Top Curr Chem (Z) (2018) 376:6
1 3
THz detection methods [77] could drastically reduce the long data acquisition times
that presently hinder virtually all 2D THz measurements. As in other frequency
ranges including radio, microwave, infrared, and visible, multidimensional spectroscopy in the THz regime can reveal otherwise elusive structure, interactions, and
dynamics. With further advances in the relevant technologies and refinements of the
measurement methodology, 2D THz spectroscopy can be expected to take its place
among the multidimensional spectroscopies that have produced broad and deep
advances in all areas of chemistry.
Acknowledgements We thank Sharly Fleischer, Takayuki Kurihara, and Tohru Suemoto for contributions to this work. This work was supported, in part, by Office of Naval Research Grant N00014-13-10509 and Defense University Research Instrumentation Program Grant N00014-15-1-2879, National Science Foundation Grants CHE-1111557 and CHE-1665383, and the Samsung Global Research Outreach
program.
References
1. Hamm P, Zanni MT (2011) Concepts and methods of 2D infrared spectroscopy. Cambridge University Press, Cambridge
2. Mukamel S (2000) Multidimensional femtosecond correlation spectroscopies of electronic and
vibrational excitations. Annu Rev Phys Chem 51:691–729. http s://doi.org/10.1146 /annu rev.phys
chem .51.1.691
3. Jonas DM (2003) Two-dimensional femtosecond spectroscopy. Annu Rev Phys Chem 54:425–463.
http s://doi.org/10.1146 /annu rev.phys chem .54.0110 02.1039 07
4. Zheng J, Kwak K, Fayer MD (2007) Ultrafast 2D IR vibrational echo spectroscopy. Acc Chem Res
40:75–83. http s://doi.org/10.1021 /ar06 8010 d
5. Ramasesha K, De Marco L, Mandal A, Tokmakoff A (2013) Water vibrations have strongly mixed
intra- and intermolecular character. Nat Chem 5:935–940. http s://doi.org/10.1038 /nche m.1757
6. Baiz CR, Reppert M, Tokmakoff A (2013) Amide I two-dimensional infrared spectroscopy: methods for visualizing the vibrational structure of large proteins. J Phys Chem A 117:5955–5961. http
s://doi.org/10.1021 /jp31 0689 a
7. Krummel AT, Mukherjee P, Zanni MT (2003) Inter and intrastrand vibrational coupling in DNA
studied with heterodyned 2D-IR spectroscopy. J Phys Chem B 107:9165–9169. http s://doi.
org/10.1021 /JP03 5473 H
8. Fuller FD, Ogilvie JP (2015) Experimental implementations of two-dimensional Fourier transform
electronic spectroscopy. Annu Rev Phys Chem 66:667–690. http s://doi.org/10.1146 /annu rev-phys
chem -0405 13-1036 23
9. Stone KW, Gundogdu K, Turner DB et al (2009) Two-quantum 2D FT electronic spectroscopy
of biexcitons in GaAs quantum wells. Science (80-) 324:1169–1173. http s://doi.org/10.1126 /scie
nce.1170 274
10. Turner DB, Nelson KA (2010) Coherent measurements of high-order electronic correlations in
quantum wells. Nature 466:1089–1092. http s://doi.org/10.1038 /natu re09 286
11. Brixner T, Stenger J, Vaswani HM et al (2005) Two-dimensional spectroscopy of electronic couplings in photosynthesis. Nature 434:625–628. http s://doi.org/10.1038 /natu re03 429
12. Cheng Y-C, Fleming GR (2009) Dynamics of light harvesting in photosynthesis. Annu Rev Phys
Chem 60:241–262. http s://doi.org/10.1146 /annu rev.phys chem .0408 08.0902 59
13. Eisele DM, Arias DH, Fu X et al (2014) Robust excitons inhabit soft supramolecular nanotubes.
Proc Natl Acad Sci 111:E3367–E3375. http s://doi.org/10.1073 /pnas .1408 3421 11
14. Krebs N, Pugliesi I, Hauer J, Riedle E (2013) Two-dimensional Fourier transform spectroscopy
in the ultraviolet with sub-20 fs pump pulses and 250–720 nm supercontinuum probe. New J Phys
15:85016. http s://doi.org/10.1088 /1367 -2630 /15/8/0850 16
15. Lee Y-S (2009) Principles of terahertz science and technology. Springer, Berlin
316
Reprinted from the journal
1 3
THz detection methods [77] could drastically reduce the long data acquisition times
that presently hinder virtually all 2D THz measurements. As in other frequency
ranges including radio, microwave, infrared, and visible, multidimensional spectroscopy in the THz regime can reveal otherwise elusive structure, interactions, and
dynamics. With further advances in the relevant technologies and refinements of the
measurement methodology, 2D THz spectroscopy can be expected to take its place
among the multidimensional spectroscopies that have produced broad and deep
advances in all areas of chemistry.
Acknowledgements We thank Sharly Fleischer, Takayuki Kurihara, and Tohru Suemoto for contributions to this work. This work was supported, in part, by Office of Naval Research Grant N00014-13-10509 and Defense University Research Instrumentation Program Grant N00014-15-1-2879, National Science Foundation Grants CHE-1111557 and CHE-1665383, and the Samsung Global Research Outreach
program.
References
1. Hamm P, Zanni MT (2011) Concepts and methods of 2D infrared spectroscopy. Cambridge University Press, Cambridge
2. Mukamel S (2000) Multidimensional femtosecond correlation spectroscopies of electronic and
vibrational excitations. Annu Rev Phys Chem 51:691–729. http s://doi.org/10.1146 /annu rev.phys
chem .51.1.691
3. Jonas DM (2003) Two-dimensional femtosecond spectroscopy. Annu Rev Phys Chem 54:425–463.
http s://doi.org/10.1146 /annu rev.phys chem .54.0110 02.1039 07
4. Zheng J, Kwak K, Fayer MD (2007) Ultrafast 2D IR vibrational echo spectroscopy. Acc Chem Res
40:75–83. http s://doi.org/10.1021 /ar06 8010 d
5. Ramasesha K, De Marco L, Mandal A, Tokmakoff A (2013) Water vibrations have strongly mixed
intra- and intermolecular character. Nat Chem 5:935–940. http s://doi.org/10.1038 /nche m.1757
6. Baiz CR, Reppert M, Tokmakoff A (2013) Amide I two-dimensional infrared spectroscopy: methods for visualizing the vibrational structure of large proteins. J Phys Chem A 117:5955–5961. http
s://doi.org/10.1021 /jp31 0689 a
7. Krummel AT, Mukherjee P, Zanni MT (2003) Inter and intrastrand vibrational coupling in DNA
studied with heterodyned 2D-IR spectroscopy. J Phys Chem B 107:9165–9169. http s://doi.
org/10.1021 /JP03 5473 H
8. Fuller FD, Ogilvie JP (2015) Experimental implementations of two-dimensional Fourier transform
electronic spectroscopy. Annu Rev Phys Chem 66:667–690. http s://doi.org/10.1146 /annu rev-phys
chem -0405 13-1036 23
9. Stone KW, Gundogdu K, Turner DB et al (2009) Two-quantum 2D FT electronic spectroscopy
of biexcitons in GaAs quantum wells. Science (80-) 324:1169–1173. http s://doi.org/10.1126 /scie
nce.1170 274
10. Turner DB, Nelson KA (2010) Coherent measurements of high-order electronic correlations in
quantum wells. Nature 466:1089–1092. http s://doi.org/10.1038 /natu re09 286
11. Brixner T, Stenger J, Vaswani HM et al (2005) Two-dimensional spectroscopy of electronic couplings in photosynthesis. Nature 434:625–628. http s://doi.org/10.1038 /natu re03 429
12. Cheng Y-C, Fleming GR (2009) Dynamics of light harvesting in photosynthesis. Annu Rev Phys
Chem 60:241–262. http s://doi.org/10.1146 /annu rev.phys chem .0408 08.0902 59
13. Eisele DM, Arias DH, Fu X et al (2014) Robust excitons inhabit soft supramolecular nanotubes.
Proc Natl Acad Sci 111:E3367–E3375. http s://doi.org/10.1073 /pnas .1408 3421 11
14. Krebs N, Pugliesi I, Hauer J, Riedle E (2013) Two-dimensional Fourier transform spectroscopy
in the ultraviolet with sub-20 fs pump pulses and 250–720 nm supercontinuum probe. New J Phys
15:85016. http s://doi.org/10.1088 /1367 -2630 /15/8/0850 16
15. Lee Y-S (2009) Principles of terahertz science and technology. Springer, Berlin
316
Reprinted from the journal