of THz photoconductivity in monolayer graphene manifests an extraordinary dropping with pressure, compared with that from the counterparts such as bulk silicon and bilayer graphene.Concomitantly, the time constant is reduced with increasing pressure, highlighting the pressure-induced hot carrier cooling.The pressure dependence of photocarrier dynamics in monolayer graphene is likely related with the enhancement of the interfacial coupling between diamond surface and sample, allowing for the activity of new electron–phonon scattering. Our work is expected to provide an impetus for the studies of high-pressure THz spectroscopy of two-dimensional materials.展开更多
The adsorption and diffusion of hydrogen atoms on Cu(001)are studied using first-principles calculations.By taking into account the contribution of zero-point energy(ZPE),the originally identical barriers are shown to...The adsorption and diffusion of hydrogen atoms on Cu(001)are studied using first-principles calculations.By taking into account the contribution of zero-point energy(ZPE),the originally identical barriers are shown to be different for H and D,which are respectively calculated to be~158 me V and~139 me V in height.Using the transfer matrix method(TMM),we are able to calculate the accurate probability of transmission across the barriers.The crucial role of quantum tunneling is clearly demonstrated at low-temperature region.By introducing a temperature-dependent attempting frequency prefactor,the rate constants and diffusion coefficients are calculated.The results are in agreement with the experimental measurements at temperatures from~50 K to 80 K.展开更多
Recently,near-ambient superconductivity was claimed in nitrogen-doped lutetium hydride(LuH_(3-δ)N_(ε)).Unfortunately,all follow-up research still cannot find superconductivity signs in successfully synthesized lutet...Recently,near-ambient superconductivity was claimed in nitrogen-doped lutetium hydride(LuH_(3-δ)N_(ε)).Unfortunately,all follow-up research still cannot find superconductivity signs in successfully synthesized lutetium dihydride(LuH_(2)) and N-doped LuH_(2±x)N_(y).However,a similar intriguing observation was the pressure-induced color changes(from blue to pink and subsequent red).The physical understanding of its origin and the correlation between the color,crystal structure,and chemical composition of Lu–H–N is still lacking.In this work,we systematically investigated the optical properties of LuH_(2) and LuH_(3),and the effects of hydrogen vacancies and nitrogen doping using the first-principles calculations by considering both interband and intraband contributions.Our results demonstrate that the evolution of reflectivity peaks near blue and red light,which is driven by changes in the band gap and Fermi velocity of free electrons,resulting in the blue-to-red color change under pressure.In contrast,LuH_(3) exhibits gray and no color change up to 50 GPa.Furthermore,we investigated the effects of hydrogen vacancies and nitrogen doping on its optical properties.Hydrogen vacancies can significantly decrease the pressure of blue-to-red color change in LuH_(2) but do not have a noticeable effect on the color of LuH_(3).The N-doped LuH_(2) with the substitution of a hydrogen atom at the tetrahedral position maintains the color change when the N-doping concentration is low.As the doping level increases,this trend becomes less obvious,while other N-doped structures do not show a blue-to-red color change.Our results can clarify the origin of the experimental observed blue-to-red color change in lutetium hydride and also provide a further understanding of the potential N-doped lutetium dihydride.展开更多
The recent report of superconductivity in nitrogen-doped lutetium hydride(Lu-H-N)at 294 K and 1 GPa brought hope for long-sought-after ambient-condition superconductors.However,the failure of scientists worldwide to i...The recent report of superconductivity in nitrogen-doped lutetium hydride(Lu-H-N)at 294 K and 1 GPa brought hope for long-sought-after ambient-condition superconductors.However,the failure of scientists worldwide to independently reproduce these results has cast intense skepticism on this exciting claim.In this work,using a reliable experimental protocol,we synthesized Lu-H-N while minimizing extrinsic influences and reproduced the sudden change in resistance near room temperature.With quantitative comparison of the temperaturedependent resistance between Lu-H-N and the pure lutetium before reaction,we were able to clarify that the drastic resistance change is most likely caused by a metal-to-poor-conductor transition rather than by superconductivity.Herein,we also briefly discuss other issues recently raised in relation to the Lu-H-N system.展开更多
Transition metal oxides are regarded as promising candidates of anode for next-generation lithium-ion batteries(LIBs)due to their ultrahigh theoretical capacity and low cost,but are restricted by their low conductivit...Transition metal oxides are regarded as promising candidates of anode for next-generation lithium-ion batteries(LIBs)due to their ultrahigh theoretical capacity and low cost,but are restricted by their low conductivity and large volume expansion during Li^(+)intercalation.Herein,we designed and constructed a structurally integrated 3D carbon tube(3D-CT)grid film with Mn_(3)O_(4)nanoparticles(Mn_(3)O_(4)-NPs)and carbon nanotubes(CNTs)filled in the inner cavity of CTs(denoted as Mn_(3)O_(4)-NPs/CNTs@3D-CT)as high-performance free-standing anode for LIBs.The Mn_(3)O_(4)-NPs/CNTs@3D-CT grid with Mn_(3)O_(4)-NPs filled in the inner cavity of 3D-CT not only afford sufficient space to overcome the damage caused by the volume expansion of Mn_(3)O_(4)-NPs during charge and discharge processes,but also achieves highly efficient channels for the fast transport of both electrons and Li+during cycling,thus offering outstanding electrochemical performance(865 mAh g^(-1)at 1 A g^(-1)after 300 cycles)and excellent rate capability(418 mAh g^(-1)at 4 A g^(-1))based on the total mass of electrode.The unique 3D-CT framework structure would open up a new route to the highly stable,high-capacity,and excellent cycle and high-rate performance free-standing electrodes for highperformance Li-ion storage.展开更多
To remove the key impurity elements,P and B,from primary Si simultaneously,Sr and Zr co-addition to Al-Si alloy systems during solvent refining has been investigated.Sr reacts with Al,Si,and P in the melt to form a P-...To remove the key impurity elements,P and B,from primary Si simultaneously,Sr and Zr co-addition to Al-Si alloy systems during solvent refining has been investigated.Sr reacts with Al,Si,and P in the melt to form a P-containing Al_(2)Si_(2)Sr phase and Zr reacts with B to form a ZrB_(2) phase.In the Al-Si-Sr-Zr system,high removal fractions of P and B in the primary Si,with 84.8%-98.4%and 90.7%-96.7%,respectively,are achieved at the same time,respectively.The best removal effect is obtained in the sample with the addition of Sr-32000+Zr-3000μg·kg^(-1),and the removal fractions of P and B in the purified Si reach 98.4%and 96.1%.Compared with the Sr/Zr single-addition,the removal effects of Sr and Zr co-addition on P and B do not show a significant downward trend,indicating that the nucleation and growth of the B/P-containing impurity phases are mutually independent.Finally,an evolution model is proposed to describe the nucleation and the growth stages of Sr/Zr-containing compound phases,which reveals the interaction between the impurity phases and the primary Si.展开更多
Arson presents a challenging crime scene for fire investigators worldwide. Key to the investigation of suspected arson cases is the analysis of fire debris for the presence of accelerants or ignitable liquids. This st...Arson presents a challenging crime scene for fire investigators worldwide. Key to the investigation of suspected arson cases is the analysis of fire debris for the presence of accelerants or ignitable liquids. This study has investigated the application and method development of vapor phase mid-Infrared (mid-IR) spectroscopy using a field portable quantum cascade laser (QCL) based system for the detection and identification of accelerant residues such as gasoline, diesel, and ethanol in fire debris. A searchable spectral library of various ignitable fluids and fuel components measured in the vapor phase was constructed that allowed for real-time identification of accelerants present in samples using software developed in-house. Measurement of vapors collected from paper material that had been doused with an accelerant followed by controlled burning and then extinguished with water showed that positive identification could be achieved for gasoline, diesel, and ethanol. This vapor phase mid-IR QCL method is rapid, easy to use, and has the sensitivity and discrimination capability that make it well suited for non-destructive crime scene sample analysis. Sampling and measurement can be performed in minutes with this 7.5 kg instrument. This vibrational spectroscopic method required no time-consuming sample pretreatment or complicated solvent extraction procedure. The results of this initial feasibility study demonstrate that this portable fire debris analyzer would greatly benefit arson investigators performing analysis on-site.展开更多
The combination of non-Hermitian physics and Majorana fermions can give rise to new effects in quantum transport systems. In this work, we investigate the interplay of PT-symmetric complex potentials, Majorana tunneli...The combination of non-Hermitian physics and Majorana fermions can give rise to new effects in quantum transport systems. In this work, we investigate the interplay of PT-symmetric complex potentials, Majorana tunneling and interdot tunneling in a non-Hermitian double quantum dots system. It is found that in the weak-coupling regime the Majorana tunneling has pronounced effects on the transport properties of such a system, manifested as splitting of the single peak into three and a reduced 1/4 peak in the transmission function. In the presence of the PT-symmetric complex potentials and interdot tunneling, the 1/4 central peak is robust against them, while the two side peaks are tuned by them. The interdot tunneling only induces asymmetry, instead of moving the conductance peak, due to the robustness of the Majorana modes. There is an exceptional point induced by the union of Majorana tunneling and interdot tunneling. With increased PT-symmetric complex potentials, the two side peaks will move towards each other. When the exceptional point is passed through, these two side peaks will disappear. In the strong-coupling regime, the Majorana fermion induces a 1/4 conductance dip instead of the three-peak structure. PT-symmetric complex potentials induce two conductance dips pinned at the exceptional point. These effects should be accessible in experiments.展开更多
We report a systematic study on layered metal SrCu_(4-x)P_(2) single crystals via transport, magnetization, thermodynamic measurements and structural characterization. We find that the crystals show large linear magne...We report a systematic study on layered metal SrCu_(4-x)P_(2) single crystals via transport, magnetization, thermodynamic measurements and structural characterization. We find that the crystals show large linear magnetoresistance without any sign of saturation with a magnetic field up to 30T. We also observe a phase transition with significant anomalies in resistivity and heat capacity at T_(p)~140 K. Thermal expansion measurement reveals a subtle lattice parameter variation near Tp, i.e.,?L_(c)/L_(c)~0.062%. The structural characterization confines that there is no structure transition below and above T_(p). All these results suggest that the nonmagnetic transition of SrCu_(4-x)P_(2) could be associated with structural distortion.展开更多
Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites...Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen(O)coordination on bacterial cellulose-converted graphitic carbon(Mn-O-C).Evidence of the atomically dispersed Mn-(O-C_(2))_(4)moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption spectroscopy.As a result,the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH_(3)yield rate(RNH_(3))of 1476.9±62.6μg h^(−1)cm^(−2)at−0.7 V(vs.reversible hydrogen electrode,RHE)and a faradaic efficiency(FE)of 89.0±3.8%at−0.5 V(vs.RHE)under ambient conditions.Further,when evaluated with a practical flow cell,Mn-O-C shows a high RNH_(3)of 3706.7±552.0μg h^(−1)cm^(−2)at a current density of 100 mA cm−2,2.5 times of that in the H cell.The in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C_(2))_(4)sites not only effectively inhibit the competitive hydrogen evolution reaction,but also greatly promote the adsorption and activation of nitrate(NO_(3)^(−)),thus boosting both the FE and selectivity of NH_(3)over Mn-(O-C_(2))_(4)sites.展开更多
A procedure is presented for the calculation of the Mn^(2+)-F^(-) bond length from the superhyperfine constants measured by magnetic resonance experiments.With the present technique it is possible to detect the variat...A procedure is presented for the calculation of the Mn^(2+)-F^(-) bond length from the superhyperfine constants measured by magnetic resonance experiments.With the present technique it is possible to detect the variation of the bond length,ΔR,down to 0.01Å.The technique is sensitive enough to determine the bond length R and its variationΔR experienced when pressure or temperature changes.展开更多
基金supported by the National Natural Science Foundation of China(52172243)。
文摘The(electro)chemical stability and Li dendrite suppression capability of sulfide solid electrolytes(SEs)need further improvement for developing all-solid-state Li batteries(ASSLBs).Here,we report advanced halogen-rich argyrodites via I and Cl co-occupation on the crystal lattice.Notably,a proper I content forms a single phase,whereas an excessive I causes precipitation of two argyrodite phases like a superlattice structure.The resultant synergistic effect of the optimized composition allows to gain high ionic conductivities at room temperature and-20℃,and enhances the(electro)chemical stability against Li and Li dendrite suppression capability.The Li|argyrodite interface is very sensitive to the ratio of I and Cl.A LiCl-and LiI-rich double-layer interface is observed from the cell using the SE with optimized composition,whereas too high I content forms only a single interface layer with a mixture of Lil and LiCl.This double-layer interface is found to effectively mitigate the Li/SE reaction.The proper designed argyrodite enables ASSLBs to achieve good electrochemical properties at a broad temperature range regardless of the electrode materials.This co-occupation strategy provides a novel exploration for advanced halogen-rich argyrodite system.
基金Funded by the National Natural Science Foundation of China(Nos.51701206 and 51671187)the Shanxi Natural Science Foundation(No.2019JQ-833)+2 种基金the Anhui Natural Science Foundation(1808085QE166)the Special Scientific Research Project of Shanxi Education Committee(No.19JQ0974)the Doctoral Research Initiation Project of Yan’an University(No.YDBD2018-21)。
文摘The mechanical behavior and microstructural evolution of an Fe-30Mn-3Al-3Si twinninginduced plasticity(TWIP)steel processed using warm forging was investigated.It is found that steel processed via warm forging improves comprehensive mechanical properties compared to the TWIP steel processed via cold rolling,with a high tensile strength(R_(m))of 793 MPa,a yield strength(R_(P))of 682 MPa,an extremely large R_(P)/R_(m)ratio as high as 0.86 as well as an excellent elongation rate of 46.8%.The microstructure observation demonstrates that steel processed by warm forging consists of large and elongated grains together with fine,equiaxed grains.Complicated micro-defect configurations were also observed within the steel,including dense dislocation networks and a few coarse deformation twins.As the plastic deformation proceeds,the densities of dislocations and deformation twins significantly increase.Moreover,a great number of slip lines could be observed in the elongated grains.These findings reveal that a much more dramatic interaction between microstructural defect and dislocations glide takes place in the forging sample,wherein the fine and equiaxed grains propagated dislocations more rapidly,together with initial defect configurations,are responsible for enhanced strength properties.Meanwhile,larger,elongated grains with more prevalently activated deformation twins result in high plasticity.
基金supported by the National Natural Science Foundation of China (Grant Nos. 12374012, 11974208, 52172212, and 52002217)Shandong Provincial Natural Science Foundation (Grant Nos. ZR2023JQ001, ZR2020YQ05, and 2019KJJ020)financial support from the Program of Distinguished Expert of Taishan Scholar (Grant No. tstp20221124)。
文摘As a sister compound of PbTe, SnTe possesses the environmentally friendly elements. However, the pristine SnTe compounds suffer from the high carrier concentration, the large valence band offset between the L and Σpositions and high thermal conductivity. Using high-pressure and high-temperature technology, we synthesized the pristine SnTe samples at different pressures and systemically investigated their thermoelectric properties.High pressure induces rich microstructures, including the high-density dislocations and lattice distortions, which serve as the strong phonon scattering centers, thereby reducing the lattice thermal conductivity. For the electrical properties, pressure reduces the harmful high carrier concentration, due to the depression of Sn vacancies.Moreover, pressure induces the valence band convergence, reducing the energy separation between the L and Σpositions. The band convergence and suppressed carrier concentration increase the Seebeck coefficient. Thus, the power factors of pressure-sintered compounds do not deteriorate significantly under the condition of decreasing electrical conductivity. Ultimately, for a pristine SnTe compound synthesized at 5 GPa, a higher ZT value of 0.51 is achieved at 750 K, representing a 140% improvement compared to the value of 0.21 obtained using SPS. Therefore, the high-pressure and high-temperature technology is demonstrated as an effectively approach to optimize thermoelectric performance.
文摘The composite internal friction peak(versus temperature)assumed to be consisted of a relaxation peak and a phase transformation peak previously observed in cold-worked Al-0.50wt%(0.21at%)Cu at temperatures below room temperature are now resolved into two separate peaks.Internal friotion peaks as a function of strain amplitude(the amplitude peak)are observed around the temperature region of both peaks for he first time.
基金financially supported by the National Natural Science Foundation of China (Nos. 52171071, 52172090, 52071159, and 51801081)Portugal National Funds through FCT project (No. 2021.04115)+4 种基金FEDER National funds FCT under the project CEMMPRE–UIDB/ 00285/2020Outstanding University Young Teachers of “Qing Lan Project” of Jiangsu ProvinceExcellent Talents of “Shenlan Project” of Jiangsu University of Science and Technologyand China Merchants Marine Scientific Research and Innovation FundFilipe Fernandes acknowledges the funding received in the aim of the projects: MCTool21– ref. “POCI-01-0247-FEDER-045940”, CEMMPRE–ref. “UIDB/00285/2020”, and SMARTLUB–ref. “POCI-010145-FEDER-031807”
文摘The need for reducing the wear in mechanical parts used in the industry makes self-lubricant films one of the sustainable solutions to achieve long-term protection under different environmental conditions.The purpose of this work is to study the influence of C additions on the tribological behavior of a magnetron-sputtered TiN film in air,water,and seawater.The results show that the addition of C into the TiN binary film induced a new amorphous phase,and the films exhibited a dual phase of fcc(face-centered cubic)-TiN and amorphous carbon.The antifriction and wear-resistance properties were enhanced in air and water by adding 19.1at%C.However,a further increase in the C concentration improved anti-frictional properties but also led to higher wear rates.Although the amorphous phase induced microbatteries and accelerated the corrosion of TiN phases in seawater,the negative abrasion state was detected for all Ti-C-N films due to the adhesion of the tribocorrosion debris on the wear track.
基金Project supported by the starting funds from Northwest University。
文摘By employing a combined approach of density-functional theory(DFT) and dynamical mean-field theory(DMFT) calculations, we examine the structural, electronic, and magnetic characteristics of two distinct strontium ruthenates: Sr2RuO4,an unconventional superconductor, and the correlated metal SrRuO3, both at 50% Fe-doping level. In both Sr2Fe0.5Ru0.5O4and SrFe0.5Ru0.5O3, the original ruthenium(Ru) and the dopant iron(Fe) atoms adopt 3-dimensional and 2-dimensional G-type structures, respectively. The hybridization between Fe-3d and Ru-4d is comparatively weaker than in other double perovskite systems. The interplay between strong correlations and reduced itinerancy results in significant spin splitting at Fe and Ru sites. Consequently, a charge transfer process, along with the super-exchange effect, leads to antiferromagnetically coupled Fe3+and Ru5+ions and establishes a semiconducting ferrimagnetic order. Subsequent DMFT calculations demonstrate the persistence of the ferrimagnetic order even at room temperature(300 K). These findings align with prior reports on Sr Fe0.5Ru0.5O3, thus reinforcing the notion that 3d–4d transition metal oxides hold considerable promise as candidates for high-performance spintronic devices, such as spin-valve sensors and spintronic giant magnetoresistance devices.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11474285 and 12074382)。
文摘The activation and dissociation of hydrogen molecules(H_(2))on the Cu(001)surface are studied theoretically.Using first-principles calculations,the activation barrier for the dissociation of H_(2) on Cu(001)is determined to be~0.59 eV in height.It is found that the electron transfer from the copper substrate to H_(2) plays a key role in the activation and breaking of the H–H bond,and the formation of the Cu–H bonds.Two stationary states are identified at around the critical height of bond breaking,corresponding to the molecular and the dissociative states,respectively.Using the transfer matrix method,we also investigate the role of quantum tunneling in the dissociation process along the minimum energy pathway(MEP),which is found to be significant at or below room temperature.At a given temperature,the tunneling contributions due to the translational and the vibrational motions of H_(2) are quantified for the dissociation process.Within a wide range of temperature,the effects of quantum tunneling on the effective barriers of dissociation and the rate constants are observed.The deduced energetic parameters associated with the thermal equilibrium and non-equilibrium(molecular beam)conditions are comparable to experimental data.In the low-temperature region,the crossover from classical to quantum regime is identified.
基金Project supported by the Science Challenge Project of China (Grant No.TZ2018004)the National Natural Science Foundation of China (Grant Nos.11975018 and 11775254)+1 种基金the National MCF Energy R&D Program of China (Grant No.2018YEF0308100)the outstanding member of Youth Innovation Promotion Association CAS (Grant No.Y202087)。
文摘The total ionizing dose(TID) effect is a key cause for the degradation/failure of semiconductor device performance under energetic-particle irradiation. We developed a dynamic model of mobile particles and defects by solving the rate equations and Poisson's equation simultaneously, to understand threshold voltage shifts induced by TID in silicon-based metal–oxide–semiconductor(MOS) devices. The calculated charged defect distribution and corresponding electric field under different TIDs are consistent with experiments. TID changes the electric field at the Si/SiO_(2) interface by inducing the accumulation of oxide charged defects nearby, thus shifting the threshold voltage accordingly. With increasing TID, the oxide charged defects increase to saturation, and the electric field increases following the universal 2/3 power law. Through analyzing the influence of TID on the interfacial electric field by different factors, we recommend that the radiation-hardened performance of devices can be improved by choosing a thin oxide layer with high permittivity and under high gate voltages.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12174398,12004387,51727806,51672279,11874361,and 12204484)the Innovation Program of Chinese Academy of Sciences(Grant No.CXJJ-19B08)+2 种基金the Youth Innovation Promotion Association of Chinese Academy of Sciences(Grant No.2021446)the HFIPS Director’s Fund of Chinese Academy of Sciences(Grant Nos.2021YZGH03 and YZJJKX202202)China Postdoctoral Science Foundation(Grant No.2021M703255)。
文摘Graphene hosts intriguing photocarrier dynamics such as negative transient terahertz(THz) photoconductivity, high electron temperature, benefiting from the unique linear Dirac dispersion. In this work, the pressure effects of photocarrier dynamics of graphene have been investigated using in situ time-resolved THz spectroscopy in combination with diamond anvil cell exceeding 9 GPa. We find that the negative THz conductivity maintains in our studied pressure range both for monolayer and bilayer graphene. In particular, the amplitude of THz photoconductivity in monolayer graphene manifests an extraordinary dropping with pressure, compared with that from the counterparts such as bulk silicon and bilayer graphene.Concomitantly, the time constant is reduced with increasing pressure, highlighting the pressure-induced hot carrier cooling.The pressure dependence of photocarrier dynamics in monolayer graphene is likely related with the enhancement of the interfacial coupling between diamond surface and sample, allowing for the activity of new electron–phonon scattering. Our work is expected to provide an impetus for the studies of high-pressure THz spectroscopy of two-dimensional materials.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11474285 and 12074382)。
文摘The adsorption and diffusion of hydrogen atoms on Cu(001)are studied using first-principles calculations.By taking into account the contribution of zero-point energy(ZPE),the originally identical barriers are shown to be different for H and D,which are respectively calculated to be~158 me V and~139 me V in height.Using the transfer matrix method(TMM),we are able to calculate the accurate probability of transmission across the barriers.The crucial role of quantum tunneling is clearly demonstrated at low-temperature region.By introducing a temperature-dependent attempting frequency prefactor,the rate constants and diffusion coefficients are calculated.The results are in agreement with the experimental measurements at temperatures from~50 K to 80 K.
基金supported by the National Key Research and Development Program of China(Grant Nos.2022YFA1403203 and 2021YFA1600200)the National Natural Science Foundation of China(Grant Nos.U2032215 and 12241405)。
文摘Recently,near-ambient superconductivity was claimed in nitrogen-doped lutetium hydride(LuH_(3-δ)N_(ε)).Unfortunately,all follow-up research still cannot find superconductivity signs in successfully synthesized lutetium dihydride(LuH_(2)) and N-doped LuH_(2±x)N_(y).However,a similar intriguing observation was the pressure-induced color changes(from blue to pink and subsequent red).The physical understanding of its origin and the correlation between the color,crystal structure,and chemical composition of Lu–H–N is still lacking.In this work,we systematically investigated the optical properties of LuH_(2) and LuH_(3),and the effects of hydrogen vacancies and nitrogen doping using the first-principles calculations by considering both interband and intraband contributions.Our results demonstrate that the evolution of reflectivity peaks near blue and red light,which is driven by changes in the band gap and Fermi velocity of free electrons,resulting in the blue-to-red color change under pressure.In contrast,LuH_(3) exhibits gray and no color change up to 50 GPa.Furthermore,we investigated the effects of hydrogen vacancies and nitrogen doping on its optical properties.Hydrogen vacancies can significantly decrease the pressure of blue-to-red color change in LuH_(2) but do not have a noticeable effect on the color of LuH_(3).The N-doped LuH_(2) with the substitution of a hydrogen atom at the tetrahedral position maintains the color change when the N-doping concentration is low.As the doping level increases,this trend becomes less obvious,while other N-doped structures do not show a blue-to-red color change.Our results can clarify the origin of the experimental observed blue-to-red color change in lutetium hydride and also provide a further understanding of the potential N-doped lutetium dihydride.
文摘The recent report of superconductivity in nitrogen-doped lutetium hydride(Lu-H-N)at 294 K and 1 GPa brought hope for long-sought-after ambient-condition superconductors.However,the failure of scientists worldwide to independently reproduce these results has cast intense skepticism on this exciting claim.In this work,using a reliable experimental protocol,we synthesized Lu-H-N while minimizing extrinsic influences and reproduced the sudden change in resistance near room temperature.With quantitative comparison of the temperaturedependent resistance between Lu-H-N and the pure lutetium before reaction,we were able to clarify that the drastic resistance change is most likely caused by a metal-to-poor-conductor transition rather than by superconductivity.Herein,we also briefly discuss other issues recently raised in relation to the Lu-H-N system.
基金supported by the Natural Science Foundation of China(91963202 and 52072372)the Key Research Program of Frontier Sciences(CAS,Grant,QYZDJ-SSW-SLH046)the CAS/SAFEA International Partnership Program for Creative Research Teams,and the Hefei Institutes of Physical Science,Chinese Academy of Sciences Director’s Fund(YZJ ZX202018)
文摘Transition metal oxides are regarded as promising candidates of anode for next-generation lithium-ion batteries(LIBs)due to their ultrahigh theoretical capacity and low cost,but are restricted by their low conductivity and large volume expansion during Li^(+)intercalation.Herein,we designed and constructed a structurally integrated 3D carbon tube(3D-CT)grid film with Mn_(3)O_(4)nanoparticles(Mn_(3)O_(4)-NPs)and carbon nanotubes(CNTs)filled in the inner cavity of CTs(denoted as Mn_(3)O_(4)-NPs/CNTs@3D-CT)as high-performance free-standing anode for LIBs.The Mn_(3)O_(4)-NPs/CNTs@3D-CT grid with Mn_(3)O_(4)-NPs filled in the inner cavity of 3D-CT not only afford sufficient space to overcome the damage caused by the volume expansion of Mn_(3)O_(4)-NPs during charge and discharge processes,but also achieves highly efficient channels for the fast transport of both electrons and Li+during cycling,thus offering outstanding electrochemical performance(865 mAh g^(-1)at 1 A g^(-1)after 300 cycles)and excellent rate capability(418 mAh g^(-1)at 4 A g^(-1))based on the total mass of electrode.The unique 3D-CT framework structure would open up a new route to the highly stable,high-capacity,and excellent cycle and high-rate performance free-standing electrodes for highperformance Li-ion storage.
基金supported by the National Natural Science Foundation of China(Nos.51804294,51874272,52111540265)Anhui Provincial Natural Science Foundation(No.1808085ME121)+4 种基金the Key Laboratory of Photovoltaic and Energy Conservation Materials,Chinese Academy of Science(No.PECL2021QN003)Hefei Institutes of Physical Science,Chinese Academy of Sciences Director’s Fund(No.YZJJZX202018)International Clean Energy Talent Program by China Scholarship CouncilOpen Foundation of State Key Laboratory of Mineral Processing(No.BGRIMM-KJSKL-2022-23)Open Foundation of State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization(No.CNMRCUKF2205)。
文摘To remove the key impurity elements,P and B,from primary Si simultaneously,Sr and Zr co-addition to Al-Si alloy systems during solvent refining has been investigated.Sr reacts with Al,Si,and P in the melt to form a P-containing Al_(2)Si_(2)Sr phase and Zr reacts with B to form a ZrB_(2) phase.In the Al-Si-Sr-Zr system,high removal fractions of P and B in the primary Si,with 84.8%-98.4%and 90.7%-96.7%,respectively,are achieved at the same time,respectively.The best removal effect is obtained in the sample with the addition of Sr-32000+Zr-3000μg·kg^(-1),and the removal fractions of P and B in the purified Si reach 98.4%and 96.1%.Compared with the Sr/Zr single-addition,the removal effects of Sr and Zr co-addition on P and B do not show a significant downward trend,indicating that the nucleation and growth of the B/P-containing impurity phases are mutually independent.Finally,an evolution model is proposed to describe the nucleation and the growth stages of Sr/Zr-containing compound phases,which reveals the interaction between the impurity phases and the primary Si.
文摘Arson presents a challenging crime scene for fire investigators worldwide. Key to the investigation of suspected arson cases is the analysis of fire debris for the presence of accelerants or ignitable liquids. This study has investigated the application and method development of vapor phase mid-Infrared (mid-IR) spectroscopy using a field portable quantum cascade laser (QCL) based system for the detection and identification of accelerant residues such as gasoline, diesel, and ethanol in fire debris. A searchable spectral library of various ignitable fluids and fuel components measured in the vapor phase was constructed that allowed for real-time identification of accelerants present in samples using software developed in-house. Measurement of vapors collected from paper material that had been doused with an accelerant followed by controlled burning and then extinguished with water showed that positive identification could be achieved for gasoline, diesel, and ethanol. This vapor phase mid-IR QCL method is rapid, easy to use, and has the sensitivity and discrimination capability that make it well suited for non-destructive crime scene sample analysis. Sampling and measurement can be performed in minutes with this 7.5 kg instrument. This vibrational spectroscopic method required no time-consuming sample pretreatment or complicated solvent extraction procedure. The results of this initial feasibility study demonstrate that this portable fire debris analyzer would greatly benefit arson investigators performing analysis on-site.
基金Project supported by the National Natural Science Foundation of China (Grant No.11834005)。
文摘The combination of non-Hermitian physics and Majorana fermions can give rise to new effects in quantum transport systems. In this work, we investigate the interplay of PT-symmetric complex potentials, Majorana tunneling and interdot tunneling in a non-Hermitian double quantum dots system. It is found that in the weak-coupling regime the Majorana tunneling has pronounced effects on the transport properties of such a system, manifested as splitting of the single peak into three and a reduced 1/4 peak in the transmission function. In the presence of the PT-symmetric complex potentials and interdot tunneling, the 1/4 central peak is robust against them, while the two side peaks are tuned by them. The interdot tunneling only induces asymmetry, instead of moving the conductance peak, due to the robustness of the Majorana modes. There is an exceptional point induced by the union of Majorana tunneling and interdot tunneling. With increased PT-symmetric complex potentials, the two side peaks will move towards each other. When the exceptional point is passed through, these two side peaks will disappear. In the strong-coupling regime, the Majorana fermion induces a 1/4 conductance dip instead of the three-peak structure. PT-symmetric complex potentials induce two conductance dips pinned at the exceptional point. These effects should be accessible in experiments.
基金Project supported by the National Key Research and Development Program of China (Grant Nos.2023YFA1607403,2021YFA1600201,and 2022YFA1602603)the Natural Science Foundation of China (Grant Nos.U19A2093,U2032214,and U2032163)+5 种基金the Collaborative Innovation Program of Hefei Science Center,CAS (Grant No.2019HSC-CIP 001)the Youth Innovation Promotion Association of CAS (Grant No.2021117)the Natural Science Foundation of Anhui Province (No.1908085QA15)the HFIPS Director’s Fund (Grant No.YZJJQY202304)the CASHIPS Director’s Fund (Grant No.YZJJ2022QN36)supported by the High Magnetic Field Laboratory of Anhui Province。
文摘We report a systematic study on layered metal SrCu_(4-x)P_(2) single crystals via transport, magnetization, thermodynamic measurements and structural characterization. We find that the crystals show large linear magnetoresistance without any sign of saturation with a magnetic field up to 30T. We also observe a phase transition with significant anomalies in resistivity and heat capacity at T_(p)~140 K. Thermal expansion measurement reveals a subtle lattice parameter variation near Tp, i.e.,?L_(c)/L_(c)~0.062%. The structural characterization confines that there is no structure transition below and above T_(p). All these results suggest that the nonmagnetic transition of SrCu_(4-x)P_(2) could be associated with structural distortion.
基金the financial support from the Natural Science Foundation of China(Grant No.52172106)Anhui Provincial Natural Science Foundation(Grant Nos.2108085QB60 and 2108085QB61)China Postdoctoral Science Foundation(Grant Nos.2020M682057 and 2023T160651).
文摘Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen(O)coordination on bacterial cellulose-converted graphitic carbon(Mn-O-C).Evidence of the atomically dispersed Mn-(O-C_(2))_(4)moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption spectroscopy.As a result,the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH_(3)yield rate(RNH_(3))of 1476.9±62.6μg h^(−1)cm^(−2)at−0.7 V(vs.reversible hydrogen electrode,RHE)and a faradaic efficiency(FE)of 89.0±3.8%at−0.5 V(vs.RHE)under ambient conditions.Further,when evaluated with a practical flow cell,Mn-O-C shows a high RNH_(3)of 3706.7±552.0μg h^(−1)cm^(−2)at a current density of 100 mA cm−2,2.5 times of that in the H cell.The in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C_(2))_(4)sites not only effectively inhibit the competitive hydrogen evolution reaction,but also greatly promote the adsorption and activation of nitrate(NO_(3)^(−)),thus boosting both the FE and selectivity of NH_(3)over Mn-(O-C_(2))_(4)sites.
基金Supported by tke National Natural Science Foundation of China under Grant No.19574036.
文摘A procedure is presented for the calculation of the Mn^(2+)-F^(-) bond length from the superhyperfine constants measured by magnetic resonance experiments.With the present technique it is possible to detect the variation of the bond length,ΔR,down to 0.01Å.The technique is sensitive enough to determine the bond length R and its variationΔR experienced when pressure or temperature changes.