skip to main content


Search for: All records

Creators/Authors contains: "Zakutayev, Andriy"

Note: When clicking on a Digital Object Identifier (DOI) number, you will be taken to an external site maintained by the publisher. Some full text articles may not yet be available without a charge during the embargo (administrative interval).
What is a DOI Number?

Some links on this page may take you to non-federal websites. Their policies may differ from this site.

  1. Wurtzite-type ferroelectrics have drawn increasing attention due to the promise of better performance and integration than traditional oxide ferroelectrics with semiconductors such as Si, SiC, and III-V compounds. However, wurtzite-type ferroelectrics generally require enormous electric fields, approaching breakdown, to reverse their polarization. The underlying switching mechanism(s), especially for multinary compounds and alloys, remains elusive. Here, we examine the switching behaviors in Al1−xScxN alloys and wurtzite-type multinary candidate compounds we recently computationally identified. We find that switching in these tetrahedrally coordinated materials proceeds via a variety of nonpolar intermediate structures and that switching barriers are dominated by the more-electronegative cations. For Al1−xScxN alloys, we find that the switching pathway changes from a collective mechanism to a lower-barrier mechanism enabled by inversion of individual tetrahedra with increased Sc composition. Our findings provide insights for future engineering and realization of wurtzite-type materials and open a door to understanding domain motion.

     
    more » « less
    Free, publicly-accessible full text available May 17, 2025
  2. Low-energy compute-in-memory architectures promise to reduce the energy demand for computation and data storage. Wurtzite- type ferroelectrics are promising options for both performance and integration with existing semiconductor processes. The Al1-xScxN alloy is among the few tetrahedral materials that exhibit polarization switching, but the electric field required to switch the polarization is too high (few MV/cm). Going beyond binary com- pounds, we explore the search space of multinary wurtzite-type compounds. Through this large-scale search, we identify four prom- ising ternary nitrides and oxides, including Mg2PN3, MgSiN2, Li2SiO3, and Li2GeO3, for future experimental realization and engi- neering. In >90% of the considered multinary materials, we identify unique switching pathways and non-polar structures that are distinct from the commonly assumed switching mechanism in AlN-based materials. Our results disprove the existing design principle based on the reduction of the wurtzite c/a lattice parameter ratio when comparing different chemistries while sup- porting two emerging design principles—ionicity and bond strength. 
    more » « less
    Free, publicly-accessible full text available April 1, 2025
  3. Free, publicly-accessible full text available February 14, 2025
  4. Anomalously abrupt nucleation and growth kinetics in polarization switching of wurtzite ferroelectrics are demonstrated. The anomaly inspires an extension of the traditional model to a regime that simultaneous non-linear nucleation and growth occur.

     
    more » « less
    Free, publicly-accessible full text available July 31, 2024
  5. A high-speed and high-power current measurement instrument is described for measuring rapid switching of ferroelectric samples with large spontaneous polarization and coercive field. Instrument capabilities (±200 V, 200 mA, and 200 ns order response) are validated with a LiTaO3 single crystal whose switching kinetics are well known. The new instrument described here enables measurements that are not possible using existing commercial measurement systems, including the observation of ferroelectric switching in large coercive field and large spontaneous polarization Al0.7Sc0.3N thin films. 
    more » « less
  6. Ferroelectricity enables key modern technologies from non-volatile memory to precision ultrasound. The first known wurtzite ferroelectric Al 1− x Sc x N has recently attracted attention because of its robust ferroelectricity and Si process compatibility, but the chemical and structural origins of ferroelectricity in wurtzite materials are not yet fully understood. Here we show that ferroelectric behavior in wurtzite nitrides has local chemical rather than extended structural origin. According to our coupled experimental and computational results, the local bond ionicity and ionic displacement, rather than simply the change in the lattice parameter of the wurtzite structure, is key to controlling the macroscopic ferroelectric response in these materials. Across gradients in composition and thickness of 0 < x < 0.35 and 140–260 nm, respectively, in combinatorial thin films of Al 1− x Sc x N, the pure wurtzite phase exhibits a similar c / a ratio regardless of the Sc content due to elastic interaction with neighboring crystals. The coercive field and spontaneous polarization significantly decrease with increasing Sc content despite this invariant c / a ratio. This property change is due to the more ionic bonding nature of Sc–N relative to the more covalent Al–N bonds, and the local displacement of the neighboring Al atoms caused by Sc substitution, according to DFT calculations. Based on these insights, ionicity engineering is introduced as an approach to reduce coercive field of Al 1− x Sc x N for memory and other applications and to control ferroelectric properties in other wurtzites. 
    more » « less
  7. We present a thermodynamic analysis of the recently discovered nitride ferroelectric materials using the classic Landau–Devonshire approach. Electrostrictive and dielectric stiffness coefficients of Al 1− x Sc x N with a wurtzite structure ( 6 mm) are determined using a free energy density function assuming a hexagonal parent phase (6/ mmm), with the first-order phase transition based on the dielectric stiffness relationships. The results of this analysis show that the strain sensitivity of the energy barrier is one order of magnitude larger than that of the spontaneous polarization in these wurtzite ferroelectrics, yet both are less sensitive to strain compared to classic perovskite ferroelectrics. These analysis results reported here explain experimentally reported sensitivity of the coercive field to elastic strain/stress in Al 1− x Sc x N films and would enable further thermodynamic analysis via phase field simulation and related methods. 
    more » « less
  8. We investigate electronic structure and dopability of an ultrawide bandgap (UWBG) AlScO3 perovskite, a known high-pressure and long-lived metastable oxide. From first-principles electronic structure calculations, HSE06(+G0W0), we find this material to exhibit an indirect bandgap of around 8.0 eV. Defect calculations point to cation and oxygen vacancies as the dominant intrinsic point defects limiting extrinsic doping. While acceptor behaving Al and Sc vacancies prevent n-type doping, oxygen vacancies permit the Fermi energy to reach ∼0.3 eV above the valence band maximum, rendering AlScO3 p-type dopable. Furthermore, we find that both Mg and Zn could serve as extrinsic p-type dopants. Specifically, Mg is predicted to have achievable net acceptor concentrations of ∼1017 cm−3 with ionization energy of bound small hole polarons of ∼0.49 eV and free ones below 0.1 eV. These values place AlScO3 among the UWBG oxides with lowest bound small hole polaron ionization energies, which, as we find, is likely due to large ionic dielectric constant that correlates well with low hole polaron ionization energies across various UWBG oxides.

     
    more » « less