Abstract

We use multiphoton quantum-control spectroscopy to discriminate between unbound and enzyme-bound NADH (reduced nicotinamide adenine dinucleotide) molecules in solution. Shaped ultrafast laser pulses are used to illuminate both forms of NADH, and the ratio of the fluorescence from the bound and unbound molecules for different pulse shapes allows us to measure binding without spectrally resolving the emitted fluorescence or relying on the absolute fluorescence yield. This permits determination of enzyme binding in situations where spectrally resolved measurements and absolute fluorescence yields are difficult to obtain, and makes the approach ideal for multiphoton microscopy with molecular discrimination.

© 2011 OSA

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2010 (1)

2009 (6)

A. C. W. van Rhijn, S. Postma, J. P. Korterik, J. L. Herek, and H. L. Offerhaus, “Chemically selective imaging by spectral phase shaping for broadband CARS around 3000 cm−1,” J. Opt. Soc. Am. B 26, 559–563 (2009).
[CrossRef]

R. S. Pillai, C. Boudoux, G. Labroille, N. Olivier, I. Veilleux, E. Farge, M. Joffre, and E. Beaurepaire, “Multiplexed two-photon microscopy of dynamic biological samples with shaped broadband pulses,” Opt. Express 17, 12741–12752 (2009).
[CrossRef] [PubMed]

M. Roth, L. Guyon, J. Roslund, V. Boutou, F. Courvoisier, J.-P. Wolf, and H. Rabitz, “Quantum control of tightly competitive product channels,” Phys. Rev. Lett. 102, 253001 (2009).
[CrossRef] [PubMed]

T. Weinacht, “Distinguishing between molecules that look the same,” Physics 2, 51 (2009).
[CrossRef]

S. D. Clow, U. C. Hölscher, and T. C. Weinacht, “Achieving “perfect” molecular discrimination via coherent control and stimulated emission,” New J. Phys. 11, 115007 (2009).
[CrossRef]

Y. Silberberg, “Quantum coherent control for nonlinear spectroscopy and microscopy,” Ann. Rev. Phys. Chem. 60, 277–292 (2009).
[CrossRef]

2008 (2)

X. G. Xu, S. O. Konorov, J. W. Hepburn, and V. Milner, “Noise autocorrelation spectroscopy with coherent Raman scattering,” Nature Phys. 4, 125–129 (2008).
[CrossRef]

B. von Vacano and M. Motzkus, “Time-resolving molecular vibration for microanalytics: single laser beam nonlinear Raman spectroscopy in simulation and experiment,” Phys. Chem. Chem. Phys. 10, 681–691 (2008).
[CrossRef] [PubMed]

2007 (3)

B. von Vacano and M. Motzkus, “Molecular discrimination of a mixture with single-beam Raman control,” J. Chem. Phys. 127, 144514 (2007).
[CrossRef] [PubMed]

A. Gandman, L. Chuntonov, L. Rybak, and Z. Amitay, “Coherent phase control of resonance-mediated (2 + 1) three-photon absorption,” Phys. Rev. A 75, 031401 (2007).
[CrossRef]

C. Trallero-Herrero and T. C. Weinacht, “Transition from weak- to strong-field coherent control,” Phys. Rev. A 75, 063401 (2007).
[CrossRef]

2006 (2)

J. M. D. Cruz, V. V. Lozovoy, and M. Dantus, “Coherent control improves biomedical imaging with ultrashort shaped pulses,” J. Photochem. Photobio. A 180, 307 – 313 (2006).
[CrossRef]

J. P. Ogilvie, D. Débarre, X. Solinas, J.-L. Martin, E. Beaurepaire, and M. Joffre, “Use of coherent control for selective two-photon fluorescence microscopy in live organisms,” Opt. Express 14, 759–766 (2006).
[CrossRef] [PubMed]

2005 (2)

H. D. Vishwasrao, A. A. Heikal, K. A. Kasischke, and W. W. Webb, “Conformational dependence of intracellular NADH on metabolic state revealed by associated fluorescence anisotropy,” J. Bio. Chem. 280, 25119–25126 (2005).
[CrossRef]

W. Wohlleben, T. Buckup, J. L. Herek, and M. Motzkus, “Coherent control for spectroscopy and manipulation of biological dynamics,” ChemPhysChem 6, 850–857 (2005).
[CrossRef] [PubMed]

2004 (2)

J.-X. Cheng and X. S. Xie, “Coherent anti-Stokes Raman scattering microscopy: Instrumentation, theory, and applications,” J. Phys. Chem. B 108, 827–840 (2004).
[CrossRef]

K. A. Kasischke, H. D. Vishwasrao, P. J. Fisher, W. R. Zipfel, and W. W. Webb, “Neural activity triggers neuronal oxidative metabolism followed by astrocytic glycolysis,” Science 305, 99–103 (2004).
[CrossRef] [PubMed]

2003 (3)

I. Pastirk, J. M. D. Cruz, K. A. Walowicz, V. V. Lozovoy, and M. Dantus, “Selective two-photon microscopy with shaped femtosecond pulses,” Opt. Express 11, 1695–1701 (2003).
[CrossRef] [PubMed]

T. Brixner and G. Gerber, “Quantum control of gas-phase and liquid-phase femtochemistry,” ChemPhysChem 4, 418–438 (2003).
[CrossRef] [PubMed]

W. R. Zipfel, R. M. Williams, and W. W. Webb, “Nonlinear magic: multiphoton microscopy in the biosciences,” Nature Biotech. 21, 1369–1377 (2003).
[CrossRef]

2002 (2)

N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy,” Nature 418, 512–514 (2002).
[CrossRef] [PubMed]

K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, “Multiphoton intrapulse interference. 1. Control of multiphoton processes in condensed phases,” J. Phys. Chem. A 106, 9369–9373 (2002).
[CrossRef]

2001 (1)

T. Brixner, N. H. Damrauer, P. Niklaus, and G. Gerber, “Photoselective adaptive femtosecond quantum control in the liquid phase,” Nature 414, 57–60 (2001).
[CrossRef] [PubMed]

2000 (2)

H. Rabitz, R. de Vivie-Riedle, M. Motzkus, and K. Kompa, “Whither the future of controlling quantum phenomena?” Science 288, 824–828 (2000).
[CrossRef] [PubMed]

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

1999 (1)

D. Meshulach and Y. Silberberg, “Coherent quantum control of multiphoton transitions by shaped ultrashort optical pulses,” Phys. Rev. A 60, 1287–1292 (1999).
[CrossRef]

1997 (2)

R. Trebino, K. W. DeLong, D. N. Fittinghoff, J. N. Sweetser, M. A. Krumbugel, B. A. Richman, and D. J. Kane, “Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating,” Rev. Sci. Inst. 68, 3277–3295 (1997).
[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]

1992 (1)

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

1990 (1)

W. Denk, J. Strickler, and W. W. Webb, “Two-photon laser scanning fluorescence microscopy,” Science 248, 73–76 (1990).
[CrossRef] [PubMed]

1986 (2)

P. Brumer and M. Shapiro, “Control of unimolecular reactions using coherent light,” Chem. Phys. Lett. 126, 541–546 (1986).
[CrossRef]

D. J. Tannor, R. Kosloff, and S. A. Rice, “Control pulse sequence induced control of selectivity of reactions: Exact quantum mechanical calculations,” J. Chem. Phys. 85, 5805–5820 (1986).
[CrossRef]

1972 (1)

J. J. Holbrook and R. G. Wolfe, “Malate dehydrogenase. X. fluorescence microtitration studies of d-malate, hydroxymalonate, nicotinamide dinucleotide, and dihydronicotinamide-adenine dinucleotide binding by mitochondrial and supernatant porcine heart enzymes,” Biochemistry 11, 2499 (1972).
[CrossRef] [PubMed]

Amitay, Z.

A. Gandman, L. Chuntonov, L. Rybak, and Z. Amitay, “Coherent phase control of resonance-mediated (2 + 1) three-photon absorption,” Phys. Rev. A 75, 031401 (2007).
[CrossRef]

Beaurepaire, E.

Boudoux, C.

Boutou, V.

M. Roth, L. Guyon, J. Roslund, V. Boutou, F. Courvoisier, J.-P. Wolf, and H. Rabitz, “Quantum control of tightly competitive product channels,” Phys. Rev. Lett. 102, 253001 (2009).
[CrossRef] [PubMed]

Brixner, T.

T. Brixner and G. Gerber, “Quantum control of gas-phase and liquid-phase femtochemistry,” ChemPhysChem 4, 418–438 (2003).
[CrossRef] [PubMed]

T. Brixner, N. H. Damrauer, P. Niklaus, and G. Gerber, “Photoselective adaptive femtosecond quantum control in the liquid phase,” Nature 414, 57–60 (2001).
[CrossRef] [PubMed]

Brumer, P.

P. Brumer and M. Shapiro, “Control of unimolecular reactions using coherent light,” Chem. Phys. Lett. 126, 541–546 (1986).
[CrossRef]

Buckup, T.

J. Rehbinder, C. Pohling, T. Buckup, and M. Motzkus, “Multiplex coherent anti-Stokes Raman microspectroscopy with tailored Stokes spectrum,” Opt. Lett. 35, 3721–3723 (2010).
[CrossRef] [PubMed]

W. Wohlleben, T. Buckup, J. L. Herek, and M. Motzkus, “Coherent control for spectroscopy and manipulation of biological dynamics,” ChemPhysChem 6, 850–857 (2005).
[CrossRef] [PubMed]

Cheng, J.-X.

J.-X. Cheng and X. S. Xie, “Coherent anti-Stokes Raman scattering microscopy: Instrumentation, theory, and applications,” J. Phys. Chem. B 108, 827–840 (2004).
[CrossRef]

Chuntonov, L.

A. Gandman, L. Chuntonov, L. Rybak, and Z. Amitay, “Coherent phase control of resonance-mediated (2 + 1) three-photon absorption,” Phys. Rev. A 75, 031401 (2007).
[CrossRef]

Clow, S. D.

S. D. Clow, U. C. Hölscher, and T. C. Weinacht, “Achieving “perfect” molecular discrimination via coherent control and stimulated emission,” New J. Phys. 11, 115007 (2009).
[CrossRef]

Courvoisier, F.

M. Roth, L. Guyon, J. Roslund, V. Boutou, F. Courvoisier, J.-P. Wolf, and H. Rabitz, “Quantum control of tightly competitive product channels,” Phys. Rev. Lett. 102, 253001 (2009).
[CrossRef] [PubMed]

Cruz, J. M. D.

J. M. D. Cruz, V. V. Lozovoy, and M. Dantus, “Coherent control improves biomedical imaging with ultrashort shaped pulses,” J. Photochem. Photobio. A 180, 307 – 313 (2006).
[CrossRef]

I. Pastirk, J. M. D. Cruz, K. A. Walowicz, V. V. Lozovoy, and M. Dantus, “Selective two-photon microscopy with shaped femtosecond pulses,” Opt. Express 11, 1695–1701 (2003).
[CrossRef] [PubMed]

Damrauer, N. H.

T. Brixner, N. H. Damrauer, P. Niklaus, and G. Gerber, “Photoselective adaptive femtosecond quantum control in the liquid phase,” Nature 414, 57–60 (2001).
[CrossRef] [PubMed]

Dantus, M.

J. M. D. Cruz, V. V. Lozovoy, and M. Dantus, “Coherent control improves biomedical imaging with ultrashort shaped pulses,” J. Photochem. Photobio. A 180, 307 – 313 (2006).
[CrossRef]

I. Pastirk, J. M. D. Cruz, K. A. Walowicz, V. V. Lozovoy, and M. Dantus, “Selective two-photon microscopy with shaped femtosecond pulses,” Opt. Express 11, 1695–1701 (2003).
[CrossRef] [PubMed]

K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, “Multiphoton intrapulse interference. 1. Control of multiphoton processes in condensed phases,” J. Phys. Chem. A 106, 9369–9373 (2002).
[CrossRef]

de Vivie-Riedle, R.

H. Rabitz, R. de Vivie-Riedle, M. Motzkus, and K. Kompa, “Whither the future of controlling quantum phenomena?” Science 288, 824–828 (2000).
[CrossRef] [PubMed]

Débarre, D.

DeLong, K. W.

R. Trebino, K. W. DeLong, D. N. Fittinghoff, J. N. Sweetser, M. A. Krumbugel, B. A. Richman, and D. J. Kane, “Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating,” Rev. Sci. Inst. 68, 3277–3295 (1997).
[CrossRef]

Denk, W.

W. Denk, J. Strickler, and W. W. Webb, “Two-photon laser scanning fluorescence microscopy,” Science 248, 73–76 (1990).
[CrossRef] [PubMed]

Dudovich, N.

N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy,” Nature 418, 512–514 (2002).
[CrossRef] [PubMed]

Dugan, M. A.

Farge, E.

Fisher, P. J.

K. A. Kasischke, H. D. Vishwasrao, P. J. Fisher, W. R. Zipfel, and W. W. Webb, “Neural activity triggers neuronal oxidative metabolism followed by astrocytic glycolysis,” Science 305, 99–103 (2004).
[CrossRef] [PubMed]

Fittinghoff, D. N.

R. Trebino, K. W. DeLong, D. N. Fittinghoff, J. N. Sweetser, M. A. Krumbugel, B. A. Richman, and D. J. Kane, “Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating,” Rev. Sci. Inst. 68, 3277–3295 (1997).
[CrossRef]

Gandman, A.

A. Gandman, L. Chuntonov, L. Rybak, and Z. Amitay, “Coherent phase control of resonance-mediated (2 + 1) three-photon absorption,” Phys. Rev. A 75, 031401 (2007).
[CrossRef]

Gerber, G.

T. Brixner and G. Gerber, “Quantum control of gas-phase and liquid-phase femtochemistry,” ChemPhysChem 4, 418–438 (2003).
[CrossRef] [PubMed]

T. Brixner, N. H. Damrauer, P. Niklaus, and G. Gerber, “Photoselective adaptive femtosecond quantum control in the liquid phase,” Nature 414, 57–60 (2001).
[CrossRef] [PubMed]

Guyon, L.

M. Roth, L. Guyon, J. Roslund, V. Boutou, F. Courvoisier, J.-P. Wolf, and H. Rabitz, “Quantum control of tightly competitive product channels,” Phys. Rev. Lett. 102, 253001 (2009).
[CrossRef] [PubMed]

Heikal, A. A.

H. D. Vishwasrao, A. A. Heikal, K. A. Kasischke, and W. W. Webb, “Conformational dependence of intracellular NADH on metabolic state revealed by associated fluorescence anisotropy,” J. Bio. Chem. 280, 25119–25126 (2005).
[CrossRef]

Hepburn, J. W.

X. G. Xu, S. O. Konorov, J. W. Hepburn, and V. Milner, “Noise autocorrelation spectroscopy with coherent Raman scattering,” Nature Phys. 4, 125–129 (2008).
[CrossRef]

Herek, J. L.

A. C. W. van Rhijn, S. Postma, J. P. Korterik, J. L. Herek, and H. L. Offerhaus, “Chemically selective imaging by spectral phase shaping for broadband CARS around 3000 cm−1,” J. Opt. Soc. Am. B 26, 559–563 (2009).
[CrossRef]

W. Wohlleben, T. Buckup, J. L. Herek, and M. Motzkus, “Coherent control for spectroscopy and manipulation of biological dynamics,” ChemPhysChem 6, 850–857 (2005).
[CrossRef] [PubMed]

Holbrook, J. J.

J. J. Holbrook and R. G. Wolfe, “Malate dehydrogenase. X. fluorescence microtitration studies of d-malate, hydroxymalonate, nicotinamide dinucleotide, and dihydronicotinamide-adenine dinucleotide binding by mitochondrial and supernatant porcine heart enzymes,” Biochemistry 11, 2499 (1972).
[CrossRef] [PubMed]

Hölscher, U. C.

S. D. Clow, U. C. Hölscher, and T. C. Weinacht, “Achieving “perfect” molecular discrimination via coherent control and stimulated emission,” New J. Phys. 11, 115007 (2009).
[CrossRef]

Joffre, M.

Judson, R. S.

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

Kane, D. J.

R. Trebino, K. W. DeLong, D. N. Fittinghoff, J. N. Sweetser, M. A. Krumbugel, B. A. Richman, and D. J. Kane, “Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating,” Rev. Sci. Inst. 68, 3277–3295 (1997).
[CrossRef]

Kasischke, K. A.

H. D. Vishwasrao, A. A. Heikal, K. A. Kasischke, and W. W. Webb, “Conformational dependence of intracellular NADH on metabolic state revealed by associated fluorescence anisotropy,” J. Bio. Chem. 280, 25119–25126 (2005).
[CrossRef]

K. A. Kasischke, H. D. Vishwasrao, P. J. Fisher, W. R. Zipfel, and W. W. Webb, “Neural activity triggers neuronal oxidative metabolism followed by astrocytic glycolysis,” Science 305, 99–103 (2004).
[CrossRef] [PubMed]

Kompa, K.

H. Rabitz, R. de Vivie-Riedle, M. Motzkus, and K. Kompa, “Whither the future of controlling quantum phenomena?” Science 288, 824–828 (2000).
[CrossRef] [PubMed]

Konorov, S. O.

X. G. Xu, S. O. Konorov, J. W. Hepburn, and V. Milner, “Noise autocorrelation spectroscopy with coherent Raman scattering,” Nature Phys. 4, 125–129 (2008).
[CrossRef]

Korterik, J. P.

Kosloff, R.

D. J. Tannor, R. Kosloff, and S. A. Rice, “Control pulse sequence induced control of selectivity of reactions: Exact quantum mechanical calculations,” J. Chem. Phys. 85, 5805–5820 (1986).
[CrossRef]

Krumbugel, M. A.

R. Trebino, K. W. DeLong, D. N. Fittinghoff, J. N. Sweetser, M. A. Krumbugel, B. A. Richman, and D. J. Kane, “Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating,” Rev. Sci. Inst. 68, 3277–3295 (1997).
[CrossRef]

Labroille, G.

Lozovoy, V. V.

J. M. D. Cruz, V. V. Lozovoy, and M. Dantus, “Coherent control improves biomedical imaging with ultrashort shaped pulses,” J. Photochem. Photobio. A 180, 307 – 313 (2006).
[CrossRef]

I. Pastirk, J. M. D. Cruz, K. A. Walowicz, V. V. Lozovoy, and M. Dantus, “Selective two-photon microscopy with shaped femtosecond pulses,” Opt. Express 11, 1695–1701 (2003).
[CrossRef] [PubMed]

K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, “Multiphoton intrapulse interference. 1. Control of multiphoton processes in condensed phases,” J. Phys. Chem. A 106, 9369–9373 (2002).
[CrossRef]

Martin, J.-L.

Meshulach, D.

D. Meshulach and Y. Silberberg, “Coherent quantum control of multiphoton transitions by shaped ultrashort optical pulses,” Phys. Rev. A 60, 1287–1292 (1999).
[CrossRef]

Milner, V.

X. G. Xu, S. O. Konorov, J. W. Hepburn, and V. Milner, “Noise autocorrelation spectroscopy with coherent Raman scattering,” Nature Phys. 4, 125–129 (2008).
[CrossRef]

Motzkus, M.

J. Rehbinder, C. Pohling, T. Buckup, and M. Motzkus, “Multiplex coherent anti-Stokes Raman microspectroscopy with tailored Stokes spectrum,” Opt. Lett. 35, 3721–3723 (2010).
[CrossRef] [PubMed]

B. von Vacano and M. Motzkus, “Time-resolving molecular vibration for microanalytics: single laser beam nonlinear Raman spectroscopy in simulation and experiment,” Phys. Chem. Chem. Phys. 10, 681–691 (2008).
[CrossRef] [PubMed]

B. von Vacano and M. Motzkus, “Molecular discrimination of a mixture with single-beam Raman control,” J. Chem. Phys. 127, 144514 (2007).
[CrossRef] [PubMed]

W. Wohlleben, T. Buckup, J. L. Herek, and M. Motzkus, “Coherent control for spectroscopy and manipulation of biological dynamics,” ChemPhysChem 6, 850–857 (2005).
[CrossRef] [PubMed]

H. Rabitz, R. de Vivie-Riedle, M. Motzkus, and K. Kompa, “Whither the future of controlling quantum phenomena?” Science 288, 824–828 (2000).
[CrossRef] [PubMed]

Niklaus, P.

T. Brixner, N. H. Damrauer, P. Niklaus, and G. Gerber, “Photoselective adaptive femtosecond quantum control in the liquid phase,” Nature 414, 57–60 (2001).
[CrossRef] [PubMed]

Offerhaus, H. L.

Ogilvie, J. P.

Olivier, N.

Oron, D.

N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy,” Nature 418, 512–514 (2002).
[CrossRef] [PubMed]

Pastirk, I.

I. Pastirk, J. M. D. Cruz, K. A. Walowicz, V. V. Lozovoy, and M. Dantus, “Selective two-photon microscopy with shaped femtosecond pulses,” Opt. Express 11, 1695–1701 (2003).
[CrossRef] [PubMed]

K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, “Multiphoton intrapulse interference. 1. Control of multiphoton processes in condensed phases,” J. Phys. Chem. A 106, 9369–9373 (2002).
[CrossRef]

Pillai, R. S.

Pohling, C.

Postma, S.

Rabitz, H.

M. Roth, L. Guyon, J. Roslund, V. Boutou, F. Courvoisier, J.-P. Wolf, and H. Rabitz, “Quantum control of tightly competitive product channels,” Phys. Rev. Lett. 102, 253001 (2009).
[CrossRef] [PubMed]

H. Rabitz, R. de Vivie-Riedle, M. Motzkus, and K. Kompa, “Whither the future of controlling quantum phenomena?” Science 288, 824–828 (2000).
[CrossRef] [PubMed]

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

Rehbinder, J.

Rice, S. A.

D. J. Tannor, R. Kosloff, and S. A. Rice, “Control pulse sequence induced control of selectivity of reactions: Exact quantum mechanical calculations,” J. Chem. Phys. 85, 5805–5820 (1986).
[CrossRef]

Richman, B. A.

R. Trebino, K. W. DeLong, D. N. Fittinghoff, J. N. Sweetser, M. A. Krumbugel, B. A. Richman, and D. J. Kane, “Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating,” Rev. Sci. Inst. 68, 3277–3295 (1997).
[CrossRef]

Roslund, J.

M. Roth, L. Guyon, J. Roslund, V. Boutou, F. Courvoisier, J.-P. Wolf, and H. Rabitz, “Quantum control of tightly competitive product channels,” Phys. Rev. Lett. 102, 253001 (2009).
[CrossRef] [PubMed]

Roth, M.

M. Roth, L. Guyon, J. Roslund, V. Boutou, F. Courvoisier, J.-P. Wolf, and H. Rabitz, “Quantum control of tightly competitive product channels,” Phys. Rev. Lett. 102, 253001 (2009).
[CrossRef] [PubMed]

Rybak, L.

A. Gandman, L. Chuntonov, L. Rybak, and Z. Amitay, “Coherent phase control of resonance-mediated (2 + 1) three-photon absorption,” Phys. Rev. A 75, 031401 (2007).
[CrossRef]

Shapiro, M.

P. Brumer and M. Shapiro, “Control of unimolecular reactions using coherent light,” Chem. Phys. Lett. 126, 541–546 (1986).
[CrossRef]

Silberberg, Y.

Y. Silberberg, “Quantum coherent control for nonlinear spectroscopy and microscopy,” Ann. Rev. Phys. Chem. 60, 277–292 (2009).
[CrossRef]

N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy,” Nature 418, 512–514 (2002).
[CrossRef] [PubMed]

D. Meshulach and Y. Silberberg, “Coherent quantum control of multiphoton transitions by shaped ultrashort optical pulses,” Phys. Rev. A 60, 1287–1292 (1999).
[CrossRef]

Solinas, X.

Strickler, J.

W. Denk, J. Strickler, and W. W. Webb, “Two-photon laser scanning fluorescence microscopy,” Science 248, 73–76 (1990).
[CrossRef] [PubMed]

Sweetser, J. N.

R. Trebino, K. W. DeLong, D. N. Fittinghoff, J. N. Sweetser, M. A. Krumbugel, B. A. Richman, and D. J. Kane, “Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating,” Rev. Sci. Inst. 68, 3277–3295 (1997).
[CrossRef]

Tannor, D. J.

D. J. Tannor, R. Kosloff, and S. A. Rice, “Control pulse sequence induced control of selectivity of reactions: Exact quantum mechanical calculations,” J. Chem. Phys. 85, 5805–5820 (1986).
[CrossRef]

Trallero-Herrero, C.

C. Trallero-Herrero and T. C. Weinacht, “Transition from weak- to strong-field coherent control,” Phys. Rev. A 75, 063401 (2007).
[CrossRef]

Trebino, R.

R. Trebino, K. W. DeLong, D. N. Fittinghoff, J. N. Sweetser, M. A. Krumbugel, B. A. Richman, and D. J. Kane, “Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating,” Rev. Sci. Inst. 68, 3277–3295 (1997).
[CrossRef]

Tull, J. X.

van Rhijn, A. C. W.

Veilleux, I.

Vishwasrao, H. D.

H. D. Vishwasrao, A. A. Heikal, K. A. Kasischke, and W. W. Webb, “Conformational dependence of intracellular NADH on metabolic state revealed by associated fluorescence anisotropy,” J. Bio. Chem. 280, 25119–25126 (2005).
[CrossRef]

K. A. Kasischke, H. D. Vishwasrao, P. J. Fisher, W. R. Zipfel, and W. W. Webb, “Neural activity triggers neuronal oxidative metabolism followed by astrocytic glycolysis,” Science 305, 99–103 (2004).
[CrossRef] [PubMed]

H. D. Vishwasrao, “Quantitative two-photon redox fluorescence microscopy of neurometabolic dynamics,” Ph.D. thesis, Cornell University (2005).

von Vacano, B.

B. von Vacano and M. Motzkus, “Time-resolving molecular vibration for microanalytics: single laser beam nonlinear Raman spectroscopy in simulation and experiment,” Phys. Chem. Chem. Phys. 10, 681–691 (2008).
[CrossRef] [PubMed]

B. von Vacano and M. Motzkus, “Molecular discrimination of a mixture with single-beam Raman control,” J. Chem. Phys. 127, 144514 (2007).
[CrossRef] [PubMed]

Walowicz, K. A.

I. Pastirk, J. M. D. Cruz, K. A. Walowicz, V. V. Lozovoy, and M. Dantus, “Selective two-photon microscopy with shaped femtosecond pulses,” Opt. Express 11, 1695–1701 (2003).
[CrossRef] [PubMed]

K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, “Multiphoton intrapulse interference. 1. Control of multiphoton processes in condensed phases,” J. Phys. Chem. A 106, 9369–9373 (2002).
[CrossRef]

Warren, W. S.

Webb, W. W.

H. D. Vishwasrao, A. A. Heikal, K. A. Kasischke, and W. W. Webb, “Conformational dependence of intracellular NADH on metabolic state revealed by associated fluorescence anisotropy,” J. Bio. Chem. 280, 25119–25126 (2005).
[CrossRef]

K. A. Kasischke, H. D. Vishwasrao, P. J. Fisher, W. R. Zipfel, and W. W. Webb, “Neural activity triggers neuronal oxidative metabolism followed by astrocytic glycolysis,” Science 305, 99–103 (2004).
[CrossRef] [PubMed]

W. R. Zipfel, R. M. Williams, and W. W. Webb, “Nonlinear magic: multiphoton microscopy in the biosciences,” Nature Biotech. 21, 1369–1377 (2003).
[CrossRef]

W. Denk, J. Strickler, and W. W. Webb, “Two-photon laser scanning fluorescence microscopy,” Science 248, 73–76 (1990).
[CrossRef] [PubMed]

Weinacht, T.

T. Weinacht, “Distinguishing between molecules that look the same,” Physics 2, 51 (2009).
[CrossRef]

Weinacht, T. C.

S. D. Clow, U. C. Hölscher, and T. C. Weinacht, “Achieving “perfect” molecular discrimination via coherent control and stimulated emission,” New J. Phys. 11, 115007 (2009).
[CrossRef]

C. Trallero-Herrero and T. C. Weinacht, “Transition from weak- to strong-field coherent control,” Phys. Rev. A 75, 063401 (2007).
[CrossRef]

Weiner, A. M.

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

Williams, R. M.

W. R. Zipfel, R. M. Williams, and W. W. Webb, “Nonlinear magic: multiphoton microscopy in the biosciences,” Nature Biotech. 21, 1369–1377 (2003).
[CrossRef]

Wohlleben, W.

W. Wohlleben, T. Buckup, J. L. Herek, and M. Motzkus, “Coherent control for spectroscopy and manipulation of biological dynamics,” ChemPhysChem 6, 850–857 (2005).
[CrossRef] [PubMed]

Wolf, J.-P.

M. Roth, L. Guyon, J. Roslund, V. Boutou, F. Courvoisier, J.-P. Wolf, and H. Rabitz, “Quantum control of tightly competitive product channels,” Phys. Rev. Lett. 102, 253001 (2009).
[CrossRef] [PubMed]

Wolfe, R. G.

J. J. Holbrook and R. G. Wolfe, “Malate dehydrogenase. X. fluorescence microtitration studies of d-malate, hydroxymalonate, nicotinamide dinucleotide, and dihydronicotinamide-adenine dinucleotide binding by mitochondrial and supernatant porcine heart enzymes,” Biochemistry 11, 2499 (1972).
[CrossRef] [PubMed]

Xie, X. S.

J.-X. Cheng and X. S. Xie, “Coherent anti-Stokes Raman scattering microscopy: Instrumentation, theory, and applications,” J. Phys. Chem. B 108, 827–840 (2004).
[CrossRef]

Xu, X. G.

X. G. Xu, S. O. Konorov, J. W. Hepburn, and V. Milner, “Noise autocorrelation spectroscopy with coherent Raman scattering,” Nature Phys. 4, 125–129 (2008).
[CrossRef]

Zipfel, W. R.

K. A. Kasischke, H. D. Vishwasrao, P. J. Fisher, W. R. Zipfel, and W. W. Webb, “Neural activity triggers neuronal oxidative metabolism followed by astrocytic glycolysis,” Science 305, 99–103 (2004).
[CrossRef] [PubMed]

W. R. Zipfel, R. M. Williams, and W. W. Webb, “Nonlinear magic: multiphoton microscopy in the biosciences,” Nature Biotech. 21, 1369–1377 (2003).
[CrossRef]

Ann. Rev. Phys. Chem. (1)

Y. Silberberg, “Quantum coherent control for nonlinear spectroscopy and microscopy,” Ann. Rev. Phys. Chem. 60, 277–292 (2009).
[CrossRef]

Biochemistry (1)

J. J. Holbrook and R. G. Wolfe, “Malate dehydrogenase. X. fluorescence microtitration studies of d-malate, hydroxymalonate, nicotinamide dinucleotide, and dihydronicotinamide-adenine dinucleotide binding by mitochondrial and supernatant porcine heart enzymes,” Biochemistry 11, 2499 (1972).
[CrossRef] [PubMed]

Chem. Phys. Lett. (1)

P. Brumer and M. Shapiro, “Control of unimolecular reactions using coherent light,” Chem. Phys. Lett. 126, 541–546 (1986).
[CrossRef]

ChemPhysChem (2)

T. Brixner and G. Gerber, “Quantum control of gas-phase and liquid-phase femtochemistry,” ChemPhysChem 4, 418–438 (2003).
[CrossRef] [PubMed]

W. Wohlleben, T. Buckup, J. L. Herek, and M. Motzkus, “Coherent control for spectroscopy and manipulation of biological dynamics,” ChemPhysChem 6, 850–857 (2005).
[CrossRef] [PubMed]

J. Bio. Chem. (1)

H. D. Vishwasrao, A. A. Heikal, K. A. Kasischke, and W. W. Webb, “Conformational dependence of intracellular NADH on metabolic state revealed by associated fluorescence anisotropy,” J. Bio. Chem. 280, 25119–25126 (2005).
[CrossRef]

J. Chem. Phys. (2)

D. J. Tannor, R. Kosloff, and S. A. Rice, “Control pulse sequence induced control of selectivity of reactions: Exact quantum mechanical calculations,” J. Chem. Phys. 85, 5805–5820 (1986).
[CrossRef]

B. von Vacano and M. Motzkus, “Molecular discrimination of a mixture with single-beam Raman control,” J. Chem. Phys. 127, 144514 (2007).
[CrossRef] [PubMed]

J. Opt. Soc. Am. B (2)

J. Photochem. Photobio. A (1)

J. M. D. Cruz, V. V. Lozovoy, and M. Dantus, “Coherent control improves biomedical imaging with ultrashort shaped pulses,” J. Photochem. Photobio. A 180, 307 – 313 (2006).
[CrossRef]

J. Phys. Chem. A (1)

K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, “Multiphoton intrapulse interference. 1. Control of multiphoton processes in condensed phases,” J. Phys. Chem. A 106, 9369–9373 (2002).
[CrossRef]

J. Phys. Chem. B (1)

J.-X. Cheng and X. S. Xie, “Coherent anti-Stokes Raman scattering microscopy: Instrumentation, theory, and applications,” J. Phys. Chem. B 108, 827–840 (2004).
[CrossRef]

Nature (2)

N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy,” Nature 418, 512–514 (2002).
[CrossRef] [PubMed]

T. Brixner, N. H. Damrauer, P. Niklaus, and G. Gerber, “Photoselective adaptive femtosecond quantum control in the liquid phase,” Nature 414, 57–60 (2001).
[CrossRef] [PubMed]

Nature Biotech. (1)

W. R. Zipfel, R. M. Williams, and W. W. Webb, “Nonlinear magic: multiphoton microscopy in the biosciences,” Nature Biotech. 21, 1369–1377 (2003).
[CrossRef]

Nature Phys. (1)

X. G. Xu, S. O. Konorov, J. W. Hepburn, and V. Milner, “Noise autocorrelation spectroscopy with coherent Raman scattering,” Nature Phys. 4, 125–129 (2008).
[CrossRef]

New J. Phys. (1)

S. D. Clow, U. C. Hölscher, and T. C. Weinacht, “Achieving “perfect” molecular discrimination via coherent control and stimulated emission,” New J. Phys. 11, 115007 (2009).
[CrossRef]

Opt. Express (3)

Opt. Lett. (1)

Phys. Chem. Chem. Phys. (1)

B. von Vacano and M. Motzkus, “Time-resolving molecular vibration for microanalytics: single laser beam nonlinear Raman spectroscopy in simulation and experiment,” Phys. Chem. Chem. Phys. 10, 681–691 (2008).
[CrossRef] [PubMed]

Phys. Rev. A (3)

D. Meshulach and Y. Silberberg, “Coherent quantum control of multiphoton transitions by shaped ultrashort optical pulses,” Phys. Rev. A 60, 1287–1292 (1999).
[CrossRef]

A. Gandman, L. Chuntonov, L. Rybak, and Z. Amitay, “Coherent phase control of resonance-mediated (2 + 1) three-photon absorption,” Phys. Rev. A 75, 031401 (2007).
[CrossRef]

C. Trallero-Herrero and T. C. Weinacht, “Transition from weak- to strong-field coherent control,” Phys. Rev. A 75, 063401 (2007).
[CrossRef]

Phys. Rev. Lett. (2)

M. Roth, L. Guyon, J. Roslund, V. Boutou, F. Courvoisier, J.-P. Wolf, and H. Rabitz, “Quantum control of tightly competitive product channels,” Phys. Rev. Lett. 102, 253001 (2009).
[CrossRef] [PubMed]

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

Physics (1)

T. Weinacht, “Distinguishing between molecules that look the same,” Physics 2, 51 (2009).
[CrossRef]

Rev. Sci. Inst. (2)

R. Trebino, K. W. DeLong, D. N. Fittinghoff, J. N. Sweetser, M. A. Krumbugel, B. A. Richman, and D. J. Kane, “Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating,” Rev. Sci. Inst. 68, 3277–3295 (1997).
[CrossRef]

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

Science (3)

H. Rabitz, R. de Vivie-Riedle, M. Motzkus, and K. Kompa, “Whither the future of controlling quantum phenomena?” Science 288, 824–828 (2000).
[CrossRef] [PubMed]

W. Denk, J. Strickler, and W. W. Webb, “Two-photon laser scanning fluorescence microscopy,” Science 248, 73–76 (1990).
[CrossRef] [PubMed]

K. A. Kasischke, H. D. Vishwasrao, P. J. Fisher, W. R. Zipfel, and W. W. Webb, “Neural activity triggers neuronal oxidative metabolism followed by astrocytic glycolysis,” Science 305, 99–103 (2004).
[CrossRef] [PubMed]

Other (2)

H. D. Vishwasrao, “Quantitative two-photon redox fluorescence microscopy of neurometabolic dynamics,” Ph.D. thesis, Cornell University (2005).

Developmental Resource for Biophysical Imaging Opto-Electronics (DRBIO) at Cornell University, “Two-photon action cross sections,” http://www.drbio.cornell.edu/cross_sections.html .

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Figures (6)

Fig. 1
Fig. 1

Experimental set-up showing the computer-controlled pulse shaper and cuvettes containing NADH or NADH + enzyme in solution. As discussed in the text, the pulse shaper scans the position of a π-spectral phase step across the bandwidth of the laser pulse.

Fig. 2
Fig. 2

Left panel: one-photon absorption spectrum of NADH and NADH plus MDH. Right panel: one-photon fluorescence spectrum of NADH and NADH plus MDH at various concentrations as measured in a spectrofluorometer. The excitation wavelength was 385 nm.

Fig. 3
Fig. 3

SHG-FROG plots showing both an unshaped pulse (left panel) and a shaped pulse with a π-phase step in the middle of the spectral bandwidth (middle panel). The right panel shows the second-order power spectrum, or the Fourier transform of the square of the electric field in time, for an unshaped pulse and two π-phase step pulses that are representative of the control pulses used in Fig. 4.

Fig. 4
Fig. 4

Normalized fluorescence as a function of π-step position for both NADH alone (solid red) and NADH with MDH (dashed blue). The fluorescence from the Trizma buffer and MDH alone were negligible and did not affect the control. Measurements from two separate days are shown in the left and right panels to illustrate the fact that while the details of the scans vary from day to day, the main discrimination feature remains.

Fig. 5
Fig. 5

Ratio of the fluorescence signal at the short-wavelength minimum to that at the long-wavelength minimum as a function of enzyme concentration. The binding fraction (as calculated based on the Kd value given in [35]) is shown on the top of the graph. The error bars show the standard deviation of the mean for repeated measurements.

Fig. 6
Fig. 6

Histograms showing the ratio of fluorescence between two pulse shapes for both unbound NADH (pink shaded) and enzyme-bound NADH (solid blue). The clear distinction between the peaks implies easy selectivity between the two forms of NADH. The peaks were constructed from 100 measurements, with 500 laser shots contributing to each measurement.

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