We report a low-cost water-in-salt electrolyte, of 30 m ZnCl2, which enables dendrite-free Zn metal anode to possess high coulombic efficiency (CE). In asymmetric Zn‖Zn cells with limited mass plated as the working electrode, ZnCl2 WiSE improves average CE 95.4% from 73.2% in 5 ZnCl2.

Abstract A great challenge for all aqueous batteries, including Zn‐metal is the parasitic hydrogen evolution reaction on low‐potential anode. Herein, we report formula of a highly concentrated electrolyte that mitigates by transforming water molecules more inert. The comprises primarily ZnCl 2 and LiCl as an additive, both which are inexpensive salts. O–H covalent bonds in get strengthened chemical environment has fewer bonding interactions greater number Zn–Cl superhalides, suggested...

Primary events that power ultrafast excited state proton transfer in water are revealed to involve coupled intermolecular and intramolecular motions.

We demonstrate a versatile and efficient setup to perform femtosecond stimulated Raman spectroscopy (FSRS). Technical innovations are implemented achieve the wavelength tunability for both picosecond narrowband pump pulse broadband probe pulse. Using simplified one-grating scheme in home-built second harmonic bandwidth compressor followed by two-stage noncollinear optical parametric amplifier, we tune from ca. 480 750 nm. To generate suitable tandem, rely on our recently demonstrated...

Tracking molecular motions in real time remains a formidable challenge science and engineering fields because the experimental methodology requires simultaneously high spatial temporal resolutions. Building on early successes future potential of femtosecond stimulated Raman spectroscopy (FSRS) as structural dynamics technique, we present comprehensive study line shapes photosensitive molecule solution with tunable pump probe pulses. Following 400 nm electronic excitation, model photoacid...

Oxidative anion insertion into graphite in an aqueous environment represents a significant challenge the construction of dual-ion batteries. In dilute electrolytes, oxygen evolution reaction (OER) dominates anodic current before anions can be inserted gallery. Herein, we report that reversible Mg-Cl superhalides delivers record-high capacity 150 mAh g-1 from deep eutectic solvent comprising magnesium chloride and choline chloride. The does not form staged intercalation compounds; instead,...

Green fluorescent protein (GFP) has revolutionized bioimaging and life sciences. Its successes have inspired modification of the chromophore structure environment to tune emission properties, but outside cage, is essentially non-fluorescent. In this study, we employ tunable femtosecond stimulated Raman spectroscopy (FSRS) transient absorption (TA) map energy dissipation pathways GFP model (HBDI) in basic aqueous solution. Strategic tuning pump 550 nm exploits band enhance excited state...

Superphotoacidity involves ultrafast proton motions implicated in numerous chemical and biological processes. We used conformational locking strategic addition of electron-withdrawing substituents to synthesize a new GFP chromophore analogue: p-HO-3,5-diF-BDI:BF2 (diF). It is highly fluorescent exhibits excited-state transfer (ESPT) various solvents, placing it among the strongest photoacids. Tunable femtosecond stimulated Raman spectroscopy with unique resonance conditions transient...

We strategically modified the GFP core via chemical synthesis to make redder and brighter biomimetic fluorophores. Based on quantum calculations, solvatochromism analysis, femtosecond Raman, we unveiled additive effect of tuning electronic ground excited states, respectively, achieve a dramatic emission redshift with "double-donor-one-acceptor" structure.

Tracking vibrational motions during a photochemical or photophysical process has gained momentum, due to its sensitivity the progression of reaction and change environment. In this work, we implemented an advanced ultrafast technique, femtosecond-stimulated Raman spectroscopy (FSRS), monitor excited state structural evolution engineered green fluorescent protein (GFP) single-site mutant S205V. This mutation alters original proton transfer (ESPT) chain. By strategically tuning pump different...

When considering the optimal molecular packing to realize charge multiplication in organic photovoltaic materials, subtle changes intermolecular transfer (CT) coupling can strongly modulate singlet fission. To understand why certain morphologies are more conducive by triplet pair (TT) formation, we measure diffraction-limited transient absorption (TA) response from four single-crystal functionalized derivatives of fluorinated anthradithiophene: diF R-ADT (R = TES, TSBS, TDMS, TBDMS). TES-ADT...

Proton transfer remains one of the most fundamental processes in chemistry and biology. Superphotoacids provide an excellent platform to delineate excited-state proton (ESPT) mechanism on ultrafast time scales enable precisely control photoacidity other pertinent functionalities such as fluorescence. We modified GFP core ( p-HBDI chromophore) into two series highly fluorescent photoacids by fluorinating phenolic ring conformationally locking backbone (i.e., biomimetics). The trifluorinated...

Abstract Plating battery electrodes typically deliver higher specific capacity values than insertion or conversion because the ion charge carriers represent sole electrode active mass, and a host is unnecessary. However, reversible plating are rare for electronically insulating nonmetals. Now, highly iodine cathode presented that operates on redox couples of I 2 /[ZnI x (OH ) 4− ] 2− in water‐in‐salt electrolyte. The with theoretical 211 mAh g −1 plates carbon fiber paper as current...

Understanding excited-state structural dynamics of fluorescent-protein-based biosensors for Ca2+ imaging is crucial developing new in vivo indicators and advancing bioimaging. We implemented wavelength-tunable femtosecond stimulated Raman spectroscopy (FSRS) with a 530 nm pump to uncover the working mechanism an intensiometric fluorescent-protein biosensor, G-GECO1.1, highlighting deprotonation process its embedded chromophore. Besides confirming dynamic difference proton transfer (ESPT)...

The molecular mechanisms for the photoconversion of fluorescent proteins remain elusive owing to challenges monitoring chromophore structural dynamics during light-induced processes. We implemented time-resolved electronic and stimulated Raman spectroscopies reveal two hidden species an engineered ancestral GFP-like protein LEA, involving semi-trapped protonated trapped deprotonated chromophores en route in pH 7.9 buffer. A new dual-illumination approach was examined, using 400 505 nm light...

Natural and laboratory-guided evolution has created a rich diversity of fluorescent protein (FP)-based sensors for chloride (Cl-). To date, such have been limited to the Aequorea victoria green (avGFP) family, fusions with other FPs unlocked ratiometric imaging applications. Recently, we identified yellow from jellyfish Phialidium sp. (phiYFP) as turn-on, self-ratiometric Cl- sensor. elucidate its working mechanism rare example single FP this capability, tracked excited-state dynamics phiYFP...

We demonstrate the versatile broadband wavelength tunability of frequency upconverted multicolor cascaded four-wave-mixing (CFWM) signals spanning continuous range from UV to near IR in a thin type-I BBO crystal using 35 fs, 800 nm fundamental and chirped supercontinuum white light pulses. Two sets spatially dispersed CFWM laser sidebands are concomitantly generated two incident pulses as well their second-harmonic-generation sum-frequency-generation crossing geometry. The tunable with...

The ultrafast hydrogen bond breaking and reformation dynamics at the carbonyl site of a coumarin 102 dye molecule in ethanol is captured by femtosecond stimulated Raman spectroscopy (FSRS) on picosecond timescales.

Resonance enhancement has been increasingly employed in the emergent femtosecond stimulated Raman spectroscopy (FSRS) to selectively monitor molecular structure and dynamics with improved spectral temporal resolutions signal-to-noise ratios. Such joint efforts by technique- application-oriented scientists engineers have laid foundation for exploiting tunable FSRS methodology investigate a great variety of photosensitive systems elucidate underlying functional mechanisms on time scales....

We demonstrate the simultaneous generation of multicolor femtosecond laser pulses spanning wavelength range from UV to near IR in a 0.1 mm Type I beta-barium borate crystal 800 nm fundamental and weak super-continuum white light (SCWL) pulses. The broadband observed are attributed two concomitant cascaded four-wave mixing (CFWM) processes as corroborated by calculation: (1) directly incident pulses; (2) sum-frequency (SFG) induced CFWM process (SFGFWM). latter signal arises interaction...

Photoactivated proton transfer (PT) wire is responsible for the glow of green fluorescent protein (GFP), which crucial bioimaging and biomedicine. In this work, a new GFP-S65T/S205V double mutant developed from wild-type GFP in PT significantly modified. We implement femtosecond transient absorption (fs-TA) stimulated Raman spectroscopy (FSRS) to delineate process action. The excited state proceeds on ∼110 ps timescale, infers that distance one key link (water T203) GFP-S205V shortened by...

Metal–organic complexes are widely used across disciplines for energy and biological applications, however, their photophysical photochemical reaction coordinates remain unclear in solution due to pertaining molecular motions on ultrafast time scales. In this study, we apply transient absorption tunable femtosecond stimulated Raman spectroscopy (FSRS) investigate the UV photolysis of tungsten hexacarbonyl subsequent solvent binding events. On macroscopic scale with lamp irradiation, no...

In this paper, the crystal growth, polarized spectra, and laser performance of Yb:CaGdAlO4 were reported. The segregation coefficient Yb3+ ions was calculated to be 0.47. cell parameters determined a = b 0.3658 nm, c 1.1985 nm. peak absorption cross-section 2.65 × 10−20 cm2 at 979 nm stimulated emission 2.23 980 for π polarization. continuous-wave (CW) operations uncoated crystals with 5 3 mm3 in size demonstrated. A maximum output power 1.6 W 1048 obtained slope efficiency 28%. results show...