Tunable stochastic memristors for energy-efficient encryption and computing.

Information security and computing, two critical technological challenges for post-digital computation, pose opposing requirements - security (encryption) requires a source of unpredictability, while computing generally requires predictability. Each of these contrasting requirements presently necessitates distinct conventional Si-based hardware units with power-hungry overheads. This work demonstrates Cu0.3Te0.7/HfO2 ('CuTeHO') ion-migration-driven memristors that satisfy the contrasting requirements. Under specific operating biases, CuTeHO memristors generate truly random and physically unclonable functions, while under other biases, they perform universal Boolean logic. Using these computing primitives, this work experimentally demonstrates a single system that performs cryptographic key generation, universal Boolean logic operations, and encryption/decryption. Circuit-based calculations reveal the energy and latency advantages of the CuTeHO memristors in these operations. This work illustrates the functional flexibility of memristors in implementing operations with varying component-level requirements.

Energy and Space Efficient Parallel Adder Using Molecular Memristors.

A breakthrough in in-memory computing technologies hinges on the development of appropriate material platforms that can overcome their existing limitations, such as larger than optimal footprint and multiple serial computational steps, with potential accumulation of errors. Using a molecular switching element with multiple non-monotonic and deterministic transitions, the device count and the number of computational steps can be substantially reduced. With molecular materials, however, the realization of a reliable and robust platform is an unattained goal for decades. Here, crossbar arrays with up to 64 molecular memristors are fabricated to experimentally demonstrate 8-bit serial and 4-bit parallel adders that operate for thousands of measurement cycles with an estimated error probability of 10-16 . For performance benchmarking, a 32-bit parallel adder is designed and simulated with 268 million inputs including contributions from the peripheral circuitry showing a 47× higher energy efficiency, 93× faster operation, and 9% of the footprint, leading to 4390 times improved energy-delay product compared to a special purpose complementary metal-oxide-semiconductor (CMOS)-based multicore adder.

High Thermal Conductivity of Submicrometer Aluminum Nitride Thin Films Sputter-Deposited at Low Temperature.

Aluminum nitride (AlN) is one of the few electrically insulating materials with excellent thermal conductivity, but high-quality films typically require exceedingly hot deposition temperatures (>1000 °C). For thermal management applications in dense or high-power integrated circuits, it is important to deposit heat spreaders at low temperatures (<500 °C), without affecting the underlying electronics. Here, we demonstrate 100 nm to 1.7 µm thick AlN films achieved by low-temperature (<100 °C) sputtering, correlating their thermal properties with their grain size and interfacial quality, which we analyze by X-ray diffraction, transmission X-ray microscopy, as well as Raman and Auger spectroscopy. Controlling the deposition conditions through the partial pressure of reactive N2, we achieve an ∼3× variation in thermal conductivity (∼36-104 W m-1 K-1) of ∼600 nm films, with the upper range representing one of the highest values for such film thicknesses at room temperature, especially at deposition temperatures below 100 °C. Defect densities are also estimated from the thermal conductivity measurements, providing insight into the thermal engineering of AlN that can be optimized for application-specific heat spreading or thermal confinement.

Novel Program Scheme of Vertical NAND Flash Memory for Reduction of Z-Interference.

Minimizing the variation in threshold voltage (Vt) of programmed cells is required to the extreme level for realizing multi-level-cells; as many as even 5 bits per cell recently. In this work, a recent program scheme to write the cells from the top, for instance the 170th layer, to the bottom, the 1st layer, (T-B scheme) in vertical NAND (VNAND) Flash Memory, is investigated to minimize Vt variation by reducing Z-interference. With the aid of Technology Computer Aided Design (TCAD) the Z-Interference for T-B (84 mV) is found to be better than B-T (105 mV). Moreover, under scaled cell dimensions (e.g., Lg: 31→24 nm), the improvement becomes protruding (T-B: 126 mV and B-T: 162 mV), emphasizing the significance of the T-B program scheme for the next generation VNAND products with the higher bit density.

Promoting Dual Electronic and Ionic Transport in PEDOT by Embedding Carbon Nanotubes for Large Thermoelectric Responses.

Thermoelectric (TE) energy conversion with nontraditional organic materials is promising in wearable electronics and roll-to-roll manufacturing because of mechanical flexibility, lightweight, and easy processing. Although typical organic materials have a benefit of low thermal conductivity that creates a large temperature gradient, relatively small thermopower (or Seebeck coefficient) often requires copious number of TE legs to fabricate practical TE devices. Here, we show that hybrids of poly(3,4-ethylenedioxythiophene)-tosylate (PEDOT-Tos) and carbon nanotubes (CNTs) can produce extremely large thermopower, ∼14 mV/K at room temperature by a chemical reduction. With decent electrical conductivity, an extraordinary power factor of ∼1200 µW/m K2 at room temperature was observed. The large power factor could be attributed to prominent dual electronic and ionic conduction, which is likely to be promoted by embedding the CNTs in PEDOT  due to the improvement in the carrier mobility, in comparison with the inferior and widely varying  TE properties of PEDOT-only samples in the literature. While a higher CNT concentration gave a larger electronic contribution, a longer reduction or a lower CNT concentration provided a larger ionic contribution. Meanwhile, well-separated CNTs created CNT junctions intervened by PEDOT-Tos, suppressing the thermal transport. Further research utilizing the high TE responses could greatly help to develop practical wearable and/or mass-producible thermal energy harvesting and storage devices.

Morphology dependent catalysis and surface enhanced Raman scattering (SERS) studies using Pd nanostructures in DNA, CTAB and PVA scaffolds.

Palladium nanoparticles (Pd NPs) of three different morphologies viz., nanocubes with cetyltrimethylammonium bromide (CTAB), nanowires with polyvinyl alcohol (PVA) and Pd NPs with deoxyribonucleic acid (DNA) scaffolds were synthesized by UV-irradiation. Catalysis and surface enhanced Raman scattering (SERS) studies were done with the synthesized morphologically distinct Pd nanostructures for the very first time. The catalytic rate was extremely high with Pd nanowires templated with PVA and the order of the catalytic rate was Pd nanowires in PVA > Pd nanocubes in CTAB > DNA-Pd wire-like assemblies. The highest catalytic rate was observed for PVA capped Pd nanowires which is a few hundred fold higher than other metal NP catalysts. Methylene blue (MB) was used as a Raman analyte for the SERS study and the largest EF of 1.9 × 105 at a peak position of 1391 cm-1 was observed with Pd nanowires in the DNA scaffold as a SERS substrate. The order of the SERS EF values was DNA-Pd wire-like assemblies > Pd nanocubes in CTAB > Pd nanowires in PVA. Beyond everything, the present synthesis route is easy, faster, candid, highly reproducible and cost-effective. In the near future, the same protocol could be applied to synthesize other materials for various applications.

Thermal Transport Driven by Extraneous Nanoparticles and Phase Segregation in Nanostructured Mg2(Si,Sn) and Estimation of Optimum Thermoelectric Performance.

Solid solutions of magnesium silicide and magnesium stannide were recently reported to have high thermoelectric figure-of-merits (ZT) due to remarkably low thermal conductivity, which was conjectured to come from phonon scattering by segregated Mg2Si and Mg2Sn phases without detailed study. However, it is essential to identify the main cause for further improving ZT as well as estimating its upper bound. Here we synthesized Mg2(Si,Sn) with nanoparticles and segregated phases, and theoretically analyzed and estimated the thermal conductivity upon segregated fraction and extraneous nanoparticle addition by fitting experimentally obtained thermal conductivity, electrical conductivity, and thermopower. In opposition to the previous speculation that segregated phases intensify phonon scattering, we found that lattice thermal conductivity was increased by the phase segregation, which is difficult to avoid due to the miscibility gap. We selected extraneous TiO2 nanoparticles dissimilar to the host materials as additives to reduce lattice thermal conductivity. Our experimental results showed the maximum ZT was improved from ∼0.9 without the nanoparticles to ∼1.1 with 2 and 5 vol % TiO2 nanoparticles at 550 °C. According to our theoretical analysis, this ZT increase by the nanoparticle addition mainly comes from suppressed lattice thermal conductivity in addition to lower bipolar thermal conductivity at high temperatures. The upper bound of ZT was predicted to be ∼1.8 for the ideal case of no phase segregation and addition of 5 vol % TiO2 nanoparticles. We believe this study offers a new direction toward improved thermoelectric performance of Mg2(Si,Sn).

Simultaneously improving electrical conductivity and thermopower of polyaniline composites by utilizing carbon nanotubes as high mobility conduits.

Electrical conductivity and thermopower of isotropic materials typically have inversely proportional correlation because both are strongly affected in the opposite way by the electronic carrier concentration. This behavior has been one of the major hurdles in developing high-performance thermoelectrics whose figure-of-merit enhances with large thermopower and high electrical conductivity. Here we report a promising method of simultaneously improving both properties with polyaniline (PANI) composites filled by carbon nanotubes (CNTs). With addition of double-wall CNTs (DWCNTs), the electronic mobility of PANI doped with camphorsulfonic acid (PANI-CSA) was raised from ∼0.15 to ∼7.3 cm(2)/(V s) (∼50 time improvement) while the carrier concentration was decreased from ∼2.1 × 10(21) to ∼5.6 × 10(20) cm(-3) (∼4 time reduction). The larger increase of mobility increased electrical conductivity despite the carrier concentration reduction that enlarges thermopower. The improvement in the carrier mobility could be attributed to the band alignment that attracts hole carriers to CNTs whose mobility is much higher than that of PANI-CSA. The electrical conductivity of the PANI-CSA composites with 30-wt % DWCNTs was measured to be ∼610 S/cm with a thermopower value of ∼61 µV/K at room temperature, resulting in a power factor value of ∼220 µW/(m K(2)), which is more than two orders higher than that of PANI-CSA as well as the highest among those of the previously reported PANI composites. Further study may result in high performance thermoelectric organic composites uniquely offering mechanical flexibility, light weight, low toxicity, and easy manufacturing. unlike conventional inorganic semiconductors.

Thermally Driven Large N-Type Voltage Responses from Hybrids of Carbon Nanotubes and Poly(3,4-ethylenedioxythiophene) with Tetrakis(dimethylamino)ethylene.

Hybrids of carbon nanotubes (CNTs) and poly(3,4-ethylenedioxythiophene) (PEDOT) treated by tetrakis(dimethylamino)ethylene (TDAE) have large n-type voltages in response to temperature differences. The reduced carrier concentration by TDAE reduction and partially percolated CNT networks embedded in the PEDOT matrix result in high thermopower and low thermal conductivity. The high electron mobility in the CNTs helps to minimally reduce the electrical conductivity of the hybrid, resulting in a large figure-of-merit.