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FAIR DEAL Grand Challenge Overview

Allemang, Christopher R.; Anderson, Evan M.; Baczewski, Andrew D.; Bussmann, Ezra B.; Butera, Robert E.; Campbell, DeAnna M.; Campbell, Quinn C.; Carr, Stephen M.; Frederick, Esther F.; Gamache, Phillip G.; Gao, Xujiao G.; Grine, Albert D.; Gunter, Mathew M.; Halsey, Connor H.; Ivie, Jeffrey A.; Katzenmeyer, Aaron M.; Leenheer, Andrew J.; Lepkowski, William L.; Lu, Tzu-Ming L.; Mamaluy, Denis M.; Mendez Granado, Juan P.; Pena, Luis F.; Schmucker, Scott W.; Scrymgeour, David S.; Tracy, Lisa A.; Wang, George T.; Ward, Dan W.; Young, Steve M.

While it is likely practically a bad idea to shrink a transistor to the size of an atom, there is no arguing that it would be fantastic to have atomic-scale control over every aspect of a transistor – a kind of crystal ball to understand and evaluate new ideas. This project showed that it was possible to take a niche technique used to place dopants in silicon with atomic precision and apply it broadly to study opportunities and limitations in microelectronics. In addition, it laid the foundation to attaining atomic-scale control in semiconductor manufacturing more broadly.

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Characterization of suspended membrane waveguides towards a photonic atom trap integrated platform

Optics Express

Gehl, M.; Kindel, William K.; Karl, Nicholas J.; Orozco, Adrian S.; Musick, Katherine M.; Trotter, Douglas C.; Dallo, Christina M.; Starbuck, Andrew L.; Leenheer, Andrew J.; DeRose, Christopher T.; Biedermann, Grant; Jau, Yuan-Yu J.; Lee, Jongmin L.

We demonstrate an optical waveguide device, capable of supporting the high, invacuum, optical power necessary for trapping a single atom or a cold atom ensemble with evanescent fields. Our photonic integrated platform, with suspended membrane waveguides, successfully manages optical powers of 6 mW (500 μm span) to nearly 30 mW (125 μm span) over an un-tethered waveguide span. This platform is compatible with laser cooling and magnetooptical traps (MOTs) in the vicinity of the suspended waveguide, called the membrane MOT and the needle MOT, a key ingredient for efficient trap loading. We evaluate two novel designs that explore critical thermal management features that enable this large power handling. This work represents a significant step toward an integrated platform for coupling neutral atom quantum systems to photonic and electronic integrated circuits on silicon.

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CMOS-compatible, piezo-optomechanically tunable photonics for visible wavelengths and cryogenic temperatures

Optics Express

Stanfield, Paul S.; Leenheer, Andrew J.; Michael, C.P.; Sims, R.; Eichenfield, Matthew S.

We demonstrate a platform for phase and amplitude modulation in silicon nitride photonic integrated circuits via piezo-optomechanical coupling using tightly mechanically coupled aluminum nitride actuators. The platform, fabricated in a CMOS foundry, enables scalable active photonic integrated circuits for visible wavelengths, and the piezoelectric actuation functions without performance degradation down to cryogenic temperatures. As an example of the potential of the platform, we demonstrate a compact (∼40 µm diameter) silicon nitride ring resonator modulator operating at 780 nm with intrinsic quality factors in excess of 1.5 million, >10 dB change in extinction ratio with 2 V applied, a switching time less than 4 ns, and a switching energy of 0.5 pJ/bit. We characterize the exemplary device at room temperature and 7 K. At 7 K, the device obtains a resistance of approximately 20 teraohms, allowing it to operate with sub-picowatt electrical power dissipation. We further demonstrate a Mach-Zehnder modulator constructed in the same platform with piezoelectrically tunable phase shifting arms, with 750 ns switching time constant and 20 nW steady-state power dissipation at room temperature.

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Optimization of Si-photonics compatible AlN waveguides for integrated nonlinear optics applications

Optics InfoBase Conference Papers

Siddiqui, Aleem M.; Dominguez, Daniel D.; Michael, Christopher M.; Sims, Ryan; Stanfield, Paul S.; Hackett, Lisa A.; Leenheer, Andrew J.; Eichenfield, Matthew S.

We explore fabrication-process dependencies on optical losses of AlN films and demonstrate Second Harmonic Generation through modal phase-matching in integrated AlN waveguides. A loss-dependent conversion efficiency model is developed to better design waveguides in lossy AlN media.

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Phase Boundary Propagation in Li-Alloying Battery Electrodes Revealed by Liquid-Cell Transmission Electron Microscopy

ACS Nano

Leenheer, Andrew J.; Jungjohann, Katherine L.; Zavadil, Kevin R.; Harris, Charles T.

Battery cycle life is directly influenced by the microstructural changes occurring in the electrodes during charge and discharge cycles. Here, we image in situ the nanoscale phase evolution in negative electrode materials for Li-ion batteries using a fully enclosed liquid cell in a transmission electron microscope (TEM) to reveal early degradation that is not evident in the charge-discharge curves. To compare the electrochemical phase transformation behavior between three model materials, thin films of amorphous Si, crystalline Al, and crystalline Au were lithiated and delithiated at controlled rates while immersed in a commercial liquid electrolyte. This method allowed for the direct observation of lithiation mechanisms in nanoscale negative electrodes, revealing that a simplistic model of a surface-to-interior lithiation front is insufficient. For the crystalline films, a lithiation front spread laterally from a few initial nucleation points, with continued grain nucleation along the growing interface. The intermediate lithiated phases were identified using electron diffraction, and high-resolution postmortem imaging revealed the details of the final microstructure. Our results show that electrochemically induced solid-solid phase transformations can lead to highly concentrated stresses at the laterally propagating phase boundary which should be considered for future designs of nanostructured electrodes for Li-ion batteries.

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How voltage drops are manifested by lithium ion configurations at interfaces and in thin films on battery electrodes

Journal of Physical Chemistry C

Leung, Kevin L.; Leenheer, Andrew J.

Battery electrode surfaces are generally coated with electronically insulating solid films of thickness 1-50 nm. Both electrons and Li+ can move at the electrode-surface film interface in response to the voltage, which adds complexity to the "electric double layer" (EDL). We apply Density Functional Theory (DFT) to investigate how the applied voltage is manifested as changes in the EDL at atomic length scales, including charge separation and interfacial dipole moments. Illustrating examples include Li3PO4, Li2CO3, and LixMn2O4 thin films on Au(111) surfaces under ultrahigh vacuum conditions. Adsorbed organic solvent molecules can strongly reduce voltages predicted in vacuum. We propose that manipulating surface dipoles, seldom discussed in battery studies, may be a viable strategy to improve electrode passivation. We also distinguish the computed potential governing electrons, which is the actual or instantaneous voltage, and the "lithium cohesive energy"-based voltage governing Li content widely reported in DFT calculations, which is a slower-responding self-consistency criterion at interfaces. This distinction is critical for a comprehensive description of electrochemical activities on electrode surfaces, including Li+ insertion dynamics, parasitic electrolyte decomposition, and electrodeposition at overpotentials.

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Lithium electrodeposition dynamics in aprotic electrolyte observed in situ via transmission electron Microscopy

ACS Nano

Leenheer, Andrew J.; Jungjohann, Katherine L.; Zavadil, Kevin R.; Sullivan, John P.; Harris, C.T.

Electrodeposited metallic lithium is an ideal negative battery electrode, but nonuniform microstructure evolution during cycling leads to degradation and safety issues. A better understanding of the Li plating and stripping processes is needed to enable practical Li-metal batteries. Here we use a custom microfabricated, sealed liquid cell for in situ scanning transmission electron microscopy (STEM) to image the first few cycles of lithium electrodeposition/dissolution in liquid aprotic electrolyte at submicron resolution. Cycling at current densities from 1 to 25 mA/cm2 leads to variations in grain structure, with higher current densities giving a more needle-like, higher surface area deposit. The effect of the electron beam was explored, and it was found that, even with minimal beam exposure, beam-induced surface film formation could alter the Li microstructure. The electrochemical dissolution was seen to initiate from isolated points on grains rather than uniformly across the Li surface, due to the stabilizing solid electrolyte interphase surface film. We discuss the implications for operando STEM liquid-cell imaging and Li-battery applications.

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47 Results
47 Results