The multiple quantum transitions within d-band correlation oxides such as rare-earth nickelates(RENiO_(3))triggered by critical temperatures and/or hydrogenation opened up a new paradigm for correlated electronics app...The multiple quantum transitions within d-band correlation oxides such as rare-earth nickelates(RENiO_(3))triggered by critical temperatures and/or hydrogenation opened up a new paradigm for correlated electronics applications,e.g.ocean electric field sensor,bio-sensor,and neuron synapse logical devices.Nevertheless,these applications are obstructed by the present ineffectiveness in the thin film growth of the metastable RENiO_(3)with flexibly adjustable rare-earth compositions and electronic structures.Herein,we demonstrate a metal-organic decompositions(MOD)approach that can effectively grow metastable RENiO_(3)covering a large variety of the rare-earth composition without introducing any vacuum process.Unlike the previous chemical growths for RENiO_(3)relying on strict interfacial coherency that limit the film thickness,the MOD growth using reactive isooctanoate percussors is tolerant to lattice defects and therefore achieves comparable film thickness to vacuum depositions.Further indicated by positron annihilation spectroscopy,the RENiO_(3)grown by MOD exhibit large amount of lattice defects that improves their hydrogen incorporation amount and electron transfers,as demonstrated by the resonant nuclear reaction analysis and near edge X-ray absorption fine structure analysis.This effectively enlarges the magnitude in the resistance regulations in particular for RENiO_(3)with lighter RE,shedding a light on the extrinsic regulation of the hydrogen induced quantum transitions for correlated oxides semiconductors kinetically via defect engineering.展开更多
While the metal to insulator transition(MIT)of d-band correlated perovskite nickelates(RENiO_(3))are widely adjustable via their rare-earth composition,the roles of potential valence variabilities associated with the ...While the metal to insulator transition(MIT)of d-band correlated perovskite nickelates(RENiO_(3))are widely adjustable via their rare-earth composition,the roles of potential valence variabilities associated with the rare-earth elements were rarely concerned.Herein,we demonstrate the material synthesis and MIT properties of RENiO_(3) containing valence variable rare-earth compositions,such as Ce,Pr,Sm,Eu and Tb.The metastable perovskite structure of SmNiO_(3) and EuNiO_(3) with a rare-earth valence states variable towards+2 can be effectively synthesized under high oxygen pressures as it is necessary to reduce their formation free energies.This is in contrast to Ce and Tb,in which situations the variable rare-earth valence state towards+4 reduces their ionic radius and prohibits their occupation or co-occupation of the rare-earth site within the perovskite structured RENiO_(3).Nevertheless,PrNiO_(3) with MIT properties can be effectively synthesized at lower oxygen pressures,owing to the higher stability to form a fully occupied 6s orbit associated Pr3+compared to the half-filled one related to Pr4+.The present work provides guidance for regulating the MIT properties of RENiO_(3).展开更多
Although the metal to insulator transition(MIT)observed in d-band correlated metal oxides enables promising applications(e.g.,correlated logical devices and Mottronic devices),its present recognition is mainly limited...Although the metal to insulator transition(MIT)observed in d-band correlated metal oxides enables promising applications(e.g.,correlated logical devices and Mottronic devices),its present recognition is mainly limited on the direct current(DC)electrical transports.Up to date,the MIT from the perspective of alternation current(AC)transport and its potential electronic applications remains yet unclear.Herein,we demonstrate the frequency(f_(AC))dependence in the impedance(Z=Z’+iZ″)of typical MIT materials,such as thin film rare-earth nickelates(Re NiO_(3)),across the critical MIT temperature(T_(MIT)).Apart from the abrupt change in the impedance modulus(|Z|)across the critical temperature(T_(MIT))similar to the DC transport,the MIT also triggers non-continuous variation in the impedance phase(θ),and this enables the f_(AC)-regulations in the Z’-T tendencies(Z’=|Z|cosθ).At the critical f_(AC) range(e.g.,104-106 Hz),the con-versing variations in|Z|-T and cosθ-T across T_(MIT) result in non-monotonic delta-shape Z’-T tendency in Sm_(x) Nd_(1-x) NiO_(3),the full width half maximum of which is effectively narrowed compared to the situation with the absence of MIT.Further imparting lower or higher f_(AC) elevate the domination in|Z|-T and cosθ-T,respectively,but also enables abrupt Z’-T tendencies across T_(MIT) showing negative temperature coefficient of resistance(NTCR)or positive temperature coefficient of resistance(PTCR).By introducing f_(AC) as a new freedom,the MIT behavior can be more comprehensively regulated electronically,and this extends the vision in exploring the new electronic applications based on the correlated MIT materials from the AC perspective.展开更多
The United Nations has proclaimed 1994 as the International Year of the Family and has defined its objectives to stimulate local, national and international actions as part of a sustained longterm effort to: a. Increa...The United Nations has proclaimed 1994 as the International Year of the Family and has defined its objectives to stimulate local, national and international actions as part of a sustained longterm effort to: a. Increase awareness of family issues among Governments as well as in the private sector. IYF would serve to highlight the importance of families; increase a better understanding of their unctions and problems; promote nowledge of the economic, social and emographic processes affecting展开更多
基金financially supported by the National Key Research and Development Program of China(No.2021YFA0718900)National Natural Science Foundation of China(Nos.62074014,52073090,and 52103284)。
文摘The multiple quantum transitions within d-band correlation oxides such as rare-earth nickelates(RENiO_(3))triggered by critical temperatures and/or hydrogenation opened up a new paradigm for correlated electronics applications,e.g.ocean electric field sensor,bio-sensor,and neuron synapse logical devices.Nevertheless,these applications are obstructed by the present ineffectiveness in the thin film growth of the metastable RENiO_(3)with flexibly adjustable rare-earth compositions and electronic structures.Herein,we demonstrate a metal-organic decompositions(MOD)approach that can effectively grow metastable RENiO_(3)covering a large variety of the rare-earth composition without introducing any vacuum process.Unlike the previous chemical growths for RENiO_(3)relying on strict interfacial coherency that limit the film thickness,the MOD growth using reactive isooctanoate percussors is tolerant to lattice defects and therefore achieves comparable film thickness to vacuum depositions.Further indicated by positron annihilation spectroscopy,the RENiO_(3)grown by MOD exhibit large amount of lattice defects that improves their hydrogen incorporation amount and electron transfers,as demonstrated by the resonant nuclear reaction analysis and near edge X-ray absorption fine structure analysis.This effectively enlarges the magnitude in the resistance regulations in particular for RENiO_(3)with lighter RE,shedding a light on the extrinsic regulation of the hydrogen induced quantum transitions for correlated oxides semiconductors kinetically via defect engineering.
基金Project supported by the National Key Research and Development Program of China(2021YFA0718900)the National Natural Science Foundation of China(62074014,52073090)。
文摘While the metal to insulator transition(MIT)of d-band correlated perovskite nickelates(RENiO_(3))are widely adjustable via their rare-earth composition,the roles of potential valence variabilities associated with the rare-earth elements were rarely concerned.Herein,we demonstrate the material synthesis and MIT properties of RENiO_(3) containing valence variable rare-earth compositions,such as Ce,Pr,Sm,Eu and Tb.The metastable perovskite structure of SmNiO_(3) and EuNiO_(3) with a rare-earth valence states variable towards+2 can be effectively synthesized under high oxygen pressures as it is necessary to reduce their formation free energies.This is in contrast to Ce and Tb,in which situations the variable rare-earth valence state towards+4 reduces their ionic radius and prohibits their occupation or co-occupation of the rare-earth site within the perovskite structured RENiO_(3).Nevertheless,PrNiO_(3) with MIT properties can be effectively synthesized at lower oxygen pressures,owing to the higher stability to form a fully occupied 6s orbit associated Pr3+compared to the half-filled one related to Pr4+.The present work provides guidance for regulating the MIT properties of RENiO_(3).
基金financially supported by the National Key Re-search and Development Program of China(No.2021YFA0718900)the National Natural Science Foundation of China(Nos.62074014 and 52073090)the Beijing New-star Plan of Science and Tech-nology(No.Z191100001119071).
文摘Although the metal to insulator transition(MIT)observed in d-band correlated metal oxides enables promising applications(e.g.,correlated logical devices and Mottronic devices),its present recognition is mainly limited on the direct current(DC)electrical transports.Up to date,the MIT from the perspective of alternation current(AC)transport and its potential electronic applications remains yet unclear.Herein,we demonstrate the frequency(f_(AC))dependence in the impedance(Z=Z’+iZ″)of typical MIT materials,such as thin film rare-earth nickelates(Re NiO_(3)),across the critical MIT temperature(T_(MIT)).Apart from the abrupt change in the impedance modulus(|Z|)across the critical temperature(T_(MIT))similar to the DC transport,the MIT also triggers non-continuous variation in the impedance phase(θ),and this enables the f_(AC)-regulations in the Z’-T tendencies(Z’=|Z|cosθ).At the critical f_(AC) range(e.g.,104-106 Hz),the con-versing variations in|Z|-T and cosθ-T across T_(MIT) result in non-monotonic delta-shape Z’-T tendency in Sm_(x) Nd_(1-x) NiO_(3),the full width half maximum of which is effectively narrowed compared to the situation with the absence of MIT.Further imparting lower or higher f_(AC) elevate the domination in|Z|-T and cosθ-T,respectively,but also enables abrupt Z’-T tendencies across T_(MIT) showing negative temperature coefficient of resistance(NTCR)or positive temperature coefficient of resistance(PTCR).By introducing f_(AC) as a new freedom,the MIT behavior can be more comprehensively regulated electronically,and this extends the vision in exploring the new electronic applications based on the correlated MIT materials from the AC perspective.
文摘The United Nations has proclaimed 1994 as the International Year of the Family and has defined its objectives to stimulate local, national and international actions as part of a sustained longterm effort to: a. Increase awareness of family issues among Governments as well as in the private sector. IYF would serve to highlight the importance of families; increase a better understanding of their unctions and problems; promote nowledge of the economic, social and emographic processes affecting
