Abstract

We demonstrate a “drop-in” modification of the pulse-shaped pump-probe geometry two-dimensional Fourier transform spectrometer that significantly improves its performance by making the measurement background-free. The modification uses a hybrid diffractive optic/pulse-shaping approach that combines the advantages of background-free detection with the precise timing and phase-cycling capabilities enabled by pulse-shaping. In addition, we present a simple new method for accurate phasing of optically heterodyned two-dimensional spectra. We demonstrate the high quality of data obtainable with this approach by reporting two-dimensional Fourier transform electronic spectra of chlorophyll a in glycerol/water at 77 K.

© 2014 Optical Society of America

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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef]
  25. J. M. Anna, E. E. Ostroumov, K. Maghlaoui, J. Barber, G. D. Scholes, “Two-dimensional electronic spectroscopy reveals ultrafast downhill energy transfer in photosystem I trimers of the cyanobacterium Thermosynechococcus elongatus,” J. Phys. Chem. Lett. 3(24), 3677–3684 (2012).
    [CrossRef]
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    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef] [PubMed]
  35. Z. Y. Zhang, K. L. Wells, E. W. J. Hyland, H. S. Tan, “Phase-cycling schemes for pump-probe beam geometry two-dimensional electronic spectroscopy,” Chem. Phys. Lett. 550, 156–161 (2012).
    [CrossRef]
  36. S. H. Shim, M. T. Zanni, “How to turn your pump-probe instrument into a multidimensional spectrometer: 2D IR and Vis spectroscopies via pulse shaping,” Phys. Chem. Chem. Phys. 11(5), 748–761 (2009).
    [CrossRef] [PubMed]
  37. D. Keusters, H. S. Tan, W. S. Warren, “Role of pulse phase and direction in two-dimensional optical spectroscopy,” J. Phys. Chem. A 103(49), 10369–10380 (1999).
    [CrossRef]
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    [CrossRef]
  41. J. P. Ogilvie, M. Plazanet, G. Dadusc, R. J. D. Miller, “Dynamics of ligand escape in myoglobin: Q-band transient absorption and four-wave mixing studies,” J. Phys. Chem. B 106(40), 10460–10467 (2002).
    [CrossRef]
  42. V. P. Singh, A. F. Fidler, B. S. Rolczynski, G. S. Engel, “Independent phasing of rephasing and non-rephasing 2D electronic spectra,” J. Chem. Phys. 139(8), 084201 (2013).
    [CrossRef] [PubMed]

2013

P. Tyagi, J. I. Saari, B. Walsh, A. Kabir, V. Crozatier, N. Forget, P. Kambhampati, “Two-color two-dimensional electronic spectroscopy using dual acousto-optic pulse shapers for complete amplitude, phase, and polarization control of femtosecond laser pulses,” J. Phys. Chem. A 117(29), 6264–6269 (2013).
[CrossRef] [PubMed]

W. Rock, Y. L. Li, P. Pagano, C. M. Cheatum, “2D IR spectroscopy using four-wave mixing, pulse shaping, and IR upconversion: a quantitative comparison,” J. Phys. Chem. A 117(29), 6073–6083 (2013).
[CrossRef] [PubMed]

V. P. Singh, A. F. Fidler, B. S. Rolczynski, G. S. Engel, “Independent phasing of rephasing and non-rephasing 2D electronic spectra,” J. Chem. Phys. 139(8), 084201 (2013).
[CrossRef] [PubMed]

F. Milota, C. N. Lincoln, J. Hauer, “Precise phasing of 2D-electronic spectra in a fully non-collinear phase-matching geometry,” Opt. Express 21(13), 15904–15911 (2013).
[CrossRef] [PubMed]

D. E. Wilcox, F. D. Fuller, J. P. Ogilvie, “Fast second-harmonic generation frequency-resolved optical gating using only a pulse shaper,” Opt. Lett. 38(16), 2980–2983 (2013).
[CrossRef] [PubMed]

2012

Z. Y. Zhang, K. L. Wells, E. W. J. Hyland, H. S. Tan, “Phase-cycling schemes for pump-probe beam geometry two-dimensional electronic spectroscopy,” Chem. Phys. Lett. 550, 156–161 (2012).
[CrossRef]

J. M. Anna, E. E. Ostroumov, K. Maghlaoui, J. Barber, G. D. Scholes, “Two-dimensional electronic spectroscopy reveals ultrafast downhill energy transfer in photosystem I trimers of the cyanobacterium Thermosynechococcus elongatus,” J. Phys. Chem. Lett. 3(24), 3677–3684 (2012).
[CrossRef]

K. L. M. Lewis, J. P. Ogilvie, “Probing photosynthetic energy and charge transfer with two-dimensional electronic spectroscopy,” J. Phys. Chem. Lett. 3(4), 503–510 (2012).
[CrossRef]

2011

2010

P. F. Tekavec, J. A. Myers, K. L. M. Lewis, F. D. Fuller, J. P. Ogilvie, “Effects of chirp on two-dimensional Fourier transform electronic spectra,” Opt. Express 18(11), 11015–11024 (2010).
[CrossRef] [PubMed]

N. Christensson, F. Milota, A. Nemeth, I. Pugliesi, E. Riedle, J. Sperling, T. Pullerits, H. F. Kauffmann, J. Hauer, “Electronic double-quantum coherences and their impact on ultrafast spectroscopy: the example of β-carotene,” J. Phys. Chem. Lett. 1(23), 3366–3370 (2010).
[CrossRef] [PubMed]

E. Harel, A. F. Fidler, G. S. Engel, “Real-time mapping of electronic structure with single-shot two-dimensional electronic spectroscopy,” Proc. Natl. Acad. Sci. U. S. A. 107(38), 16444–16447 (2010).
[CrossRef] [PubMed]

2009

S. H. Shim, M. T. Zanni, “How to turn your pump-probe instrument into a multidimensional spectrometer: 2D IR and Vis spectroscopies via pulse shaping,” Phys. Chem. Chem. Phys. 11(5), 748–761 (2009).
[CrossRef] [PubMed]

V. I. Prokhorenko, A. Halpin, R. J. D. Miller, “Coherently-controlled two-dimensional photon echo electronic spectroscopy,” Opt. Express 17(12), 9764–9779 (2009).
[CrossRef] [PubMed]

A. Nemeth, J. Sperling, J. Hauer, H. F. Kauffmann, F. Milota, “Compact phase-stable design for single- and double-quantum two-dimensional electronic spectroscopy,” Opt. Lett. 34(21), 3301–3303 (2009).
[CrossRef] [PubMed]

K. W. Stone, D. B. Turner, K. Gundogdu, S. T. Cundiff, K. A. Nelson, “Exciton-exciton correlations revealed by two-quantum, two-dimensional Fourier transform optical spectroscopy,” Acc. Chem. Res. 42(9), 1452–1461 (2009).
[CrossRef] [PubMed]

K. W. Stone, K. Gundogdu, D. B. Turner, X. Q. Li, S. T. Cundiff, K. A. Nelson, “Two-quantum 2D FT electronic spectroscopy of biexcitons in GaAs quantum wells,” Science 324(5931), 1169–1173 (2009).
[CrossRef] [PubMed]

2008

2007

E. M. Grumstrup, S. H. Shim, M. A. Montgomery, N. H. Damrauer, M. T. Zanni, “Facile collection of two-dimensional electronic spectra using femtosecond pulse-shaping technology,” Opt. Express 15(25), 16681–16689 (2007).
[CrossRef] [PubMed]

E. L. Read, G. S. Engel, T. R. Calhoun, T. Mancal, T. K. Ahn, R. E. Blankenship, G. R. Fleming, “Cross-peak-specific two-dimensional electronic spectroscopy,” Proc. Natl. Acad. Sci. U. S. A. 104(36), 14203–14208 (2007).
[CrossRef] [PubMed]

S. H. Shim, D. B. Strasfeld, Y. L. Ling, M. T. Zanni, “Automated 2D IR spectroscopy using a mid-IR pulse shaper and application of this technology to the human islet amyloid polypeptide,” Proc. Natl. Acad. Sci. U. S. A. 104(36), 14197–14202 (2007).
[CrossRef] [PubMed]

J. C. Vaughan, T. Hornung, K. W. Stone, K. A. Nelson, “Coherently controlled ultrafast four-wave mixing spectroscopy,” J. Phys. Chem. A 111(23), 4873–4883 (2007).
[CrossRef] [PubMed]

P. F. Tekavec, G. A. Lott, A. H. Marcus, “Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation,” J. Chem. Phys. 127(21), 214307 (2007).
[CrossRef] [PubMed]

2005

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, G. R. Fleming, “Two-dimensional spectroscopy of electronic couplings in photosynthesis,” Nature 434(7033), 625–628 (2005).
[CrossRef] [PubMed]

2004

M. L. Cowan, J. P. Ogilvie, R. J. D. Miller, “Two-dimensional spectroscopy using diffractive optics based phased-locked photon echoes,” Chem. Phys. Lett. 386(1-3), 184–189 (2004).
[CrossRef]

T. Brixner, T. Mancal, I. V. Stiopkin, G. R. Fleming, “Phase-stabilized two-dimensional electronic spectroscopy,” J. Chem. Phys. 121(9), 4221–4236 (2004).
[CrossRef] [PubMed]

2003

D. M. Jonas, “Two-dimensional femtosecond spectroscopy,” Annu. Rev. Phys. Chem. 54(1), 425–463 (2003).
[CrossRef] [PubMed]

P. F. Tian, D. Keusters, Y. Suzaki, W. S. Warren, “Femtosecond phase-coherent two-dimensional spectroscopy,” Science 300(5625), 1553–1555 (2003).
[CrossRef] [PubMed]

2002

J. D. Hybl, A. Yu, D. A. Farrow, D. M. Jonas, “Polar solvation dynamics in the femtosecond evolution of two-dimensional Fourier transform spectra,” J. Phys. Chem. A 106(34), 7651–7654 (2002).
[CrossRef]

J. P. Ogilvie, M. Plazanet, G. Dadusc, R. J. D. Miller, “Dynamics of ligand escape in myoglobin: Q-band transient absorption and four-wave mixing studies,” J. Phys. Chem. B 106(40), 10460–10467 (2002).
[CrossRef]

2000

A. M. Weiner, “Femtosecond pulse shaping using spatial light modulators,” Rev. Sci. Instrum. 71(5), 1929–1960 (2000).
[CrossRef]

1999

S. M. G. Faeder, D. M. Jonas, “Two-dimensional electronic correlation and relaxation spectra: Theory and model calculations,” J. Phys. Chem. A 103(49), 10489–10505 (1999).
[CrossRef]

D. Keusters, H. S. Tan, W. S. Warren, “Role of pulse phase and direction in two-dimensional optical spectroscopy,” J. Phys. Chem. A 103(49), 10369–10380 (1999).
[CrossRef]

1998

G. D. Goodno, G. Dadusc, R. J. D. Miller, “Ultrafast heterodyne-detected transient-grating spectroscopy using diffractive optics,” J. Opt. Soc. Am. B 15(6), 1791–1794 (1998).
[CrossRef]

J. D. Hybl, A. W. Albrecht, S. M. G. Faeder, D. M. Jonas, “Two-dimensional electronic spectroscopy,” Chem. Phys. Lett. 297(3-4), 307–313 (1998).
[CrossRef]

1997

1995

1994

1979

M. D. Levenson, G. L. Eesley, “Polarization selective optical heterodyne-detection for dramatically improved sensitivity in laser spectroscopy,” Appl. Phys. 19(1), 1–17 (1979).
[CrossRef]

Ahn, T. K.

E. L. Read, G. S. Engel, T. R. Calhoun, T. Mancal, T. K. Ahn, R. E. Blankenship, G. R. Fleming, “Cross-peak-specific two-dimensional electronic spectroscopy,” Proc. Natl. Acad. Sci. U. S. A. 104(36), 14203–14208 (2007).
[CrossRef] [PubMed]

Albrecht, A. W.

J. D. Hybl, A. W. Albrecht, S. M. G. Faeder, D. M. Jonas, “Two-dimensional electronic spectroscopy,” Chem. Phys. Lett. 297(3-4), 307–313 (1998).
[CrossRef]

Anna, J. M.

J. M. Anna, E. E. Ostroumov, K. Maghlaoui, J. Barber, G. D. Scholes, “Two-dimensional electronic spectroscopy reveals ultrafast downhill energy transfer in photosystem I trimers of the cyanobacterium Thermosynechococcus elongatus,” J. Phys. Chem. Lett. 3(24), 3677–3684 (2012).
[CrossRef]

Augulis, R.

Barber, J.

J. M. Anna, E. E. Ostroumov, K. Maghlaoui, J. Barber, G. D. Scholes, “Two-dimensional electronic spectroscopy reveals ultrafast downhill energy transfer in photosystem I trimers of the cyanobacterium Thermosynechococcus elongatus,” J. Phys. Chem. Lett. 3(24), 3677–3684 (2012).
[CrossRef]

Blankenship, R. E.

E. L. Read, G. S. Engel, T. R. Calhoun, T. Mancal, T. K. Ahn, R. E. Blankenship, G. R. Fleming, “Cross-peak-specific two-dimensional electronic spectroscopy,” Proc. Natl. Acad. Sci. U. S. A. 104(36), 14203–14208 (2007).
[CrossRef] [PubMed]

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, G. R. Fleming, “Two-dimensional spectroscopy of electronic couplings in photosynthesis,” Nature 434(7033), 625–628 (2005).
[CrossRef] [PubMed]

Brixner, T.

U. Selig, F. Langhojer, F. Dimler, T. Löhrig, C. Schwarz, B. Gieseking, T. Brixner, “Inherently phase-stable coherent two-dimensional spectroscopy using only conventional optics,” Opt. Lett. 33(23), 2851–2853 (2008).
[CrossRef] [PubMed]

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, G. R. Fleming, “Two-dimensional spectroscopy of electronic couplings in photosynthesis,” Nature 434(7033), 625–628 (2005).
[CrossRef] [PubMed]

T. Brixner, T. Mancal, I. V. Stiopkin, G. R. Fleming, “Phase-stabilized two-dimensional electronic spectroscopy,” J. Chem. Phys. 121(9), 4221–4236 (2004).
[CrossRef] [PubMed]

Calhoun, T. R.

E. L. Read, G. S. Engel, T. R. Calhoun, T. Mancal, T. K. Ahn, R. E. Blankenship, G. R. Fleming, “Cross-peak-specific two-dimensional electronic spectroscopy,” Proc. Natl. Acad. Sci. U. S. A. 104(36), 14203–14208 (2007).
[CrossRef] [PubMed]

Cheatum, C. M.

W. Rock, Y. L. Li, P. Pagano, C. M. Cheatum, “2D IR spectroscopy using four-wave mixing, pulse shaping, and IR upconversion: a quantitative comparison,” J. Phys. Chem. A 117(29), 6073–6083 (2013).
[CrossRef] [PubMed]

Cheriaux, G.

Cho, M.

T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, G. R. Fleming, “Two-dimensional spectroscopy of electronic couplings in photosynthesis,” Nature 434(7033), 625–628 (2005).
[CrossRef] [PubMed]

Christensson, N.

N. Christensson, F. Milota, A. Nemeth, I. Pugliesi, E. Riedle, J. Sperling, T. Pullerits, H. F. Kauffmann, J. Hauer, “Electronic double-quantum coherences and their impact on ultrafast spectroscopy: the example of β-carotene,” J. Phys. Chem. Lett. 1(23), 3366–3370 (2010).
[CrossRef] [PubMed]

Cowan, M. L.

M. L. Cowan, J. P. Ogilvie, R. J. D. Miller, “Two-dimensional spectroscopy using diffractive optics based phased-locked photon echoes,” Chem. Phys. Lett. 386(1-3), 184–189 (2004).
[CrossRef]

Crozatier, V.

P. Tyagi, J. I. Saari, B. Walsh, A. Kabir, V. Crozatier, N. Forget, P. Kambhampati, “Two-color two-dimensional electronic spectroscopy using dual acousto-optic pulse shapers for complete amplitude, phase, and polarization control of femtosecond laser pulses,” J. Phys. Chem. A 117(29), 6264–6269 (2013).
[CrossRef] [PubMed]

Cundiff, S. T.

K. W. Stone, D. B. Turner, K. Gundogdu, S. T. Cundiff, K. A. Nelson, “Exciton-exciton correlations revealed by two-quantum, two-dimensional Fourier transform optical spectroscopy,” Acc. Chem. Res. 42(9), 1452–1461 (2009).
[CrossRef] [PubMed]

K. W. Stone, K. Gundogdu, D. B. Turner, X. Q. Li, S. T. Cundiff, K. A. Nelson, “Two-quantum 2D FT electronic spectroscopy of biexcitons in GaAs quantum wells,” Science 324(5931), 1169–1173 (2009).
[CrossRef] [PubMed]

Dadusc, G.

J. P. Ogilvie, M. Plazanet, G. Dadusc, R. J. D. Miller, “Dynamics of ligand escape in myoglobin: Q-band transient absorption and four-wave mixing studies,” J. Phys. Chem. B 106(40), 10460–10467 (2002).
[CrossRef]

G. D. Goodno, G. Dadusc, R. J. D. Miller, “Ultrafast heterodyne-detected transient-grating spectroscopy using diffractive optics,” J. Opt. Soc. Am. B 15(6), 1791–1794 (1998).
[CrossRef]

Damrauer, N. H.

Dimler, F.

Eesley, G. L.

M. D. Levenson, G. L. Eesley, “Polarization selective optical heterodyne-detection for dramatically improved sensitivity in laser spectroscopy,” Appl. Phys. 19(1), 1–17 (1979).
[CrossRef]

Engel, G. S.

V. P. Singh, A. F. Fidler, B. S. Rolczynski, G. S. Engel, “Independent phasing of rephasing and non-rephasing 2D electronic spectra,” J. Chem. Phys. 139(8), 084201 (2013).
[CrossRef] [PubMed]

E. Harel, A. F. Fidler, G. S. Engel, “Real-time mapping of electronic structure with single-shot two-dimensional electronic spectroscopy,” Proc. Natl. Acad. Sci. U. S. A. 107(38), 16444–16447 (2010).
[CrossRef] [PubMed]

E. L. Read, G. S. Engel, T. R. Calhoun, T. Mancal, T. K. Ahn, R. E. Blankenship, G. R. Fleming, “Cross-peak-specific two-dimensional electronic spectroscopy,” Proc. Natl. Acad. Sci. U. S. A. 104(36), 14203–14208 (2007).
[CrossRef] [PubMed]

Faeder, S. M. G.

S. M. G. Faeder, D. M. Jonas, “Two-dimensional electronic correlation and relaxation spectra: Theory and model calculations,” J. Phys. Chem. A 103(49), 10489–10505 (1999).
[CrossRef]

J. D. Hybl, A. W. Albrecht, S. M. G. Faeder, D. M. Jonas, “Two-dimensional electronic spectroscopy,” Chem. Phys. Lett. 297(3-4), 307–313 (1998).
[CrossRef]

Farrow, D. A.

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