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Zuerch, Michael; Kohrell, Finn; Nebgen, Bailey R; Spies, Jacob A; Hollinger, Richard; Zong, Alfred; Uzundal, Can; Spielmann, Christian (, Dryad)Solid-state high harmonic generation (sHHG) spectroscopy is a promising technique for studying electronic structure, symmetry, and dynamics in condensed matter systems. Here, we report on the implementation of an advanced sHHG spectrometer based on a vacuum chamber and closed-cycle helium cryostat. Using an in situ temperature probe, it is demonstrated that the sample interaction region retains cryogenic temperature during the application of high-intensity femtosecond laser pulses that generate high harmonics. The presented implementation opens the door for temperature-dependent sHHG measurements down to a few Kelvin, which makes sHHG spectroscopy a new tool for studying phases of matter that emerge at low temperatures, which is particularly interesting for highly correlated materials.more » « less
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Tayvah, Uriel; Spies, Jacob A.; Neu, Jens; Schmuttenmaer, Charles A. (, Analytical Chemistry)
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Neu, Jens; Shipps, Catharine C.; Guberman-Pfeffer, Matthew J.; Shen, Cong; Srikanth, Vishok; Spies, Jacob A.; Kirchhofer, Nathan D.; Yalcin, Sibel Ebru; Brudvig, Gary W.; Batista, Victor S.; et al (, Nature Communications)Abstract Light-induced microbial electron transfer has potential for efficient production of value-added chemicals, biofuels and biodegradable materials owing to diversified metabolic pathways. However, most microbes lack photoactive proteins and require synthetic photosensitizers that suffer from photocorrosion, photodegradation, cytotoxicity, and generation of photoexcited radicals that are harmful to cells, thus severely limiting the catalytic performance. Therefore, there is a pressing need for biocompatible photoconductive materials for efficient electronic interface between microbes and electrodes. Here we show that living biofilms ofGeobacter sulfurreducensuse nanowires of cytochrome OmcS as intrinsic photoconductors. Photoconductive atomic force microscopy shows up to 100-fold increase in photocurrent in purified individual nanowires. Photocurrents respond rapidly (<100 ms) to the excitation and persist reversibly for hours. Femtosecond transient absorption spectroscopy and quantum dynamics simulations reveal ultrafast (~200 fs) electron transfer between nanowire hemes upon photoexcitation, enhancing carrier density and mobility. Our work reveals a new class of natural photoconductors for whole-cell catalysis.more » « less
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