R E V I E W
Ultrafast structural molecular dynamics investigated
with 2D infrared spectroscopy methods
Jan Philip Kraack
1
Received: 31 March 2017 / Accepted: 2 October 2017 / Published online: 25 October 2017
Ó Springer International Publishing AG 2017
Abstract Ultrafast, multi-dimensional infrared (IR) spectroscopy has been
advanced in recent years to a versatile analytical tool with a broad range of
applications to elucidate molecular structure on ultrafast timescales, and it can be
used for samples in a many different environments. Following a short and general
introduction on the benefits of 2D IR spectroscopy, the first part of this chapter contains a brief discussion on basic descriptions and conceptual considerations
of 2D IR spectroscopy. Outstanding classical applications of 2D IR are used
afterwards to highlight the strengths and basic applicability of the method. This
includes the identification of vibrational coupling in molecules, characterization of
spectral diffusion dynamics, chemical exchange of chemical bond formation and
breaking, as well as dynamics of intra- and intermolecular energy transfer for
molecules in bulk solution and thin films. In the second part, several important,
recently developed variants and new applications of 2D IR spectroscopy are
introduced. These methods focus on (i) applications to molecules under two- and
three-dimensional confinement, (ii) the combination of 2D IR with electrochemistry, (iii) ultrafast 2D IR in conjunction with diffraction-limited microscopy, (iv)
several variants of non-equilibrium 2D IR spectroscopy such as transient 2D IR and
3D IR, and (v) extensions of the pump and probe spectral regions for multi-dimensional vibrational spectroscopy towards mixed vibrational-electronic spectroscopies. In light of these examples, the important open scientific and conceptual
questions with regard to intra- and intermolecular dynamics are highlighted. Such
& Jan Philip Kraack
philip.kraack@chem.uzh.ch
1
Department of Chemistry, University of Zu ¨rich, Winterthurerstrasse 190, 8057 Zurich,
Switzerland
123
Top Curr Chem (Z) (2017) 375:86
https://doi.org/10.1007/s41061-017-0172-1
113
Reprinted from the journal
Chapter 4 was originally published as Kraack, J. P. Top Curr Chem (Z) (2017) 375: 86. https://doi.org/
10.1007/s41061-017-0172-1.
Ultrafast structural molecular dynamics investigated
with 2D infrared spectroscopy methods
Jan Philip Kraack
1
Received: 31 March 2017 / Accepted: 2 October 2017 / Published online: 25 October 2017
Ó Springer International Publishing AG 2017
Abstract Ultrafast, multi-dimensional infrared (IR) spectroscopy has been
advanced in recent years to a versatile analytical tool with a broad range of
applications to elucidate molecular structure on ultrafast timescales, and it can be
used for samples in a many different environments. Following a short and general
introduction on the benefits of 2D IR spectroscopy, the first part of this chapter contains a brief discussion on basic descriptions and conceptual considerations
of 2D IR spectroscopy. Outstanding classical applications of 2D IR are used
afterwards to highlight the strengths and basic applicability of the method. This
includes the identification of vibrational coupling in molecules, characterization of
spectral diffusion dynamics, chemical exchange of chemical bond formation and
breaking, as well as dynamics of intra- and intermolecular energy transfer for
molecules in bulk solution and thin films. In the second part, several important,
recently developed variants and new applications of 2D IR spectroscopy are
introduced. These methods focus on (i) applications to molecules under two- and
three-dimensional confinement, (ii) the combination of 2D IR with electrochemistry, (iii) ultrafast 2D IR in conjunction with diffraction-limited microscopy, (iv)
several variants of non-equilibrium 2D IR spectroscopy such as transient 2D IR and
3D IR, and (v) extensions of the pump and probe spectral regions for multi-dimensional vibrational spectroscopy towards mixed vibrational-electronic spectroscopies. In light of these examples, the important open scientific and conceptual
questions with regard to intra- and intermolecular dynamics are highlighted. Such
& Jan Philip Kraack
philip.kraack@chem.uzh.ch
1
Department of Chemistry, University of Zu ¨rich, Winterthurerstrasse 190, 8057 Zurich,
Switzerland
123
Top Curr Chem (Z) (2017) 375:86
https://doi.org/10.1007/s41061-017-0172-1
113
Reprinted from the journal
Chapter 4 was originally published as Kraack, J. P. Top Curr Chem (Z) (2017) 375: 86. https://doi.org/
10.1007/s41061-017-0172-1.