Abstract

Quantum photonics offers much promise for the development of new technologies. The ability to control the interaction of light and matter at the level of single quantum excitations is a prerequisite for the construction of potentially powerful devices. Here we use the rotational levels of a room temperature ensemble of hydrogen molecules to couple two distinct optical modes at the single photon level using femtosecond pulses with 2 THz bandwidth. We observe photon correlations that violate a Cauchy–Schwarz inequality, thereby verifying the creation of a nonclassical state. This work demonstrates the rich potential of molecules for use in ultrafast quantum photonic devices.

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References

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2013 (1)

P. J. Bustard, R. Lausten, D. G. England, and B. J. Sussman, Phys. Rev. Lett. 111, 083901 (2013).
[Crossref]

2012 (1)

2011 (6)

M. D. Eisaman, J. Fan, A. Migdall, and S. V. Polyakov, Rev. Sci. Instrum. 82, 071101 (2011).
[Crossref]

P. J. Bustard, D. Moffatt, R. Lausten, G. Wu, I. A. Walmsley, and B. J. Sussman, Opt. Express 19, 25173 (2011).
[Crossref]

K. C. Lee, B. J. Sussman, M. R. Sprague, P. Michelberger, K. F. Reim, J. Nunn, N. K. Langford, P. J. Bustard, D. Jaksch, and I. A. Walmsley, Nat. Photonics 6, 41 (2011).
[Crossref]

N. Sangouard, C. Simon, H. de Riedmatten, and N. Gisin, Rev. Mod. Phys. 83, 33 (2011).
[Crossref]

C. Clausen, I. Usmani, F. Bussières, N. Sangouard, M. Afzelius, H. de Riedmatten, and N. Gisin, Nature 469, 508 (2011).
[Crossref]

E. Saglamyurek, N. Sinclair, J. Jin, J. A. Slater, D. Oblak, F. Bussières, M. George, R. Ricken, W. Sohler, and W. Tittel, Nature 469, 512 (2011).
[Crossref]

2010 (4)

B. Lauritzen, J. Minář, H. de Riedmatten, M. Afzelius, N. Sangouard, C. Simon, and N. Gisin, Phys. Rev. Lett. 104, 080502 (2010).
[Crossref]

M. Afzelius, I. Usmani, A. Amari, B. Lauritzen, A. Walther, C. Simon, N. Sangouard, J. Minář, H. de Riedmatten, N. Gisin, and S. Kröll, Phys. Rev. Lett. 104, 040503 (2010).
[Crossref]

K. F. Reim, J. Nunn, V. O. Lorenz, B. J. Sussman, K. C. Lee, N. K. Langford, D. Jaksch, and I. A. Walmsley, Nat. Photonics 4, 218 (2010).
[Crossref]

M. Hedges, J. Longdell, Y. Li, and M. Sellars, Nature 465, 1052 (2010).
[Crossref]

2009 (2)

A. Lvovsky, B. Sanders, and W. Tittel, Nat. Photonics 3, 706 (2009).
[Crossref]

M. Hosseini, B. Sparkes, G. Hétet, J. Longdell, P. Lam, and B. Buchler, Nature 461, 241 (2009).
[Crossref]

2008 (1)

G. Hétet, J. J. Longdell, A. L. Alexander, P. K. Lam, and M. J. Sellars, Phys. Rev. Lett. 100, 023601 (2008).
[Crossref]

2007 (2)

A. Alexander, J. Longdell, M. Sellars, and N. Manson, J. Lumin. 127, 94 (2007).
[Crossref]

P. Kok, W. J. Munro, K. Nemoto, T. C. Ralph, J. P. Dowling, and G. J. Milburn, Rev. Mod. Phys. 79, 135 (2007).
[Crossref]

2006 (2)

D. N. Matsukevich, T. Chanelière, S. D. Jenkins, S.-Y. Lan, T. A. B. Kennedy, and A. Kuzmich, Phys. Rev. Lett. 97, 013601 (2006).
[Crossref]

S. Chen, Y.-A. Chen, T. Strassel, Z.-S. Yuan, B. Zhao, J. Schmiedmayer, and J.-W. Pan, Phys. Rev. Lett. 97, 173004 (2006).
[Crossref]

2005 (1)

M. D. Eisaman, A. André, F. Massou, M. Fleischhauer, A. S. Zibrov, and M. D. Lukin, Nature 438, 837 (2005).
[Crossref]

2003 (2)

A. Kuzmich, W. Bowen, A. Boozer, A. Boca, C. Chou, L.-M. Duan, and H. Kimble, Nature 423, 731 (2003).
[Crossref]

C. H. van der Wal, M. D. Eisaman, A. André, R. L. Walsworth, D. F. Phillips, A. S. Zibrov, and M. D. Lukin, Science 301, 196 (2003).
[Crossref]

2002 (1)

M. Fleischhauer and M. D. Lukin, Phys. Rev. A 65, 022314 (2002).
[Crossref]

2001 (3)

D. F. Phillips, A. Fleischhauer, A. Mair, R. L. Walsworth, and M. D. Lukin, Phys. Rev. Lett. 86, 783 (2001).
[Crossref]

C. Liu, Z. Dutton, C. H. Behroozi, and L. V. Hau, Nature 409, 490 (2001).
[Crossref]

L.-M. Duan, M. D. Lukin, J. I. Cirac, and P. Zoller, Nature 414, 413 (2001).
[Crossref]

2000 (1)

A. E. Kozhekin, K. Mølmer, and E. Polzik, Phys. Rev. A 62, 033809 (2000).
[Crossref]

1998 (1)

H.-J. Briegel, W. Dür, J. I. Cirac, and P. Zoller, Phys. Rev. Lett. 81, 5932 (1998).
[Crossref]

1990 (1)

K. J. Miller, J. Am. Chem. Soc. 112, 8543 (1990).
[Crossref]

1986 (1)

G. C. Herring, M. J. Dyer, and W. K. Bischel, Phys. Rev. A 34, 1944 (1986).
[Crossref]

1979 (1)

A. Penzkofer, A. Laubereau, and W. Kaiser, Prog. Quant. Electron. 6, 55 (1979).
[Crossref]

1966 (1)

R. W. Minck, E. E. Hagenlocker, and W. G. Rado, Phys. Rev. Lett. 17, 229 (1966).
[Crossref]

Afzelius, M.

C. Clausen, I. Usmani, F. Bussières, N. Sangouard, M. Afzelius, H. de Riedmatten, and N. Gisin, Nature 469, 508 (2011).
[Crossref]

M. Afzelius, I. Usmani, A. Amari, B. Lauritzen, A. Walther, C. Simon, N. Sangouard, J. Minář, H. de Riedmatten, N. Gisin, and S. Kröll, Phys. Rev. Lett. 104, 040503 (2010).
[Crossref]

B. Lauritzen, J. Minář, H. de Riedmatten, M. Afzelius, N. Sangouard, C. Simon, and N. Gisin, Phys. Rev. Lett. 104, 080502 (2010).
[Crossref]

Alexander, A.

A. Alexander, J. Longdell, M. Sellars, and N. Manson, J. Lumin. 127, 94 (2007).
[Crossref]

Alexander, A. L.

G. Hétet, J. J. Longdell, A. L. Alexander, P. K. Lam, and M. J. Sellars, Phys. Rev. Lett. 100, 023601 (2008).
[Crossref]

Amari, A.

M. Afzelius, I. Usmani, A. Amari, B. Lauritzen, A. Walther, C. Simon, N. Sangouard, J. Minář, H. de Riedmatten, N. Gisin, and S. Kröll, Phys. Rev. Lett. 104, 040503 (2010).
[Crossref]

André, A.

M. D. Eisaman, A. André, F. Massou, M. Fleischhauer, A. S. Zibrov, and M. D. Lukin, Nature 438, 837 (2005).
[Crossref]

C. H. van der Wal, M. D. Eisaman, A. André, R. L. Walsworth, D. F. Phillips, A. S. Zibrov, and M. D. Lukin, Science 301, 196 (2003).
[Crossref]

Bashkansky, M.

Behroozi, C. H.

C. Liu, Z. Dutton, C. H. Behroozi, and L. V. Hau, Nature 409, 490 (2001).
[Crossref]

Bischel, W. K.

G. C. Herring, M. J. Dyer, and W. K. Bischel, Phys. Rev. A 34, 1944 (1986).
[Crossref]

Boca, A.

A. Kuzmich, W. Bowen, A. Boozer, A. Boca, C. Chou, L.-M. Duan, and H. Kimble, Nature 423, 731 (2003).
[Crossref]

Boozer, A.

A. Kuzmich, W. Bowen, A. Boozer, A. Boca, C. Chou, L.-M. Duan, and H. Kimble, Nature 423, 731 (2003).
[Crossref]

Bowen, W.

A. Kuzmich, W. Bowen, A. Boozer, A. Boca, C. Chou, L.-M. Duan, and H. Kimble, Nature 423, 731 (2003).
[Crossref]

Briegel, H.-J.

H.-J. Briegel, W. Dür, J. I. Cirac, and P. Zoller, Phys. Rev. Lett. 81, 5932 (1998).
[Crossref]

Buchler, B.

M. Hosseini, B. Sparkes, G. Hétet, J. Longdell, P. Lam, and B. Buchler, Nature 461, 241 (2009).
[Crossref]

Bussières, F.

E. Saglamyurek, N. Sinclair, J. Jin, J. A. Slater, D. Oblak, F. Bussières, M. George, R. Ricken, W. Sohler, and W. Tittel, Nature 469, 512 (2011).
[Crossref]

C. Clausen, I. Usmani, F. Bussières, N. Sangouard, M. Afzelius, H. de Riedmatten, and N. Gisin, Nature 469, 508 (2011).
[Crossref]

Bustard, P. J.

P. J. Bustard, R. Lausten, D. G. England, and B. J. Sussman, Phys. Rev. Lett. 111, 083901 (2013).
[Crossref]

K. C. Lee, B. J. Sussman, M. R. Sprague, P. Michelberger, K. F. Reim, J. Nunn, N. K. Langford, P. J. Bustard, D. Jaksch, and I. A. Walmsley, Nat. Photonics 6, 41 (2011).
[Crossref]

P. J. Bustard, D. Moffatt, R. Lausten, G. Wu, I. A. Walmsley, and B. J. Sussman, Opt. Express 19, 25173 (2011).
[Crossref]

Chanelière, T.

D. N. Matsukevich, T. Chanelière, S. D. Jenkins, S.-Y. Lan, T. A. B. Kennedy, and A. Kuzmich, Phys. Rev. Lett. 97, 013601 (2006).
[Crossref]

Chen, S.

S. Chen, Y.-A. Chen, T. Strassel, Z.-S. Yuan, B. Zhao, J. Schmiedmayer, and J.-W. Pan, Phys. Rev. Lett. 97, 173004 (2006).
[Crossref]

Chen, Y.-A.

S. Chen, Y.-A. Chen, T. Strassel, Z.-S. Yuan, B. Zhao, J. Schmiedmayer, and J.-W. Pan, Phys. Rev. Lett. 97, 173004 (2006).
[Crossref]

Chou, C.

A. Kuzmich, W. Bowen, A. Boozer, A. Boca, C. Chou, L.-M. Duan, and H. Kimble, Nature 423, 731 (2003).
[Crossref]

Cirac, J. I.

L.-M. Duan, M. D. Lukin, J. I. Cirac, and P. Zoller, Nature 414, 413 (2001).
[Crossref]

H.-J. Briegel, W. Dür, J. I. Cirac, and P. Zoller, Phys. Rev. Lett. 81, 5932 (1998).
[Crossref]

Clausen, C.

C. Clausen, I. Usmani, F. Bussières, N. Sangouard, M. Afzelius, H. de Riedmatten, and N. Gisin, Nature 469, 508 (2011).
[Crossref]

de Riedmatten, H.

C. Clausen, I. Usmani, F. Bussières, N. Sangouard, M. Afzelius, H. de Riedmatten, and N. Gisin, Nature 469, 508 (2011).
[Crossref]

N. Sangouard, C. Simon, H. de Riedmatten, and N. Gisin, Rev. Mod. Phys. 83, 33 (2011).
[Crossref]

B. Lauritzen, J. Minář, H. de Riedmatten, M. Afzelius, N. Sangouard, C. Simon, and N. Gisin, Phys. Rev. Lett. 104, 080502 (2010).
[Crossref]

M. Afzelius, I. Usmani, A. Amari, B. Lauritzen, A. Walther, C. Simon, N. Sangouard, J. Minář, H. de Riedmatten, N. Gisin, and S. Kröll, Phys. Rev. Lett. 104, 040503 (2010).
[Crossref]

Dowling, J. P.

P. Kok, W. J. Munro, K. Nemoto, T. C. Ralph, J. P. Dowling, and G. J. Milburn, Rev. Mod. Phys. 79, 135 (2007).
[Crossref]

Duan, L.-M.

A. Kuzmich, W. Bowen, A. Boozer, A. Boca, C. Chou, L.-M. Duan, and H. Kimble, Nature 423, 731 (2003).
[Crossref]

L.-M. Duan, M. D. Lukin, J. I. Cirac, and P. Zoller, Nature 414, 413 (2001).
[Crossref]

Dür, W.

H.-J. Briegel, W. Dür, J. I. Cirac, and P. Zoller, Phys. Rev. Lett. 81, 5932 (1998).
[Crossref]

Dutton, Z.

C. Liu, Z. Dutton, C. H. Behroozi, and L. V. Hau, Nature 409, 490 (2001).
[Crossref]

Dyer, M. J.

G. C. Herring, M. J. Dyer, and W. K. Bischel, Phys. Rev. A 34, 1944 (1986).
[Crossref]

Eisaman, M. D.

M. D. Eisaman, J. Fan, A. Migdall, and S. V. Polyakov, Rev. Sci. Instrum. 82, 071101 (2011).
[Crossref]

M. D. Eisaman, A. André, F. Massou, M. Fleischhauer, A. S. Zibrov, and M. D. Lukin, Nature 438, 837 (2005).
[Crossref]

C. H. van der Wal, M. D. Eisaman, A. André, R. L. Walsworth, D. F. Phillips, A. S. Zibrov, and M. D. Lukin, Science 301, 196 (2003).
[Crossref]

England, D. G.

P. J. Bustard, R. Lausten, D. G. England, and B. J. Sussman, Phys. Rev. Lett. 111, 083901 (2013).
[Crossref]

Fan, J.

M. D. Eisaman, J. Fan, A. Migdall, and S. V. Polyakov, Rev. Sci. Instrum. 82, 071101 (2011).
[Crossref]

Fatemi, F. K.

Fleischhauer, A.

D. F. Phillips, A. Fleischhauer, A. Mair, R. L. Walsworth, and M. D. Lukin, Phys. Rev. Lett. 86, 783 (2001).
[Crossref]

Fleischhauer, M.

M. D. Eisaman, A. André, F. Massou, M. Fleischhauer, A. S. Zibrov, and M. D. Lukin, Nature 438, 837 (2005).
[Crossref]

M. Fleischhauer and M. D. Lukin, Phys. Rev. A 65, 022314 (2002).
[Crossref]

George, M.

E. Saglamyurek, N. Sinclair, J. Jin, J. A. Slater, D. Oblak, F. Bussières, M. George, R. Ricken, W. Sohler, and W. Tittel, Nature 469, 512 (2011).
[Crossref]

Gisin, N.

N. Sangouard, C. Simon, H. de Riedmatten, and N. Gisin, Rev. Mod. Phys. 83, 33 (2011).
[Crossref]

C. Clausen, I. Usmani, F. Bussières, N. Sangouard, M. Afzelius, H. de Riedmatten, and N. Gisin, Nature 469, 508 (2011).
[Crossref]

M. Afzelius, I. Usmani, A. Amari, B. Lauritzen, A. Walther, C. Simon, N. Sangouard, J. Minář, H. de Riedmatten, N. Gisin, and S. Kröll, Phys. Rev. Lett. 104, 040503 (2010).
[Crossref]

B. Lauritzen, J. Minář, H. de Riedmatten, M. Afzelius, N. Sangouard, C. Simon, and N. Gisin, Phys. Rev. Lett. 104, 080502 (2010).
[Crossref]

Hagenlocker, E. E.

R. W. Minck, E. E. Hagenlocker, and W. G. Rado, Phys. Rev. Lett. 17, 229 (1966).
[Crossref]

Hau, L. V.

C. Liu, Z. Dutton, C. H. Behroozi, and L. V. Hau, Nature 409, 490 (2001).
[Crossref]

Hedges, M.

M. Hedges, J. Longdell, Y. Li, and M. Sellars, Nature 465, 1052 (2010).
[Crossref]

Herring, G. C.

G. C. Herring, M. J. Dyer, and W. K. Bischel, Phys. Rev. A 34, 1944 (1986).
[Crossref]

Herzberg, G.

G. Herzberg, Molecular Spectra and Molecular Structure (Van Nostrand, 1950), Vol. 1.

Hétet, G.

M. Hosseini, B. Sparkes, G. Hétet, J. Longdell, P. Lam, and B. Buchler, Nature 461, 241 (2009).
[Crossref]

G. Hétet, J. J. Longdell, A. L. Alexander, P. K. Lam, and M. J. Sellars, Phys. Rev. Lett. 100, 023601 (2008).
[Crossref]

Hosseini, M.

M. Hosseini, B. Sparkes, G. Hétet, J. Longdell, P. Lam, and B. Buchler, Nature 461, 241 (2009).
[Crossref]

Jaksch, D.

K. C. Lee, B. J. Sussman, M. R. Sprague, P. Michelberger, K. F. Reim, J. Nunn, N. K. Langford, P. J. Bustard, D. Jaksch, and I. A. Walmsley, Nat. Photonics 6, 41 (2011).
[Crossref]

K. F. Reim, J. Nunn, V. O. Lorenz, B. J. Sussman, K. C. Lee, N. K. Langford, D. Jaksch, and I. A. Walmsley, Nat. Photonics 4, 218 (2010).
[Crossref]

Jenkins, S. D.

D. N. Matsukevich, T. Chanelière, S. D. Jenkins, S.-Y. Lan, T. A. B. Kennedy, and A. Kuzmich, Phys. Rev. Lett. 97, 013601 (2006).
[Crossref]

Jin, J.

E. Saglamyurek, N. Sinclair, J. Jin, J. A. Slater, D. Oblak, F. Bussières, M. George, R. Ricken, W. Sohler, and W. Tittel, Nature 469, 512 (2011).
[Crossref]

Kaiser, W.

A. Penzkofer, A. Laubereau, and W. Kaiser, Prog. Quant. Electron. 6, 55 (1979).
[Crossref]

Kennedy, T. A. B.

D. N. Matsukevich, T. Chanelière, S. D. Jenkins, S.-Y. Lan, T. A. B. Kennedy, and A. Kuzmich, Phys. Rev. Lett. 97, 013601 (2006).
[Crossref]

Kimble, H.

A. Kuzmich, W. Bowen, A. Boozer, A. Boca, C. Chou, L.-M. Duan, and H. Kimble, Nature 423, 731 (2003).
[Crossref]

Kok, P.

P. Kok, W. J. Munro, K. Nemoto, T. C. Ralph, J. P. Dowling, and G. J. Milburn, Rev. Mod. Phys. 79, 135 (2007).
[Crossref]

Kozhekin, A. E.

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Science (1)

C. H. van der Wal, M. D. Eisaman, A. André, R. L. Walsworth, D. F. Phillips, A. S. Zibrov, and M. D. Lukin, Science 301, 196 (2003).
[Crossref]

Other (3)

R. Loudon, The Quantum Theory of Light (Oxford University, 2004).

G. Herzberg, Molecular Spectra and Molecular Structure (Van Nostrand, 1950), Vol. 1.

D. A. Long, The Raman Effect: A Unified Treatment of the Theory of Raman Scattering by Molecules (Wiley, 2002).

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Figures (2)

Fig. 1.
Fig. 1.

(a) Right-circular polarized (SR) Stokes photons are created by spontaneous Raman scattering from the left-circular polarized (WL) write pulse, with rotational population transfer from |g|e. (b) Left-circular polarized anti-Stokes photons (AL) are created by Raman scattering from the right-circular polarized read pulse (RR); commensurate population completes the |e|g transition. (c) Write and read pulses of duration 150 fs are generated using an 80 MHz repetition rate, 3.7 W Ti:sapphire oscillator (Ti:sapph) centered at 805 nm. We reduce the full width at half-maximum bandwidth of the laser output to 2 THz by spectral filtering. The beam is subsequently split using a polarizing beamspliter (PBS); orthogonal linearly polarized write (V-polarized) and read (H-polarized) pulses are recombined with a variable delay τ. The write and read pulses are converted to left-circular (WL) and right-circular (RR) polarization, respectively, using a quarter-wave plate (λ/4) and focussed collinearly using an f=50mm singlet, into a 7 cm cell filled with hydrogen at pressure p=18bar and temperature T=295K. The output light is collimated using an f=75mm singlet and converted back to linear polarization using an achromatic quarter-wave plate (λ/4). Pump radiation is separated from rotational Raman Stokes and anti-Stokes photons using notch filter F1. Stokes photons are partitioned from anti-Stokes photons using a dichroic mirror (DM). H-polarized Stokes photons are transmitted at a polarizer (POL), spectrally filtered by filter F2, coupled into a single mode fiber, and detected using an avalanche photodiode (APD1); V-polarized anti-Stokes photons are reflected at a polarizer, spectrally filtered by filter F3, coupled into a single mode fiber, and detected using APD2. Detection events are recorded using a coincidence counting module (&).

Fig. 2.
Fig. 2.

Plot of measured gS,A(2) as a function of write pulse–read pulse delay (blue cross). At positive delays gS,A(2)>2, indicating nonclassical correlations between the detected Stokes and anti-Stokes photons. Standard errors are shown as error bars. A theoretical model shows close agreement with the measured values (solid red line).

Equations (7)

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PSth=NLNwσΔΩ,
gS,A(2)=PS,APSPA,
PS=ηSPSth,
PA=ηAβχ+ηAPAth,
PS,A=ηSηAαPSth+PSPA,
gS,A(2)(τ0)=1+(α0/PSth)e2Γτ(χβ0/PSth)e2Γτ+n¯(λS/λr)4,
α(τ0)=α0e2Γτ;β(τ0)=β0e2Γτ

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