Abstract

This Letter demonstrates polarization spectroscopy of a velocity selected and vibrationally excited molecular sample. Specifically, the anisotropy induced by a circularly polarized IR pump beam tuned to the R(14.5)1/2v=1v=0 transition of nitric oxide is observed using an IR probe resonant with the R(15.5)1/2v=2v=1 hot band transition. Using two detectors in combination with the rapidly swept probe allows both the absorptive and dispersive components of the excited state polarization to be observed for the first time. The data are well described by simulations based upon a three-level density matrix model.

© 2014 Optical Society of America

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  1. C. Wieman and T. W. Hänsch, Phys. Rev. Lett. 36, 1170 (1976).
    [CrossRef]
  2. C. P. Pearman, C. S. Adams, S. G. Cox, P. F. Griffin, D. A. Smith, and I. G. Hughes, J. Phys. B 35, 5141 (2002).
    [CrossRef]
  3. C. Carr, C. S. Adams, and K. J. Weatherill, Opt. Lett. 37, 118 (2012).
    [CrossRef]
  4. M. L. Harris, C. S. Adams, S. L. Cornish, I. C. McLeod, E. Tarleton, and I. G. Hughes, Phys. Rev. A 73, 062509 (2006).
    [CrossRef]
  5. G. Hancock, G. A. D. Ritchie, J.-P. van Helden, R. Walker, and D. Weidmann, Opt. Eng. 49, 111121 (2010).
    [CrossRef]
  6. R. J. Walker, J. H. van Helden, and G. A. D. Ritchie, Chem. Phys. Lett. 501, 20 (2010).
    [CrossRef]
  7. J. M. R. Kirkbride, S. K. Causier, E. A. McCormack, D. Weidmann, and G. A. D. Ritchie, Phys. Chem. Chem. Phys. 15, 2684 (2013).
    [CrossRef]
  8. J. M. R. Kirkbride, S. K. Causier, A. R. Dalton, D. Weidmann, and G. A. D. Ritchie, J. Chem. Phys. 140, 054311 (2014).
    [CrossRef]
  9. Y. S. Bartalini, S. Borri, and P. De Natale, Opt. Express 17, 7440 (2009).
    [CrossRef]
  10. W. Demtröder, Laser Spectroscopy: Basic Concepts and Instrumentation, 3rd ed. (Springer, 2003), pp. 507–509.
  11. R. J. Walker, J. H. van Helden, J. Kirkbride, E. A. McCormack, M. T. Bell, D. Weidmann, and G. A. D. Ritchie, Opt. Lett. 36, 4725 (2011).
    [CrossRef]
  12. N. Mukherjee and R. N. Zare, J. Chem. Phys 132, 154302 (2010).
    [CrossRef]
  13. N. Mukherjee and R. N. Zare, J. Chem. Phys 133, 094301 (2010).
    [CrossRef]
  14. L. Rothman, I. Gordon, A. Barbe, D. Benner, P. Bernath, M. Birk, V. Boudon, L. Brown, A. Campargue, and J.-P. Champion, J. Quant. Spectrosc. Radiat. Transfer 110, 533 (2009).
    [CrossRef]

2014 (1)

J. M. R. Kirkbride, S. K. Causier, A. R. Dalton, D. Weidmann, and G. A. D. Ritchie, J. Chem. Phys. 140, 054311 (2014).
[CrossRef]

2013 (1)

J. M. R. Kirkbride, S. K. Causier, E. A. McCormack, D. Weidmann, and G. A. D. Ritchie, Phys. Chem. Chem. Phys. 15, 2684 (2013).
[CrossRef]

2012 (1)

2011 (1)

2010 (4)

N. Mukherjee and R. N. Zare, J. Chem. Phys 132, 154302 (2010).
[CrossRef]

N. Mukherjee and R. N. Zare, J. Chem. Phys 133, 094301 (2010).
[CrossRef]

G. Hancock, G. A. D. Ritchie, J.-P. van Helden, R. Walker, and D. Weidmann, Opt. Eng. 49, 111121 (2010).
[CrossRef]

R. J. Walker, J. H. van Helden, and G. A. D. Ritchie, Chem. Phys. Lett. 501, 20 (2010).
[CrossRef]

2009 (2)

Y. S. Bartalini, S. Borri, and P. De Natale, Opt. Express 17, 7440 (2009).
[CrossRef]

L. Rothman, I. Gordon, A. Barbe, D. Benner, P. Bernath, M. Birk, V. Boudon, L. Brown, A. Campargue, and J.-P. Champion, J. Quant. Spectrosc. Radiat. Transfer 110, 533 (2009).
[CrossRef]

2006 (1)

M. L. Harris, C. S. Adams, S. L. Cornish, I. C. McLeod, E. Tarleton, and I. G. Hughes, Phys. Rev. A 73, 062509 (2006).
[CrossRef]

2002 (1)

C. P. Pearman, C. S. Adams, S. G. Cox, P. F. Griffin, D. A. Smith, and I. G. Hughes, J. Phys. B 35, 5141 (2002).
[CrossRef]

1976 (1)

C. Wieman and T. W. Hänsch, Phys. Rev. Lett. 36, 1170 (1976).
[CrossRef]

Adams, C. S.

C. Carr, C. S. Adams, and K. J. Weatherill, Opt. Lett. 37, 118 (2012).
[CrossRef]

M. L. Harris, C. S. Adams, S. L. Cornish, I. C. McLeod, E. Tarleton, and I. G. Hughes, Phys. Rev. A 73, 062509 (2006).
[CrossRef]

C. P. Pearman, C. S. Adams, S. G. Cox, P. F. Griffin, D. A. Smith, and I. G. Hughes, J. Phys. B 35, 5141 (2002).
[CrossRef]

Barbe, A.

L. Rothman, I. Gordon, A. Barbe, D. Benner, P. Bernath, M. Birk, V. Boudon, L. Brown, A. Campargue, and J.-P. Champion, J. Quant. Spectrosc. Radiat. Transfer 110, 533 (2009).
[CrossRef]

Bartalini, Y. S.

Bell, M. T.

Benner, D.

L. Rothman, I. Gordon, A. Barbe, D. Benner, P. Bernath, M. Birk, V. Boudon, L. Brown, A. Campargue, and J.-P. Champion, J. Quant. Spectrosc. Radiat. Transfer 110, 533 (2009).
[CrossRef]

Bernath, P.

L. Rothman, I. Gordon, A. Barbe, D. Benner, P. Bernath, M. Birk, V. Boudon, L. Brown, A. Campargue, and J.-P. Champion, J. Quant. Spectrosc. Radiat. Transfer 110, 533 (2009).
[CrossRef]

Birk, M.

L. Rothman, I. Gordon, A. Barbe, D. Benner, P. Bernath, M. Birk, V. Boudon, L. Brown, A. Campargue, and J.-P. Champion, J. Quant. Spectrosc. Radiat. Transfer 110, 533 (2009).
[CrossRef]

Borri, S.

Boudon, V.

L. Rothman, I. Gordon, A. Barbe, D. Benner, P. Bernath, M. Birk, V. Boudon, L. Brown, A. Campargue, and J.-P. Champion, J. Quant. Spectrosc. Radiat. Transfer 110, 533 (2009).
[CrossRef]

Brown, L.

L. Rothman, I. Gordon, A. Barbe, D. Benner, P. Bernath, M. Birk, V. Boudon, L. Brown, A. Campargue, and J.-P. Champion, J. Quant. Spectrosc. Radiat. Transfer 110, 533 (2009).
[CrossRef]

Campargue, A.

L. Rothman, I. Gordon, A. Barbe, D. Benner, P. Bernath, M. Birk, V. Boudon, L. Brown, A. Campargue, and J.-P. Champion, J. Quant. Spectrosc. Radiat. Transfer 110, 533 (2009).
[CrossRef]

Carr, C.

Causier, S. K.

J. M. R. Kirkbride, S. K. Causier, A. R. Dalton, D. Weidmann, and G. A. D. Ritchie, J. Chem. Phys. 140, 054311 (2014).
[CrossRef]

J. M. R. Kirkbride, S. K. Causier, E. A. McCormack, D. Weidmann, and G. A. D. Ritchie, Phys. Chem. Chem. Phys. 15, 2684 (2013).
[CrossRef]

Champion, J.-P.

L. Rothman, I. Gordon, A. Barbe, D. Benner, P. Bernath, M. Birk, V. Boudon, L. Brown, A. Campargue, and J.-P. Champion, J. Quant. Spectrosc. Radiat. Transfer 110, 533 (2009).
[CrossRef]

Cornish, S. L.

M. L. Harris, C. S. Adams, S. L. Cornish, I. C. McLeod, E. Tarleton, and I. G. Hughes, Phys. Rev. A 73, 062509 (2006).
[CrossRef]

Cox, S. G.

C. P. Pearman, C. S. Adams, S. G. Cox, P. F. Griffin, D. A. Smith, and I. G. Hughes, J. Phys. B 35, 5141 (2002).
[CrossRef]

Dalton, A. R.

J. M. R. Kirkbride, S. K. Causier, A. R. Dalton, D. Weidmann, and G. A. D. Ritchie, J. Chem. Phys. 140, 054311 (2014).
[CrossRef]

De Natale, P.

Demtröder, W.

W. Demtröder, Laser Spectroscopy: Basic Concepts and Instrumentation, 3rd ed. (Springer, 2003), pp. 507–509.

Gordon, I.

L. Rothman, I. Gordon, A. Barbe, D. Benner, P. Bernath, M. Birk, V. Boudon, L. Brown, A. Campargue, and J.-P. Champion, J. Quant. Spectrosc. Radiat. Transfer 110, 533 (2009).
[CrossRef]

Griffin, P. F.

C. P. Pearman, C. S. Adams, S. G. Cox, P. F. Griffin, D. A. Smith, and I. G. Hughes, J. Phys. B 35, 5141 (2002).
[CrossRef]

Hancock, G.

G. Hancock, G. A. D. Ritchie, J.-P. van Helden, R. Walker, and D. Weidmann, Opt. Eng. 49, 111121 (2010).
[CrossRef]

Hänsch, T. W.

C. Wieman and T. W. Hänsch, Phys. Rev. Lett. 36, 1170 (1976).
[CrossRef]

Harris, M. L.

M. L. Harris, C. S. Adams, S. L. Cornish, I. C. McLeod, E. Tarleton, and I. G. Hughes, Phys. Rev. A 73, 062509 (2006).
[CrossRef]

Hughes, I. G.

M. L. Harris, C. S. Adams, S. L. Cornish, I. C. McLeod, E. Tarleton, and I. G. Hughes, Phys. Rev. A 73, 062509 (2006).
[CrossRef]

C. P. Pearman, C. S. Adams, S. G. Cox, P. F. Griffin, D. A. Smith, and I. G. Hughes, J. Phys. B 35, 5141 (2002).
[CrossRef]

Kirkbride, J.

Kirkbride, J. M. R.

J. M. R. Kirkbride, S. K. Causier, A. R. Dalton, D. Weidmann, and G. A. D. Ritchie, J. Chem. Phys. 140, 054311 (2014).
[CrossRef]

J. M. R. Kirkbride, S. K. Causier, E. A. McCormack, D. Weidmann, and G. A. D. Ritchie, Phys. Chem. Chem. Phys. 15, 2684 (2013).
[CrossRef]

McCormack, E. A.

J. M. R. Kirkbride, S. K. Causier, E. A. McCormack, D. Weidmann, and G. A. D. Ritchie, Phys. Chem. Chem. Phys. 15, 2684 (2013).
[CrossRef]

R. J. Walker, J. H. van Helden, J. Kirkbride, E. A. McCormack, M. T. Bell, D. Weidmann, and G. A. D. Ritchie, Opt. Lett. 36, 4725 (2011).
[CrossRef]

McLeod, I. C.

M. L. Harris, C. S. Adams, S. L. Cornish, I. C. McLeod, E. Tarleton, and I. G. Hughes, Phys. Rev. A 73, 062509 (2006).
[CrossRef]

Mukherjee, N.

N. Mukherjee and R. N. Zare, J. Chem. Phys 133, 094301 (2010).
[CrossRef]

N. Mukherjee and R. N. Zare, J. Chem. Phys 132, 154302 (2010).
[CrossRef]

Pearman, C. P.

C. P. Pearman, C. S. Adams, S. G. Cox, P. F. Griffin, D. A. Smith, and I. G. Hughes, J. Phys. B 35, 5141 (2002).
[CrossRef]

Ritchie, G. A. D.

J. M. R. Kirkbride, S. K. Causier, A. R. Dalton, D. Weidmann, and G. A. D. Ritchie, J. Chem. Phys. 140, 054311 (2014).
[CrossRef]

J. M. R. Kirkbride, S. K. Causier, E. A. McCormack, D. Weidmann, and G. A. D. Ritchie, Phys. Chem. Chem. Phys. 15, 2684 (2013).
[CrossRef]

R. J. Walker, J. H. van Helden, J. Kirkbride, E. A. McCormack, M. T. Bell, D. Weidmann, and G. A. D. Ritchie, Opt. Lett. 36, 4725 (2011).
[CrossRef]

R. J. Walker, J. H. van Helden, and G. A. D. Ritchie, Chem. Phys. Lett. 501, 20 (2010).
[CrossRef]

G. Hancock, G. A. D. Ritchie, J.-P. van Helden, R. Walker, and D. Weidmann, Opt. Eng. 49, 111121 (2010).
[CrossRef]

Rothman, L.

L. Rothman, I. Gordon, A. Barbe, D. Benner, P. Bernath, M. Birk, V. Boudon, L. Brown, A. Campargue, and J.-P. Champion, J. Quant. Spectrosc. Radiat. Transfer 110, 533 (2009).
[CrossRef]

Smith, D. A.

C. P. Pearman, C. S. Adams, S. G. Cox, P. F. Griffin, D. A. Smith, and I. G. Hughes, J. Phys. B 35, 5141 (2002).
[CrossRef]

Tarleton, E.

M. L. Harris, C. S. Adams, S. L. Cornish, I. C. McLeod, E. Tarleton, and I. G. Hughes, Phys. Rev. A 73, 062509 (2006).
[CrossRef]

van Helden, J. H.

van Helden, J.-P.

G. Hancock, G. A. D. Ritchie, J.-P. van Helden, R. Walker, and D. Weidmann, Opt. Eng. 49, 111121 (2010).
[CrossRef]

Walker, R.

G. Hancock, G. A. D. Ritchie, J.-P. van Helden, R. Walker, and D. Weidmann, Opt. Eng. 49, 111121 (2010).
[CrossRef]

Walker, R. J.

Weatherill, K. J.

Weidmann, D.

J. M. R. Kirkbride, S. K. Causier, A. R. Dalton, D. Weidmann, and G. A. D. Ritchie, J. Chem. Phys. 140, 054311 (2014).
[CrossRef]

J. M. R. Kirkbride, S. K. Causier, E. A. McCormack, D. Weidmann, and G. A. D. Ritchie, Phys. Chem. Chem. Phys. 15, 2684 (2013).
[CrossRef]

R. J. Walker, J. H. van Helden, J. Kirkbride, E. A. McCormack, M. T. Bell, D. Weidmann, and G. A. D. Ritchie, Opt. Lett. 36, 4725 (2011).
[CrossRef]

G. Hancock, G. A. D. Ritchie, J.-P. van Helden, R. Walker, and D. Weidmann, Opt. Eng. 49, 111121 (2010).
[CrossRef]

Wieman, C.

C. Wieman and T. W. Hänsch, Phys. Rev. Lett. 36, 1170 (1976).
[CrossRef]

Zare, R. N.

N. Mukherjee and R. N. Zare, J. Chem. Phys 132, 154302 (2010).
[CrossRef]

N. Mukherjee and R. N. Zare, J. Chem. Phys 133, 094301 (2010).
[CrossRef]

Chem. Phys. Lett. (1)

R. J. Walker, J. H. van Helden, and G. A. D. Ritchie, Chem. Phys. Lett. 501, 20 (2010).
[CrossRef]

J. Chem. Phys (2)

N. Mukherjee and R. N. Zare, J. Chem. Phys 132, 154302 (2010).
[CrossRef]

N. Mukherjee and R. N. Zare, J. Chem. Phys 133, 094301 (2010).
[CrossRef]

J. Chem. Phys. (1)

J. M. R. Kirkbride, S. K. Causier, A. R. Dalton, D. Weidmann, and G. A. D. Ritchie, J. Chem. Phys. 140, 054311 (2014).
[CrossRef]

J. Phys. B (1)

C. P. Pearman, C. S. Adams, S. G. Cox, P. F. Griffin, D. A. Smith, and I. G. Hughes, J. Phys. B 35, 5141 (2002).
[CrossRef]

J. Quant. Spectrosc. Radiat. Transfer (1)

L. Rothman, I. Gordon, A. Barbe, D. Benner, P. Bernath, M. Birk, V. Boudon, L. Brown, A. Campargue, and J.-P. Champion, J. Quant. Spectrosc. Radiat. Transfer 110, 533 (2009).
[CrossRef]

Opt. Eng. (1)

G. Hancock, G. A. D. Ritchie, J.-P. van Helden, R. Walker, and D. Weidmann, Opt. Eng. 49, 111121 (2010).
[CrossRef]

Opt. Express (1)

Opt. Lett. (2)

Phys. Chem. Chem. Phys. (1)

J. M. R. Kirkbride, S. K. Causier, E. A. McCormack, D. Weidmann, and G. A. D. Ritchie, Phys. Chem. Chem. Phys. 15, 2684 (2013).
[CrossRef]

Phys. Rev. A (1)

M. L. Harris, C. S. Adams, S. L. Cornish, I. C. McLeod, E. Tarleton, and I. G. Hughes, Phys. Rev. A 73, 062509 (2006).
[CrossRef]

Phys. Rev. Lett. (1)

C. Wieman and T. W. Hänsch, Phys. Rev. Lett. 36, 1170 (1976).
[CrossRef]

Other (1)

W. Demtröder, Laser Spectroscopy: Basic Concepts and Instrumentation, 3rd ed. (Springer, 2003), pp. 507–509.

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Figures (3)

Fig. 1.
Fig. 1.

Polarization signals (ΣI and ΔI [θ=45°]) obtained at a pressure of 36 mTorr and probe chirp rate of 0.92MHzμs1. The pure absorption signal is shown in (a) and shows the velocity selection induced by the pump beam with a width of 2 MHz. The difference detection method also gives rise to the dispersion signal shown in (b) and is shown with a fit using Eq. (1).

Fig. 2.
Fig. 2.

Polarization signals (ΣI and ΔI [θ=45°]) as a function of chirp rate obtained at a pressure of 36 mTorr and probe chirp rates of 0.92, 4.1, and 15.2MHzμs1. The chirp rate is increasing from top to bottom, and (a)–(c) show ΣI, while (d)–(f) show ΔI. As the chirp rate increases, RP oscillations become apparent in both the absorption and dispersion with a phase difference of π/2 between the two as expected from the optical Bloch equations.

Fig. 3.
Fig. 3.

Comparison of polarization signals obtained at a chirp rate of 68.6MHzμs1 with a simulation based upon the three-level density matrix model of Zare and Mukherjee. The simulation displays excellent agreement with the measured data in (a). The populations of the three levels are shown in (b) as the probe laser is swept through resonance. The simulation predicts 38% population transfer.

Equations (8)

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

ΔI=I0eα¯L(ξ+|sin(θ+Φ)|2|cos(θ+Φ)|2),
Φ(ω)=ω2c(LΔn(ω)+Δbr)+i(LΔα4+Δbi2),
Δα=Δα0Γ2Γ2+(ωω0)2,
Δn=Δα0cω0Γ2(ωω0)Γ2+(ωω0).
Ω=μ4Pπr2cε0,
γ01=Δpump2+Γ012,
γ12=Δprobe2+Γ122,
γ02=Δpump2+Δprobe2.

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