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DOE OSTI2023

Redox-enabled electronic interrogation and feedback control of hierarchical and networked biological systems

Abstract Microelectronic devices can directly communicate with biology, as electronic information can be transmitted via redox reactions within biological systems. By engineering biology’s native redox networks, we enable electronic interrogation and control of biological systems at several hierarchical levels: proteins, cells, and cell consortia. First, electro-biofabrication facilitates on-device biological component assembly. Then, electrode-actuated redox data transmission and redox-linked synthetic biology allows programming of enzyme activity and closed-loop electrogenetic control of cellular function. Specifically, horseradish peroxidase is assembled onto interdigitated electrodes where electrode-generated hydrogen peroxide controls its activity. E. coli ’s stress response regulon, oxyRS , is rewired to enable algorithm-based feedback control of gene expression, including an eCRISPR module that switches cell-cell quorum sensing communication from one autoinducer to another—creating an electronically controlled ‘bilingual’ cell. Then, these disparate redox-guided devices are wirelessly connected, enabling real-time communication and user-based control. We suggest these methodologies will help us to better understand and develop sophisticated control for biology.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2026

Switching speed limits in electrically driven VO 2 structural Mott–Peierls transition

Mott materials are archetypal quantum systems actively explored as next-generation electronic and photonic platforms, with potential applications spanning non-Von Neumann computing, robotics, energy storage, and microwave technologies. Among these, vanadium dioxide (VO 2 ) has emerged as one of the most intensively studied compounds, owing to its sharp, near-room-temperature insulator-to-metal phase transition. VO 2 also serves as a benchmark system for testing cutting-edge theories and experimental techniques. Here, we directly visualize the electrically driven transition dynamics in VO 2 using a microwave-driven, frequency-tunable pulsed transmission electron microscope that combines nanometer spatial and picosecond temporal resolution. Under high-frequency (MHz–GHz) excitation, we capture the ultrafast nucleation, propagation, and dissolution of metallic domains within an operating device over millions of reversible cycles. We observe the ultrafast formation of consistent metallic nuclei beneath the electrodes, followed by the propagation of a structural phase front at 4.54 nm/ns. Our experiments show that phonon-mediated structural recovery ultimately limits reversible switching of VO 2 at GHz frequencies, and that a tunable regime for reversible operation spans from kHz to GHz through device engineering. Beyond VO 2 , our approach provides a powerful framework for probing non-equilibrium structural transformations in correlated and functional materials under realistic electrical stimuli.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Novel inverse oxide/metal catalysts for methanol synthesis: impact of oxide–metal interactions and reversible morphological changes

Inverse oxide/metal catalysts have proved to be excellent systems for the generation of methanol by CO 2 hydrogenation or the partial oxidation of methane. These systems can exhibit unique structural and chemical properties due to the nano size of the oxide component and strong oxide–metal interactions. Recent studies for ZnO/Cu, CeO 2 /Cu, TiO 2/ Cu, MgO/Cu, In 2 O 3 /Cu, and In 2 O 3 /Au catalysts have shown large variations in the composition and morphology of the oxide overlayer as a function of temperature and chemical environment. These oxide–metal interfaces are able to react with CO 2 and CH 4 at room temperature, and both reactants have a strong influence on the physical and chemical properties of the catalysts. Under reaction conditions, switches between oxide–metal and metal–metal interfaces can take in the catalyst surface. A dynamic behavior that can be linked to a high selectivity for methanol production over systems such as ZnO/Cu, CeO 2 /Cu and In 2 O 3 /Au. Finally, this type of correlation deserves additional systematic studies since it could be a powerful tool for designing highly efficient catalysts for methanol synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Design Space Exploration of Ferroelectric Tunnel Junction Toward Crossbar Memories

We perform a simulation-based analysis on the potential of emerging ferroelectric tunnel junctions (FTJs) as a memory device for crossbar arrays. Though FTJs are promising due to their low power switching characteristics compared to other emerging technologies, the greatest challenge for FTJs is the tradeoff between integration density and read performance. Our analysis highlights the need to co-optimize the ferroelectric thickness of the FTJ and read/write voltages to achieve proper functionality at large array sizes. Our analysis shows that FTJ-based crossbar achieves 93% higher sense margin at isoread power of 116 nW (per bit), but this FTJ design comes at a cost of 9.28× higher write power at isowrite time of 250 ns. In response, we study the potential tradeoffs of design points outside the feasible region to understand what device characteristics are desired to overcome such challenges.

Jao, Nicholas↗

DOE OSTI2019

Functionalizing Oxide Surfaces with Molecular Assemblies

In the research funded by this research grant, a series of key areas were explored. 1. Molecular Self-Assembled p/n Junctions for Solar Fuel Generation. 2. Functionalized Chromophore Assemblies for Dye-Sensitized Photoelectrosynthesis Cells with applications based on perylene diimides for water splitting in photocathode applications and in molecularly modified quantum dots. 3. Highly conjugated supramolecular chromophores in sensitized photoanodes for water reduction and excitation dependent photocurrent switching. 4. Electropolymerized molecular assemblies for Dye Sensitized Photoelectrosynthesis Cells, in excitation-energy dependent photocurrent switching, and a stable molecular photocathode for solar-driven CO 2 reduction. 5. Electropolymerized molecular assemblies for solar CO 2 reduction and water oxidation and preparing stable surface structures by silane and click chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

Structures of two aptamers with differing ligand specificity reveal ruggedness in the functional landscape of RNA

Two classes of riboswitches related to the ykkC guanidine-I riboswitch bind phosphoribosyl pyrophosphate (PRPP) and guanosine tetraphosphate (ppGpp). Here we report the co-crystal structure of the PRPP aptamer and its ligand. We also report the structure of the G96A point mutant that prefers ppGpp over PRPP with a dramatic 40,000-fold switch in specificity. The ends of the aptamer form a helix that is not present in the guanidine aptamer and is involved in the expression platform. In the mutant, the base of ppGpp replaces G96 in three-dimensional space. This disrupts the S-turn, which is a primary structural feature of the ykkC RNA motif. These dramatic differences in ligand specificity are achieved with minimal mutations. ykkC aptamers are therefore a prime example of an RNA fold with a rugged fitness landscape. The ease with which the ykkC aptamer acquires new specificity represents a striking case of evolvability in RNA.

Knappenberger, Andrew John↗

NASA NTRS1991

'Self-consistent' production of ion conics on return current region auroral field lines - A time-dependent, semi-kinetic model

We describe initial results from a time-dependent, semi-kinetic model of plasma outflow incorporating wave-particle interactions along current-carrying auroral field lines. Electrostatic waves are generated by the current driven ion cyclotron instability (CDICI), causing perpendicular velocity diffusion of ions plus electron heating via anomalous resistivity when and where the relative drift between electrons and ions exceeds certain critical velocities. Using the local bulk parameters we calculate these critical velocities, and so are able to self-consistently switch on and off the heating of the various particle species. Due to the dependence of these critical velocities on the bulk parameters of the species the heating effects exhibit quite complex spatial and temporal variations. A wide range of ion distribution functions are observed in these simulations, including conics with energies of a few electron volts and 'ring' distributions. The rings are seen to be a natural result of transverse heating and velocity filter effects and do not require coherent acceleration processes. We also observe the formation of a density depletion in hydrogen and enhanced oxygen densities at high altitudes.

Brown, David G.↗

NASA NTRS1993

Site diversity for satellite earth terminals and measurements at 28 GHz

This paper reviews site diversity concepts and models and presents the results of a site diversity experiment, in which radiometers were used to measure attenuation on earth-space paths, performed at Columbus, Ohio, for a period of one year. Attenuation statistics are presented first in the form of the joint probability density function of attenuation at the two sites. From these are derived the cumulative two-dimensional distribution of attenuation at both sites, the cumulative distribution of attenuation at each site, the effective cumulative distribution of attenuation for a diversity system that always switches to the better of two signals, and the effective cumulative distribution of attenuation for a system with maximal-ratio signal combining. The switched-system diversity gain is compared with Hodge's predictive model, and the diversity improvement is compared with Boithias' model. Fade-duration and interfade-interval statistics are also presented for each site and for systems that employ switching and maximal-ratio combining. Rain-rate and interrainfall interval statistics are also included.

Lin, Kuan-Ting↗

NASA NTRS1994

Applying Analog Integrated Circuits for Hero Protection

One of the most efficient methods for protecting electro-explosive devices (EED's) from HERO and ESD is to shield the EED in a conducting shell (Faraday cage). Electrical energy is transferred to the bridge by means of a magnetic coupling which passes through a portion of the conducting shell that is made from a magnetically permeable but electrically conducting material. This technique was perfected by ML Aviation, a U.K. company, in the early 80's, and was called a Radio Frequency Attenuation Connector (RFAC). It is now in wide use in the U.K. Previously, the disadvantage of RFAC over more conventional methods was its relatively high cost, largely driven by a thick film hybrid circuit used to switch the primary of the transformer. Recently, through a licensing agreement, this technology has been transferred to the U.S. and significant cost reductions and performance improvements have been achieved by the introduction of analog integrated circuits. An integrated circuit performs the following functions: (1) Chops the DC input to a signal suitable for driving the primary of the transformer; (2) Verifies the input voltage is above a threshold; (3) Verifies the input voltage is valid for a pre set time before enabling the device; (4) Provides thermal protection of the circuit; and (5) Provides an external input for independent logic level enabling of the power transfer mechanism. This paper describes the new RFAC product and its applications.

Kenneth E Willis↗

NASA NTRS2002

Energy Storage Flywheels on Spacecraft

With advances in carbon composite material, magnetic bearings, microprocessors, and high-speed power switching devices, work has begun on a space qualifiable Energy Momentum Wheel (EMW). An EMW is a device that can be used on a satellite to store energy, like a chemical battery, and manage angular momentum, like a reaction wheel. These combined functions are achieved by the simultaneous and balanced operation of two or more energy storage flywheels. An energy storage flywheel typically consists of a carbon composite rotor driven by a brushless DC motor/generator. Each rotor has a relatively large angular moment of inertia and is suspended on magnetic bearings to minimize energy loss. The use of flywheel batteries on spacecraft will increase system efficiencies (mass and power), while reducing design-production time and life-cycle cost. This paper will present a discussion of flywheel battery design considerations and a simulation of spacecraft system performance utilizing four flywheel batteries to combine energy storage and momentum management for a typical LEO satellite. A proposed set of control laws and an engineering animation will also be presented. Once flight qualified and demonstrated, space flywheel batteries may alter the architecture of most medium and high-powered spacecraft.

Bartlett, Robert O.↗

NASA NTRS1992

Optically intraconnected computer employing dynamically reconfigurable holographic optical element

An optically intraconnected computer and a reconfigurable holographic optical element employed therein. The basic computer comprises a memory for holding a sequence of instructions to be executed; logic for accessing the instructions in sequence; logic for determining for each the instruction the function to be performed and the effective address thereof; a plurality of individual elements on a common support substrate optimized to perform certain logical sequences employed in executing the instructions; and, element selection logic connected to the logic determining the function to be performed for each the instruction for determining the class of each function and for causing the instruction to be executed by those the elements which perform those associated the logical sequences affecting the instruction execution in an optimum manner. In the optically intraconnected version, the element selection logic is adapted for transmitting and switching signals to the elements optically.

Bergman, Larry A.↗

DOE OSTI2024

Modular DC circuit breaker with integrated energy storage for future DC networks

A T-breaker is an all-in-one solution for dc microgrid fault protection, power flow control, and power quality improvement. A T-breaker features a modular multilevel “T” structure with integrated energy storage devices. The two horizontal arms of the T-breaker realize fault current breaking, load voltage compensation, and power flow control; and the vertical arm of the T-breaker realizes shunt compensation. The configuration provides excellent voltage scalability and relaxes the requirements on the switching signal synchronization during fault transients. The local energy storage in sub-modules eases the fault energy dissipation requirement placed on the traditionally-adopted surge arrestors. The modular multilevel structure also offers immense control flexibility for all types of targeted functions of the provided T-breaker.

Wang, Jin↗

DOE OSTI2019

Nonlinear manipulation of surface plasmons on graphene-TMDC Bragg reflectors

In this study, we benefit from the nonlinear optical tunability of the graphene-transition metal dichalcogenide (G-TMDC) heterostructure and the strong confinement of the electromagnetic fields of surface plasmon polaritons (SPPs) on graphene in order to propose a highly tunable nonlinear optical Bragg reflector. Recently, two-dimensional (2D) TMDCs are the subject of intense researches because of their nonlinear optical properties at near infrared wavelengths which are very intriguing for various optical applications. We choose two kinds of 2D-TMDCs, MoSe{sub 2} and WSe{sub 2}, with the strongest second order optical nonlinearity at near infrared range to properly design the periodic variation of the propagating SPP waves on the graphene layer. We utilize theoretical method of quantum electrostatic heterostructure to compute the dielectric function of graphene-TMDCs. Different nonlinearities of two TMDCs lead to noticeable tuning of the full width at half maximum (FWHM) and the central Bragg wavelength of the reflector which let design various optical devices. We design an add/drop filter, a nonlinear switch, and an AND/OR optical logic gate based on our proposed Bragg reflector. Our finite difference time domain numerical and transfer matrix analytical results reveal that by increment of the optical intensity up to 6 MW/cm{sup 2} which is below the pulse damage threshold of graphene, due to the second order nonlinearity, a 10-nm red-shift in central Bragg wavelength is observed and the 20-nm FWHM at linear regime decreases to 1.5 nm. The SPP intensities of 0.8 MW/cm{sup 2} and 1.53 MW/cm{sup 2} fulfill the requirements for AND and OR logical operations with 57 and 66.51 dB extinction ratios, respectively.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Born effective charges and electric polarization in bulk ε-Fe 2 O 3 : An ab-initio approach

Limitation in the synthesis of single-crystal has restricted the complete understanding of the magnetoelectric properties of bulk ε-Fe 2 O 3 . In order to understand the electric polarization of bulk ε-Fe 2 O 3 , we have employed a first-principles Berry-phase method and the density functional perturbation theory to calculate the spontaneous electric polarization and Born effective charges (BECs) of ε-Fe 2 O 3 . The polarization quanta of the ferroelectric bulk ε-Fe 2 O 3 and its polarization lattice are also reported. The polarization switching through a paraelectric transition phase of a low barrier is found to be favorable. The polarization and BECs calculated by both methods are in good agreement.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Origin of Stabilization of Ligand-Centered Mixed Valence Ruthenium Azopyridine Complexes: DFT Insights for Neuromorphic Applications

Redox-driven conductance changes are critical processes in molecular- and coordination-complex-based memristive thin films and devices that are envisioned for neuromorphic technologies, but fundamental mechanisms of conductance switching are not fully understood. Here, we explore charge disproportionation (CD) processes in [Ru II L 2 ](PF 6 ) 2 molecular systems that intrinsically involve interfragment charge transfer (IFCT). Using a combination of ab initio molecular dynamics simulation (AIMD), time-dependent density functional theory (TD-DFT), and density functional theory (DFT) calculations, we investigate the electron transfer mechanisms and the roles of temperature and cell volumetric expansion in facilitating the counterion movements and electronic transitions required for low-cost IFCT and charge redistribution. A detailed analysis of the density of states and TD-DFT calculations highlights that unpaired electrons play a crucial role in low-energy transitions, with the azo (N=N) groups of the ligand serving as the primary sites for electronic transport between molecular fragments, further stabilizing the asymmetric state. Localization of added electrons on azo ligands occurs with negligible change at the Ru centers, supported by atomic volume expansions up to +4.74 bohr 3 , and goes along with a progressive reduction of the HOMO−LUMO gap across redox states, suggesting enhanced conductivity. The TD-DFT analysis reveals a dominant IFCT excitation at 2082.76 nm in the doubly reduced (22) state, while a stabilization energy of 1.20 eV of the asymmetric (13) state relative to the symmetric (22) state is predicted by constrained DFT. Periodic DFT and AIMD simulations emulating a molecular film show that the stabilization of the asymmetric state, relative to a symmetric one, translates in net charge separation values (order of ∼0.33 e) that are strongly linked to increased counterion mobility (average counterion displacements exceeding 0.7 Å per atom during CD events) and the involvement of azo groups in electron redistribution. These findings, which align with previously reported experimental and computational data, provide key insights into the IFCT mechanisms and electronic transport facilitated by azo groups, with important implications for redox-driven memristive and neuromorphic technologies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Cryo-EM captures the coordination of asymmetric electron transfer through a di-copper site in DPOR

Enzymes that catalyze long-range electron transfer (ET) reactions often function as higher order complexes that possess two structurally symmetrical halves. The functional advantages for such an architecture remain a mystery. Using cryoelectron microscopy we capture snapshots of the nitrogenase-like dark-operative protochlorophyllide oxidoreductase (DPOR) during substrate binding and turnover. DPOR catalyzes reduction of the C17 = C18 double bond in protochlorophyllide during the dark chlorophyll biosynthetic pathway. DPOR is composed of electron donor (L-protein) and acceptor (NB-protein) component proteins that transiently form a complex in the presence of ATP to facilitate ET. NB-protein is an α 2 β 2 heterotetramer with two structurally identical halves. However, our structures reveal that NB-protein becomes functionally asymmetric upon substrate binding. Asymmetry results in allosteric inhibition of L-protein engagement and ET in one half. Residues that form a conduit for ET are aligned in one half while misaligned in the other. An ATP hydrolysis-coupled conformational switch is triggered once ET is accomplished in one half. These structural changes are then relayed to the other half through a di-nuclear copper center at the tetrameric interface of the NB-protein and leads to activation of ET and substrate reduction. These findings provide a mechanistic blueprint for regulation of long-range electron transfer reactions.

Computational biophysics↗

DOE OSTI2026

Alignment switching in 3D-printed smectic liquid crystal elastomers

Extrusion-based additive manufacturing has emerged as a powerful platform for designing shape-morphing materials through controlled orientation. However, existing approaches primarily rely on a single mode of flow-induced alignment, limiting orientation programmability. Herein, we present a direct-ink-writing approach for smectic liquid crystal elastics that exploits two distinct alignment modes within a single ink. The smectic ink exhibits shear- and temperature-dependent orientation switching, enabling molecular alignment either perpendicular or parallel to the print direction. Combined rheological, X-ray, and molecular dynamics analyses reveal that this alignment inversion arises from the preservation or collapse of smectic layers under flow. This reversible switching encodes both contractile and elongational actuation within individual filaments, greatly expanding the design freedom of printed liquid crystal elastomers. We demonstrate 2D and 3D structures with diverse programmed shape transformations, highlighting the potential of this platform for adaptive soft actuators and architected functional materials.

Lee, Jin Hyeong [Pusan National University, Busan,↗

DOE OSTI2024

Cavity-modified molecular dipole switching dynamics

Polaritonic states, which are formed by resonances between a molecular excitation and the photonic mode of a cavity, have a number of useful properties that offer new routes to control molecular photochemistry using electric fields. To provide a theoretical description of how polaritonic states affect the real-time electron dynamics in molecules, a new method is described where the effects of strong light–molecule coupling are implemented using real-time electronic structure theory. The coupling between the molecular electronic states and the cavity is described by the Pauli–Fierz Hamiltonian, and transitions between polaritonic states are induced via an external time-dependent electric field using time-dependent configuration interaction (TDCI) theory, producing quantum electrodynamics TDCI (QED-TDCI). This method is used to study laser-induced ultrafast charge transfer and dipole-switching dynamics of the LiCN molecule inside a cavity. The increase in cavity coupling strength is found to have a significant impact on the energies and transition dipole moments of the molecule–cavity system. The convergence of the polaritonic state energies as a function of the number of included electronic and photonic basis states is discussed.

Chemistry↗