Abstract

This letter reports a straightforward means of collecting two-dimensional electronic (2D-E) spectra using optical tools common to many research groups involved in ultrafast spectroscopy and quantum control. In our method a femtosecond pulse shaper is used to generate a pair of phase stable collinear laser pulses which are then incident on a gas or liquid sample. The pulse pair is followed by an ultrashort probe pulse that is spectrally resolved. The delay between the collinear pulses is incremented using phase and amplitude shaping and a 2D-E spectrum is generated following Fourier transformation. The partially collinear beam geometry results in perfectly phased absorptive spectra without phase twist. Our approach is much simpler to implement than standard non-collinear beam geometries, which are challenging to phase stabilize and require complicated calibrations. Using pulse shaping, many new experiments are now also possible in both 2D-E spectroscopy and coherent control.

© 2007 Optical Society of America

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2007

"Multidimensional Ultrafast Spectroscopy Special Feature," Proc. Natl. Acad. Sci. USA 104, 14189-14544 (2007).
[PubMed]

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

S.-H. Shim, D. B. Strasfeld, Y. L. Ling, and 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. USA 104, 14197-14202 (2007).
[CrossRef] [PubMed]

P. F. Tekavec, G. A. Lott, and A. H. Marcus, "Flourescence-Detected Two-Dimensional Electronic Coherence Spectroscopy by Acousto-Optic Phase Modulation," J. Chem. Phys., Submitted (2007).
[CrossRef] [PubMed]

M. A. Montgomery, and N. H. Damrauer, "Elucidation of control mechanisms discovered during adaptive manipulation of [Ru(dpb)3](PF6)2 emission in the solution phase," J. Phys. Chem. A 111, 1426-1433 (2007).
[CrossRef] [PubMed]

M. A. Montgomery, R. R. Meglen, and N. H. Damrauer, "General method for reducing adaptive laser pulse-shaping experiments to a single control variable," J. Phys. Chem. A 111, 5126-5129 (2007).
[CrossRef] [PubMed]

2006

J. C. Vaughan, T. Feurer, K. W. Stone, and K. A. Nelson, "Analysis of replica pulses in femtosecond pulse shaping with pixelated devices," Opt. Express 14, 1314-1328 (2006).
[CrossRef] [PubMed]

M. A. Montgomery, R. R. Meglen, and N. H. Damrauer, "General method for the dimension reduction of adaptive control experiments," J. Phys. Chem. A 110, 6391-6394 (2006).
[CrossRef] [PubMed]

E. B. W. Lerch, X. C. Dai, S. Gilb, E. A. Torres, and S. R. Leone, "Control of Li2 wave packet dynamics by modification of the quantum mechanical amplitude of a single state," J. Chem. Phys. 124 (2006).
[CrossRef] [PubMed]

F. Ding, P. Mukherjee, and M. T. Zanni, "Passively correcting phase drift in two-dimensional infrared spectroscopy," Opt. Lett. 31, 2918-2920 (2006).
[CrossRef] [PubMed]

2005

2004

E. C. Fulmer, P. Mukherjee, A. T. Krummel, and M. T. Zanni, "A pulse sequence for directly measuring the anharmonicities of coupled vibrations: Two-quantum two-dimensional infrared spectroscopy," J. Chem. Phys. 120, 8067-8078 (2004).
[CrossRef] [PubMed]

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

J. B. Asbury, T. Steinel, and M. D. Fayer, "Vibrational echo correlation spectroscopy probes of hydrogen bond dynamics in water and methanol," J. Lumin. 107, 271-286 (2004).
[CrossRef] [PubMed]

2003

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

T. Brixner, N. H. Damrauer, B. Kiefer, and G. Gerber, "Liquid-phase adaptive femtosecond quantum control: Removing intrinsic intensity dependencies," J. Chem. Phys. 118, 3692-3701 (2003).
[CrossRef]

2001

M. Khalil, and A. Tokmakoff, "Signatures of vibrational interactions in coherent two-dimensional infrared spectroscopy," Chem. Phys. 266, 213-230 (2001).
[CrossRef]

C. Scheurer and S. Mukamel, "Design strategies for pulse sequences in multidimensional optical spectroscopies," J. Chem. Phys. 115, 4989-5004 (2001).
[CrossRef]

"Special Issue on Multidimensional Spectroscopies," Chem. Phys. 266, 135-352 (2001).

1999

T. Weinacht, J. Ahn, and P. Bucksbaum, "Controlling the shape of a quantum wavefunction," Nature 397, 233-235 (1999).
[CrossRef]

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

W. M. Zhang, V. Chernyak, and S. Mukamel, "Multidimensional femtosecond correlation spectroscopies of electronic and vibrational excitons," J. Chem. Phys. 110, 5011-5028 (1999).
[CrossRef]

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

1998

T. C. Weinacht, J. Ahn, and P. H. Bucksbaum, "Measurement of the amplitude and phase of a sculpted Rydberg wave packet," Phys. Rev. Lett. 80, 5508-5511 (1998).
[CrossRef]

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

1997

1995

H. Kawashima, M. M. Wefers, and K. A. Nelson, "Femtosecond Pulse Shaping, Multiple-Pulse Spectroscopy, and Optical Control," Annu. Rev. Phys. Chem. 46, 627-656 (1995).
[CrossRef]

1992

R. S. Judson and H. Rabitz, "Teaching lasers to control molecules," Phys. Rev. Lett. 68, 1500-1503 (1992).
[CrossRef] [PubMed]

Ahn, J.

T. Weinacht, J. Ahn, and P. Bucksbaum, "Controlling the shape of a quantum wavefunction," Nature 397, 233-235 (1999).
[CrossRef]

T. C. Weinacht, J. Ahn, and P. H. Bucksbaum, "Measurement of the amplitude and phase of a sculpted Rydberg wave packet," Phys. Rev. Lett. 80, 5508-5511 (1998).
[CrossRef]

Asbury, J. B.

J. B. Asbury, T. Steinel, and M. D. Fayer, "Vibrational echo correlation spectroscopy probes of hydrogen bond dynamics in water and methanol," J. Lumin. 107, 271-286 (2004).
[CrossRef] [PubMed]

Borca, C. N.

Brixner, T.

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

T. Brixner, N. H. Damrauer, B. Kiefer, and G. Gerber, "Liquid-phase adaptive femtosecond quantum control: Removing intrinsic intensity dependencies," J. Chem. Phys. 118, 3692-3701 (2003).
[CrossRef]

Bucksbaum, P.

T. Weinacht, J. Ahn, and P. Bucksbaum, "Controlling the shape of a quantum wavefunction," Nature 397, 233-235 (1999).
[CrossRef]

Bucksbaum, P. H.

T. C. Weinacht, J. Ahn, and P. H. Bucksbaum, "Measurement of the amplitude and phase of a sculpted Rydberg wave packet," Phys. Rev. Lett. 80, 5508-5511 (1998).
[CrossRef]

Chernyak, V.

W. M. Zhang, V. Chernyak, and S. Mukamel, "Multidimensional femtosecond correlation spectroscopies of electronic and vibrational excitons," J. Chem. Phys. 110, 5011-5028 (1999).
[CrossRef]

Cundiff, S. T.

Dadusc, G.

Dai, X. C.

E. B. W. Lerch, X. C. Dai, S. Gilb, E. A. Torres, and S. R. Leone, "Control of Li2 wave packet dynamics by modification of the quantum mechanical amplitude of a single state," J. Chem. Phys. 124 (2006).
[CrossRef] [PubMed]

Damrauer, N. H.

M. A. Montgomery, and N. H. Damrauer, "Elucidation of control mechanisms discovered during adaptive manipulation of [Ru(dpb)3](PF6)2 emission in the solution phase," J. Phys. Chem. A 111, 1426-1433 (2007).
[CrossRef] [PubMed]

M. A. Montgomery, R. R. Meglen, and N. H. Damrauer, "General method for reducing adaptive laser pulse-shaping experiments to a single control variable," J. Phys. Chem. A 111, 5126-5129 (2007).
[CrossRef] [PubMed]

M. A. Montgomery, R. R. Meglen, and N. H. Damrauer, "General method for the dimension reduction of adaptive control experiments," J. Phys. Chem. A 110, 6391-6394 (2006).
[CrossRef] [PubMed]

T. Brixner, N. H. Damrauer, B. Kiefer, and G. Gerber, "Liquid-phase adaptive femtosecond quantum control: Removing intrinsic intensity dependencies," J. Chem. Phys. 118, 3692-3701 (2003).
[CrossRef]

Ding, F.

F. Ding, P. Mukherjee, and M. T. Zanni, "Passively correcting phase drift in two-dimensional infrared spectroscopy," Opt. Lett. 31, 2918-2920 (2006).
[CrossRef] [PubMed]

E. C. Fulmer, F. Ding, P. Mukherjee, and M. T. Zanni, "Vibrational dynamics of ions in glass from fifth-order two-dimensional infrared spectroscopy," Phys. Rev. Lett. 94,067402 (2005).
[CrossRef] [PubMed]

Dugan, M. A.

Faeder, S. M. G.

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

Fayer, M. D.

J. B. Asbury, T. Steinel, and M. D. Fayer, "Vibrational echo correlation spectroscopy probes of hydrogen bond dynamics in water and methanol," J. Lumin. 107, 271-286 (2004).
[CrossRef] [PubMed]

Feurer, T.

Fleming, G. R.

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

Fulmer, E. C.

E. C. Fulmer, F. Ding, P. Mukherjee, and M. T. Zanni, "Vibrational dynamics of ions in glass from fifth-order two-dimensional infrared spectroscopy," Phys. Rev. Lett. 94,067402 (2005).
[CrossRef] [PubMed]

E. C. Fulmer, P. Mukherjee, A. T. Krummel, and M. T. Zanni, "A pulse sequence for directly measuring the anharmonicities of coupled vibrations: Two-quantum two-dimensional infrared spectroscopy," J. Chem. Phys. 120, 8067-8078 (2004).
[CrossRef] [PubMed]

Gerber, G.

T. Brixner, N. H. Damrauer, B. Kiefer, and G. Gerber, "Liquid-phase adaptive femtosecond quantum control: Removing intrinsic intensity dependencies," J. Chem. Phys. 118, 3692-3701 (2003).
[CrossRef]

Gilb, S.

E. B. W. Lerch, X. C. Dai, S. Gilb, E. A. Torres, and S. R. Leone, "Control of Li2 wave packet dynamics by modification of the quantum mechanical amplitude of a single state," J. Chem. Phys. 124 (2006).
[CrossRef] [PubMed]

Goodno, G. D.

Hamm, P.

Hornung, T.

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

Jonas, D. M.

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

Judson, R. S.

R. S. Judson and H. Rabitz, "Teaching lasers to control molecules," Phys. Rev. Lett. 68, 1500-1503 (1992).
[CrossRef] [PubMed]

Kawashima, H.

H. Kawashima, M. M. Wefers, and K. A. Nelson, "Femtosecond Pulse Shaping, Multiple-Pulse Spectroscopy, and Optical Control," Annu. Rev. Phys. Chem. 46, 627-656 (1995).
[CrossRef]

Keusters, D.

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

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

Khalil, M.

M. Khalil, and A. Tokmakoff, "Signatures of vibrational interactions in coherent two-dimensional infrared spectroscopy," Chem. Phys. 266, 213-230 (2001).
[CrossRef]

Kiefer, B.

T. Brixner, N. H. Damrauer, B. Kiefer, and G. Gerber, "Liquid-phase adaptive femtosecond quantum control: Removing intrinsic intensity dependencies," J. Chem. Phys. 118, 3692-3701 (2003).
[CrossRef]

Krummel, A. T.

E. C. Fulmer, P. Mukherjee, A. T. Krummel, and M. T. Zanni, "A pulse sequence for directly measuring the anharmonicities of coupled vibrations: Two-quantum two-dimensional infrared spectroscopy," J. Chem. Phys. 120, 8067-8078 (2004).
[CrossRef] [PubMed]

Leone, S. R.

E. B. W. Lerch, X. C. Dai, S. Gilb, E. A. Torres, and S. R. Leone, "Control of Li2 wave packet dynamics by modification of the quantum mechanical amplitude of a single state," J. Chem. Phys. 124 (2006).
[CrossRef] [PubMed]

Lerch, E. B. W.

E. B. W. Lerch, X. C. Dai, S. Gilb, E. A. Torres, and S. R. Leone, "Control of Li2 wave packet dynamics by modification of the quantum mechanical amplitude of a single state," J. Chem. Phys. 124 (2006).
[CrossRef] [PubMed]

Li, X. Q.

Ling, Y. L.

S.-H. Shim, D. B. Strasfeld, Y. L. Ling, and 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. USA 104, 14197-14202 (2007).
[CrossRef] [PubMed]

Lott, G. A.

P. F. Tekavec, G. A. Lott, and A. H. Marcus, "Flourescence-Detected Two-Dimensional Electronic Coherence Spectroscopy by Acousto-Optic Phase Modulation," J. Chem. Phys., Submitted (2007).
[CrossRef] [PubMed]

Mancal, T.

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

Marcus, A. H.

P. F. Tekavec, G. A. Lott, and A. H. Marcus, "Flourescence-Detected Two-Dimensional Electronic Coherence Spectroscopy by Acousto-Optic Phase Modulation," J. Chem. Phys., Submitted (2007).
[CrossRef] [PubMed]

Meglen, R. R.

M. A. Montgomery, R. R. Meglen, and N. H. Damrauer, "General method for reducing adaptive laser pulse-shaping experiments to a single control variable," J. Phys. Chem. A 111, 5126-5129 (2007).
[CrossRef] [PubMed]

M. A. Montgomery, R. R. Meglen, and N. H. Damrauer, "General method for the dimension reduction of adaptive control experiments," J. Phys. Chem. A 110, 6391-6394 (2006).
[CrossRef] [PubMed]

Miller, R. J. D.

Montgomery, M. A.

M. A. Montgomery, R. R. Meglen, and N. H. Damrauer, "General method for reducing adaptive laser pulse-shaping experiments to a single control variable," J. Phys. Chem. A 111, 5126-5129 (2007).
[CrossRef] [PubMed]

M. A. Montgomery, and N. H. Damrauer, "Elucidation of control mechanisms discovered during adaptive manipulation of [Ru(dpb)3](PF6)2 emission in the solution phase," J. Phys. Chem. A 111, 1426-1433 (2007).
[CrossRef] [PubMed]

M. A. Montgomery, R. R. Meglen, and N. H. Damrauer, "General method for the dimension reduction of adaptive control experiments," J. Phys. Chem. A 110, 6391-6394 (2006).
[CrossRef] [PubMed]

Mukamel, S.

C. Scheurer and S. Mukamel, "Design strategies for pulse sequences in multidimensional optical spectroscopies," J. Chem. Phys. 115, 4989-5004 (2001).
[CrossRef]

W. M. Zhang, V. Chernyak, and S. Mukamel, "Multidimensional femtosecond correlation spectroscopies of electronic and vibrational excitons," J. Chem. Phys. 110, 5011-5028 (1999).
[CrossRef]

Mukherjee, P.

F. Ding, P. Mukherjee, and M. T. Zanni, "Passively correcting phase drift in two-dimensional infrared spectroscopy," Opt. Lett. 31, 2918-2920 (2006).
[CrossRef] [PubMed]

E. C. Fulmer, F. Ding, P. Mukherjee, and M. T. Zanni, "Vibrational dynamics of ions in glass from fifth-order two-dimensional infrared spectroscopy," Phys. Rev. Lett. 94,067402 (2005).
[CrossRef] [PubMed]

E. C. Fulmer, P. Mukherjee, A. T. Krummel, and M. T. Zanni, "A pulse sequence for directly measuring the anharmonicities of coupled vibrations: Two-quantum two-dimensional infrared spectroscopy," J. Chem. Phys. 120, 8067-8078 (2004).
[CrossRef] [PubMed]

Nelson, K. A.

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

J. C. Vaughan, T. Feurer, K. W. Stone, and K. A. Nelson, "Analysis of replica pulses in femtosecond pulse shaping with pixelated devices," Opt. Express 14, 1314-1328 (2006).
[CrossRef] [PubMed]

H. Kawashima, M. M. Wefers, and K. A. Nelson, "Femtosecond Pulse Shaping, Multiple-Pulse Spectroscopy, and Optical Control," Annu. Rev. Phys. Chem. 46, 627-656 (1995).
[CrossRef]

Rabitz, H.

R. S. Judson and H. Rabitz, "Teaching lasers to control molecules," Phys. Rev. Lett. 68, 1500-1503 (1992).
[CrossRef] [PubMed]

Schanz, R.

Scheurer, C.

C. Scheurer and S. Mukamel, "Design strategies for pulse sequences in multidimensional optical spectroscopies," J. Chem. Phys. 115, 4989-5004 (2001).
[CrossRef]

Shim, S.-H.

S.-H. Shim, D. B. Strasfeld, Y. L. Ling, and 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. USA 104, 14197-14202 (2007).
[CrossRef] [PubMed]

Steinel, T.

J. B. Asbury, T. Steinel, and M. D. Fayer, "Vibrational echo correlation spectroscopy probes of hydrogen bond dynamics in water and methanol," J. Lumin. 107, 271-286 (2004).
[CrossRef] [PubMed]

Stiopkin, I. V.

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

Stone, K. W.

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

J. C. Vaughan, T. Feurer, K. W. Stone, and K. A. Nelson, "Analysis of replica pulses in femtosecond pulse shaping with pixelated devices," Opt. Express 14, 1314-1328 (2006).
[CrossRef] [PubMed]

Strasfeld, D. B.

S.-H. Shim, D. B. Strasfeld, Y. L. Ling, and 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. USA 104, 14197-14202 (2007).
[CrossRef] [PubMed]

Suzaki, Y.

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

Tan, H. S.

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

Tekavec, P. F.

P. F. Tekavec, G. A. Lott, and A. H. Marcus, "Flourescence-Detected Two-Dimensional Electronic Coherence Spectroscopy by Acousto-Optic Phase Modulation," J. Chem. Phys., Submitted (2007).
[CrossRef] [PubMed]

Tian, P. F.

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

Tokmakoff, A.

M. Khalil, and A. Tokmakoff, "Signatures of vibrational interactions in coherent two-dimensional infrared spectroscopy," Chem. Phys. 266, 213-230 (2001).
[CrossRef]

Torres, E. A.

E. B. W. Lerch, X. C. Dai, S. Gilb, E. A. Torres, and S. R. Leone, "Control of Li2 wave packet dynamics by modification of the quantum mechanical amplitude of a single state," J. Chem. Phys. 124 (2006).
[CrossRef] [PubMed]

Tull, J. X.

Vaughan, J. C.

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

J. C. Vaughan, T. Feurer, K. W. Stone, and K. A. Nelson, "Analysis of replica pulses in femtosecond pulse shaping with pixelated devices," Opt. Express 14, 1314-1328 (2006).
[CrossRef] [PubMed]

Volkov, V.

Warren, W. S.

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

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

M. A. Dugan, J. X. Tull, and W. S. Warren, "High-resolution acousto-optic shaping of unamplified and amplified femtosecond laser pulses," J. Opt. Soc. Am. B 14, 2348-2358 (1997).
[CrossRef]

Wefers, M. M.

H. Kawashima, M. M. Wefers, and K. A. Nelson, "Femtosecond Pulse Shaping, Multiple-Pulse Spectroscopy, and Optical Control," Annu. Rev. Phys. Chem. 46, 627-656 (1995).
[CrossRef]

Weinacht, T.

T. Weinacht, J. Ahn, and P. Bucksbaum, "Controlling the shape of a quantum wavefunction," Nature 397, 233-235 (1999).
[CrossRef]

Weinacht, T. C.

T. C. Weinacht, J. Ahn, and P. H. Bucksbaum, "Measurement of the amplitude and phase of a sculpted Rydberg wave packet," Phys. Rev. Lett. 80, 5508-5511 (1998).
[CrossRef]

Zanni, M. T.

S.-H. Shim, D. B. Strasfeld, Y. L. Ling, and 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. USA 104, 14197-14202 (2007).
[CrossRef] [PubMed]

F. Ding, P. Mukherjee, and M. T. Zanni, "Passively correcting phase drift in two-dimensional infrared spectroscopy," Opt. Lett. 31, 2918-2920 (2006).
[CrossRef] [PubMed]

E. C. Fulmer, F. Ding, P. Mukherjee, and M. T. Zanni, "Vibrational dynamics of ions in glass from fifth-order two-dimensional infrared spectroscopy," Phys. Rev. Lett. 94,067402 (2005).
[CrossRef] [PubMed]

E. C. Fulmer, P. Mukherjee, A. T. Krummel, and M. T. Zanni, "A pulse sequence for directly measuring the anharmonicities of coupled vibrations: Two-quantum two-dimensional infrared spectroscopy," J. Chem. Phys. 120, 8067-8078 (2004).
[CrossRef] [PubMed]

Zhang, T. H.

Zhang, W. M.

W. M. Zhang, V. Chernyak, and S. Mukamel, "Multidimensional femtosecond correlation spectroscopies of electronic and vibrational excitons," J. Chem. Phys. 110, 5011-5028 (1999).
[CrossRef]

Annu. Rev. Phys. Chem.

H. Kawashima, M. M. Wefers, and K. A. Nelson, "Femtosecond Pulse Shaping, Multiple-Pulse Spectroscopy, and Optical Control," Annu. Rev. Phys. Chem. 46, 627-656 (1995).
[CrossRef]

Chem. Phys.

"Special Issue on Multidimensional Spectroscopies," Chem. Phys. 266, 135-352 (2001).

M. Khalil, and A. Tokmakoff, "Signatures of vibrational interactions in coherent two-dimensional infrared spectroscopy," Chem. Phys. 266, 213-230 (2001).
[CrossRef]

J. Chem. Phys.

C. Scheurer and S. Mukamel, "Design strategies for pulse sequences in multidimensional optical spectroscopies," J. Chem. Phys. 115, 4989-5004 (2001).
[CrossRef]

P. F. Tekavec, G. A. Lott, and A. H. Marcus, "Flourescence-Detected Two-Dimensional Electronic Coherence Spectroscopy by Acousto-Optic Phase Modulation," J. Chem. Phys., Submitted (2007).
[CrossRef] [PubMed]

E. C. Fulmer, P. Mukherjee, A. T. Krummel, and M. T. Zanni, "A pulse sequence for directly measuring the anharmonicities of coupled vibrations: Two-quantum two-dimensional infrared spectroscopy," J. Chem. Phys. 120, 8067-8078 (2004).
[CrossRef] [PubMed]

W. M. Zhang, V. Chernyak, and S. Mukamel, "Multidimensional femtosecond correlation spectroscopies of electronic and vibrational excitons," J. Chem. Phys. 110, 5011-5028 (1999).
[CrossRef]

T. Brixner, N. H. Damrauer, B. Kiefer, and G. Gerber, "Liquid-phase adaptive femtosecond quantum control: Removing intrinsic intensity dependencies," J. Chem. Phys. 118, 3692-3701 (2003).
[CrossRef]

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

E. B. W. Lerch, X. C. Dai, S. Gilb, E. A. Torres, and S. R. Leone, "Control of Li2 wave packet dynamics by modification of the quantum mechanical amplitude of a single state," J. Chem. Phys. 124 (2006).
[CrossRef] [PubMed]

J. Lumin.

J. B. Asbury, T. Steinel, and M. D. Fayer, "Vibrational echo correlation spectroscopy probes of hydrogen bond dynamics in water and methanol," J. Lumin. 107, 271-286 (2004).
[CrossRef] [PubMed]

J. Opt. Soc. Am. B

J. Phys. Chem. A

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

M. A. Montgomery, and N. H. Damrauer, "Elucidation of control mechanisms discovered during adaptive manipulation of [Ru(dpb)3](PF6)2 emission in the solution phase," J. Phys. Chem. A 111, 1426-1433 (2007).
[CrossRef] [PubMed]

M. A. Montgomery, R. R. Meglen, and N. H. Damrauer, "General method for reducing adaptive laser pulse-shaping experiments to a single control variable," J. Phys. Chem. A 111, 5126-5129 (2007).
[CrossRef] [PubMed]

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

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

M. A. Montgomery, R. R. Meglen, and N. H. Damrauer, "General method for the dimension reduction of adaptive control experiments," J. Phys. Chem. A 110, 6391-6394 (2006).
[CrossRef] [PubMed]

Nature

T. Weinacht, J. Ahn, and P. Bucksbaum, "Controlling the shape of a quantum wavefunction," Nature 397, 233-235 (1999).
[CrossRef]

Opt. Express

Opt. Lett.

Phys. Rev. Lett.

T. C. Weinacht, J. Ahn, and P. H. Bucksbaum, "Measurement of the amplitude and phase of a sculpted Rydberg wave packet," Phys. Rev. Lett. 80, 5508-5511 (1998).
[CrossRef]

E. C. Fulmer, F. Ding, P. Mukherjee, and M. T. Zanni, "Vibrational dynamics of ions in glass from fifth-order two-dimensional infrared spectroscopy," Phys. Rev. Lett. 94,067402 (2005).
[CrossRef] [PubMed]

R. S. Judson and H. Rabitz, "Teaching lasers to control molecules," Phys. Rev. Lett. 68, 1500-1503 (1992).
[CrossRef] [PubMed]

Proc. Natl. Acad. Sci. USA

"Multidimensional Ultrafast Spectroscopy Special Feature," Proc. Natl. Acad. Sci. USA 104, 14189-14544 (2007).
[PubMed]

S.-H. Shim, D. B. Strasfeld, Y. L. Ling, and 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. USA 104, 14197-14202 (2007).
[CrossRef] [PubMed]

Science

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

Other

S. A. Rice and M. Zhao, Optical Control of MolecularDdynamics. (Wiley, New York, 2000).

T. Brixner, N. H. Damrauer, and G. Gerber, "Femtosecond quantum control," in Advances in Atomic, Molecular, and Optical Physics, Vol 46(2001), pp. 1-54.
[CrossRef]

R. Trebino, Frequency-Resolved Optical Gating (Kluwer Avademic Publishers, Norwell, MA, 2000).

S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford University Press, New York, 1995).

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Figures (5)

Fig. 1.
Fig. 1.

Methods for collecting 2D spectra. kn are the wavevectors (directions) of the excitation pulses and ks is the wavevector of the emitted signal. (a) An entirely collinear pulse sequence in which fluorescence is collected orthogonally to the beam path. (b) A boxcar type of geometry in which all four beams propagate at different angles. (c) The partially collinear geometry employed here in which two “pump” pulses are followed by an off axis “probe” pulse which is then spectrally resolved.

Fig. 2.
Fig. 2.

Time domain data collected at λprobe=780 nm and t2=1.0 ps. Fast oscillations of the signal (see inset) are superimposed on slow modulation of transient absorption signal.

Fig. 3.
Fig. 3.

(color) (a) 2D spectrum of Rb vapor. (b) Detail of the peak at λpumpprobe=780 nm.

Fig. 4.
Fig. 4.

Phase stability as measured over 35 hours by repeatedly scanning the signal from t1=200-220 fs. Phase drift was measured to be λ/67.

Fig. 5.
Fig. 5.

(a). Simulated pulse pair (t1=4 ps) produced with a perfect shaper. (b). Pulse pair produced with simulated gaps, but otherwise continuous shaping ability. Arrows point to small pulses caused by gaps. (c). Spurious pulses produced as a result of mask pixilation. The double arrow points to a spurious peak that interferes with the signal for t1>2 ps.

Equations (3)

Equations on this page are rendered with MathJax. Learn more.

S ( t 1 , t 2 , ω probe ) = n ( R n ( t 1 , t 2 , t 3 ) E 1 E 2 E probe + E probe ) e i ω probe t dt 2
S ( ω pump , t 2 , ω probe ) = S ( t 1 , t 2 , ω probe ) e i ω pump t 1 dt 1
R n ( t 1 , t 2 , t 3 ) = R n rephase ( t 1 , t 2 , t 3 ) + R n nonrephase ( t 1 , t 2 , t 3 ) + R n two-quantum ( t 1 , t 2 , t 3 )

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