Hafnium-based ferroelectric films,remaining their ferroelectricity down to nanoscale thickness,present a promising application for low-power logic devices and nonvolatile memories.It has been appealing for researchers...Hafnium-based ferroelectric films,remaining their ferroelectricity down to nanoscale thickness,present a promising application for low-power logic devices and nonvolatile memories.It has been appealing for researchers to reduce the required temperature to obtain the ferroelectric phase in hafnium-based ferroelectric films for applications such as flexible and wearable electronics.This work demonstrates that a remanent polarization(P_(r))value of>5μC/cm^(2)can be obtained in asdeposited Hf_(0.5)Zr_(0.5)O_(2)(HZO)films that are fabricated by thermal atomic layer deposition(TALD)under low temperature of 250℃.The ferroelectric orthorhombic phase(o-phase)in the as-deposited HZO films is detected by scanning transmission electron microscopy(STEM).This low fabrication temperature further extends the compatibility of ferroelectric HZO films to flexible electronics and avoids the cost imposed by following high-temperature annealing treatments.展开更多
Crystallization annealing is a crucial process for the formation of the ferroelectric phase in HfO_(2)-based ferroelectric thin films.Here,we systematically investigate the impact of the annealing process,with tempera...Crystallization annealing is a crucial process for the formation of the ferroelectric phase in HfO_(2)-based ferroelectric thin films.Here,we systematically investigate the impact of the annealing process,with temperature varied from 350℃to 550℃,on the electricity,ferroelectricity and reliability of a Hf_(0.5)Zr_(0.5)O_(2)(HZO;7.5 nm)film capacitor.It was found that HZO film annealed at a low temperature of 400℃can effectively suppress the formation of the monoclinic phase and reduce the leakage current.HZO film annealed at 400℃also exhibits better ferroelectric properties than those annealed at 350℃and 550℃.Specifically,the 400℃-annealed HZO film shows an outstanding 2Pr value of 54.6μC·cm^(-2)at±3.0 MV·cm^(-1),which is relatively high compared with previously reported values for HZO film under the same electric field and annealing temperature.When the applied electric field increases to±5.0 MV·cm^(-1),the 2Pr value can reach a maximum of 69.6μC·cm^(-2).In addition,the HZO films annealed at 400℃and 550℃can endure up to bout 2.3×10^(8)cycles under a cycling field of 2.0 MV·cm^(-1)before the occurrence of breakdown.In the 400℃-annealed HZO film,72.1%of the initial polarization is maintained while only 44.9%is maintained in the 550℃-annealed HZO film.Our work demonstrates that HZO film with a low crystallization temperature(400℃)has quite a high ferroelectric polarization,which is of significant importance in applications in ferroelectric memory and negative capacitance transistors.展开更多
Owing to the utilization of lithium metal as anode with the ultrahigh theoretical capacity density of 3860 mA h g^(-1)and oxide-based ceramic solid-state electrolytes(SE),e.g.,garnet-type Li7La_(3)Zr_(2)O_(12)(LLZO),a...Owing to the utilization of lithium metal as anode with the ultrahigh theoretical capacity density of 3860 mA h g^(-1)and oxide-based ceramic solid-state electrolytes(SE),e.g.,garnet-type Li7La_(3)Zr_(2)O_(12)(LLZO),all-state-state lithium metal batteries(ASLMBs)have been widely accepted as the promising alternatives for providing the satisfactory energy density and safety.However,its applications are still challenged by plenty of technical and scientific issues.In this contribution,the co-sintering temperature at 500℃is proved as a compromise method to fabricate the composite cathode with structural integrity and declined capacity fading of LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2)(NCM).On the other hand,it tends to form weaker grain boundary(GB)inside polycrystalline LLZO at inadequate sintering temperature for LLZO,which can induce the intergranular failure of SE during the growth of Li filament inside the unavoidable defect on the interface of SE.Therefore,increasing the strength of GB,refining the grain to 0.4μm,and precluding the interfacial defect are suggested to postpone the electro-chemo-mechanical failure of SE with weak GB.Moreover,the advanced sintering techniques to lower the co-sintering temperature for both NCM-LLZO composite cathode and LLZO SE can be posted out to realize the viability of state-of-the-art ASLMBs with higher energy density as well as the guaranteed safety.展开更多
Ultra-high temperature ceramic(UHTC)nanowires are potential reinforcement materials due to it combines the perfect properties of bulk materials and unique geometric properties of one-dimensional(1D)nanostructures.Thus...Ultra-high temperature ceramic(UHTC)nanowires are potential reinforcement materials due to it combines the perfect properties of bulk materials and unique geometric properties of one-dimensional(1D)nanostructures.Thus,developing 1D nanomaterials that have excellent morphology and structure retention in ultra-high temperature environments is of prime importance to bring their outstanding performance into full play.Herein,we report the novel solid solution((Hf_(0.5)Ta_(0.5))C)ceramic nanowires,which could not only maintain morphological and structural stability at 1900°C but also exhibit 1D nanostructures under oxyacetylene scouring and ablation at 2300°C.The morphology evolution of nanowires obeys the Rayleigh instability mechanism,and the internal structure and element distribution of nanowires remain unchanged even if the surface atoms are rearranged.The fascinating nanowires are demonstrated to have great potential as ideal reinforcement materials of composite materials and toughening phases of ceramics that are applied in ultra-high temperature environments,as well as excellent performance enhancement phases of functional materials.Our work may provide new insights into the development of ceramic nanowires and widen their applications.展开更多
This paper reports the improvement of electrical,ferroelectric and endurance of Hf_(0.5)Zr_(0.5)O_(2)(HZO)thinfilm capacitors by implementing W electrode.The W/HZO/W capacitor shows excellent pristine 2 P_(r)values of...This paper reports the improvement of electrical,ferroelectric and endurance of Hf_(0.5)Zr_(0.5)O_(2)(HZO)thinfilm capacitors by implementing W electrode.The W/HZO/W capacitor shows excellent pristine 2 P_(r)values of 45.1 gC/cm^(2)at±6 V,which are much higher than those of TiN/HZO/W(34.4μC/cm^(2))and W/HZO/TiN(26.9μC/cm^(2))capacitors.Notably,the maximum initial 2 P_(r)value of W/HZO/W capacitor can reach as high as 57.9μC/cm^(2)at±7.5 V.These strong ferroelectric polarization effects are ascribed to the W electrode with a fairly low thermal expansion coefficient which provides a larger in-plane tensile strain compared with TiN electrode,allowing for enhancement of o-phase formation.Moreover,the W/HZO/W capacitor also exhibits higher endurance,smaller wake-up effect(10.1%)and superior fatigue properties up to 1.5×10^(10)cycles compared to the TiN/HZO/W and W/HZO/TiN capacitors.Such improvements of W/HZO/W capacitor are mainly due to the decreased leakage current by more than an order of magnitude compared to the W/HZO/TiN capacitor.These results demonstrate that capping electrode material plays an important role in the enhancement of o-phase formation,reduces oxygen vacancies,mitigates wake-up effect and improves reliability.展开更多
Flexible memory devices are promising for information storage and data processing applications in portable,wearable,and smart electronics operating under curved conditions.In this work,we realized high-performance fle...Flexible memory devices are promising for information storage and data processing applications in portable,wearable,and smart electronics operating under curved conditions.In this work,we realized high-performance flexible ferroelectric capacitors based on Hf_(0.5)Zr_(0.5)O_(2)(HZO)thin film by depositing a buffer layer of Al_(2)O_(3)on polyimide(PI)substrates using atomic layer deposition(ALD).The flexible ferroelectric HZO films exhibit high remnant polarization(Pr)of 21μC/cm^(2).Furthermore,deterioration of polarization,retention,and endurance performance was not observed even at a bending radius of 2 mm after 5,000 bending cycles.This work marks a critical step in the development of high-performance flexible HfO_(2)-based ferroelectric memories for next-generation wearable electronic devices.展开更多
The n-type ultrathin fully depleted silicon-on-insulator(FDSOI) metal-oxide-semiconductor field-effect transistors(MOSFETs),with a Hf_(0.5)Zr_(0.5)O_(2) high dielectric permittivity(high-k) dielectric as gate insulato...The n-type ultrathin fully depleted silicon-on-insulator(FDSOI) metal-oxide-semiconductor field-effect transistors(MOSFETs),with a Hf_(0.5)Zr_(0.5)O_(2) high dielectric permittivity(high-k) dielectric as gate insulator,were fabricated.The total ionizing dose effects were investigated,and an X-ray radiation dose up to 1500 krad(Si) was applied for both long-and short-channel devices.The short-channel devices(0.025-0.100 μm) exhibited less irradiation sensitivity compared with the long-channel devices(0.35-16 μm),leading to a 71% reduction in the irradiation-induced drain current growth and a 26% decrease in the shift of the threshold voltage.It was experimentally demonstrated that the OFF mode is the worst case among the three working conditions(OFF,ON and A110) for short-channel devices.Also,the determined effective electron mobility was enhanced by 38% after X-ray irradiation,attributed to the different compensations for charges triggered by radiation between the highk dielectric and buried oxide.By extracting the carrier mobility,gate length modulation,and source/drain(S/D)parasitic resistance,the degradation mechanism on X-ray irradiation was revealed.Finally,the split capacitance-voltage measurements were used to validate the analysis.展开更多
Multilevel ferroelectric field-effect transistors(FeFETs)integrated with HfO_(2)-based ferroelectric thin films demonstrate tremendous potential in high-speed massive data storage and neuromorphic computing applicatio...Multilevel ferroelectric field-effect transistors(FeFETs)integrated with HfO_(2)-based ferroelectric thin films demonstrate tremendous potential in high-speed massive data storage and neuromorphic computing applications.However,few works have focused on the stability of the multiple memory states in the HfO_(2)-based FeFETs.Here we firstly report the write/read disturb effects on the multiple memory states in the Hf_(0.5)Zr_(0.5)O_(2)(HZO)-based FeFETs.The multiple memory states in HZO-based FeFETs do not show obvious degradation with the write and read disturb cycles.Moreover,the retention characteristics of the intermediate memory states in HZO-based FeFETs with unsaturated ferroelectric polarizations are better than that of the memory state with saturated ferroelectric polarization.Through the deep analysis of the operation principle of in HZO-based FeFETs,we speculate that the better retention properties of intermediate memory states are determined by the less ferroelectric polarization degradation and the weaker ferroelectric polarization shielding.The experimental and theoretical evidences confirm that the long-term stability of the intermediate memory states in HZO-based FeFETs are as robust as that of the saturated memory state,laying a solid foundation for their practical applications.展开更多
基金Project supported by the National Key Research and Development Program of China(Grant No.2021YFA1200700)the National Natural Science Foundation of China(Grant Nos.T2222025 and 62174053)+5 种基金the Open Research Projects of Zhejiang Laboratory(Grant No.2021MD0AB03)the Shanghai Science and Technology Innovation Action Plan(Grant Nos.21JC1402000 and 21520714100)the Guangdong Provincial Key Laboratory Program(Grant No.2021B1212040001)the Fundamental Research Funds for the Central Universitiessupport from the Zuckerman STEM Leadership ProgramPazy Research Foundation(Grant No.149-2020)。
文摘Hafnium-based ferroelectric films,remaining their ferroelectricity down to nanoscale thickness,present a promising application for low-power logic devices and nonvolatile memories.It has been appealing for researchers to reduce the required temperature to obtain the ferroelectric phase in hafnium-based ferroelectric films for applications such as flexible and wearable electronics.This work demonstrates that a remanent polarization(P_(r))value of>5μC/cm^(2)can be obtained in asdeposited Hf_(0.5)Zr_(0.5)O_(2)(HZO)films that are fabricated by thermal atomic layer deposition(TALD)under low temperature of 250℃.The ferroelectric orthorhombic phase(o-phase)in the as-deposited HZO films is detected by scanning transmission electron microscopy(STEM).This low fabrication temperature further extends the compatibility of ferroelectric HZO films to flexible electronics and avoids the cost imposed by following high-temperature annealing treatments.
基金Hainan Provincial Natural Science Foundation of China(Grant No.523QN257)Collegelevel Scientific Research Foundation of Qiongtai Normal University(Grant No.qtqn202215)+6 种基金the Innovation and Entrepreneurship Training Program for College Students(Grant No.202213811016)Science and Technology Program of Henan(Grant No.232102210182)Scientific Research Foundation of Henan Normal University(Grant No.20230196)Natural Science Foundation of Shandong Province(Grant No.ZR2023QA047)Foundation of PeiXin(Grant No.2023PX027)Science and technology smes innovation ability improvement project(Grant No.2023TSGC0154)the National Natural Science Foundation of China(Grant No.62174059)。
文摘Crystallization annealing is a crucial process for the formation of the ferroelectric phase in HfO_(2)-based ferroelectric thin films.Here,we systematically investigate the impact of the annealing process,with temperature varied from 350℃to 550℃,on the electricity,ferroelectricity and reliability of a Hf_(0.5)Zr_(0.5)O_(2)(HZO;7.5 nm)film capacitor.It was found that HZO film annealed at a low temperature of 400℃can effectively suppress the formation of the monoclinic phase and reduce the leakage current.HZO film annealed at 400℃also exhibits better ferroelectric properties than those annealed at 350℃and 550℃.Specifically,the 400℃-annealed HZO film shows an outstanding 2Pr value of 54.6μC·cm^(-2)at±3.0 MV·cm^(-1),which is relatively high compared with previously reported values for HZO film under the same electric field and annealing temperature.When the applied electric field increases to±5.0 MV·cm^(-1),the 2Pr value can reach a maximum of 69.6μC·cm^(-2).In addition,the HZO films annealed at 400℃and 550℃can endure up to bout 2.3×10^(8)cycles under a cycling field of 2.0 MV·cm^(-1)before the occurrence of breakdown.In the 400℃-annealed HZO film,72.1%of the initial polarization is maintained while only 44.9%is maintained in the 550℃-annealed HZO film.Our work demonstrates that HZO film with a low crystallization temperature(400℃)has quite a high ferroelectric polarization,which is of significant importance in applications in ferroelectric memory and negative capacitance transistors.
基金the National Natural Science Foundation of China(12102328)for supporting this work。
文摘Owing to the utilization of lithium metal as anode with the ultrahigh theoretical capacity density of 3860 mA h g^(-1)and oxide-based ceramic solid-state electrolytes(SE),e.g.,garnet-type Li7La_(3)Zr_(2)O_(12)(LLZO),all-state-state lithium metal batteries(ASLMBs)have been widely accepted as the promising alternatives for providing the satisfactory energy density and safety.However,its applications are still challenged by plenty of technical and scientific issues.In this contribution,the co-sintering temperature at 500℃is proved as a compromise method to fabricate the composite cathode with structural integrity and declined capacity fading of LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2)(NCM).On the other hand,it tends to form weaker grain boundary(GB)inside polycrystalline LLZO at inadequate sintering temperature for LLZO,which can induce the intergranular failure of SE during the growth of Li filament inside the unavoidable defect on the interface of SE.Therefore,increasing the strength of GB,refining the grain to 0.4μm,and precluding the interfacial defect are suggested to postpone the electro-chemo-mechanical failure of SE with weak GB.Moreover,the advanced sintering techniques to lower the co-sintering temperature for both NCM-LLZO composite cathode and LLZO SE can be posted out to realize the viability of state-of-the-art ASLMBs with higher energy density as well as the guaranteed safety.
基金supported by the National Natural Science Foundation of China(62174059,52250281 and 91963102)the Hong Kong Research Grant Council(15300619)+3 种基金the Science and Technology Projects in Guangzhou(202201000008)Guangdong Science and Technology Project-International Cooperation(2021A0505030064)Guangdong Provincial Key Laboratory of Optical Information Materials and Technology(2017B030301007)the Joint Funds of Basic and Applied Basic Research Foundation of Guangdong Province(2019A1515110605)。
基金supported by the National Natural Science Foundation of China(Nos.52130205 and 51727804)the National Key R&D Program of China(No.2021YFA0715803)Innovation Foundation for Doctor Dissertation of Northwestern Polytechnical University(CX2022010).
文摘Ultra-high temperature ceramic(UHTC)nanowires are potential reinforcement materials due to it combines the perfect properties of bulk materials and unique geometric properties of one-dimensional(1D)nanostructures.Thus,developing 1D nanomaterials that have excellent morphology and structure retention in ultra-high temperature environments is of prime importance to bring their outstanding performance into full play.Herein,we report the novel solid solution((Hf_(0.5)Ta_(0.5))C)ceramic nanowires,which could not only maintain morphological and structural stability at 1900°C but also exhibit 1D nanostructures under oxyacetylene scouring and ablation at 2300°C.The morphology evolution of nanowires obeys the Rayleigh instability mechanism,and the internal structure and element distribution of nanowires remain unchanged even if the surface atoms are rearranged.The fascinating nanowires are demonstrated to have great potential as ideal reinforcement materials of composite materials and toughening phases of ceramics that are applied in ultra-high temperature environments,as well as excellent performance enhancement phases of functional materials.Our work may provide new insights into the development of ceramic nanowires and widen their applications.
基金financially supported by the National Natural Science Foundation of China(No.51872099)the Hong Kong Research Grant Council(No.15300619)+2 种基金the Science and Technology Program of Guangzhou(No.201905-0001)the Guangdong Science and Technology Project-International Cooperation(No.2021A0505030064)financial support by the Hong Kong Scholars Program(No.XJ2019006)。
文摘This paper reports the improvement of electrical,ferroelectric and endurance of Hf_(0.5)Zr_(0.5)O_(2)(HZO)thinfilm capacitors by implementing W electrode.The W/HZO/W capacitor shows excellent pristine 2 P_(r)values of 45.1 gC/cm^(2)at±6 V,which are much higher than those of TiN/HZO/W(34.4μC/cm^(2))and W/HZO/TiN(26.9μC/cm^(2))capacitors.Notably,the maximum initial 2 P_(r)value of W/HZO/W capacitor can reach as high as 57.9μC/cm^(2)at±7.5 V.These strong ferroelectric polarization effects are ascribed to the W electrode with a fairly low thermal expansion coefficient which provides a larger in-plane tensile strain compared with TiN electrode,allowing for enhancement of o-phase formation.Moreover,the W/HZO/W capacitor also exhibits higher endurance,smaller wake-up effect(10.1%)and superior fatigue properties up to 1.5×10^(10)cycles compared to the TiN/HZO/W and W/HZO/TiN capacitors.Such improvements of W/HZO/W capacitor are mainly due to the decreased leakage current by more than an order of magnitude compared to the W/HZO/TiN capacitor.These results demonstrate that capping electrode material plays an important role in the enhancement of o-phase formation,reduces oxygen vacancies,mitigates wake-up effect and improves reliability.
基金This work was supported in part by the National Natural Science Foundation of China(Nos.61922083,61804167,61834009,61904200,and 61821091)in part by the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB44000000).
文摘Flexible memory devices are promising for information storage and data processing applications in portable,wearable,and smart electronics operating under curved conditions.In this work,we realized high-performance flexible ferroelectric capacitors based on Hf_(0.5)Zr_(0.5)O_(2)(HZO)thin film by depositing a buffer layer of Al_(2)O_(3)on polyimide(PI)substrates using atomic layer deposition(ALD).The flexible ferroelectric HZO films exhibit high remnant polarization(Pr)of 21μC/cm^(2).Furthermore,deterioration of polarization,retention,and endurance performance was not observed even at a bending radius of 2 mm after 5,000 bending cycles.This work marks a critical step in the development of high-performance flexible HfO_(2)-based ferroelectric memories for next-generation wearable electronic devices.
基金financially supported by the National Natural Science Foundation of China (Nos.61874135,61904194 and 11905287)the National Major Project of Science and Technology of China (No.2017ZX02315001)+1 种基金the Youth Innovation Promotion Association,CAS (No.Y9YQ01R004)the Opening Project of Key Laboratory of Microelectronic Devices & Integrated Technology,Institute of Microelectronics,CAS (No.Y9YS05X002)。
文摘The n-type ultrathin fully depleted silicon-on-insulator(FDSOI) metal-oxide-semiconductor field-effect transistors(MOSFETs),with a Hf_(0.5)Zr_(0.5)O_(2) high dielectric permittivity(high-k) dielectric as gate insulator,were fabricated.The total ionizing dose effects were investigated,and an X-ray radiation dose up to 1500 krad(Si) was applied for both long-and short-channel devices.The short-channel devices(0.025-0.100 μm) exhibited less irradiation sensitivity compared with the long-channel devices(0.35-16 μm),leading to a 71% reduction in the irradiation-induced drain current growth and a 26% decrease in the shift of the threshold voltage.It was experimentally demonstrated that the OFF mode is the worst case among the three working conditions(OFF,ON and A110) for short-channel devices.Also,the determined effective electron mobility was enhanced by 38% after X-ray irradiation,attributed to the different compensations for charges triggered by radiation between the highk dielectric and buried oxide.By extracting the carrier mobility,gate length modulation,and source/drain(S/D)parasitic resistance,the degradation mechanism on X-ray irradiation was revealed.Finally,the split capacitance-voltage measurements were used to validate the analysis.
基金This work was partly supported by the National Natural Science Foundation of China(Grant Nos.52122205,51902274,52072324,and 11932016)the Science and Technology Innovation Program of Hunan Province(Grant No.2020RC2077)the Natural Science Foundation of Hunan Province(Grant No.2019JJ50617).
文摘Multilevel ferroelectric field-effect transistors(FeFETs)integrated with HfO_(2)-based ferroelectric thin films demonstrate tremendous potential in high-speed massive data storage and neuromorphic computing applications.However,few works have focused on the stability of the multiple memory states in the HfO_(2)-based FeFETs.Here we firstly report the write/read disturb effects on the multiple memory states in the Hf_(0.5)Zr_(0.5)O_(2)(HZO)-based FeFETs.The multiple memory states in HZO-based FeFETs do not show obvious degradation with the write and read disturb cycles.Moreover,the retention characteristics of the intermediate memory states in HZO-based FeFETs with unsaturated ferroelectric polarizations are better than that of the memory state with saturated ferroelectric polarization.Through the deep analysis of the operation principle of in HZO-based FeFETs,we speculate that the better retention properties of intermediate memory states are determined by the less ferroelectric polarization degradation and the weaker ferroelectric polarization shielding.The experimental and theoretical evidences confirm that the long-term stability of the intermediate memory states in HZO-based FeFETs are as robust as that of the saturated memory state,laying a solid foundation for their practical applications.
