Research On The Application Of Combinatorial Methon In Solid-state Reaction Of Multilayer Thinfilm

Nano-multilayer thin-film became more integrated into microelectronics and manufacturing applications due to the unique properties and physical effects by means of artificially modulated thin-film layers.While,with the development of industrialization,higher performance is required for nano-multilayer thin-film.The performance of the nano-multilayer thin-film is mainly affected by the microstructure,which is determined by the solid-state reaction process.Therefore,mastering the evolution of the microstructure of the nano-multilayer thin-film during the solid-state reaction,and ultimately adjusting the microstructure of the multilayer thin-film by adjusting the solid-state reaction parameters is the key to accelerating the use of the multilayer thin-film.Aiming at the phenomenon of insufficient research on the formation order of the crystalline phase and the amorphous transformation of the phase structure in the solid-state reaction research of the multilayer thin-film,we propose a combinatorial method which is integration of combinatorial multilayer thin-film preparation,high-throughput experimental characterization and automated data processing.Using this method,the systematic analysis of the evolution of the phase structure of the combinatorial multilayer thin-film under different isothermal solid-state reaction parameters is performed quickly.At the same time,in-situ characterization techniques for analysis of multi-component multilayer thin-films were developed on the basis of isothermal solid-state reaction research.This study accelerates the research process of the solid-state reaction mechanism of multilayer thin-films and provides a new research perspective for the development and screening of multilayer thin-film materials with excellent performance.At the same time,it laid the foundation for the application of combinatorial multilayer thin-film technology in the field of phase diagrams and rapid screening of amorphous alloys.The main conclusion is as follows:1)Taking the Cu-Cr-Co combinatorial multilayer thin-film as an example,the structural evolution of the crystalline phase of the combinatorial multilayer thin-film at different modulation period was studied.The combinatorial multilayer thin-films with different modulation periods were quickly prepared by the high-throughput ion beam sputtering system and then annealed at 973K and 1073K.The high-throughput synchrotron X-ray diffraction(XRD)+micro X-ray fluorescence(XRF)characterization was simultaneously used to quickly characterize the structure and chemical composition of the combinatorial multilayer thin-film,and the composition-phase distribution diagram of the Cu-Cr-Co ternary system was quickly constructed through an automated data processing program.At the same time,combined with time-of-flight secondary ion mass spectroscopy(To F-SIMS),the element distribution in the depth direction of the multilayer thin-film was analyzed.The results showed that the evolution of the phase distribution of the Cu-Cr-Co combinatorial multilayer thin-film at different thermal treatment temperatures is almost consistent with the traditional equilibrium phase diagram,but the corresponding temperature is about 200K higher.At the same time,the shorter the modulation period,the longer the isothermal solid-state reaction time,the closer the phase distribution range is to the high-temperature equilibrium phase diagram,and the more uniform the element distribution in the depth direction.2)Taking Ti-Ni-Cu and Ge-Sb-Te combinatorial multilayer thin-films as representatives of the crystalline precursors and the amorphous precursors respectively,the trend of amorphization phase evolution of combinatorial multilayer thin-films under different precursors was systematically studied.By adjusting the deposition sequence,annealing temperature,modulation period,etc.to study its effect on the amorphization during the solid-state reaction.The synchrotron high-throughput XRD,-XRF,and Rutherford backscattering spectrometry(RBS)were used to characterize the structure and chemical composition of the combinatorial multilayer thin-film.Transmission electron microscopy(TEM)and To F-SIMS were used to analyze the microstructure and elemental distribution in the depth direction of the multilayer thin-film under different synthesis parameters before and after the long-time solid-state reaction at low temperature.The results show that when the precursor is crystalline,the crystal structure gradually transforms to the amorphous structure during the low-temperature and long-term solid-state reaction process,due to the rapid diffusion of the amorphous component Ti element in the Ti-Ni-Cu system.The coating sequence has a greater impact on the final product than the modulation ratio.When the precursor is an amorphous structure,the thermal stability of the amorphous structure of the Ge-Sb-Te combinatorial multilayer thin-film during the low-temperature and long-term solid-state reaction is affected by the modulation period and deposition sequence.The smaller the modulation period,the more intense the interdiffusion,the better the thermal stability.At the same time,the high efficiency of the combinatorial method in the study of the multilayer thin-film amorphization during solid-state reaction and its feasibility in the field of rapid screening of amorphous alloy were verified.3)Ge₂Sb₂Te₅(GST)and Sc_0.2Sb₂Te₃(SST)single-component multilayer thin-films and GST+SST multi-component multilayer thin-films were fabricated on Nano-FDSC devices using a high-throughput ion beam sputtering system.A new Nano-FDSC in-situ characterization technology suitable for high-temperature field was developed and the glass-like transition temperature,crystallization temperature,solid-solid phase transition temperature,and the melting point of the multilayer thin-film during the solid-state reaction were analyzed.By comparing with single-component experimental data,it is verified that the method can achieve in-situ characterization of multi-component multilayer films.It laid the foundation for the high-throughput Nano-FDSC in-situ characterization of solid-state reactions of combinatorial thin-film.