Abstract

Our simulations show a copropagating pair of laser pulses polarized in two different directions can selectively excite clockwise or counterclockwise molecular rotation in a gas of linear molecules. The resulting birefringence of the gas rotates on a femtosecond timescale and shows a periodic revival structure. The total duration of the pulse pair can be subpicosecond, allowing molecular alignment at the high densities and temperatures necessary to create a transient spinning waveplate.

© 2009 Optical Society of America

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  1. R. Bartels, T. Weinacht, N. Wagner, M. Baertschy, C. Greene, M. Murnane, and H. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88(1) (2002).
    [PubMed]
  2. N. Zhavoronkov and G. Korn, "Generation of single intense short optical pulses by ultrafast molecular phase modulation," Phys. Rev. Lett. 88(20), 203901 (2002).
    [CrossRef] [PubMed]
  3. S. Varma, Y.-H. Chen, and H. M. Milchberg, "Trapping and destruction of long-range high-intensity optical filaments by molecular quantum wakes in air," Phys. Rev. Lett. 101(20), 205001 (2008).
    [CrossRef] [PubMed]
  4. F. Calegari, C. Vozzi, and S. Stagira, "Optical propagation in molecular gases undergoing filamentation-assisted field-free alignment," Phys. Rev. A 79(2), 023827 (2009).
    [CrossRef]
  5. A. G. York and H. M. Milchberg, "Broadband terahertz lasing in aligned molecules," Opt. Express,  16(14), 10557-10564 (2008).
    [CrossRef] [PubMed]
  6. Y.-H. Chen, S. Varma, A. York, and H. M. Milchberg, "Single-shot space- and time-resolved measurement of rotational wavepacket revivals in H2, D2, N2, O2, and N2O," Opt. Express 15(18), 1341-11357 (2007).
    [CrossRef] [PubMed]
  7. K. Hartinger and R. A. Bartels, "Single-shot measurement of ultrafast time-varying phase modulation induced by femtosecond laser pulses with arbitrary polarization," Applied Physics Letters 92(2), 021126 (2008).
    [CrossRef]
  8. D. M. Villeneuve, S. A. Aseyev, P. Dietrich, M. Spanner, M. Yu. Ivanov, and P. B. Corkum, "Forced molecular rotation in an optical centrifuge," Phys. Rev. Lett. 85(3), 542-545 (2000).
    [CrossRef] [PubMed]
  9. T. Brixner, G. Krampert, T. Pfeifer, R. Selle, G. Gerber, M. Wollenhaupt, O. Graefe, C. Horn, D. Liese, and T. Baumert. "Quantum control by ultrafast polarization shaping," Phys. Rev. Lett. 92(20), 208301 (2004).
    [CrossRef] [PubMed]
  10. K. Hartinger and R. A. Bartels, "Pulse polarization splitting in a transient wave plate," Opt. Lett. 31(23), 3526- 3528 (2006).
    [CrossRef] [PubMed]
  11. C. Marceau, Y. Chen, F. Th’eberge, M. Chateauneuf, J. Dubois, and S. L. Chin, "Ultrafast birefringence induced by a femtosecond laser filament in gases," Opt. Lett. 34(9), :417-1419 (2009).
    [CrossRef] [PubMed]
  12. P. Bejot, Y. Petit, L. Bonacina, J. Kasparian, M. Moret, and J.-P. Wolf, "Ultrafast gaseous "half-wave plate," Opt. Express 16(10), 7564-7570 (2008).
    [CrossRef] [PubMed]
  13. A. R. Edmonds, Angular momentum in quantum mechanics (Princeton University Press, 1996).
  14. W. Schweizer, Numerical quantum dynamics (Springer, 2001).

2009

F. Calegari, C. Vozzi, and S. Stagira, "Optical propagation in molecular gases undergoing filamentation-assisted field-free alignment," Phys. Rev. A 79(2), 023827 (2009).
[CrossRef]

C. Marceau, Y. Chen, F. Th’eberge, M. Chateauneuf, J. Dubois, and S. L. Chin, "Ultrafast birefringence induced by a femtosecond laser filament in gases," Opt. Lett. 34(9), :417-1419 (2009).
[CrossRef] [PubMed]

2008

P. Bejot, Y. Petit, L. Bonacina, J. Kasparian, M. Moret, and J.-P. Wolf, "Ultrafast gaseous "half-wave plate," Opt. Express 16(10), 7564-7570 (2008).
[CrossRef] [PubMed]

A. G. York and H. M. Milchberg, "Broadband terahertz lasing in aligned molecules," Opt. Express,  16(14), 10557-10564 (2008).
[CrossRef] [PubMed]

K. Hartinger and R. A. Bartels, "Single-shot measurement of ultrafast time-varying phase modulation induced by femtosecond laser pulses with arbitrary polarization," Applied Physics Letters 92(2), 021126 (2008).
[CrossRef]

S. Varma, Y.-H. Chen, and H. M. Milchberg, "Trapping and destruction of long-range high-intensity optical filaments by molecular quantum wakes in air," Phys. Rev. Lett. 101(20), 205001 (2008).
[CrossRef] [PubMed]

2007

2006

2004

T. Brixner, G. Krampert, T. Pfeifer, R. Selle, G. Gerber, M. Wollenhaupt, O. Graefe, C. Horn, D. Liese, and T. Baumert. "Quantum control by ultrafast polarization shaping," Phys. Rev. Lett. 92(20), 208301 (2004).
[CrossRef] [PubMed]

2002

R. Bartels, T. Weinacht, N. Wagner, M. Baertschy, C. Greene, M. Murnane, and H. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88(1) (2002).
[PubMed]

N. Zhavoronkov and G. Korn, "Generation of single intense short optical pulses by ultrafast molecular phase modulation," Phys. Rev. Lett. 88(20), 203901 (2002).
[CrossRef] [PubMed]

2000

D. M. Villeneuve, S. A. Aseyev, P. Dietrich, M. Spanner, M. Yu. Ivanov, and P. B. Corkum, "Forced molecular rotation in an optical centrifuge," Phys. Rev. Lett. 85(3), 542-545 (2000).
[CrossRef] [PubMed]

Aseyev, S. A.

D. M. Villeneuve, S. A. Aseyev, P. Dietrich, M. Spanner, M. Yu. Ivanov, and P. B. Corkum, "Forced molecular rotation in an optical centrifuge," Phys. Rev. Lett. 85(3), 542-545 (2000).
[CrossRef] [PubMed]

Baertschy, M.

R. Bartels, T. Weinacht, N. Wagner, M. Baertschy, C. Greene, M. Murnane, and H. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88(1) (2002).
[PubMed]

Bartels, R.

R. Bartels, T. Weinacht, N. Wagner, M. Baertschy, C. Greene, M. Murnane, and H. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88(1) (2002).
[PubMed]

Bartels, R. A.

K. Hartinger and R. A. Bartels, "Single-shot measurement of ultrafast time-varying phase modulation induced by femtosecond laser pulses with arbitrary polarization," Applied Physics Letters 92(2), 021126 (2008).
[CrossRef]

K. Hartinger and R. A. Bartels, "Pulse polarization splitting in a transient wave plate," Opt. Lett. 31(23), 3526- 3528 (2006).
[CrossRef] [PubMed]

Baumert, T.

T. Brixner, G. Krampert, T. Pfeifer, R. Selle, G. Gerber, M. Wollenhaupt, O. Graefe, C. Horn, D. Liese, and T. Baumert. "Quantum control by ultrafast polarization shaping," Phys. Rev. Lett. 92(20), 208301 (2004).
[CrossRef] [PubMed]

Brixner, T.

T. Brixner, G. Krampert, T. Pfeifer, R. Selle, G. Gerber, M. Wollenhaupt, O. Graefe, C. Horn, D. Liese, and T. Baumert. "Quantum control by ultrafast polarization shaping," Phys. Rev. Lett. 92(20), 208301 (2004).
[CrossRef] [PubMed]

Calegari, F.

F. Calegari, C. Vozzi, and S. Stagira, "Optical propagation in molecular gases undergoing filamentation-assisted field-free alignment," Phys. Rev. A 79(2), 023827 (2009).
[CrossRef]

Chen, Y.

Chen, Y.-H.

S. Varma, Y.-H. Chen, and H. M. Milchberg, "Trapping and destruction of long-range high-intensity optical filaments by molecular quantum wakes in air," Phys. Rev. Lett. 101(20), 205001 (2008).
[CrossRef] [PubMed]

Y.-H. Chen, S. Varma, A. York, and H. M. Milchberg, "Single-shot space- and time-resolved measurement of rotational wavepacket revivals in H2, D2, N2, O2, and N2O," Opt. Express 15(18), 1341-11357 (2007).
[CrossRef] [PubMed]

Corkum, P. B.

D. M. Villeneuve, S. A. Aseyev, P. Dietrich, M. Spanner, M. Yu. Ivanov, and P. B. Corkum, "Forced molecular rotation in an optical centrifuge," Phys. Rev. Lett. 85(3), 542-545 (2000).
[CrossRef] [PubMed]

Dietrich, P.

D. M. Villeneuve, S. A. Aseyev, P. Dietrich, M. Spanner, M. Yu. Ivanov, and P. B. Corkum, "Forced molecular rotation in an optical centrifuge," Phys. Rev. Lett. 85(3), 542-545 (2000).
[CrossRef] [PubMed]

Gerber, G.

T. Brixner, G. Krampert, T. Pfeifer, R. Selle, G. Gerber, M. Wollenhaupt, O. Graefe, C. Horn, D. Liese, and T. Baumert. "Quantum control by ultrafast polarization shaping," Phys. Rev. Lett. 92(20), 208301 (2004).
[CrossRef] [PubMed]

Graefe, O.

T. Brixner, G. Krampert, T. Pfeifer, R. Selle, G. Gerber, M. Wollenhaupt, O. Graefe, C. Horn, D. Liese, and T. Baumert. "Quantum control by ultrafast polarization shaping," Phys. Rev. Lett. 92(20), 208301 (2004).
[CrossRef] [PubMed]

Greene, C.

R. Bartels, T. Weinacht, N. Wagner, M. Baertschy, C. Greene, M. Murnane, and H. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88(1) (2002).
[PubMed]

Hartinger, K.

K. Hartinger and R. A. Bartels, "Single-shot measurement of ultrafast time-varying phase modulation induced by femtosecond laser pulses with arbitrary polarization," Applied Physics Letters 92(2), 021126 (2008).
[CrossRef]

K. Hartinger and R. A. Bartels, "Pulse polarization splitting in a transient wave plate," Opt. Lett. 31(23), 3526- 3528 (2006).
[CrossRef] [PubMed]

Horn, C.

T. Brixner, G. Krampert, T. Pfeifer, R. Selle, G. Gerber, M. Wollenhaupt, O. Graefe, C. Horn, D. Liese, and T. Baumert. "Quantum control by ultrafast polarization shaping," Phys. Rev. Lett. 92(20), 208301 (2004).
[CrossRef] [PubMed]

Ivanov, M. Yu.

D. M. Villeneuve, S. A. Aseyev, P. Dietrich, M. Spanner, M. Yu. Ivanov, and P. B. Corkum, "Forced molecular rotation in an optical centrifuge," Phys. Rev. Lett. 85(3), 542-545 (2000).
[CrossRef] [PubMed]

Kapteyn, H.

R. Bartels, T. Weinacht, N. Wagner, M. Baertschy, C. Greene, M. Murnane, and H. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88(1) (2002).
[PubMed]

Korn, G.

N. Zhavoronkov and G. Korn, "Generation of single intense short optical pulses by ultrafast molecular phase modulation," Phys. Rev. Lett. 88(20), 203901 (2002).
[CrossRef] [PubMed]

Krampert, G.

T. Brixner, G. Krampert, T. Pfeifer, R. Selle, G. Gerber, M. Wollenhaupt, O. Graefe, C. Horn, D. Liese, and T. Baumert. "Quantum control by ultrafast polarization shaping," Phys. Rev. Lett. 92(20), 208301 (2004).
[CrossRef] [PubMed]

Liese, D.

T. Brixner, G. Krampert, T. Pfeifer, R. Selle, G. Gerber, M. Wollenhaupt, O. Graefe, C. Horn, D. Liese, and T. Baumert. "Quantum control by ultrafast polarization shaping," Phys. Rev. Lett. 92(20), 208301 (2004).
[CrossRef] [PubMed]

Marceau, C.

Milchberg, H. M.

Murnane, M.

R. Bartels, T. Weinacht, N. Wagner, M. Baertschy, C. Greene, M. Murnane, and H. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88(1) (2002).
[PubMed]

Pfeifer, T.

T. Brixner, G. Krampert, T. Pfeifer, R. Selle, G. Gerber, M. Wollenhaupt, O. Graefe, C. Horn, D. Liese, and T. Baumert. "Quantum control by ultrafast polarization shaping," Phys. Rev. Lett. 92(20), 208301 (2004).
[CrossRef] [PubMed]

Selle, R.

T. Brixner, G. Krampert, T. Pfeifer, R. Selle, G. Gerber, M. Wollenhaupt, O. Graefe, C. Horn, D. Liese, and T. Baumert. "Quantum control by ultrafast polarization shaping," Phys. Rev. Lett. 92(20), 208301 (2004).
[CrossRef] [PubMed]

Spanner, M.

D. M. Villeneuve, S. A. Aseyev, P. Dietrich, M. Spanner, M. Yu. Ivanov, and P. B. Corkum, "Forced molecular rotation in an optical centrifuge," Phys. Rev. Lett. 85(3), 542-545 (2000).
[CrossRef] [PubMed]

Stagira, S.

F. Calegari, C. Vozzi, and S. Stagira, "Optical propagation in molecular gases undergoing filamentation-assisted field-free alignment," Phys. Rev. A 79(2), 023827 (2009).
[CrossRef]

Th’eberge, F.

Varma, S.

S. Varma, Y.-H. Chen, and H. M. Milchberg, "Trapping and destruction of long-range high-intensity optical filaments by molecular quantum wakes in air," Phys. Rev. Lett. 101(20), 205001 (2008).
[CrossRef] [PubMed]

Y.-H. Chen, S. Varma, A. York, and H. M. Milchberg, "Single-shot space- and time-resolved measurement of rotational wavepacket revivals in H2, D2, N2, O2, and N2O," Opt. Express 15(18), 1341-11357 (2007).
[CrossRef] [PubMed]

Villeneuve, D. M.

D. M. Villeneuve, S. A. Aseyev, P. Dietrich, M. Spanner, M. Yu. Ivanov, and P. B. Corkum, "Forced molecular rotation in an optical centrifuge," Phys. Rev. Lett. 85(3), 542-545 (2000).
[CrossRef] [PubMed]

Vozzi, C.

F. Calegari, C. Vozzi, and S. Stagira, "Optical propagation in molecular gases undergoing filamentation-assisted field-free alignment," Phys. Rev. A 79(2), 023827 (2009).
[CrossRef]

Wagner, N.

R. Bartels, T. Weinacht, N. Wagner, M. Baertschy, C. Greene, M. Murnane, and H. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88(1) (2002).
[PubMed]

Weinacht, T.

R. Bartels, T. Weinacht, N. Wagner, M. Baertschy, C. Greene, M. Murnane, and H. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88(1) (2002).
[PubMed]

Wollenhaupt, M.

T. Brixner, G. Krampert, T. Pfeifer, R. Selle, G. Gerber, M. Wollenhaupt, O. Graefe, C. Horn, D. Liese, and T. Baumert. "Quantum control by ultrafast polarization shaping," Phys. Rev. Lett. 92(20), 208301 (2004).
[CrossRef] [PubMed]

York, A.

York, A. G.

Zhavoronkov, N.

N. Zhavoronkov and G. Korn, "Generation of single intense short optical pulses by ultrafast molecular phase modulation," Phys. Rev. Lett. 88(20), 203901 (2002).
[CrossRef] [PubMed]

Applied Physics Letters

K. Hartinger and R. A. Bartels, "Single-shot measurement of ultrafast time-varying phase modulation induced by femtosecond laser pulses with arbitrary polarization," Applied Physics Letters 92(2), 021126 (2008).
[CrossRef]

Opt. Express

Opt. Lett.

Phys. Rev. A

F. Calegari, C. Vozzi, and S. Stagira, "Optical propagation in molecular gases undergoing filamentation-assisted field-free alignment," Phys. Rev. A 79(2), 023827 (2009).
[CrossRef]

Phys. Rev. Lett.

R. Bartels, T. Weinacht, N. Wagner, M. Baertschy, C. Greene, M. Murnane, and H. Kapteyn, "Phase modulation of ultrashort light pulses using molecular rotational wave packets," Phys. Rev. Lett. 88(1) (2002).
[PubMed]

N. Zhavoronkov and G. Korn, "Generation of single intense short optical pulses by ultrafast molecular phase modulation," Phys. Rev. Lett. 88(20), 203901 (2002).
[CrossRef] [PubMed]

S. Varma, Y.-H. Chen, and H. M. Milchberg, "Trapping and destruction of long-range high-intensity optical filaments by molecular quantum wakes in air," Phys. Rev. Lett. 101(20), 205001 (2008).
[CrossRef] [PubMed]

D. M. Villeneuve, S. A. Aseyev, P. Dietrich, M. Spanner, M. Yu. Ivanov, and P. B. Corkum, "Forced molecular rotation in an optical centrifuge," Phys. Rev. Lett. 85(3), 542-545 (2000).
[CrossRef] [PubMed]

T. Brixner, G. Krampert, T. Pfeifer, R. Selle, G. Gerber, M. Wollenhaupt, O. Graefe, C. Horn, D. Liese, and T. Baumert. "Quantum control by ultrafast polarization shaping," Phys. Rev. Lett. 92(20), 208301 (2004).
[CrossRef] [PubMed]

Other

A. R. Edmonds, Angular momentum in quantum mechanics (Princeton University Press, 1996).

W. Schweizer, Numerical quantum dynamics (Springer, 2001).

Supplementary Material (1)

» Media 1: MPG (1640 KB)     

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Figures (5)

Fig. 1.
Fig. 1.

Degree of alignment A=〈cos2(θ)〉-1/3 driven by a copropagating pair of 100 fs, 2×1011 W/cm2 alignment pulses with Δθ=π/4, Δt=100 fs, versus probe delay and probe polarization θ p . (Media 1) illustrates the sense of rotation in polar coordinates.

Fig. 2.
Fig. 2.

(a) Maximum (blue) and minimum (red) of A(θ p ) for the same conditions as Fig. 1, (b) θ p,max (blue) and θ p,min (red), (c) ΔA, proportional to birefringence magnitude, all plotted vs. probe delay.

Fig. 3.
Fig. 3.

Effect of alignment pulse relative delay Δt on transient birefringence. Solid green line corresponds to birefringence magnitude (left axis). Dotted blue line gives the direction of birefringence (right axis).

Fig. 4.
Fig. 4.

Effects of alignment pulse relative polarization angle Δθ on transient birefringence. Solid green line corresponds to birefringence magnitude (left axis). Dotted blue line gives the direction of birefringence (right axis).

Fig. 5.
Fig. 5.

Effects of HCN gas temperature T on transient birefringence. Solid green line corresponds to birefringence magnitude (left axis). Dotted blue line gives the direction of birefringence (right axis).

Equations (4)

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

tλj,j+2m,n=λj,j+2m,nP(t)δjm,n+Δjm,nP(t)ej,j+2t
λ (t)=AΔiωδA eiωt0 (eiω(tt0)eδA(tt0)) +λ0eδA(tt0)(t0<t<t0+τ)
j,mρk,n=Σm,nρj,km,nDmmjDn,nk
Dm,mj(α,β,γ)j,m(α,β,γ)j,m =eimαdm,mj(β) eimγ .

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