Solvent dynamics play a decisive role in the complex formation of biologically relevant redox proteins

Adams, Ellen M.; Lampret, Oliver; König, Benedikt; Happe, Thomas; Havenith, Martina

doi:10.1039/d0cp00267d

Cited by 11 publications

(9 citation statements)

References 56 publications

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“…We characterized previously the optical properties of the diamond windows of the sample holder with linear, tabletop terahertz time-domain spectroscopy (THz-TDS). The details of this linear spectroscopy technique are reported elsewhere [36]. The diamond windows display a small absorption in the THz range (orange diamonds, Figure 2a).…”

Section: Methodsmentioning

confidence: 99%

Nonlinear TeraHertz Transmission by Liquid Water at 1 THz

Novelli

Adhlakha

et al. 2020

Applied Sciences

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The solvation properties of liquid water originate from the transient network of hydrogen-bonded molecules. In order to probe the coupling between the different modes of this network, nonlinear terahertz (THz) spectroscopy techniques are required. Ideally, these techniques should use a minimal volume and capitalize on sensitive field-resolved detection. Here we performed open aperture z-scan transmission experiments on static liquid cells, and detect the THz fields with electro-optical techniques. We show that it is possible to quantify the nonlinear response of liquid water at ~1 THz even when large signals originate from the sample holder windows.

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Section: Methodsmentioning

confidence: 99%

Nonlinear TeraHertz Transmission by Liquid Water at 1 THz

Novelli

Adhlakha

et al. 2020

Applied Sciences

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“…The absorption coefficient (and refractive index if applicable) of the sample was determined from previously described methods. 60,61 Error of THz-TDS and FTIR measurements are 0.6 and 5 cm −1 , respectively.…”

Section: Terahertz Spectroscopymentioning

confidence: 99%

“…Terahertz (THz) absorption spectra were measured with a THz time domain spectrometer (THz-TDS, range 10–80 cm –1 ) and a FTIR spectrometer (80–600 cm –1 ). The THz-TDS is a custom-built spectrometer system that has been previously described, 60 while the FTIR spectrometer is a commercially available spectrometer (Bruker Vertex 80 v) equipped with a helium cooled silicon bolometer detector. For the THz-TDS measurements, a demountable cell consisting of two z -cut quartz windows (4 mm thick) and a Teflon spacer (100 μm thick) was used.…”

Section: Experimental and Simulation Detailsmentioning

confidence: 99%

“…The sample cell temperature was kept constant at 20 °C with an external chiller, and the sample compartment was purged with nitrogen. The absorption coefficient (and refractive index if applicable) of the sample was determined from previously described methods. , Error of THz-TDS and FTIR measurements are 0.6 and 5 cm –1 , respectively.…”

Section: Experimental and Simulation Detailsmentioning

confidence: 99%

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Local Mutations Can Serve as a Game Changer for Global Protein Solvent Interaction

Adams

Pezzotti

Ahlers

et al. 2021

JACS Au

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Although it is well-known that limited local mutations of enzymes, such as matrix metalloproteinases (MMPs), may change enzyme activity by orders of magnitude as well as its stability, the completely rational design of proteins is still challenging. These local changes alter the electrostatic potential and thus local electrostatic fields, which impacts the dynamics of water molecules close the protein surface. Here we show by a combined computational design, experimental, and molecular dynamics (MD) study that local mutations have not only a local but also a global effect on the solvent: In the specific case of the matrix metalloprotease MMP14, we found that the nature of local mutations, coupled with surface morphology, have the ability to influence large patches of the water hydrogen-bonding network at the protein surface, which is correlated with stability. The solvent contribution can be experimentally probed via terahertz (THz) spectroscopy, thus opening the door to the exciting perspective of rational protein design in which a systematic tuning of hydration water properties allows manipulation of protein stability and enzymatic activity.

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“…In this context, an important body of research in the field of molecular electronics is being done with proteins both at a single-molecule level [214][215][216][217][218] and thin-films comprising a monolayer or a short number of layers [219][220][221][222][223]. Additionally, it has been experimentally and theoretically proved that it is possible to tune molecular electron transfer rates in electron transfer proteins (ETpr's) through (i) chemical modifications and changes in the redox center, as well as the locations of the donor, the acceptor, and the bridge moieties within the ETpr's structure [220,[224][225][226][227][228] (ii) modifying the solvent environment [229], and importantly, (iii) orientation relative to the electrode and changing the strength of the protein-electrode coupling [230][231][232]. The study of large-area protein-based molecular electronic devices has been carried out mainly by the self-assembly method [148,149] via an appropriate linker.…”

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confidence: 99%

Nanofabrication Techniques in Large-Area Molecular Electronic Devices

2020

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The societal impact of the electronics industry is enormous—not to mention how this industry impinges on the global economy. The foreseen limits of the current technology—technical, economic, and sustainability issues—open the door to the search for successor technologies. In this context, molecular electronics has emerged as a promising candidate that, at least in the short-term, will not likely replace our silicon-based electronics, but improve its performance through a nascent hybrid technology. Such technology will take advantage of both the small dimensions of the molecules and new functionalities resulting from the quantum effects that govern the properties at the molecular scale. An optimization of interface engineering and integration of molecules to form densely integrated individually addressable arrays of molecules are two crucial aspects in the molecular electronics field. These challenges should be met to establish the bridge between organic functional materials and hard electronics required for the incorporation of such hybrid technology in the market. In this review, the most advanced methods for fabricating large-area molecular electronic devices are presented, highlighting their advantages and limitations. Special emphasis is focused on bottom-up methodologies for the fabrication of well-ordered and tightly-packed monolayers onto the bottom electrode, followed by a description of the top-contact deposition methods so far used.

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Solvent dynamics play a decisive role in the complex formation of biologically relevant redox proteins

Abstract: THz absorption spectroscopy reveals that water is a critical factor that governs the transient complex formation of redox proteins. Binding of the substrate creates an entropically favorable complex with bulk-like solvent dynamics.

Cited by 11 publications

References 56 publications

Nonlinear TeraHertz Transmission by Liquid Water at 1 THz

Nonlinear TeraHertz Transmission by Liquid Water at 1 THz

Local Mutations Can Serve as a Game Changer for Global Protein Solvent Interaction

Nanofabrication Techniques in Large-Area Molecular Electronic Devices

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