Transition metal dichalcogenides(TMDs), exhibit a range of crystal structures and topological quantum states. The1T phase, in particular, shows promise for superconductivity driven by electron–phonon coupling(EPC), s...Transition metal dichalcogenides(TMDs), exhibit a range of crystal structures and topological quantum states. The1T phase, in particular, shows promise for superconductivity driven by electron–phonon coupling(EPC), strain, pressure,and chemical doping. In this theoretical investigation, we explore 1T-Rh Se Te as a novel type of TMD superconductor with topological electronic states. The optimal doping structure and atomic arrangement of 1T-Rh Se Te are constructed.Phonon spectrum calculations validate the integrity of the constructed doping structure. The analysis of the electron–phonon coupling using the electron–phonon Wannier(EPW) method has confirmed the existence of a robust electron–phonon interaction in 1T-Rh Se Te, resulting in total EPC constant λ = 2.02, the logarithmic average frequency ω_(log)= 3.15 me V and T_c = 4.61 K, consistent with experimental measurements and indicative of its classification as a BCS superconductor.The band structure analysis revealed the presence of Dirac-like band crossing points. The topological non-trivial electronic structures of the 1T-Rh Se Te are confirmed via the evolution of Wannier charge centers(WCCs) and time-reversal symmetryprotected topological surface states(TSSs). These distinctive properties underscore 1T-Rh Se Te as a possible candidate for a topological superconductor, warranting further investigation into its potential implications and applications.展开更多
Facile preparation of cost-effective and durable porous carbon-supported non-precious-metal/nitrogen electrocatalysts for oxygen reduction reaction(ORR)is extremely important for promoting the commercialized applicati...Facile preparation of cost-effective and durable porous carbon-supported non-precious-metal/nitrogen electrocatalysts for oxygen reduction reaction(ORR)is extremely important for promoting the commercialized applications of such catalysts.In this work,the FeCl3-containing porphyrinato iron-based covalent porous polymer(FeCl3·FeP or-CPP)was fabricated in-situ onto porous corncob biomass supports via a simple one-pot method.Subsequent thermal-reduction pyrolysis at 700℃-900℃with CO2 gas as an activating agent resulted in Fe2O3-decorated and N-doped graphitic carbon composite Fe2O3@NC&bio-C with a high degree of graphitization of Fe-involved promotion during pyrolysis(Fe2O3=FeCl3·FePor-CPP derived Fe2O3;NC=N-doped graphene analog;bio-C=the corncob-derived hierarchically porous graphitic biomass carbon framework).The derivedα-Fe2O3 andγ-Fe2O3 nanocrystals(5-10 nm particle diameter)were all immobilized on the N-doped bio-C micro/nanofibers.Notably,the Fe2O3@NC&bio-C obtained at the pyrolysis temperature of 800℃(Fe2O3@NC&bio-C-800),exhibited unusual ORR catalytic efficiency via a 4-electron pathway with the onset and half-wave potentials of 0.96 V and 0.85 V vs.RHE,respectively.In addition,Fe2O3@NC&bio-C-800 also exhibited a high and stable limiting current density of-6.0 mA cm-2,remarkably stability(larger than 91%retention after 10000 s),and good methanol tolerance.The present work represents one of the best results for iron-based biomass material ORR catalysts reported to date.The high ORR activity is attributed to the uniformly distributedα-Fe2O3 andγ-Fe2O3 nanoparticles on the N-enriched carbon matrix with a large specific surface area of 772.6 m^2 g^-1.This facilitates favor faster electron movement and better adsorption of oxygen molecules on the surface of the catalyst.Nevertheless,comparative studies on the structure and ORR catalytic activity of Fe2O3@NC&bioC-800 with Fe2O3@bio-C-800 and NC&bio-C-800 clearly highlight the synergistic effect of the coexisting Fe2O3 nanocrystals,NC,and bio-C on the ORR performance.展开更多
Distinctive superconducting behaviors between bulk and monolayer FeSe make it challenging to obtain a unified picture of all FeSe-based superconductors.We investigate the ultrafast quasiparticle(QP)dynamics of an inte...Distinctive superconducting behaviors between bulk and monolayer FeSe make it challenging to obtain a unified picture of all FeSe-based superconductors.We investigate the ultrafast quasiparticle(QP)dynamics of an intercalated superconductor(Li1-xFex)OHFe1-ySe,which is a bulk crystal but shares a similar electronic structure with single-layer FeSe on SrTiO3.We obtain the electron-phonon coupling(EPC)constant(0.22±0.04),which well bridges that of bulk FeSe crystal and single-layer FeSe on SrTiO3.Significantly,we find that such a positive correlation betweenλA1 g and superconducting Tc holds among all known FeSe-based superconductors,even in line with reported FeAs-based superconductors.Our observation indicates possible universal role of EPC in the superconductivity of all known categories of iron-based superconductors,which is a critical step towards achieving a unified superconducting mechanism for all iron-based superconductors.展开更多
By integrating pump-probe ultrafast spectroscopy with diamond anvil cell(DAC)technique,we demonstrate a time-resolved ultrafast dynamics study on non-equilibrium quasiparticle(QP)states in.SVo/rQi under high pressure....By integrating pump-probe ultrafast spectroscopy with diamond anvil cell(DAC)technique,we demonstrate a time-resolved ultrafast dynamics study on non-equilibrium quasiparticle(QP)states in.SVo/rQi under high pressure.On-site in situ condition is realized,where both the sample and DAC have fixed position during the experiment.The QP dynamics exhibits a salient pressure-induced phonon bottleneck feature at 20GPa,which corresponds to a gap shrinkage in the electronic structure.A structural transition is also observed at 32 GPa.In addition,the slowest relaxation component reveals possible heat diffusion or pressure-controlled local spin fluctuation associated with the gap shrinkage.Our work enables precise pressure dependence investigations of ultrafast dynamics,paving the way for reliable studies of high-pressure excited state physics.展开更多
基金Project supported by the National Natural Science Foundation of China (Grant No. 12204400)Science Research Project of Hebei Education Department (Grant No. QN2022169)+1 种基金the Natural Science Foundation of Hebei Province (Grant Nos. A2022203010 and A2024203011)Innovation Capability Improvement Project of Hebei Province (Grant No. 22567605H)。
文摘Transition metal dichalcogenides(TMDs), exhibit a range of crystal structures and topological quantum states. The1T phase, in particular, shows promise for superconductivity driven by electron–phonon coupling(EPC), strain, pressure,and chemical doping. In this theoretical investigation, we explore 1T-Rh Se Te as a novel type of TMD superconductor with topological electronic states. The optimal doping structure and atomic arrangement of 1T-Rh Se Te are constructed.Phonon spectrum calculations validate the integrity of the constructed doping structure. The analysis of the electron–phonon coupling using the electron–phonon Wannier(EPW) method has confirmed the existence of a robust electron–phonon interaction in 1T-Rh Se Te, resulting in total EPC constant λ = 2.02, the logarithmic average frequency ω_(log)= 3.15 me V and T_c = 4.61 K, consistent with experimental measurements and indicative of its classification as a BCS superconductor.The band structure analysis revealed the presence of Dirac-like band crossing points. The topological non-trivial electronic structures of the 1T-Rh Se Te are confirmed via the evolution of Wannier charge centers(WCCs) and time-reversal symmetryprotected topological surface states(TSSs). These distinctive properties underscore 1T-Rh Se Te as a possible candidate for a topological superconductor, warranting further investigation into its potential implications and applications.
基金the National Natural Science Foundation of China(Nos.21771192,21631003,21871024)the Major Program of Shandong Province Natural Science Foundation(No.ZR2017ZB0315)+2 种基金Fundamental Research Funds for the Central Universities(Nos.18CX06001A,19CX05001A)Research Foundation from China University of Petroleum(East China)(No.Y1510051)Taishan Scholar Program of Shandong Province(ts201712019,ts201511019).
文摘Facile preparation of cost-effective and durable porous carbon-supported non-precious-metal/nitrogen electrocatalysts for oxygen reduction reaction(ORR)is extremely important for promoting the commercialized applications of such catalysts.In this work,the FeCl3-containing porphyrinato iron-based covalent porous polymer(FeCl3·FeP or-CPP)was fabricated in-situ onto porous corncob biomass supports via a simple one-pot method.Subsequent thermal-reduction pyrolysis at 700℃-900℃with CO2 gas as an activating agent resulted in Fe2O3-decorated and N-doped graphitic carbon composite Fe2O3@NC&bio-C with a high degree of graphitization of Fe-involved promotion during pyrolysis(Fe2O3=FeCl3·FePor-CPP derived Fe2O3;NC=N-doped graphene analog;bio-C=the corncob-derived hierarchically porous graphitic biomass carbon framework).The derivedα-Fe2O3 andγ-Fe2O3 nanocrystals(5-10 nm particle diameter)were all immobilized on the N-doped bio-C micro/nanofibers.Notably,the Fe2O3@NC&bio-C obtained at the pyrolysis temperature of 800℃(Fe2O3@NC&bio-C-800),exhibited unusual ORR catalytic efficiency via a 4-electron pathway with the onset and half-wave potentials of 0.96 V and 0.85 V vs.RHE,respectively.In addition,Fe2O3@NC&bio-C-800 also exhibited a high and stable limiting current density of-6.0 mA cm-2,remarkably stability(larger than 91%retention after 10000 s),and good methanol tolerance.The present work represents one of the best results for iron-based biomass material ORR catalysts reported to date.The high ORR activity is attributed to the uniformly distributedα-Fe2O3 andγ-Fe2O3 nanoparticles on the N-enriched carbon matrix with a large specific surface area of 772.6 m^2 g^-1.This facilitates favor faster electron movement and better adsorption of oxygen molecules on the surface of the catalyst.Nevertheless,comparative studies on the structure and ORR catalytic activity of Fe2O3@NC&bioC-800 with Fe2O3@bio-C-800 and NC&bio-C-800 clearly highlight the synergistic effect of the coexisting Fe2O3 nanocrystals,NC,and bio-C on the ORR performance.
基金Supported by the National Key Research and Development Program of China(Grant Nos.2017YFA0303603 and 2016YFA0300300)the National Natural Science Foundation of China(Grant Nos.11574383,11774408,and 11574370)+4 种基金the Frontier Program of the Chinese Academy of Sciences(Grant No.QYZDY-SSW-SLH001)the Strategic Priority Research Program of CAS(Grant No.XDB30000000)the Beijing Natural Science Foundation(Grant No.4191003)the International Partnership Program of Chinese Academy of Sciences(Grant No.GJHZ1826)CAS Interdisciplinary Innovation Team。
文摘Distinctive superconducting behaviors between bulk and monolayer FeSe make it challenging to obtain a unified picture of all FeSe-based superconductors.We investigate the ultrafast quasiparticle(QP)dynamics of an intercalated superconductor(Li1-xFex)OHFe1-ySe,which is a bulk crystal but shares a similar electronic structure with single-layer FeSe on SrTiO3.We obtain the electron-phonon coupling(EPC)constant(0.22±0.04),which well bridges that of bulk FeSe crystal and single-layer FeSe on SrTiO3.Significantly,we find that such a positive correlation betweenλA1 g and superconducting Tc holds among all known FeSe-based superconductors,even in line with reported FeAs-based superconductors.Our observation indicates possible universal role of EPC in the superconductivity of all known categories of iron-based superconductors,which is a critical step towards achieving a unified superconducting mechanism for all iron-based superconductors.
基金Supported by the National Key Research and Development Program of China(Grant Nos.2017YFA0303603,2016YFA0300303,2018YFA0305703)the National Natural Science Foundation of China(Grant Nos.11774408,11574383,11874075,U1530402)+4 种基金the Strategic Priority Research Program of CAS(Grant No.XDB30000000)the International Partnership Program of Chinese Academy of Sciences(Grant Nos.GJHZ1826,GJHZ1403)the Beijing Natural Science Foundation(Grant No.4191003)the Science Challenge Project(Grant No.TZ2016001)the CAS Interdisciplinary Innovation Team.
文摘By integrating pump-probe ultrafast spectroscopy with diamond anvil cell(DAC)technique,we demonstrate a time-resolved ultrafast dynamics study on non-equilibrium quasiparticle(QP)states in.SVo/rQi under high pressure.On-site in situ condition is realized,where both the sample and DAC have fixed position during the experiment.The QP dynamics exhibits a salient pressure-induced phonon bottleneck feature at 20GPa,which corresponds to a gap shrinkage in the electronic structure.A structural transition is also observed at 32 GPa.In addition,the slowest relaxation component reveals possible heat diffusion or pressure-controlled local spin fluctuation associated with the gap shrinkage.Our work enables precise pressure dependence investigations of ultrafast dynamics,paving the way for reliable studies of high-pressure excited state physics.
