OSA's Digital Library

Journal of the Optical Society of America B

Journal of the Optical Society of America B


  • Vol. 20, Iss. 11 — Nov. 1, 2003
  • pp: 2255–2261

Coherent control and phase locking of two-photon processes in the nanosecond domain

Qun Zhang, Mark Keil, and Moshe Shapiro  »View Author Affiliations

JOSA B, Vol. 20, Issue 11, pp. 2255-2261 (2003)

View Full Text Article

Enhanced HTML    Acrobat PDF (162 KB)

Browse Journals / Lookup Meetings

Browse by Journal and Year


Lookup Conference Papers

Close Browse Journals / Lookup Meetings

Article Tools



We demonstrate phase locking between two pairs of nanosecond laser pulses generated from independent sources. We achieve phase locking experimentally by separately mixing two uncorrelated dye lasers of frequencies ω1(a) and ω1(b), with a common beam of frequency ω0, thereby generating two additional frequencies ω2(b)ω1(a)+ω0 and ω2(a)ω1(b)+ω0. We demonstrate that there are well-defined phase relationships between any two-photon process using the ω1(a) and the ω2(a) pair of frequencies versus any two-photon process that uses the ω1(b) and the ω2(b) pair. In particular, interference between the two identical sum frequencies ωtotal=ω1(a)+ω2(a) and ωtotal=ω1(b)+ω2(b), which we generate in a separate pair of mixing crystals, yields stable interference fringes with measured modulation depths of ±40%. Well-defined phase relationships are especially useful for two-photon versus two-photon coherent control experiments. In addition, the system can be used to transport, with a high degree of stability, the phase of a given input laser frequency ω0 to higher frequencies ωtotal by use of carrier lasers that need not be correlated.

© 2003 Optical Society of America

OCIS Codes
(020.1670) Atomic and molecular physics : Coherent optical effects
(020.4180) Atomic and molecular physics : Multiphoton processes
(030.1640) Coherence and statistical optics : Coherence
(060.0060) Fiber optics and optical communications : Fiber optics and optical communications
(120.0120) Instrumentation, measurement, and metrology : Instrumentation, measurement, and metrology
(270.1670) Quantum optics : Coherent optical effects

Qun Zhang, Mark Keil, and Moshe Shapiro, "Coherent control and phase locking of two-photon processes in the nanosecond domain," J. Opt. Soc. Am. B 20, 2255-2261 (2003)

Sort:  Author  |  Year  |  Journal  |  Reset  


  1. M. Shapiro and P. Brumer, Principles of the Quantum Control of Molecular Processes (Wiley, Hoboken, N.J., 2003).
  2. S. A. Rice, “Interfering for the good of a chemical reaction,” Nature 409, 422–426 (2001). [CrossRef] [PubMed]
  3. R. N. Zare, “Laser control of chemical reactions,” Science 279, 1875–1879 (1998). [CrossRef] [PubMed]
  4. R. J. Gordon and S. A. Rice, “Active control of the dynamics of atoms and molecules,” Annu. Rev. Phys. Chem. 48, 601–641 (1997). [CrossRef] [PubMed]
  5. M. Shapiro and P. Brumer, “Coherent control of atomic, molecular, and electronic processes,” Adv. At., Mol., Opt. Phys. 42, 287–345 (2000). [CrossRef]
  6. R. J. Gordon, L. Zhu, and T. Seideman, “Coherent control of chemical reactions,” Acc. Chem. Res. 32, 1007–1016 (1999). [CrossRef]
  7. R. Bersohn, “Coherent control of photoexcitation processes,” J. Mol. Struct. 480–481, 231–235 (1999). [CrossRef]
  8. M. Shapiro and P. Brumer, “Quantum control of chemical reactions,” J. Chem. Soc., Faraday Trans. 93, 1263–1277 (1997). [CrossRef]
  9. P. Brumer and M. Shapiro, “Coherence chemistry: controlling chemical reactions with lasers,” Acc. Chem. Res. 22, 407–413 (1989). [CrossRef]
  10. 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]
  11. A. Assion, T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, “Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses,” Science 282, 919–922 (1998). [CrossRef] [PubMed]
  12. H. Rabitz, T. Kobayashi, R. W. Field, and D. J. Tannor, “Ramifications of feedback for control of quantum dynamics,” Adv. Chem. Phys. 101, 315–325 (1997).
  13. W. S. Warren, H. Rabitz, and M. Dahleh, “Coherent control of quantum dynamics: the dream is alive,” Science 259, 1581–1589 (1993). [CrossRef] [PubMed]
  14. D. J. Tannor and S. A. Rice, “Coherent pulse sequence control of product formation in chemical reactions,” Adv. Chem. Phys. 70, 441–523 (1988).
  15. P. Brumer and M. Shapiro, “Control of unimolecular reactions using coherent light,” Chem. Phys. Lett. 126, 541–546 (1986). [CrossRef]
  16. M. Shapiro and P. Brumer, “Laser control of product quantum state populations in unimolecular reactions,” J. Chem. Phys. 84, 4103–4104 (1986). [CrossRef]
  17. M. Shapiro, J. W. Hepburn, and P. Brumer, “Simplified laser control of unimolecular reactions: simultaneous (ω1, ω3) excitation,” Chem. Phys. Lett. 149, 451–454 (1988). [CrossRef]
  18. C. Chen, Y.-Y. Yin, and D. S. Elliott, “Interference between optical transitions,” Phys. Rev. Lett. 64, 507–510 (1990). [CrossRef] [PubMed]
  19. S. M. Park, S.-P. Lu, and R. J. Gordon, “Coherent laser control of the resonance-enhanced multiphoton ionization of HCl,” J. Chem. Phys. 94, 8622–8624 (1991). [CrossRef]
  20. S.-P. Lu, S. M. Park, Y. Xie, and R. J. Gordon, “Coherent laser control of bound-to-bound transitions of HCl and CO,” J. Chem. Phys. 96, 6613–6620 (1992). [CrossRef]
  21. V. D. Kleiman, L. Zhu, X. Li, and R. J. Gordon, “Coherent phase control of the photoionization of H2S,” J. Chem. Phys. 102, 5863–5866 (1995). [CrossRef]
  22. L. Zhu, V. D. Kleiman, X. Li, S. P. Lu, K. Trentelman, and R. J. Gordon, “Coherent laser control of the product distribution obtained in the photoexcitation of HI,” Science 270, 77–80 (1995). [CrossRef]
  23. X. Wang, R. Bersohn, K. Takahashi, M. Kawasaki, and H. L. Kim, “Phase control of absorption in large polyatomic molecules,” J. Chem. Phys. 105, 2992–2997 (1996). [CrossRef]
  24. Little modulation of the phase-sensitive signal will be ap-parent if the experimental signal from one pathway greatly exceeds that of the other.
  25. R. J. Gordon, S.-P. Lu, S. M. Park, K. Trentelman, Y. Xie, L. Zhu, A. Kumar, and W. J. Meath, “The use of coherent phase control of multiphoton ionization to measure the refractive indices of H2 and Ar between 1100 and 1150 Å,” J. Chem. Phys. 98, 9481–9486 (1993). [CrossRef]
  26. E. Papastathopoulos, D. Xenakis, and D. Charalambidis, “Phase-sensitive ionization through multiphoton-excitation schemes involving even numbers of photons,” Phys. Rev. A 59, 4840–4842 (1999). [CrossRef]
  27. Z. Chen, P. Brumer, and M. Shapiro, “Coherent radiative control of molecular photodissociation via resonant two-photon versus two-photon interference,” Chem. Phys. Lett. 198, 498–504 (1992). [CrossRef]
  28. Z. Chen, P. Brumer, and M. Shapiro, “Multiproduct coherent control of photodissociation via two-photon versus two-photon interference,” J. Chem. Phys. 98, 6843–6852 (1993). [CrossRef]
  29. S. T. Pratt, “Interference effects in the two-photon ionization of nitric oxide,” J. Chem. Phys. 104, 5776–5783 (1996). [CrossRef]
  30. F. Wang, C. Chen, and D. S. Elliott, “Product state control through interfering excitation routes,” Phys. Rev. Lett. 77, 2416–2419 (1996). [CrossRef] [PubMed]
  31. N. Ph. Georgiades, E. S. Polzik, and H. J. Kimble, “Frequency metrology by use of quantum interference,” Opt. Lett. 21, 1688–1690 (1996). [CrossRef]
  32. J. J. McFerran and A. N. Luiten, “Coherent bisection of 141 THz using sum frequency generation of 1064 nm and 709 nm radiation,” Opt. Quantum Electron. 34, 841–858 (2002). [CrossRef]
  33. N. F. Scherer, A. J. Ruggiero, M. Du, and G. R. Fleming, “Time resolved dynamics of isolated molecular systems studied with phase-locked femtosecond pulse pairs,” J. Chem. Phys. 93, 856–857 (1990). [CrossRef]
  34. J. H. Yi, S. H. Kim, and Y. K. Kwak, “A nanometric displacement measurement method using the detection of fringe peak movement,” Meas. Sci. Technol. 11, 1352–1358 (2000). [CrossRef]
  35. These red wavelengths are resonant with the transitions X 1Σg+(v=0,  J=15)→A 1Σu+(v=7,  J=14) and X 1Σg+(v=0,  J=15)→A 1Σu+(v=6,  J=14) in Na2, which are being used for coherent control photodissociation experiments currently under way in our laboratory.

Cited By

Alert me when this paper is cited

OSA is able to provide readers links to articles that cite this paper by participating in CrossRef's Cited-By Linking service. CrossRef includes content from more than 3000 publishers and societies. In addition to listing OSA journal articles that cite this paper, citing articles from other participating publishers will also be listed.

« Previous Article  |  Next Article »

OSA is a member of CrossRef.

CrossCheck Deposited