Infrared spectroscopy of nicotinamide adenine dinucleotides in one and two dimensions

Niall Simpson, Daniel J. Shaw, Pim W J M Frederix, Audrey H. Gillies, Katrin Adamczyk, Gregory M. Greetham, Michael Towrie, Anthony William Parker, Paul A. Hoskisson, Neil T. Hunt

Research output: Contribution to journalArticle

7 Citations (Scopus)

Abstract

The development of multidimensional spectroscopic tools capable of resolving site-specific information about proteins and enzymes in the solution phase is an important aid to our understanding of biomolecular mechanisms, structure, and dynamics. Nicotinamide adenine dinucleotide (NAD) is a common biological substrate and so offers significant potential as an intrinsic vibrational probe of protein-ligand interactions but its complex molecular structure and incompletely characterized infrared spectrum currently limit its usefulness. Here, we report the FTIR spectroscopy of the oxidized and reduced forms of NAD at a range of pD values that relate to the "folded" and "unfolded" forms of the molecules that exist in solution. Comparisons with structural analogs and the use of density functional theory simulations provide a full assignment of the observed modes and their complex pD dependencies. Finally, ultrafast two-dimensional infrared spectra of the oxidized and reduced forms of NAD are reported and their usefulness as biomolecular probes is discussed.
LanguageEnglish
Pages16468-16478
Number of pages11
JournalJournal of Physical Chemistry B
Volume117
Issue number51
DOIs
Publication statusPublished - 27 Dec 2013

Fingerprint

nicotinamide
adenines
NAD
Infrared spectroscopy
infrared spectroscopy
Infrared radiation
Proteins
infrared spectra
Molecular structure
proteins
Density functional theory
Enzymes
probes
Ligands
Spectroscopy
Molecules
enzymes
molecular structure
Substrates
analogs

Keywords

  • infrared spectroscopy
  • nicotinamide adenine dinucleotides
  • NAD

Cite this

Simpson, N., Shaw, D. J., Frederix, P. W. J. M., Gillies, A. H., Adamczyk, K., Greetham, G. M., ... Hunt, N. T. (2013). Infrared spectroscopy of nicotinamide adenine dinucleotides in one and two dimensions. Journal of Physical Chemistry B , 117(51), 16468-16478. https://doi.org/10.1021/jp411091f
Simpson, Niall ; Shaw, Daniel J. ; Frederix, Pim W J M ; Gillies, Audrey H. ; Adamczyk, Katrin ; Greetham, Gregory M. ; Towrie, Michael ; Parker, Anthony William ; Hoskisson, Paul A. ; Hunt, Neil T. / Infrared spectroscopy of nicotinamide adenine dinucleotides in one and two dimensions. In: Journal of Physical Chemistry B . 2013 ; Vol. 117, No. 51. pp. 16468-16478.
@article{e1258452a9d2498b8c677822b716f724,
title = "Infrared spectroscopy of nicotinamide adenine dinucleotides in one and two dimensions",
abstract = "The development of multidimensional spectroscopic tools capable of resolving site-specific information about proteins and enzymes in the solution phase is an important aid to our understanding of biomolecular mechanisms, structure, and dynamics. Nicotinamide adenine dinucleotide (NAD) is a common biological substrate and so offers significant potential as an intrinsic vibrational probe of protein-ligand interactions but its complex molecular structure and incompletely characterized infrared spectrum currently limit its usefulness. Here, we report the FTIR spectroscopy of the oxidized and reduced forms of NAD at a range of pD values that relate to the {"}folded{"} and {"}unfolded{"} forms of the molecules that exist in solution. Comparisons with structural analogs and the use of density functional theory simulations provide a full assignment of the observed modes and their complex pD dependencies. Finally, ultrafast two-dimensional infrared spectra of the oxidized and reduced forms of NAD are reported and their usefulness as biomolecular probes is discussed.",
keywords = "infrared spectroscopy, nicotinamide adenine dinucleotides, NAD",
author = "Niall Simpson and Shaw, {Daniel J.} and Frederix, {Pim W J M} and Gillies, {Audrey H.} and Katrin Adamczyk and Greetham, {Gregory M.} and Michael Towrie and Parker, {Anthony William} and Hoskisson, {Paul A.} and Hunt, {Neil T.}",
year = "2013",
month = "12",
day = "27",
doi = "10.1021/jp411091f",
language = "English",
volume = "117",
pages = "16468--16478",
journal = "Journal of Physical Chemistry B",
issn = "1520-6106",
publisher = "American Chemical Society",
number = "51",

}

Simpson, N, Shaw, DJ, Frederix, PWJM, Gillies, AH, Adamczyk, K, Greetham, GM, Towrie, M, Parker, AW, Hoskisson, PA & Hunt, NT 2013, 'Infrared spectroscopy of nicotinamide adenine dinucleotides in one and two dimensions' Journal of Physical Chemistry B , vol. 117, no. 51, pp. 16468-16478. https://doi.org/10.1021/jp411091f

Infrared spectroscopy of nicotinamide adenine dinucleotides in one and two dimensions. / Simpson, Niall; Shaw, Daniel J.; Frederix, Pim W J M; Gillies, Audrey H.; Adamczyk, Katrin; Greetham, Gregory M.; Towrie, Michael; Parker, Anthony William; Hoskisson, Paul A.; Hunt, Neil T.

In: Journal of Physical Chemistry B , Vol. 117, No. 51, 27.12.2013, p. 16468-16478.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Infrared spectroscopy of nicotinamide adenine dinucleotides in one and two dimensions

AU - Simpson, Niall

AU - Shaw, Daniel J.

AU - Frederix, Pim W J M

AU - Gillies, Audrey H.

AU - Adamczyk, Katrin

AU - Greetham, Gregory M.

AU - Towrie, Michael

AU - Parker, Anthony William

AU - Hoskisson, Paul A.

AU - Hunt, Neil T.

PY - 2013/12/27

Y1 - 2013/12/27

N2 - The development of multidimensional spectroscopic tools capable of resolving site-specific information about proteins and enzymes in the solution phase is an important aid to our understanding of biomolecular mechanisms, structure, and dynamics. Nicotinamide adenine dinucleotide (NAD) is a common biological substrate and so offers significant potential as an intrinsic vibrational probe of protein-ligand interactions but its complex molecular structure and incompletely characterized infrared spectrum currently limit its usefulness. Here, we report the FTIR spectroscopy of the oxidized and reduced forms of NAD at a range of pD values that relate to the "folded" and "unfolded" forms of the molecules that exist in solution. Comparisons with structural analogs and the use of density functional theory simulations provide a full assignment of the observed modes and their complex pD dependencies. Finally, ultrafast two-dimensional infrared spectra of the oxidized and reduced forms of NAD are reported and their usefulness as biomolecular probes is discussed.

AB - The development of multidimensional spectroscopic tools capable of resolving site-specific information about proteins and enzymes in the solution phase is an important aid to our understanding of biomolecular mechanisms, structure, and dynamics. Nicotinamide adenine dinucleotide (NAD) is a common biological substrate and so offers significant potential as an intrinsic vibrational probe of protein-ligand interactions but its complex molecular structure and incompletely characterized infrared spectrum currently limit its usefulness. Here, we report the FTIR spectroscopy of the oxidized and reduced forms of NAD at a range of pD values that relate to the "folded" and "unfolded" forms of the molecules that exist in solution. Comparisons with structural analogs and the use of density functional theory simulations provide a full assignment of the observed modes and their complex pD dependencies. Finally, ultrafast two-dimensional infrared spectra of the oxidized and reduced forms of NAD are reported and their usefulness as biomolecular probes is discussed.

KW - infrared spectroscopy

KW - nicotinamide adenine dinucleotides

KW - NAD

UR - http://www.scopus.com/inward/record.url?scp=84891469708&partnerID=8YFLogxK

U2 - 10.1021/jp411091f

DO - 10.1021/jp411091f

M3 - Article

VL - 117

SP - 16468

EP - 16478

JO - Journal of Physical Chemistry B

T2 - Journal of Physical Chemistry B

JF - Journal of Physical Chemistry B

SN - 1520-6106

IS - 51

ER -

Simpson N, Shaw DJ, Frederix PWJM, Gillies AH, Adamczyk K, Greetham GM et al. Infrared spectroscopy of nicotinamide adenine dinucleotides in one and two dimensions. Journal of Physical Chemistry B . 2013 Dec 27;117(51):16468-16478. https://doi.org/10.1021/jp411091f