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Lithium metal anodes hold great promise to enable high-energy battery systems. However, lithium dendrites at the interface between anode and separator pose risks of short circuits and fire, impeding the safe application. In contrast to conventional approaches of suppressing dendrites, here we show a deposition-regulating strategy by electrically passivating the top of a porous nickel scaffold and chemically activating the bottom of the scaffold to form conductivity/lithiophilicity gradients, whereby lithium is guided to deposit preferentially at the bottom of the anode, safely away from the separator. The resulting lithium anodes significantly reduce the probability of dendrite-induced short circuits. Crucially, excellent properties are also demonstrated at extremely high capacity (up to 40 mAh cm −2 ), high current density, and/or low temperatures (down to −15 °C), which readily induce dendrite shorts in particular. This facile and viable deposition-regulating strategy provides an approach to preferentially deposit lithium in safer positions, enabling a promising anode for next-generation lithium batteries. Here the authors report a deposition-regulating strategy to form conductivity and lithiophilicity gradients which serve to guide the preferential lithium growth away from the interface between anode and separator and mitigate the dendrite-induced short circuits.

Interfaces have crucial, but still poorly understood, roles in the performance of secondary solid-state batteries. Here, using crystallographically oriented and highly faceted thick cathodes, we directly assess the impact of cathode crystallography and morphology on the long-term performance of solid-state batteries. The controlled interface crystallography, area and microstructure of these cathodes enables an understanding of interface instabilities unknown (hidden) in conventional thin-film and composite solid-state electrodes. A generic and direct correlation between cell performance and interface stability is revealed for a variety of both lithium- and sodium-based cathodes and solid electrolytes. Our findings highlight that minimizing interfacial area, rather than its expansion as is the case in conventional composite cathodes, is key to both understanding the nature of interface instabilities and improving cell performance. Our findings also point to the use of dense and thick cathodes as a way of increasing the energy density and stability of solid-state batteries. Interfaces play crucial, but still poorly understood, roles in the performance of secondary solid-state batteries. Using crystallographically oriented and highly faceted thick cathodes, the impact of cathode crystallography and morphology on long-term performance is investigated.

The field of self-assembly has moved far beyond early work, where the focus was primarily the resultant beautiful two- and three-dimensional structures, to a focus on forming materials and devices with important properties either otherwise not available, or only available at great cost. Over the last few years, materials with unprecedented electronic, photonic, energy-storage, and chemical separation functionalities were created with self-assembly, while at the same time, the ability to form even more complex structures in two and three dimensions has only continued to advance. Self-assembly crosscuts all areas of materials. Functional structures have now been realized in polymer, ceramic, metallic, and semiconducting systems, as well as composites containing multiple classes of materials. As the field of self-assembly continues to advance, the number of highly functional systems will only continue to grow and make increasingly greater impacts in both the consumer and industrial space.

High-performance miniature power sources could enable new microelectronic systems. Here we report lithium ion microbatteries having power densities up to 7.4 mW cm −2  μm −1 , which equals or exceeds that of the best supercapacitors, and which is 2,000 times higher than that of other microbatteries. Our key insight is that the battery microarchitecture can concurrently optimize ion and electron transport for high-power delivery, realized here as a three-dimensional bicontinuous interdigitated microelectrodes. The battery microarchitecture affords trade-offs between power and energy density that result in a high-performance power source, and which is scalable to larger areas. Microbatteries offer new opportunities for microelectronics, but performance and integration remain a challenge. Pikul et al . develop a lithium ion microbattery with fully integrated nanoporous electrodes, which exceeds the power densities of most supercapacitors while retaining high-energy density.

Formation of thick, high energy density, flexible solid supercapacitors is challenging because of difficulties infilling gel electrolytes into porous electrodes. Incomplete infilling results in a low capacitance and poor mechanical properties. Here we report a bottom-up infilling method to overcome these challenges. Electrodes up to 500 μm thick, formed from multi-walled carbon nanotubes and a composite of poly(3,4-ethylenedioxythiophene), polystyrene sulfonate and multi-walled carbon nanotubes are successfully infilled with a polyvinyl alcohol/phosphoric acid gel electrolyte. The exceptional mechanical properties of the multi-walled carbon nanotube-based electrode enable it to be rolled into a radius of curvature as small as 0.5 mm without cracking and retain 95% of its initial capacitance after 5000 bending cycles. The areal capacitance of our 500 μm thick poly(3,4-ethylenedioxythiophene), polystyrene sulfonate, multi-walled carbon nanotube-based flexible solid supercapacitor is 2662 mF cm –2 at 2 mV s –1 , at least five times greater than current flexible supercapacitors. The development of high performance flexible solid supercapacitors calls for an effective approach to infill gel electrolytes into porous electrodes. Here the authors report a bottom-up method to address this technical challenge, which leads to enhanced areal capacitance and durability.

Stresses resulting from electrode material chemomechanics are strongly coupled to solid electrolyte-electrode interface failures. Such failures are significant barriers to realization of practical Li metal solid-state batteries (SSBs). Significant research efforts have been devoted to control anode chemomechanical stress. Here we show positive electrode (cathode) chemomechanical stress is also critical at commercially relevant low (e.g., <1 MPa) stack pressures. Using a series of model textured positive electrodes we provide the experimental evidence of the role of positive electrode lattice strain anisotropy during charge/discharge on positive electrode chemomechanics. Our model systems reveal that positive electrode chemomechanics significantly alter Li metal plating and stripping behavior at low stack pressure. We utilize these learnings to build long cycle-life SSBs with practical areal capacity (5 mAh/cm 2 ) operating under a 1 MPa stack pressure and at room temperature. Our findings highlight the importance of controlling positive electrode chemomechanics to realize low stack pressure SSBs. Solid-state batteries typically require high pressure to operate reliably. Here, the authors show that tuning cathode chemomechanics enables stable lithium metal battery cycling at room temperature and low pressure, eliminating the need for interlayers or elevated temperatures.

Materials that can be switched between low and high thermal conductivity states would advance the control and conversion of thermal energy. Employing in situ time-domain thermoreflectance (TDTR) and in situ synchrotron X-ray scattering, we report a reversible, light-responsive azobenzene polymer that switches between high (0.35 W m−1 K−1) and low thermal conductivity (0.10 W m−1 K−1) states. This threefold change in the thermal conductivity is achieved by modulation of chain alignment resulted from the conformational transition between planar (trans) and nonplanar (cis) azobenzene groups under UV and green light illumination. This conformational transition leads to changes in the π-π stacking geometry and drives the crystal-to-liquid transition, which is fully reversible and occurs on a time scale of tens of seconds at room temperature. This result demonstrates an effective control of the thermophysical properties of polymers by modulating interchain π-π networks by light.

Understanding how heat is transferred across interfaces is important for the efficiency of micro- and nanoscale electronic devices. Here, it is shown that there is a direct link between the bonding character of an interface and the thermal transport across it. Interfaces often dictate heat flow in micro- and nanostructured systems 1 , 2 , 3 . However, despite the growing importance of thermal management in micro- and nanoscale devices 4 , 5 , 6 , a unified understanding of the atomic-scale structural features contributing to interfacial heat transport does not exist. Herein, we experimentally demonstrate a link between interfacial bonding character and thermal conductance at the atomic level. Our experimental system consists of a gold film transfer-printed to a self-assembled monolayer (SAM) with systematically varied termination chemistries. Using a combination of ultrafast pump–probe techniques (time-domain thermoreflectance, TDTR, and picosecond acoustics) and laser spallation experiments, we independently measure and correlate changes in bonding strength and heat flow at the gold–SAM interface. For example, we experimentally demonstrate that varying the density of covalent bonds within this single bonding layer modulates both interfacial stiffness and interfacial thermal conductance. We believe that this experimental system will enable future quantification of other interfacial phenomena and will be a critical tool to stimulate and validate new theories describing the mechanisms of interfacial heat transport. Ultimately, these findings will impact applications, including thermoelectric energy harvesting, microelectronics cooling, and spatial targeting for hyperthermal therapeutics.

As sensors, wireless communication devices, personal health monitoring systems, and autonomous microelectromechanical systems (MEMS) become distributed and smaller, there is an increasing demand for miniaturized integrated power sources. Although thin-film batteries are well-suited for on-chip integration, their energy and power per unit area are limited. Three-dimensional electrode designs have potential to offer much greater power and energy per unit area; however, efforts to date to realize 3D microbatteries have led to prototypes with solid electrodes (and therefore low power) or mesostructured electrodes not compatible with manufacturing or on-chip integration. Here, we demonstrate an on-chip compatible method to fabricate high energy density (6.5 μWh cm ⁻²⋅μm ⁻¹) 3D mesostructured Li-ion microbatteries based on LiMnO ₂ cathodes, and NiSn anodes that possess supercapacitor-like power (3,600 μW cm ⁻²⋅μm ⁻¹ peak). The mesostructured electrodes are fabricated by combining 3D holographic lithography with conventional photolithography, enabling deterministic control of both the internal electrode mesostructure and the spatial distribution of the electrodes on the substrate. The resultant full cells exhibit impressive performances, for example a conventional light-emitting diode (LED) is driven with a 500-μA peak current (600-C discharge) from a 10-μm-thick microbattery with an area of 4 mm ² for 200 cycles with only 12% capacity fade. A combined experimental and modeling study where the structural parameters of the battery are modulated illustrates the unique design flexibility enabled by 3D holographic lithography and provides guidance for optimization for a given application. Significance Microscale batteries can deliver energy at the actual point of energy usage, providing capabilities for miniaturizing electronic devices and enhancing their performance. Here, we demonstrate a high-performance microbattery suitable for large-scale on-chip integration with both microelectromechanical and complementary metal-oxide–semiconductor (CMOS) devices. Enabled by a 3D holographic patterning technique, the battery possesses well-defined, periodically mesostructured porous electrodes. Such battery architectures offer both high energy and high power, and the 3D holographic patterning technique offers exceptional control of the electrode’s structural parameters, enabling customized energy and power for specific applications.

Compact visible wavelength achromats are essential for miniaturized and lightweight optics. However, fabrication of such achromats has proved to be exceptionally challenging. Here, using subsurface 3D printing inside mesoporous hosts we densely integrate aligned refractive and diffractive elements, forming thin high performance hybrid achromatic imaging micro-optics. Focusing efficiencies of 51–70% are achieved for 15μm thick, 90μm diameter, 0.3 numerical aperture microlenses. Chromatic focal length errors of less than 3% allow these microlenses to form high-quality images under broadband illumination (400–700 nm). Numerical apertures upwards of 0.47 are also achieved at the cost of some focusing efficiency, demonstrating the flexibility of this approach. Furthermore, larger area images are reconstructed from an array of hybrid achromatic microlenses, laying the groundwork for achromatic light-field imagers and displays. The presented approach precisely combines optical components within 3D space to achieve thin lens systems with high focusing efficiencies, high numerical apertures, and low chromatic focusing errors, providing a pathway towards achromatic micro-optical systems. Creating compact, lightweight and powerful optics that work well under visible light has been challenging. Here, the authors 3D print optically transparent polymers inside nanoporous glass in order to densely integrate refractive and diffractive elements, forming thin, high-performance hybrid achromatic imaging micro-optics.