Integration of lead-free ferroelectric on HfO2/Si (100) for high performance non-volatile memory applications

We introduce a novel lead-free ferroelectric thin film (1-x)BaTiO3-xBa(Cu1/3Nb2/3)O3 (x = 0.025) (BT-BCN) integrated on to HfO2 buffered Si for non-volatile memory (NVM) applications. Piezoelectric force microscopy (PFM), x-ray diffraction, and high resolution transmission electron microscopy were employed to establish the ferroelectricity in BT-BCN thin films. PFM study reveals that the domains reversal occurs with 180° phase change by applying external voltage, demonstrating its effectiveness for NVM device applications. X-ray photoelectron microscopy was used to investigate the band alignments between atomic layer deposited HfO2 and pulsed laser deposited BT-BCN films. Programming and erasing operations were explained on the basis of band-alignments. The structure offers large memory window, low leakage current, and high and low capacitance values that were easily distinguishable even after ~106 s, indicating strong charge storage potential. This study explains a new approach towards the realization of ferroelectric based memory devices integrated on Si platform and also opens up a new possibility to embed the system within current complementary metal-oxide-semiconductor processing technology.

[1]  M. Gutowski,et al.  Experimental determination of valence band maxima for SrTiO3, TiO2, and SrO and the associated valence band offsets with Si(001) , 2004 .

[2]  Lu You,et al.  Non-volatile memory based on the ferroelectric photovoltaic effect , 2013, Nature Communications.

[3]  L. You,et al.  Universal Ferroelectric Switching Dynamics of Vinylidene Fluoride-trifluoroethylene Copolymer Films , 2014, Scientific Reports.

[4]  X. Zhong,et al.  The electrical and switching properties of a metal-ferroelectric (Bi3.15Nd0.85Ti3O12)-insulator (Y2O3-stabilized ZrO2)-silicon diode , 2010 .

[5]  Marin Alexe,et al.  Atomic-scale study of electric dipoles near charged and uncharged domain walls in ferroelectric films. , 2008, Nature materials.

[6]  Wen-Chieh Shih,et al.  Fabrication and characterization of metal-ferroelectric , 2008 .

[7]  S. Priya,et al.  Local structure and piezoelectric instability in lead-free (1 − x)BaTiO3-xA(Cu1/3Nb2/3)O3 (A = Sr, Ca, Ba) solid solutions , 2014 .

[8]  S. Priya,et al.  Dielectric and ferroelectric response of compositionally graded bilayer and trilayer composites of BaTiO3 and 0.975BaTiO3–0.025Ba(Cu1/3Nb2/3)O3 , 2010 .

[9]  S. Ismail-Beigi,et al.  Interface-induced polarization and inhibition of ferroelectricity in epitaxial SrTiO₃/Si. , 2010, Physical review letters.

[10]  Sergei V. Kalinin,et al.  Intrinsic single-domain switching in ferroelectric materials on a nearly ideal surface , 2007, Proceedings of the National Academy of Sciences.

[11]  M D Rossell,et al.  Controlling tetragonality and crystalline orientation in BaTiO3 nano-layers grown on Si , 2013, Nanotechnology.

[12]  Y. Ikuhara,et al.  Possible ferroelectricity in perovskite oxynitride SrTaO2N epitaxial thin films , 2014, Scientific Reports.

[13]  T. Kanashima,et al.  Basic characteristics of metal-ferroelectric-insulator-semiconductor structure using a high-k PrOx insulator layer , 2003 .

[14]  S. Priya,et al.  Energy band alignment of atomic layer deposited HfO2 on epitaxial (110)Ge grown by molecular beam epitaxy , 2013 .

[15]  Nicolas Grandjean,et al.  From visible to white light emission by GaN quantum dots on Si(111) substrate , 1999 .

[16]  E. A. Kraut,et al.  Semiconductor core-level to valence-band maximum binding-energy differences: Precise determination by x-ray photoelectron spectroscopy , 1983 .

[17]  Complex permittivity scaling of functionally graded composites , 2014 .

[18]  R. Ivkov,et al.  CORRIGENDUM: Effect of magnetic dipolar interactions on nanoparticle heating efficiency: Implications for cancer hyperthermia , 2014, Scientific Reports.

[19]  O. Takai,et al.  Enhanced memory window of Au/BaTiO3/SrTiO3/Si(001) MFIS structure with high c-axis orientation for non-volatile memory applications , 2012 .

[20]  Nripendra N. Halder,et al.  Role of ultra thin pseudomorphic InP layer to improve the high-k dielectric/GaAs interface in realizing metal-oxide-semiconductor capacitor , 2012 .

[21]  D. Schroder Semiconductor Material and Device Characterization , 1990 .

[22]  S. Ray,et al.  Structural and electrical properties of metal–ferroelectric–insulator–semiconductor structure of Al/SrBi2Ta2O9/HfO2/Si using HfO2 as buffer layer , 2008 .

[23]  J. Liu,et al.  High‐Performance Programmable Memory Devices Based on Co‐Doped BaTiO3 , 2011, Advanced materials.

[24]  H. Ishiwara,et al.  Five-day-long ferroelectric memory effect in Pt∕(Bi,La)4Ti3O12∕HfO2∕Si structures , 2004 .

[25]  T. Ren,et al.  Characteristics of Pt/BiFeO3/TiO2/Si capacitors with TiO2 layer formed by liquid-delivery metal organic chemical vapor deposition , 2010 .

[26]  Enge Wang,et al.  Domain Dynamics During Ferroelectric Switching , 2011, Science.

[27]  S. Ray,et al.  Interfacial and electrical properties of SrBi2Ta2O9/ZrO2/Si heterostructures for ferroelectric memory devices , 2008 .

[28]  Yasuo Cho,et al.  SCANNING NONLINEAR DIELECTRIC MICROSCOPY WITH CONTACT SENSING MECHANISM FOR OBSERVATION OF NANOMETER SIZED FERROELECTRIC DOMAINS , 1999 .

[29]  Huibin Lu,et al.  Switchable diode effect and ferroelectric resistive switching in epitaxial BiFeO3 thin films , 2011 .

[30]  J. Maria,et al.  Interface magnetism in epitaxial BiFeO3-La0.7Sr0.3MnO3 heterostructures integrated on Si(100). , 2013, Nano letters.

[31]  H. Ishiwara,et al.  Characterization of HfTaO films for gate oxide and metal-ferroelectric-insulator-silicon device applications , 2008 .

[32]  S. K. Streiffer,et al.  Observation of nanoscale 180° stripe domains in ferroelectric PbTiO3 thin films , 2002 .

[33]  M. Hudait,et al.  Energy band alignment of atomic layer deposited HfO2 oxide film on epitaxial (100)Ge, (110)Ge, and (111)Ge layers , 2013 .

[34]  Hiroshi Ishiwara,et al.  Capacitance-voltage and retention characteristics of Pt/SrBi2Ta2O9/HfO2/Si structures with various buffer layer thickness , 2009 .

[35]  L. Zhang,et al.  Effect of postdeposition annealing on the thermal stability and structural characteristics of sputtered HfO2 films on Si(100) , 2005 .

[36]  P. Juan,et al.  The charge trapping effect of metal-ferroelectric (PbZr0.53Ti0.47O3)-insulator (HfO2)-silicon capacitors , 2005 .

[37]  Catherine Dubourdieu,et al.  Switching of ferroelectric polarization in epitaxial BaTiO₃ films on silicon without a conducting bottom electrode. , 2013, Nature nanotechnology.

[38]  Sergei V. Kalinin,et al.  Effect of phase transition on the surface potential of the BaTiO3 (100) surface by variable temperature scanning surface potential microscopy , 2000 .

[39]  E. A. Kraut,et al.  Precise Determination of the Valence-Band Edge in X-Ray Photoemission Spectra: Application to Measurement of Semiconductor Interface Potentials , 1980 .

[40]  Dieter K. Schroder,et al.  Semiconductor Material and Device Characterization: Schroder/Semiconductor Material and Device Characterization, Third Edition , 2005 .