Abstract

Shaped near-infrared (NIR) femtosecond pulses are used for the first time to control the generation of coherent deep-ultraviolet (UV) radiation in an atomic resonance-mediated (2+1) three-photon excitation. The broadband excitation coherently involves pathways that are on resonance with the intermediate resonance state as well as pathways that are near resonance with it. Experimental and theoretical results are presented for phase controlling the total emitted UV yield in atomic sodium. Depending on the NIR spectrum of the excitation pulse, the coherent UV emission is either predominantly due to a single excited real state that is accessed resonantly or due to a manifold of virtual states. The former leads to a narrowband UV emission, while the latter leads to a broadband UV radiation. Basic phase control is exercised in both cases, with excellent agreement between experiments and calculations. The tunability is over an order-of-magnitude UV-yield range.

© 2008 Optical Society of America

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2008 (7)

L. Chuntonov, L. Rybak, A. Gandman, and Z. Amitay, "Frequency-domain coherent control of femtosecond two-photon absorption: intermediate-field versus weak-field regime," J. Phys. B 41, 035504 (2008).
[CrossRef]

Z. Amitay, A. Gandman, L. Chuntonov, and L. Rybak, "Multichannel selective femtosecond coherent control based on symmetry properties," Phys. Rev. Lett. 100, 193002 (2008).
[CrossRef] [PubMed]

N. T. Form, B. J. Whitaker, and C. Meier, "Enhancing the probability of three-photon absorption in iodine through pulse shaping," J. Phys. B 41, 074011 (2008).
[CrossRef]

B. 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 (2008).
[CrossRef]

S. D. Clow, C. Trallero-Herrero, T. Bergeman, and T. Weinacht, "Strong field multiphoton inversion of a threelevel system using shaped ultrafast laser pulses," Phys. Rev. Lett. 100, 233603 (2008).
[CrossRef] [PubMed]

H. Li, A. D. Ahmasi; B. Xu, P. J. Wrzesinski, V. V. Lozovoy, and M. Dantus, "Coherent mode-selective Raman excitation towards standoff detection," Opt. Express 16, 5499 (2008)
[CrossRef] [PubMed]

O. Katz, A. Natan, Y. Silberberg, and S. Rosenwaks, "Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses," Appl. Phys. Lett. 92, 171116 (2008).
[CrossRef]

2007 (3)

S. H. Lim, A. G. Caster, and S. R. Leone, "Fourier transform spectral interferometric coherent anti-Stokes Raman scattering (FTSI-CARS) spectroscopy," Opt. Lett. 32, 1332 (2007).
[CrossRef] [PubMed]

A. Gandman, L. Chuntonov, L. Rybak, and Z. Amitay, "Pulse-bandwidth dependence of coherent phase control of resonance-mediated (2+1) three-photon absorption," Phys. Rev. A 76, 053419 (2007).
[CrossRef]

P. Nuernberger, G. Vogt, T. Brixner, and G. Gerber, "Femtosecond quantum control of molecular dynamics in the condensed phase," Phys. Chem. Chem. Phys. 9, 2470 (2007).
[CrossRef] [PubMed]

2006 (3)

M. Wollenhaupt, A. Praelt, C. Sarpe-Tudoran, D. Liese, T. Bayer, and T. Baumert, "Femtosecond strong-field quantum control with sinusoidally phase-modulated pulses," Phys. Rev. A 73, 063409 (2006).
[CrossRef]

X. Dai, E. W. Lerch, and S. R. Leone, "Coherent control through near-resonant Raman transitions," Phys. Rev. A 73, 023404 (2006).
[CrossRef]

C. Trallero-Herrero, J. L. Cohen, and T. Weinacht, "Strong-field atomic phase matching," Phys. Rev. Lett. 96, 063603 (2006).
[CrossRef] [PubMed]

2005 (2)

2004 (2)

M. Dantus and V. V. Lozovoy, "Experimental coherent laser control of physicochemical processes," Chem. Rev. 104, 1813 (2004).
[CrossRef] [PubMed]

A. Prakelt, M. Wollenhaupt, C. Sarpe-Tudoran, and T. Baumert, "Phase control of a two-photon transition with shaped femtosecond laser-pulse sequences," Phys. Rev. A 70, 063407 (2004).
[CrossRef]

2003 (2)

2002 (3)

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy," Nature (London) 418, 512 (2002).
[CrossRef]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Narrow-band coherent anti-stokes raman signals from broadband pulses," Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

H. U. Stauffer, J. B. Ballard, Z. Amitay, and S. R. Leone, "Simultaneous phase control of Li2 wave packets in two electronic states," J. Chem. Phys. 116, 946 (2002).
[CrossRef]

2001 (2)

N. Dudovich, B. Dayan, S. M. Gallagher Faeder, and Y. Silberberg, "Transform-limited pulses are not optimal for resonant multiphoton transitions," Phys. Rev. Lett. 86, 47 (2001).
[CrossRef] [PubMed]

T. Brixner and G. Gerber, "Femtosecond polarization pulse shaping," Opt. Lett. 26, 557 (2001).
[CrossRef]

2000 (3)

A. M. Weiner, "Femtosecond pulse shaping using spatial light modulators," Rev. Sci. Instrum. 71, 1929 (2000).
[CrossRef]

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

Q3. J. G. Eden, "From N2 (337 nm) to high-order harmonic generation: 40 years of coherent source development in the UV and VUV," IEEE J. Sel. Top. Quantum Electron. 6, 1051 (2000), and references therein.
[CrossRef]

1999 (1)

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

1998 (1)

D. Meshulach and Y. Silberberg, "Coherent quantum control of two-photon transitions by a femtosecond laser pulse," Nature (London) 396, 239 (1998).
[CrossRef]

1997 (1)

R. J. Gordon and S. A. Rice, "Active control of the dynamics of atoms and molecules," Annu. Rev. Phys. Chem. 48, 601 (1997).
[CrossRef] [PubMed]

1993 (2)

1987 (1)

G. Hilber, A. Lago, and R. Wallenstein, "Broadly tunable vacuum-ultraviolet/extreme-ultraviolet radiation generated by resonant third-order frequency conversion in krypton," J. Opt. Soc. Am. B 4, 1735 (1987).
[CrossRef]

1986 (3)

1985 (1)

P. H. Herman, P. E. LaRocque, R. H. Lipson, W. Jamroz, and B. P. Stoicheff, "Vacuum ultraviolet laser spectroscopy III: laboratory sources of coherent radiation tunable from 105 to 175 nm using Mg, Zn, and Hg vapors," Can. J. Phys. 63, 1581 (1985).
[CrossRef]

1983 (1)

R. Hilbig and R. Wallenstein, "Resonant sum and difference frequency mixing in Hg," IEEE J. Quantum Electron. 19, 1759 (1983).
[CrossRef]

1981 (1)

1978 (1)

1976 (1)

S. C. Wallace and G. Zdasiuk, "High-efficiency four-wave sum mixing in magnesium at 140 nm," Appl. Phys. Lett. 28, 449 (1976).
[CrossRef]

1974 (1)

R. T. Hodgson, P. P. Sorokin, and J. J. Wynne, "Tunable coherent vacuum-ultraviolet generation in atomic vapors," Phys. Rev. Lett. 32, 343 (1974).
[CrossRef]

1971 (1)

J. F. Young, G. C. Bjorklund, A. H. Kung, R. B. Miles, and S. E. Harris, "Third-harmonic generation in phasematched Rb vapor," Phys. Rev. Lett. 27, 1551 (1971).
[CrossRef]

Ahmasi, A. D.

Amitay, Z.

Z. Amitay, A. Gandman, L. Chuntonov, and L. Rybak, "Multichannel selective femtosecond coherent control based on symmetry properties," Phys. Rev. Lett. 100, 193002 (2008).
[CrossRef] [PubMed]

L. Chuntonov, L. Rybak, A. Gandman, and Z. Amitay, "Frequency-domain coherent control of femtosecond two-photon absorption: intermediate-field versus weak-field regime," J. Phys. B 41, 035504 (2008).
[CrossRef]

A. Gandman, L. Chuntonov, L. Rybak, and Z. Amitay, "Pulse-bandwidth dependence of coherent phase control of resonance-mediated (2+1) three-photon absorption," Phys. Rev. A 76, 053419 (2007).
[CrossRef]

H. U. Stauffer, J. B. Ballard, Z. Amitay, and S. R. Leone, "Simultaneous phase control of Li2 wave packets in two electronic states," J. Chem. Phys. 116, 946 (2002).
[CrossRef]

Ballard, J. B.

H. U. Stauffer, J. B. Ballard, Z. Amitay, and S. R. Leone, "Simultaneous phase control of Li2 wave packets in two electronic states," J. Chem. Phys. 116, 946 (2002).
[CrossRef]

Bartels, R. A.

Baumert, T.

M. Wollenhaupt, A. Praelt, C. Sarpe-Tudoran, D. Liese, T. Bayer, and T. Baumert, "Femtosecond strong-field quantum control with sinusoidally phase-modulated pulses," Phys. Rev. A 73, 063409 (2006).
[CrossRef]

Bayer, T.

M. Wollenhaupt, A. Praelt, C. Sarpe-Tudoran, D. Liese, T. Bayer, and T. Baumert, "Femtosecond strong-field quantum control with sinusoidally phase-modulated pulses," Phys. Rev. A 73, 063409 (2006).
[CrossRef]

Bergeman, T.

S. D. Clow, C. Trallero-Herrero, T. Bergeman, and T. Weinacht, "Strong field multiphoton inversion of a threelevel system using shaped ultrafast laser pulses," Phys. Rev. Lett. 100, 233603 (2008).
[CrossRef] [PubMed]

Bjorklund, G. C.

J. F. Young, G. C. Bjorklund, A. H. Kung, R. B. Miles, and S. E. Harris, "Third-harmonic generation in phasematched Rb vapor," Phys. Rev. Lett. 27, 1551 (1971).
[CrossRef]

Brixner, T.

P. Nuernberger, G. Vogt, T. Brixner, and G. Gerber, "Femtosecond quantum control of molecular dynamics in the condensed phase," Phys. Chem. Chem. Phys. 9, 2470 (2007).
[CrossRef] [PubMed]

T. Brixner and G. Gerber, "Quantum Control of Gas-Phase and Liquid-Phase Femtochemistry," ChemPhysChem 4, 418 (2003).
[CrossRef] [PubMed]

T. Brixner and G. Gerber, "Femtosecond polarization pulse shaping," Opt. Lett. 26, 557 (2001).
[CrossRef]

Caster, A. G.

Chen, T. J.

Chuntonov, L.

Z. Amitay, A. Gandman, L. Chuntonov, and L. Rybak, "Multichannel selective femtosecond coherent control based on symmetry properties," Phys. Rev. Lett. 100, 193002 (2008).
[CrossRef] [PubMed]

L. Chuntonov, L. Rybak, A. Gandman, and Z. Amitay, "Frequency-domain coherent control of femtosecond two-photon absorption: intermediate-field versus weak-field regime," J. Phys. B 41, 035504 (2008).
[CrossRef]

A. Gandman, L. Chuntonov, L. Rybak, and Z. Amitay, "Pulse-bandwidth dependence of coherent phase control of resonance-mediated (2+1) three-photon absorption," Phys. Rev. A 76, 053419 (2007).
[CrossRef]

Clow, S. D.

S. D. Clow, C. Trallero-Herrero, T. Bergeman, and T. Weinacht, "Strong field multiphoton inversion of a threelevel system using shaped ultrafast laser pulses," Phys. Rev. Lett. 100, 233603 (2008).
[CrossRef] [PubMed]

Cohen, J. L.

C. Trallero-Herrero, J. L. Cohen, and T. Weinacht, "Strong-field atomic phase matching," Phys. Rev. Lett. 96, 063603 (2006).
[CrossRef] [PubMed]

Dai, X.

X. Dai, E. W. Lerch, and S. R. Leone, "Coherent control through near-resonant Raman transitions," Phys. Rev. A 73, 023404 (2006).
[CrossRef]

Dantus, M.

Dayan, B.

N. Dudovich, B. Dayan, S. M. Gallagher Faeder, and Y. Silberberg, "Transform-limited pulses are not optimal for resonant multiphoton transitions," Phys. Rev. Lett. 86, 47 (2001).
[CrossRef] [PubMed]

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 (2000).
[CrossRef] [PubMed]

DeBeer, D.

Dudovich, N.

N. Dudovich, T. Polack, A. Pe’er, and Y. Silberberg, "Simple route to strong-field coherent control," Phys. Rev. Lett. 94,083002 (2005).
[CrossRef] [PubMed]

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy," Nature (London) 418, 512 (2002).
[CrossRef]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Narrow-band coherent anti-stokes raman signals from broadband pulses," Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

N. Dudovich, B. Dayan, S. M. Gallagher Faeder, and Y. Silberberg, "Transform-limited pulses are not optimal for resonant multiphoton transitions," Phys. Rev. Lett. 86, 47 (2001).
[CrossRef] [PubMed]

Eden, J. G.

Q3. J. G. Eden, "From N2 (337 nm) to high-order harmonic generation: 40 years of coherent source development in the UV and VUV," IEEE J. Sel. Top. Quantum Electron. 6, 1051 (2000), and references therein.
[CrossRef]

Form, N. T.

N. T. Form, B. J. Whitaker, and C. Meier, "Enhancing the probability of three-photon absorption in iodine through pulse shaping," J. Phys. B 41, 074011 (2008).
[CrossRef]

Fourkas, J. T.

Gallagher Faeder, S. M.

N. Dudovich, B. Dayan, S. M. Gallagher Faeder, and Y. Silberberg, "Transform-limited pulses are not optimal for resonant multiphoton transitions," Phys. Rev. Lett. 86, 47 (2001).
[CrossRef] [PubMed]

Gandman, A.

Z. Amitay, A. Gandman, L. Chuntonov, and L. Rybak, "Multichannel selective femtosecond coherent control based on symmetry properties," Phys. Rev. Lett. 100, 193002 (2008).
[CrossRef] [PubMed]

L. Chuntonov, L. Rybak, A. Gandman, and Z. Amitay, "Frequency-domain coherent control of femtosecond two-photon absorption: intermediate-field versus weak-field regime," J. Phys. B 41, 035504 (2008).
[CrossRef]

A. Gandman, L. Chuntonov, L. Rybak, and Z. Amitay, "Pulse-bandwidth dependence of coherent phase control of resonance-mediated (2+1) three-photon absorption," Phys. Rev. A 76, 053419 (2007).
[CrossRef]

Gerber, G.

P. Nuernberger, G. Vogt, T. Brixner, and G. Gerber, "Femtosecond quantum control of molecular dynamics in the condensed phase," Phys. Chem. Chem. Phys. 9, 2470 (2007).
[CrossRef] [PubMed]

T. Brixner and G. Gerber, "Quantum Control of Gas-Phase and Liquid-Phase Femtochemistry," ChemPhysChem 4, 418 (2003).
[CrossRef] [PubMed]

T. Brixner and G. Gerber, "Femtosecond polarization pulse shaping," Opt. Lett. 26, 557 (2001).
[CrossRef]

Gershgoren, E.

Golub, J. E.

Gordon, R. J.

R. J. Gordon and S. A. Rice, "Active control of the dynamics of atoms and molecules," Annu. Rev. Phys. Chem. 48, 601 (1997).
[CrossRef] [PubMed]

Hannemann, S.

Harris, S. E.

J. F. Young, G. C. Bjorklund, A. H. Kung, R. B. Miles, and S. E. Harris, "Third-harmonic generation in phasematched Rb vapor," Phys. Rev. Lett. 27, 1551 (1971).
[CrossRef]

Hartmann, S. R.

Herman, P. H.

P. H. Herman, P. E. LaRocque, R. H. Lipson, W. Jamroz, and B. P. Stoicheff, "Vacuum ultraviolet laser spectroscopy III: laboratory sources of coherent radiation tunable from 105 to 175 nm using Mg, Zn, and Hg vapors," Can. J. Phys. 63, 1581 (1985).
[CrossRef]

Hilber, G.

G. Hilber, A. Lago, and R. Wallenstein, "Broadly tunable vacuum-ultraviolet/extreme-ultraviolet radiation generated by resonant third-order frequency conversion in krypton," J. Opt. Soc. Am. B 4, 1735 (1987).
[CrossRef]

Hilbig, R.

R. Hilbig and R. Wallenstein, "Resonant sum and difference frequency mixing in Hg," IEEE J. Quantum Electron. 19, 1759 (1983).
[CrossRef]

Hirakawa, Y.

Hodgson, R. T.

R. T. Hodgson, P. P. Sorokin, and J. J. Wynne, "Tunable coherent vacuum-ultraviolet generation in atomic vapors," Phys. Rev. Lett. 32, 343 (1974).
[CrossRef]

Hollenstein, U.

Jamroz, W.

P. H. Herman, P. E. LaRocque, R. H. Lipson, W. Jamroz, and B. P. Stoicheff, "Vacuum ultraviolet laser spectroscopy III: laboratory sources of coherent radiation tunable from 105 to 175 nm using Mg, Zn, and Hg vapors," Can. J. Phys. 63, 1581 (1985).
[CrossRef]

Kapteyn, H. C.

Katz, O.

O. Katz, A. Natan, Y. Silberberg, and S. Rosenwaks, "Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses," Appl. Phys. Lett. 92, 171116 (2008).
[CrossRef]

Kompa, K.

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

Kosloff, R.

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

Kung, A. H.

J. F. Young, G. C. Bjorklund, A. H. Kung, R. B. Miles, and S. E. Harris, "Third-harmonic generation in phasematched Rb vapor," Phys. Rev. Lett. 27, 1551 (1971).
[CrossRef]

Lago, A.

G. Hilber, A. Lago, and R. Wallenstein, "Broadly tunable vacuum-ultraviolet/extreme-ultraviolet radiation generated by resonant third-order frequency conversion in krypton," J. Opt. Soc. Am. B 4, 1735 (1987).
[CrossRef]

LaRocque, P. E.

P. H. Herman, P. E. LaRocque, R. H. Lipson, W. Jamroz, and B. P. Stoicheff, "Vacuum ultraviolet laser spectroscopy III: laboratory sources of coherent radiation tunable from 105 to 175 nm using Mg, Zn, and Hg vapors," Can. J. Phys. 63, 1581 (1985).
[CrossRef]

Leone, S. R.

S. H. Lim, A. G. Caster, and S. R. Leone, "Fourier transform spectral interferometric coherent anti-Stokes Raman scattering (FTSI-CARS) spectroscopy," Opt. Lett. 32, 1332 (2007).
[CrossRef] [PubMed]

X. Dai, E. W. Lerch, and S. R. Leone, "Coherent control through near-resonant Raman transitions," Phys. Rev. A 73, 023404 (2006).
[CrossRef]

H. U. Stauffer, J. B. Ballard, Z. Amitay, and S. R. Leone, "Simultaneous phase control of Li2 wave packets in two electronic states," J. Chem. Phys. 116, 946 (2002).
[CrossRef]

Lerch, E. W.

X. Dai, E. W. Lerch, and S. R. Leone, "Coherent control through near-resonant Raman transitions," Phys. Rev. A 73, 023404 (2006).
[CrossRef]

Li, H.

Liese, D.

M. Wollenhaupt, A. Praelt, C. Sarpe-Tudoran, D. Liese, T. Bayer, and T. Baumert, "Femtosecond strong-field quantum control with sinusoidally phase-modulated pulses," Phys. Rev. A 73, 063409 (2006).
[CrossRef]

Lim, S. H.

Lipson, R. H.

P. H. Herman, P. E. LaRocque, R. H. Lipson, W. Jamroz, and B. P. Stoicheff, "Vacuum ultraviolet laser spectroscopy III: laboratory sources of coherent radiation tunable from 105 to 175 nm using Mg, Zn, and Hg vapors," Can. J. Phys. 63, 1581 (1985).
[CrossRef]

Lozovoy, V. V.

Maeda, M.

Mahleh, D.

W. S. Warren, H. Rabitz, and D. Mahleh, "Coherent control of quantum dynamics: the dream is alive," Science 259, 1581 (1993).
[CrossRef] [PubMed]

Mahon, R.

McKee, T. J.

Meier, C.

N. T. Form, B. J. Whitaker, and C. Meier, "Enhancing the probability of three-photon absorption in iodine through pulse shaping," J. Phys. B 41, 074011 (2008).
[CrossRef]

Meshulach, D.

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

D. Meshulach and Y. Silberberg, "Coherent quantum control of two-photon transitions by a femtosecond laser pulse," Nature (London) 396, 239 (1998).
[CrossRef]

Miles, R. B.

J. F. Young, G. C. Bjorklund, A. H. Kung, R. B. Miles, and S. E. Harris, "Third-harmonic generation in phasematched Rb vapor," Phys. Rev. Lett. 27, 1551 (1971).
[CrossRef]

Mossberg, T. W.

Motzkus, M.

B. 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 (2008).
[CrossRef]

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

Muraoka, K.

Murnane, M. M.

Nagai, A.

Natan, A.

O. Katz, A. Natan, Y. Silberberg, and S. Rosenwaks, "Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses," Appl. Phys. Lett. 92, 171116 (2008).
[CrossRef]

Nuernberger, P.

P. Nuernberger, G. Vogt, T. Brixner, and G. Gerber, "Femtosecond quantum control of molecular dynamics in the condensed phase," Phys. Chem. Chem. Phys. 9, 2470 (2007).
[CrossRef] [PubMed]

Okada, T.

Oron, D.

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Narrow-band coherent anti-stokes raman signals from broadband pulses," Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy," Nature (London) 418, 512 (2002).
[CrossRef]

Pe’er, A.

N. Dudovich, T. Polack, A. Pe’er, and Y. Silberberg, "Simple route to strong-field coherent control," Phys. Rev. Lett. 94,083002 (2005).
[CrossRef] [PubMed]

Polack, T.

N. Dudovich, T. Polack, A. Pe’er, and Y. Silberberg, "Simple route to strong-field coherent control," Phys. Rev. Lett. 94,083002 (2005).
[CrossRef] [PubMed]

Praelt, A.

M. Wollenhaupt, A. Praelt, C. Sarpe-Tudoran, D. Liese, T. Bayer, and T. Baumert, "Femtosecond strong-field quantum control with sinusoidally phase-modulated pulses," Phys. Rev. A 73, 063409 (2006).
[CrossRef]

Rabitz, H.

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

W. S. Warren, H. Rabitz, and D. Mahleh, "Coherent control of quantum dynamics: the dream is alive," Science 259, 1581 (1993).
[CrossRef] [PubMed]

Rice, S. A.

R. J. Gordon and S. A. Rice, "Active control of the dynamics of atoms and molecules," Annu. Rev. Phys. Chem. 48, 601 (1997).
[CrossRef] [PubMed]

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

Rosenwaks, S.

O. Katz, A. Natan, Y. Silberberg, and S. Rosenwaks, "Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses," Appl. Phys. Lett. 92, 171116 (2008).
[CrossRef]

Rybak, L.

Z. Amitay, A. Gandman, L. Chuntonov, and L. Rybak, "Multichannel selective femtosecond coherent control based on symmetry properties," Phys. Rev. Lett. 100, 193002 (2008).
[CrossRef] [PubMed]

L. Chuntonov, L. Rybak, A. Gandman, and Z. Amitay, "Frequency-domain coherent control of femtosecond two-photon absorption: intermediate-field versus weak-field regime," J. Phys. B 41, 035504 (2008).
[CrossRef]

A. Gandman, L. Chuntonov, L. Rybak, and Z. Amitay, "Pulse-bandwidth dependence of coherent phase control of resonance-mediated (2+1) three-photon absorption," Phys. Rev. A 76, 053419 (2007).
[CrossRef]

Sarpe-Tudoran, C.

M. Wollenhaupt, A. Praelt, C. Sarpe-Tudoran, D. Liese, T. Bayer, and T. Baumert, "Femtosecond strong-field quantum control with sinusoidally phase-modulated pulses," Phys. Rev. A 73, 063409 (2006).
[CrossRef]

Silberberg, Y.

O. Katz, A. Natan, Y. Silberberg, and S. Rosenwaks, "Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses," Appl. Phys. Lett. 92, 171116 (2008).
[CrossRef]

N. Dudovich, T. Polack, A. Pe’er, and Y. Silberberg, "Simple route to strong-field coherent control," Phys. Rev. Lett. 94,083002 (2005).
[CrossRef] [PubMed]

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy," Nature (London) 418, 512 (2002).
[CrossRef]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Narrow-band coherent anti-stokes raman signals from broadband pulses," Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

N. Dudovich, B. Dayan, S. M. Gallagher Faeder, and Y. Silberberg, "Transform-limited pulses are not optimal for resonant multiphoton transitions," Phys. Rev. Lett. 86, 47 (2001).
[CrossRef] [PubMed]

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

D. Meshulach and Y. Silberberg, "Coherent quantum control of two-photon transitions by a femtosecond laser pulse," Nature (London) 396, 239 (1998).
[CrossRef]

Sorokin, P. P.

R. T. Hodgson, P. P. Sorokin, and J. J. Wynne, "Tunable coherent vacuum-ultraviolet generation in atomic vapors," Phys. Rev. Lett. 32, 343 (1974).
[CrossRef]

Stauffer, H. U.

H. U. Stauffer, J. B. Ballard, Z. Amitay, and S. R. Leone, "Simultaneous phase control of Li2 wave packets in two electronic states," J. Chem. Phys. 116, 946 (2002).
[CrossRef]

Stoicheff, B. P.

P. H. Herman, P. E. LaRocque, R. H. Lipson, W. Jamroz, and B. P. Stoicheff, "Vacuum ultraviolet laser spectroscopy III: laboratory sources of coherent radiation tunable from 105 to 175 nm using Mg, Zn, and Hg vapors," Can. J. Phys. 63, 1581 (1985).
[CrossRef]

T. J. McKee, B. P. Stoicheff, and S. C. Wallace, "Tunable, coherent radiation in the Lyman-α region (1210-1290 A) using magnesium vapor," Opt. Lett. 3,207 (1978).
[CrossRef] [PubMed]

Tannor, D. J.

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

Tobey, R.

Tomkins, F. S.

Trallero-Herrero, C.

S. D. Clow, C. Trallero-Herrero, T. Bergeman, and T. Weinacht, "Strong field multiphoton inversion of a threelevel system using shaped ultrafast laser pulses," Phys. Rev. Lett. 100, 233603 (2008).
[CrossRef] [PubMed]

C. Trallero-Herrero, J. L. Cohen, and T. Weinacht, "Strong-field atomic phase matching," Phys. Rev. Lett. 96, 063603 (2006).
[CrossRef] [PubMed]

Ubachs, W.

Vacano, B.

B. 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 (2008).
[CrossRef]

van Duijn, E-J.

Vogt, G.

P. Nuernberger, G. Vogt, T. Brixner, and G. Gerber, "Femtosecond quantum control of molecular dynamics in the condensed phase," Phys. Chem. Chem. Phys. 9, 2470 (2007).
[CrossRef] [PubMed]

Wallace, S. C.

T. J. McKee, B. P. Stoicheff, and S. C. Wallace, "Tunable, coherent radiation in the Lyman-α region (1210-1290 A) using magnesium vapor," Opt. Lett. 3,207 (1978).
[CrossRef] [PubMed]

S. C. Wallace and G. Zdasiuk, "High-efficiency four-wave sum mixing in magnesium at 140 nm," Appl. Phys. Lett. 28, 449 (1976).
[CrossRef]

Wallenstein, R.

G. Hilber, A. Lago, and R. Wallenstein, "Broadly tunable vacuum-ultraviolet/extreme-ultraviolet radiation generated by resonant third-order frequency conversion in krypton," J. Opt. Soc. Am. B 4, 1735 (1987).
[CrossRef]

R. Hilbig and R. Wallenstein, "Resonant sum and difference frequency mixing in Hg," IEEE J. Quantum Electron. 19, 1759 (1983).
[CrossRef]

Warren, W. S.

W. S. Warren, H. Rabitz, and D. Mahleh, "Coherent control of quantum dynamics: the dream is alive," Science 259, 1581 (1993).
[CrossRef] [PubMed]

Weinacht, T.

S. D. Clow, C. Trallero-Herrero, T. Bergeman, and T. Weinacht, "Strong field multiphoton inversion of a threelevel system using shaped ultrafast laser pulses," Phys. Rev. Lett. 100, 233603 (2008).
[CrossRef] [PubMed]

C. Trallero-Herrero, J. L. Cohen, and T. Weinacht, "Strong-field atomic phase matching," Phys. Rev. Lett. 96, 063603 (2006).
[CrossRef] [PubMed]

Weiner, A. M.

A. M. Weiner, "Femtosecond pulse shaping using spatial light modulators," Rev. Sci. Instrum. 71, 1929 (2000).
[CrossRef]

Whitaker, B. J.

N. T. Form, B. J. Whitaker, and C. Meier, "Enhancing the probability of three-photon absorption in iodine through pulse shaping," J. Phys. B 41, 074011 (2008).
[CrossRef]

Wollenhaupt, M.

M. Wollenhaupt, A. Praelt, C. Sarpe-Tudoran, D. Liese, T. Bayer, and T. Baumert, "Femtosecond strong-field quantum control with sinusoidally phase-modulated pulses," Phys. Rev. A 73, 063409 (2006).
[CrossRef]

Wrzesinski, P. J.

Wynne, J. J.

R. T. Hodgson, P. P. Sorokin, and J. J. Wynne, "Tunable coherent vacuum-ultraviolet generation in atomic vapors," Phys. Rev. Lett. 32, 343 (1974).
[CrossRef]

Xu, B.

Yelin, D.

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Narrow-band coherent anti-stokes raman signals from broadband pulses," Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

Young, J. F.

J. F. Young, G. C. Bjorklund, A. H. Kung, R. B. Miles, and S. E. Harris, "Third-harmonic generation in phasematched Rb vapor," Phys. Rev. Lett. 27, 1551 (1971).
[CrossRef]

Zdasiuk, G.

S. C. Wallace and G. Zdasiuk, "High-efficiency four-wave sum mixing in magnesium at 140 nm," Appl. Phys. Lett. 28, 449 (1976).
[CrossRef]

Annu. Rev. Phys. Chem. (1)

R. J. Gordon and S. A. Rice, "Active control of the dynamics of atoms and molecules," Annu. Rev. Phys. Chem. 48, 601 (1997).
[CrossRef] [PubMed]

Appl. Phys. Lett. (2)

O. Katz, A. Natan, Y. Silberberg, and S. Rosenwaks, "Standoff detection of trace amounts of solids by nonlinear Raman spectroscopy using shaped femtosecond pulses," Appl. Phys. Lett. 92, 171116 (2008).
[CrossRef]

S. C. Wallace and G. Zdasiuk, "High-efficiency four-wave sum mixing in magnesium at 140 nm," Appl. Phys. Lett. 28, 449 (1976).
[CrossRef]

Can. J. Phys. (1)

P. H. Herman, P. E. LaRocque, R. H. Lipson, W. Jamroz, and B. P. Stoicheff, "Vacuum ultraviolet laser spectroscopy III: laboratory sources of coherent radiation tunable from 105 to 175 nm using Mg, Zn, and Hg vapors," Can. J. Phys. 63, 1581 (1985).
[CrossRef]

Chem. Rev. (1)

M. Dantus and V. V. Lozovoy, "Experimental coherent laser control of physicochemical processes," Chem. Rev. 104, 1813 (2004).
[CrossRef] [PubMed]

ChemPhysChem (1)

T. Brixner and G. Gerber, "Quantum Control of Gas-Phase and Liquid-Phase Femtochemistry," ChemPhysChem 4, 418 (2003).
[CrossRef] [PubMed]

IEEE J. Quantum Electron. (1)

R. Hilbig and R. Wallenstein, "Resonant sum and difference frequency mixing in Hg," IEEE J. Quantum Electron. 19, 1759 (1983).
[CrossRef]

IEEE J. Sel. Top. Quantum Electron. (1)

Q3. J. G. Eden, "From N2 (337 nm) to high-order harmonic generation: 40 years of coherent source development in the UV and VUV," IEEE J. Sel. Top. Quantum Electron. 6, 1051 (2000), and references therein.
[CrossRef]

J. Chem. Phys. (2)

H. U. Stauffer, J. B. Ballard, Z. Amitay, and S. R. Leone, "Simultaneous phase control of Li2 wave packets in two electronic states," J. Chem. Phys. 116, 946 (2002).
[CrossRef]

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

J. Opt. Soc. Am. B (3)

J. Phys. B (2)

N. T. Form, B. J. Whitaker, and C. Meier, "Enhancing the probability of three-photon absorption in iodine through pulse shaping," J. Phys. B 41, 074011 (2008).
[CrossRef]

L. Chuntonov, L. Rybak, A. Gandman, and Z. Amitay, "Frequency-domain coherent control of femtosecond two-photon absorption: intermediate-field versus weak-field regime," J. Phys. B 41, 035504 (2008).
[CrossRef]

Nature (London) (2)

D. Meshulach and Y. Silberberg, "Coherent quantum control of two-photon transitions by a femtosecond laser pulse," Nature (London) 396, 239 (1998).
[CrossRef]

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy," Nature (London) 418, 512 (2002).
[CrossRef]

Opt. Express (1)

Opt. Lett. (7)

Phys. Chem. Chem. Phys. (2)

B. 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 (2008).
[CrossRef]

P. Nuernberger, G. Vogt, T. Brixner, and G. Gerber, "Femtosecond quantum control of molecular dynamics in the condensed phase," Phys. Chem. Chem. Phys. 9, 2470 (2007).
[CrossRef] [PubMed]

Phys. Rev. A (5)

X. Dai, E. W. Lerch, and S. R. Leone, "Coherent control through near-resonant Raman transitions," Phys. Rev. A 73, 023404 (2006).
[CrossRef]

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

A. Prakelt, M. Wollenhaupt, C. Sarpe-Tudoran, and T. Baumert, "Phase control of a two-photon transition with shaped femtosecond laser-pulse sequences," Phys. Rev. A 70, 063407 (2004).
[CrossRef]

A. Gandman, L. Chuntonov, L. Rybak, and Z. Amitay, "Pulse-bandwidth dependence of coherent phase control of resonance-mediated (2+1) three-photon absorption," Phys. Rev. A 76, 053419 (2007).
[CrossRef]

M. Wollenhaupt, A. Praelt, C. Sarpe-Tudoran, D. Liese, T. Bayer, and T. Baumert, "Femtosecond strong-field quantum control with sinusoidally phase-modulated pulses," Phys. Rev. A 73, 063409 (2006).
[CrossRef]

Phys. Rev. Lett. (8)

Z. Amitay, A. Gandman, L. Chuntonov, and L. Rybak, "Multichannel selective femtosecond coherent control based on symmetry properties," Phys. Rev. Lett. 100, 193002 (2008).
[CrossRef] [PubMed]

N. Dudovich, B. Dayan, S. M. Gallagher Faeder, and Y. Silberberg, "Transform-limited pulses are not optimal for resonant multiphoton transitions," Phys. Rev. Lett. 86, 47 (2001).
[CrossRef] [PubMed]

D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, "Narrow-band coherent anti-stokes raman signals from broadband pulses," Phys. Rev. Lett. 88, 063004 (2002).
[CrossRef] [PubMed]

N. Dudovich, T. Polack, A. Pe’er, and Y. Silberberg, "Simple route to strong-field coherent control," Phys. Rev. Lett. 94,083002 (2005).
[CrossRef] [PubMed]

C. Trallero-Herrero, J. L. Cohen, and T. Weinacht, "Strong-field atomic phase matching," Phys. Rev. Lett. 96, 063603 (2006).
[CrossRef] [PubMed]

S. D. Clow, C. Trallero-Herrero, T. Bergeman, and T. Weinacht, "Strong field multiphoton inversion of a threelevel system using shaped ultrafast laser pulses," Phys. Rev. Lett. 100, 233603 (2008).
[CrossRef] [PubMed]

J. F. Young, G. C. Bjorklund, A. H. Kung, R. B. Miles, and S. E. Harris, "Third-harmonic generation in phasematched Rb vapor," Phys. Rev. Lett. 27, 1551 (1971).
[CrossRef]

R. T. Hodgson, P. P. Sorokin, and J. J. Wynne, "Tunable coherent vacuum-ultraviolet generation in atomic vapors," Phys. Rev. Lett. 32, 343 (1974).
[CrossRef]

Rev. Sci. Instrum. (1)

A. M. Weiner, "Femtosecond pulse shaping using spatial light modulators," Rev. Sci. Instrum. 71, 1929 (2000).
[CrossRef]

Science (2)

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

W. S. Warren, H. Rabitz, and D. Mahleh, "Coherent control of quantum dynamics: the dream is alive," Science 259, 1581 (1993).
[CrossRef] [PubMed]

Other (7)

M. Shapiro and P. Brumer, Principles of the quantum control of molecular processes (Wiley, New Jersey, 2003).

S. H. Lim, A. G. Caster, and S. R. Leone, "Single-pulse phase-control interferometric coherent anti-Stokes Raman scattering spectroscopy," Phys. Rev. A 72, 041803(R) (2005).
[CrossRef]

B. Chatel, J. Degert, S. Stock, and B. Girard, "Competition between sequential and direct paths in a two-photon transition," Phys. Rev. A 68, 041402(R) (2003).
[CrossRef]

L. Chuntonov, L. Rybak, A. Gandman, and Z. Amitay, "Enhancement of intermediate-field two-photon absorption by rationally shaped femtosecond pulses," Phys. Rev. A 77, 021403(R) (2008).
[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(R) (2007).
[CrossRef]

L. Allen and J. H. Eberly, Optical Resonance and Two-Level Atom (Dover Publications, New York, 1987).

L. Rybak, L. Chuntonov, A. Gandman, N. Shakour, and Z. Amitay are preparing a manuscript to be called "Measurements of collisional dephasing of 3s-4s Na coherent superpositions by femtosecond four-wave mixing."

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Figures (2)

Fig. 1.
Fig. 1.

The generation of coherent broadband UV radiation via resonance-mediated (2+1) three-photon excitation in Na. Several sets of three-photon pathways that are on resonance (δ=0) or near resonance (δ≠0) with the intermediate state |r〉≡4s are shown. The inset shows the two NIR excitation pulse spectra with (thick gray line) and without (thin black line) a resonant access to |v R〉≡7p.

Fig. 2.
Fig. 2.

Experimental (circles) and theoretical (solid lines) results for the total UV yield generated by shaped NIR pulses with spectral π phase step, when the excitation pulse spectrum (a1) allows and (b1) blocks the resonant access to 7p (see Fig. 1). The UV yield is shown as a function of the position of the NIR π phase step. The traces are normalized by the yield generated by the corresponding transform-limited (TL) pulse. The UV spectra generated by the NIR TL pulses in the two cases are shown in panels (a2) and (b2).

Equations (10)

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μ ( t ) = j j a j ( t ) * a j ( t ) μ j , j e i ω j , j t ,
μ ( 3 ) ( t ) = j j a j ( 3 ) ( t ) * a j ( 0 ) ( t ) μ j , j e i ω j , j t + a j ( 2 ) ( t ) * a j ( 1 ) ( t ) μ j , j e i ω j , j t + c . c . ,
a j ( n ) ( t ) = 1 i h ̅ j μ j , j t a j ( n 1 ) ( t ) E ( t ) e i ω j , j t dt ,
E UV ( ω UV ) μ r , g 2 [ D R ( UV ) ( ω UV ) + D nonR ( UV ) ] A ( 2 + 1 ) ( ω UV ) ,
A ( 2 + 1 ) ( ω UV ) = A ( 2 + 1 ) on res ( ω UV ) + A ( 2 + 1 ) near res ( ω UV ) ,
A ( 2 + 1 ) on res ( ω UV ) = i π E ( ω UV ω r , g ) A ( 2 ) ( ω r , g ) ,
A ( 2 + 1 ) near res ( ω UV ) = 1 δ A ( 2 ) ( ω r , g δ ) E ( ω UV ω r , g + δ ) d δ ,
A ( 2 ) ( Ω ) = E ( ω ) E ( Ω ω ) d ω ,
D R ( UV ) ( ω UV ) = μ g , v R μ v R , r ω v R , g ω UV + i Γ v R ,
D nonR ( UR ) = v j v R μ g , v j μ v j , r ω v j , g ( ω r , g + ω 0 ) = v j v R μ g , v j μ v j , r ω v j , r ω 0 ,

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