Abstract

We demonstrate a method to measure a purely absorptive fifth-order three-dimensional (3D) electronic spectrum based on a pulse-shaper assisted pump-probe beam geometry setup. The 3D spectra are measured as a function of two independently controlled population times. With phase-cycling and data processing, purely absorptive 3D spectra of chlorophyll a are obtained.

© 2012 Optical Society of America

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References

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  1. D. M. Jonas, Annu. Rev. Phys. Chem. 54, 425 (2003).
    [CrossRef]
  2. P. Hamm and M. T. Zanni, Concepts and Methods of 2D Infrared Spectroscopy (Cambridge University, 2011).
  3. P. Hamm, J. Chem. Phys. 124, 124506 (2006).
    [CrossRef]
  4. S. Garrett-Roe and P. Hamm, Acc. Chem. Res. 42, 1412 (2009).
    [CrossRef]
  5. F. Ding and M. T. Zanni, Chem. Phys. 341, 95 (2007).
    [CrossRef]
  6. S. Garrett-Roe and P. Hamm, J. Chem. Phys. 130, 164510 (2009).
    [CrossRef]
  7. A. F. Fidler, E. Harel, and G. S. Engel, J. Phys. Chem. Lett. 1, 2876 (2010).
    [CrossRef]
  8. S. H. Shim and M. T. Zanni, Phys. Chem. Chem. Phys. 11, 748 (2009).
    [CrossRef]
  9. J. A. Myers, K. L. M. Lewis, P. F. Tekavec, and J. P. Ogilvie, Opt. Express 16, 17420 (2008).
    [CrossRef]
  10. Z. Zhang, K. L. Wells, E. W. J. Hyland, and H.-S. Tan, Chem. Phys. Lett. 550, 156 (2012).
    [CrossRef]
  11. D. Keusters, H.-S. Tan, and W. S. Warren, J. Phys. Chem. A 103, 10369 (1999).
    [CrossRef]
  12. H.-S. Tan, J. Chem. Phys. 129, 124501 (2008).
    [CrossRef]
  13. K. L. Wells, Z. Zhang, and J. R. Rouxel, Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371, Singapore, and Laboratoire de Nanotechnologie et d’Instrumentation Optique, Université de Technologie de Troyes-Centre National de la Recherche Scientifique (FRE2671), 12 rue Marie Curie, BP 2060, 10010 Troyes Cedex, France, and H.-S. Tan are preparing a manuscript to be called “Measuring the spectral diffusion of chlorophyll a using two-dimensional electronic spectroscopy.”

2012 (1)

Z. Zhang, K. L. Wells, E. W. J. Hyland, and H.-S. Tan, Chem. Phys. Lett. 550, 156 (2012).
[CrossRef]

2010 (1)

A. F. Fidler, E. Harel, and G. S. Engel, J. Phys. Chem. Lett. 1, 2876 (2010).
[CrossRef]

2009 (3)

S. H. Shim and M. T. Zanni, Phys. Chem. Chem. Phys. 11, 748 (2009).
[CrossRef]

S. Garrett-Roe and P. Hamm, Acc. Chem. Res. 42, 1412 (2009).
[CrossRef]

S. Garrett-Roe and P. Hamm, J. Chem. Phys. 130, 164510 (2009).
[CrossRef]

2008 (2)

2007 (1)

F. Ding and M. T. Zanni, Chem. Phys. 341, 95 (2007).
[CrossRef]

2006 (1)

P. Hamm, J. Chem. Phys. 124, 124506 (2006).
[CrossRef]

2003 (1)

D. M. Jonas, Annu. Rev. Phys. Chem. 54, 425 (2003).
[CrossRef]

1999 (1)

D. Keusters, H.-S. Tan, and W. S. Warren, J. Phys. Chem. A 103, 10369 (1999).
[CrossRef]

Ding, F.

F. Ding and M. T. Zanni, Chem. Phys. 341, 95 (2007).
[CrossRef]

Engel, G. S.

A. F. Fidler, E. Harel, and G. S. Engel, J. Phys. Chem. Lett. 1, 2876 (2010).
[CrossRef]

Fidler, A. F.

A. F. Fidler, E. Harel, and G. S. Engel, J. Phys. Chem. Lett. 1, 2876 (2010).
[CrossRef]

Garrett-Roe, S.

S. Garrett-Roe and P. Hamm, Acc. Chem. Res. 42, 1412 (2009).
[CrossRef]

S. Garrett-Roe and P. Hamm, J. Chem. Phys. 130, 164510 (2009).
[CrossRef]

Hamm, P.

S. Garrett-Roe and P. Hamm, J. Chem. Phys. 130, 164510 (2009).
[CrossRef]

S. Garrett-Roe and P. Hamm, Acc. Chem. Res. 42, 1412 (2009).
[CrossRef]

P. Hamm, J. Chem. Phys. 124, 124506 (2006).
[CrossRef]

P. Hamm and M. T. Zanni, Concepts and Methods of 2D Infrared Spectroscopy (Cambridge University, 2011).

Harel, E.

A. F. Fidler, E. Harel, and G. S. Engel, J. Phys. Chem. Lett. 1, 2876 (2010).
[CrossRef]

Hyland, E. W. J.

Z. Zhang, K. L. Wells, E. W. J. Hyland, and H.-S. Tan, Chem. Phys. Lett. 550, 156 (2012).
[CrossRef]

Jonas, D. M.

D. M. Jonas, Annu. Rev. Phys. Chem. 54, 425 (2003).
[CrossRef]

Keusters, D.

D. Keusters, H.-S. Tan, and W. S. Warren, J. Phys. Chem. A 103, 10369 (1999).
[CrossRef]

Lewis, K. L. M.

Myers, J. A.

Ogilvie, J. P.

Rouxel, J. R.

K. L. Wells, Z. Zhang, and J. R. Rouxel, Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371, Singapore, and Laboratoire de Nanotechnologie et d’Instrumentation Optique, Université de Technologie de Troyes-Centre National de la Recherche Scientifique (FRE2671), 12 rue Marie Curie, BP 2060, 10010 Troyes Cedex, France, and H.-S. Tan are preparing a manuscript to be called “Measuring the spectral diffusion of chlorophyll a using two-dimensional electronic spectroscopy.”

Shim, S. H.

S. H. Shim and M. T. Zanni, Phys. Chem. Chem. Phys. 11, 748 (2009).
[CrossRef]

Tan, H.-S.

Z. Zhang, K. L. Wells, E. W. J. Hyland, and H.-S. Tan, Chem. Phys. Lett. 550, 156 (2012).
[CrossRef]

H.-S. Tan, J. Chem. Phys. 129, 124501 (2008).
[CrossRef]

D. Keusters, H.-S. Tan, and W. S. Warren, J. Phys. Chem. A 103, 10369 (1999).
[CrossRef]

K. L. Wells, Z. Zhang, and J. R. Rouxel, Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371, Singapore, and Laboratoire de Nanotechnologie et d’Instrumentation Optique, Université de Technologie de Troyes-Centre National de la Recherche Scientifique (FRE2671), 12 rue Marie Curie, BP 2060, 10010 Troyes Cedex, France, and H.-S. Tan are preparing a manuscript to be called “Measuring the spectral diffusion of chlorophyll a using two-dimensional electronic spectroscopy.”

Tekavec, P. F.

Warren, W. S.

D. Keusters, H.-S. Tan, and W. S. Warren, J. Phys. Chem. A 103, 10369 (1999).
[CrossRef]

Wells, K. L.

Z. Zhang, K. L. Wells, E. W. J. Hyland, and H.-S. Tan, Chem. Phys. Lett. 550, 156 (2012).
[CrossRef]

K. L. Wells, Z. Zhang, and J. R. Rouxel, Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371, Singapore, and Laboratoire de Nanotechnologie et d’Instrumentation Optique, Université de Technologie de Troyes-Centre National de la Recherche Scientifique (FRE2671), 12 rue Marie Curie, BP 2060, 10010 Troyes Cedex, France, and H.-S. Tan are preparing a manuscript to be called “Measuring the spectral diffusion of chlorophyll a using two-dimensional electronic spectroscopy.”

Zanni, M. T.

S. H. Shim and M. T. Zanni, Phys. Chem. Chem. Phys. 11, 748 (2009).
[CrossRef]

F. Ding and M. T. Zanni, Chem. Phys. 341, 95 (2007).
[CrossRef]

P. Hamm and M. T. Zanni, Concepts and Methods of 2D Infrared Spectroscopy (Cambridge University, 2011).

Zhang, Z.

Z. Zhang, K. L. Wells, E. W. J. Hyland, and H.-S. Tan, Chem. Phys. Lett. 550, 156 (2012).
[CrossRef]

K. L. Wells, Z. Zhang, and J. R. Rouxel, Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371, Singapore, and Laboratoire de Nanotechnologie et d’Instrumentation Optique, Université de Technologie de Troyes-Centre National de la Recherche Scientifique (FRE2671), 12 rue Marie Curie, BP 2060, 10010 Troyes Cedex, France, and H.-S. Tan are preparing a manuscript to be called “Measuring the spectral diffusion of chlorophyll a using two-dimensional electronic spectroscopy.”

Acc. Chem. Res. (1)

S. Garrett-Roe and P. Hamm, Acc. Chem. Res. 42, 1412 (2009).
[CrossRef]

Annu. Rev. Phys. Chem. (1)

D. M. Jonas, Annu. Rev. Phys. Chem. 54, 425 (2003).
[CrossRef]

Chem. Phys. (1)

F. Ding and M. T. Zanni, Chem. Phys. 341, 95 (2007).
[CrossRef]

Chem. Phys. Lett. (1)

Z. Zhang, K. L. Wells, E. W. J. Hyland, and H.-S. Tan, Chem. Phys. Lett. 550, 156 (2012).
[CrossRef]

J. Chem. Phys. (3)

S. Garrett-Roe and P. Hamm, J. Chem. Phys. 130, 164510 (2009).
[CrossRef]

H.-S. Tan, J. Chem. Phys. 129, 124501 (2008).
[CrossRef]

P. Hamm, J. Chem. Phys. 124, 124506 (2006).
[CrossRef]

J. Phys. Chem. A (1)

D. Keusters, H.-S. Tan, and W. S. Warren, J. Phys. Chem. A 103, 10369 (1999).
[CrossRef]

J. Phys. Chem. Lett. (1)

A. F. Fidler, E. Harel, and G. S. Engel, J. Phys. Chem. Lett. 1, 2876 (2010).
[CrossRef]

Opt. Express (1)

Phys. Chem. Chem. Phys. (1)

S. H. Shim and M. T. Zanni, Phys. Chem. Chem. Phys. 11, 748 (2009).
[CrossRef]

Other (2)

P. Hamm and M. T. Zanni, Concepts and Methods of 2D Infrared Spectroscopy (Cambridge University, 2011).

K. L. Wells, Z. Zhang, and J. R. Rouxel, Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371, Singapore, and Laboratoire de Nanotechnologie et d’Instrumentation Optique, Université de Technologie de Troyes-Centre National de la Recherche Scientifique (FRE2671), 12 rue Marie Curie, BP 2060, 10010 Troyes Cedex, France, and H.-S. Tan are preparing a manuscript to be called “Measuring the spectral diffusion of chlorophyll a using two-dimensional electronic spectroscopy.”

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Figures (4)

Fig. 1.
Fig. 1.

(a) Pulse sequence for a fifth-order 3D spectroscopy experiment. (b) Double-sided Feynman diagrams of the processes necessary to obtain a purely absorptive 3D spectrum.

Fig. 2.
Fig. 2.

Schematic of the setup for our 2D and 3D optical spectrometer.

Fig. 3.
Fig. 3.

(a) Isosurfaces of a 3D spectrum obtained using a 2×2×2×1 phase-cycling scheme. Positive and negative amplitudes in red and blue, respectively (negative amplitudes enhanced by ×2 for visibility). (b) 3D spectrum containing only purely absorptive peakshapes obtained after data processing of the spectrum in Fig. 3(a).

Fig. 4.
Fig. 4.

Isosurfaces of purely absorptive 3D spectrum of chlorophyll a Qy transition at waiting times (a) t2=200fs and t4=400fs, (b) t2=500fs and t4=1500fs. 2D projections are depicted on the faces of the grid cube.

Equations (2)

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S˜(ϕ14,ϕ24,ϕ34;t1,t3,ω5;t2,t4)αβγs˜(α,β,γ;t1,t3,ω5;t2,t4)exp(+iαϕ14+iβϕ24+iγϕ34),
s˜(t1,t3,ω5)=XXXXX¯XXXXX¯XX+X¯X¯XXXXX¯X+X¯XX¯X+XX¯X¯XX¯X¯X¯X,

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