Terahertz calorimetry spotlights the role of water in biological processes

Zewail, A. H. Femtochemistry: atomic-scale dynamics of the chemical bond. J. Phys. Chem. A 104, 5660–5694 (2000).

Article  CAS  Google Scholar 

Alarcos, N., Cohen, B., Ziółek, M. & Douhal, A. Photochemistry and photophysics in silica-based materials: ultrafast and single molecule spectroscopy observation. Chem. Rev. 117, 13639–13720 (2017).

Article  CAS  PubMed  Google Scholar 

Maiuri, M., Garavelli, M. & Cerullo, G. Ultrafast spectroscopy: state of the art and open challenges. J. Am. Chem. Soc. 142, 3–15 (2019).

Article  PubMed  Google Scholar 

Biswas, S., Kim, J., Zhang, X. & Scholes, G. D. Coherent two-dimensional and broadband electronic spectroscopies. Chem. Rev. 122, 4257–4321 (2022).

Article  CAS  PubMed  Google Scholar 

Ball, P. Water as an active constituent in cell biology. Chem. Rev. 108, 74–108 (2008).

Article  CAS  PubMed  Google Scholar 

Breiten, B. et al. Water networks contribute to enthalpy/entropy compensation in protein–ligand binding. J. Am. Chem. Soc. 135, 15579–15584 (2013).

Article  CAS  PubMed  Google Scholar 

Conti Nibali, V. & Havenith, M. New insights into the role of water in biological function: studying solvated biomolecules using terahertz absorption spectroscopy in conjunction with molecular dynamics simulations. J. Am. Chem. Soc. 136, 12800–12807 (2014).

Article  CAS  PubMed  Google Scholar 

Ball, P. Water is an active matrix of life for cell and molecular biology. Proc. Natl Acad. Sci. USA 114, 13327–13335 (2017).

Article  CAS  PubMed  PubMed Central  Google Scholar 

Todd, M. J. & Gomez, J. Enzyme kinetics determined using calorimetry: a general assay for enzyme activity? Anal. Biochem. 296, 179–187 (2001).

Article  CAS  PubMed  Google Scholar 

Ladbury, J. E. & Doyle, M. L. Biocalorimetry 2: Applications of Calorimetry in the Biological Sciences (Wiley, 2004).

Gill, P., Moghadam, T. T. & Ranjbar, B. Differential scanning calorimetry techniques: applications in biology and nanoscience. J. Biomol. Tech. 21, 167 (2010).

PubMed  PubMed Central  Google Scholar 

Clout, A. et al. Simultaneous differential scanning calorimetry-synchrotron X-ray powder diffraction: a powerful technique for physical form characterization in pharmaceutical materials. Anal. Chem. 88, 10111–10117 (2016).

Article  CAS  PubMed  Google Scholar 

Askin, S. et al. A simultaneous differential scanning calorimetry–X-ray diffraction study of olanzapine crystallization from amorphous solid dispersions. Mol. Pharm. 17, 4364–4374 (2020).

Article  CAS  PubMed  Google Scholar 

Fornalski, D. et al. Simultaneous thermodynamic and dynamical characterisation using in situ calorimetry with neutron spectroscopy. Low Temp. Phys. 45, 289–293 (2019).

Article  CAS  Google Scholar 

Pandita, S. D. et al. Simultaneous DSC-FTIR spectroscopy: comparison of cross-linking kinetics of an epoxy/amine resin system. Thermochim. Acta 543, 9–17 (2012).

Article  CAS  Google Scholar 

Riedel, C. et al. The heat released during catalytic turnover enhances the diffusion of an enzyme. Nature 517, 227–230 (2015).

Article  CAS  PubMed  Google Scholar 

Rego, N. B. & Patel, A. J. Understanding hydrophobic effects: insights from water density fluctuations. Annu. Rev. Condens. Matter Phys. 13, 303–324 (2022).

Article  CAS  Google Scholar 

Monroe, J. et al. Water structure and properties at hydrophilic and hydrophobic surfaces. Annu. Rev. Chem. Biomol. 11, 523–557 (2020).

Article  CAS  Google Scholar 

Jamadagni, S. N., Godawat, R. & Garde, S. Hydrophobicity of proteins and interfaces: insights from density fluctuations. Annu. Rev. Chem. Biomol. Eng. 2, 147–171 (2011).

Article  CAS  PubMed  Google Scholar 

Giovambattista, N., Lopez, C. F., Rossky, P. J. & Debenedetti, P. G. Hydrophobicity of protein surfaces: separating geometry from chemistry. Proc. Natl Acad. Sci. USA 105, 2274–2279 (2008).

Article  CAS  PubMed  PubMed Central  Google Scholar 

Cheng, Y.-K. & Rossky, P. J. Surface topography dependence of biomolecular hydrophobic hydration. Nature 392, 696–699 (1998).

Article  CAS  PubMed  Google Scholar 

Perakis, F. et al. Vibrational spectroscopy and dynamics of water. Chem. Rev. 116, 7590–7607 (2016).

Article  CAS  PubMed  Google Scholar 

Bakker, H. J. & Skinner, J. L. Vibrational spectroscopy as a probe of structure and dynamics in liquid water. Chem. Rev. 110, 1498–1517 (2010).

Article  CAS  PubMed  Google Scholar 

Davis, J. G., Gierszal, K. P., Wang, P. & Ben-Amotz, D. Water structural transformation at molecular hydrophobic interfaces. Nature 491, 582–585 (2012).

Article  CAS  PubMed  Google Scholar 

Ben-Amotz, D. Hydration-shell vibrational spectroscopy. J. Am. Chem. Soc. 141, 10569–10580 (2019).

Article  CAS  PubMed  Google Scholar 

Bredt, A. J. & Ben-Amotz, D. Influence of crowding on hydrophobic hydration-shell structure. Phys. Chem. Chem. Phys. 22, 11724–11730 (2020).

Article  CAS  PubMed  Google Scholar 

Penkov, N. V. Terahertz spectroscopy as a method for investigation of hydration shells of biomolecules. Biophys. Rev. 15, 1–17 (2023).

Article  Google Scholar 

Pal, S. K., Peon, J. & Zewail, A. H. Biological water at the protein surface: dynamical solvation probed directly with femtosecond resolution. Proc. Natl Acad. Sci. USA 99, 1763–1768 (2002).

Article  CAS  PubMed  PubMed Central  Google Scholar 

Ebbinghaus, S. et al. An extended dynamical hydration shell around proteins. Proc. Natl Acad. Sci. USA 104, 20749–20752 (2007).

Article  CAS  PubMed  PubMed Central  Google Scholar 

Qin, Y., Wang, L. & Zhong, D. Dynamics and mechanism of ultrafast water–protein interactions. Proc. Natl Acad. Sci. USA 113, 8424–8429 (2016).

Article  CAS  PubMed  PubMed Central  Google Scholar 

Savolainen, J., Uhlig, F., Ahmed, S., Hamm, P. & Jungwirth, P. Direct observation of the collapse of the delocalized excess electron in water. Nat. Chem. 6, 697–701 (2014).

Article  CAS  PubMed  Google Scholar 

Shalit, A., Ahmed, S., Savolainen, J. & Hamm, P. Terahertz echoes reveal the inhomogeneity of aqueous salt solutions. Nat. Chem. 9, 273–278 (2017).

Article  CAS  PubMed  Google Scholar 

Hoberg, C. et al. Caught in the act: real-time observation of the solvent response that promotes excited-state proton transfer in pyranine. Chem. Sci. 14, 4048–4058 (2023).

Article  CAS  PubMed  PubMed Central  Google Scholar 

Hamm, P. & Zanni, M. Concepts and Methods of 2D Infrared Spectroscopy (Cambridge Univ. Press, 2011).

Dhillon, S. et al. The 2017 terahertz science and technology roadmap. J. Phys. D Appl. Phys. 50, 043001 (2017).

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