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Temperature-Jump 2D IR Spectroscopy with Intensity-Modulated CW Optical Heating

  • Brennan Ashwood
    Brennan Ashwood
    Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United States
  • Nicholas H. C. Lewis
    Nicholas H. C. Lewis
    Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United States
  • Paul J. Sanstead
    Paul J. Sanstead
    Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United States
  • , and 
  • Andrei Tokmakoff*
    Andrei Tokmakoff
    Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United States
    *Email: [email protected]
Cite this: J. Phys. Chem. B 2020, 124, 39, 8665–8677
Publication Date (Web):September 9, 2020
https://doi.org/10.1021/acs.jpcb.0c07177
Copyright © 2020 American Chemical Society

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    Abstract

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    Pulsed temperature-jump (T-jump) spectroscopy with infrared (IR) detection has been widely used to study biophysical processes occurring from nanoseconds to ∼1 ms with structural sensitivity. However, many systems exhibit structural dynamics on time scales longer than the millisecond barrier that is set by the time scale for thermal relaxation of the sample. We developed a linear and nonlinear infrared spectrometer coupled to an intensity-modulated continuous wave (CW) laser to probe T-jump-initiated chemical reactions from <1 ms to seconds. Time-dependent modulation of the CW laser leads to a <1 ms heating time as well as a constant final temperature (±3%) for the duration of the heating time. Temperature changes of up to 75 °C in D2O are demonstrated, allowing for nonequilibrium measurements inaccessible to standard pulsed optical T-jump setups. T-jump linear absorption, pump–probe, and two-dimensional IR (2D IR) spectroscopy are applied to the unfolding and refolding of ubiquitin and a model intercalated motif (i-motif) DNA sequence, and analysis of the observed signals is used to demonstrate the limits and utility of each method. Overall, the ability to probe temperature-induced chemical processes from <1 ms to many seconds with 2D IR spectroscopy provides multiple new avenues for time-dependent spectroscopy in chemistry and biophysics.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpcb.0c07177.

    • Sample preparation; methodology of determining sample temperature change; details of solvent heating and cooling simulations; Ti-dependent solvent heating and cooling measurements; methodology of D2O background removal for t-A spectroscopy; comparison of t-A and t-PP signal amplitude and relaxation kinetics; evaluation of distortions in T-jump and T-drop data from overlap with solvent heating and cooling profile (PDF)

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    Cited By

    This article is cited by 9 publications.

    1. Kevin C. Robben, Christopher M. Cheatum. Increasing Pump–Probe Signal toward Asymptotic Limits. The Journal of Physical Chemistry B 2023, 127 (21) , 4694-4707. https://doi.org/10.1021/acs.jpcb.3c01270
    2. Adam K. Nijhawan, Arnold M. Chan, Darren J. Hsu, Lin X. Chen, Kevin L. Kohlstedt. Resolving Dynamics in the Ensemble: Finding Paths through Intermediate States and Disordered Protein Structures. The Journal of Physical Chemistry B 2021, 125 (45) , 12401-12412. https://doi.org/10.1021/acs.jpcb.1c05820
    3. K. Laouer, M. Schmid, F. Wien, P. Changenet, F. Hache. Folding Dynamics of DNA G-Quadruplexes Probed by Millisecond Temperature Jump Circular Dichroism. The Journal of Physical Chemistry B 2021, 125 (29) , 8088-8098. https://doi.org/10.1021/acs.jpcb.1c01993
    4. Alexander P. Hawkins, Amy E. Edmeades, Christopher D. M. Hutchison, Michael Towrie, Russell F. Howe, Gregory M. Greetham, Paul M. Donaldson. Laser induced temperature-jump time resolved IR spectroscopy of zeolites. Chemical Science 2024, 15 (10) , 3453-3465. https://doi.org/10.1039/D3SC06128K
    5. Tiantian Dong, Pengyun Yu, Juan Zhao, Jianping Wang. Site specifically probing the unfolding process of human telomere i-motif DNA using vibrationally enhanced alkynyl stretch. Physical Chemistry Chemical Physics 2024, 26 (5) , 3857-3868. https://doi.org/10.1039/D3CP05328H
    6. Neil T. Hunt. Biomolecular infrared spectroscopy: making time for dynamics. Chemical Science 2024, 15 (2) , 414-430. https://doi.org/10.1039/D3SC05223K
    7. Susan J. Schroeder. Insights into nucleic acid helix formation from infrared spectroscopy. Biophysical Journal 2024, 123 (2) , 115-117. https://doi.org/10.1016/j.bpj.2023.12.017
    8. Brennan Ashwood, Michael S. Jones, Yumin Lee, Joseph R. Sachleben, Andrew L. Ferguson, Andrei Tokmakoff. Molecular insight into how the position of an abasic site modifies DNA duplex stability and dynamics. Biophysical Journal 2024, 123 (2) , 118-133. https://doi.org/10.1016/j.bpj.2023.11.022
    9. Brennan Ashwood, Michael S. Jones, Aleksandar Radakovic, Smayan Khanna, Yumin Lee, Joseph R. Sachleben, Jack W. Szostak, Andrew L. Ferguson, Andrei Tokmakoff. Thermodynamics and kinetics of DNA and RNA dinucleotide hybridization to gaps and overhangs. Biophysical Journal 2023, 122 (16) , 3323-3339. https://doi.org/10.1016/j.bpj.2023.07.009

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