Top Curr Chem (Z) (2018) 376:6
https://doi.org/10.1007/s41061-018-0185-4
1 3
REVIEW
Two‑Dimensional Spectroscopy at Terahertz
Frequencies
Jian Lu
1
 · Xian Li
1
 · Yaqing Zhang
1
 · Harold Y. Hwang
1
 ·
Benjamin K. Ofori‑Okai
1
 · Keith A. Nelson
1
Received: 31 August 2017 / Accepted: 5 January 2018 / Published online: 23 January 2018
© Springer International Publishing AG, part of Springer Nature 2018
Abstract Multidimensional spectroscopy in the visible and infrared spectral
ranges has become a powerful technique to retrieve dynamic correlations and couplings in wide-ranging systems by utilizing multiple correlated light-matter interactions. Its extension to the terahertz (THz) regime of the electromagnetic spectrum, where rich material degrees of freedom reside, however, has been progressing
slowly. This chapter reviews some of the THz-frequency two-dimensional (2D)
spectroscopy techniques and experimental results realized in recent years. Examples include gas molecule rotations, spin precessions in magnetic systems, and liquid molecular dynamics studied by 2D THz or hybrid 2D THz-Raman spectroscopy
techniques. The methodology shows promising applications to different THz-frequency degrees of freedom in various chemical systems and processes.
Keywords Terahertz · Gas-phase molecular rotations · Liquid-phase molecular
dynamics · Magnetic resonances
1 Introduction
Recent years have witnessed increasing interest in two-dimensional spectroscopy
in many regions of the  electromagnetic spectrum. Two-dimensional infrared (2D
IR) vibrational spectroscopy [1–4] is a powerful technique for studying structural
dynamics and correlations between coupled molecular motions in chemical and
* Keith A. Nelson
kanelson@mit.edu
1
Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
275
Reprinted from the journal
Chapter 7 was originally published as Lu, J., Li, X., Zhang, Y., Hwang, H. Y., Ofori-Okai, B. K. &
Nelson, K. A. Top Curr Chem (Z) (2018) 376: 6. https://doi.org/10.1007/s41061-018-0185-4.
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