Abstract

We present an experimental comparison and a theoretical analysis of the signal-to-noise ratios in fluorescence and extinction spectroscopy of a single emitter. We show that because of its homodyne nature the extinction measurements can be advantageous if the emitter is weakly excited. Furthermore, we discuss the potential of this method for the detection and spectroscopy of weakly emitting systems such as rare earth ions.

© 2008 Optical Society of America

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  1. F. Kulzer and M. Orrit, Single-Molecule Optics, Annu. Rev. Phys. Chem. 55, 585-611 (2004).
    [CrossRef] [PubMed]
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  4. E. Shera, N. Seitzinger, L. Davis, R. Keller, and S. Soper, "Detection of single fluorescent molecules," Chem. Phys. Lett. 174, 553-557 (1990).
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    [CrossRef] [PubMed]
  13. G. Wrigge, I. Gerhardt, J. Hwang, G. Zumofen, and V. Sandoghdar, "Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence," Nature Phys. 4, 60-66 (2008).
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
  26. V. Jacobsen, P. Stoller, C. Brunner, V. Vogel, and V. Sandoghdar, "Interferometric optical detection and tracking of very small gold nanoparticles at a water-glass interface," Opt. Express 14, 405-414 (2006).
    [CrossRef] [PubMed]
  27. F. V. Ignatovich and L. Novotny, "Real-Time and Background-Free Detection of Nanoscale Particles," Phys. Rev. Lett. 96, 013901 (2006).
    [CrossRef] [PubMed]
  28. H. Ewers, V. Jacobsen, E. Klotzsch, A. E. Smith, A. Helenius, and V. Sandoghdar, "Label-free Optical Detection and Tracking of Single Virions Bound to their Receptor in Supported Membrane Bilayers," Nano Lett. 7, 2263-2266 (2007).
    [CrossRef] [PubMed]
  29. S. Schultz, D. R. Smith, J. J. Mock, and D. A. Schultz, "Single-target molecule detection with nonbleaching multicolor optical immunolabels," PNAS 97, 996-1001 (2000).
    [CrossRef] [PubMed]
  30. C. Sonnichsen, S. Geier, N. E. Hecker, G. von Plessen, J. Feldmann, H. Ditlbacher, b. Lamprecht, J. R. Krenn, F. R. Aussenegg, V. Z.-H. Chan, J. P. Spatz, and M. M¨oller, "Spectroscopy of single metallic nanoparticles using total internal reflection microscopy," Appl. Phys. Lett. 77, 2949-2951 (2000).
    [CrossRef]

2008

G. Wrigge, I. Gerhardt, J. Hwang, G. Zumofen, and V. Sandoghdar, "Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence," Nature Phys. 4, 60-66 (2008).
[CrossRef]

G. Zumofen, N. M. Mojarad, V. Sandoghdar, and M. Agio, "Perfect Reflection of Light by an Oscillating Dipole," Phys. Rev. Lett. (to appear), http://arxiv.org/abs/0805.3231v2 (2008).
[CrossRef] [PubMed]

P. Kukura, M. Celebrano, A. Renn, and V. Sandoghdar, "Seeing a single quantum emitter in its bright and dark states," Nano Lett. (DOI: 10.1021/nl801735y), http://arxiv.org/abs/0802.1206 (2008).
[PubMed]

2007

H. Ewers, V. Jacobsen, E. Klotzsch, A. E. Smith, A. Helenius, and V. Sandoghdar, "Label-free Optical Detection and Tracking of Single Virions Bound to their Receptor in Supported Membrane Bilayers," Nano Lett. 7, 2263-2266 (2007).
[CrossRef] [PubMed]

A. N. Vamivakas, M. Atature, J. Dreiser, S. T. Yilmaz, A. Badolato, A. K. Swan, B. B. Goldberg, A. Imamoglu, and M. S. Unlu, "Strong extinction of a far-field laser beam by a single quantum dot," Nano Lett. 7, 2892-2896 (2007).
[CrossRef] [PubMed]

I. Gerhardt, G. Wrigge, P. Bushev, G. Zumofen, M. Agio, R. Pfab, and V. Sandoghdar, "Strong extinction of a laser beam by a single molecule," Phys. Rev. Lett. 98, 033601 (2007).
[CrossRef] [PubMed]

I. Gerhardt, G. Wrigge, M. Agio, P. Bushev, G. Zumofen, and V. Sandoghdar, "Scanning Near-Field Optical Coherent Spectroscopy of Single Molecules at 1.4 Kelvin," Opt. Lett. 32, 1420-1422 (2007).
[CrossRef] [PubMed]

2006

2004

K. Lindfors, T. Kalkbrenner, P. Stoller, and V. Sandoghdar, "Detection and spectroscopy of gold nanoparticle using supercontinuum white light confocal microscopy," Phys. Rev. Lett. 93, 037401 (2004).
[CrossRef] [PubMed]

A. Arbouet, D. Christofilos, N. D. Fatti, F. Vall�??ee, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, "Direct measurement of the single-metal-cluster optical absorption," Phys. Rev. Lett. 93, 127401 (2004).
[CrossRef] [PubMed]

F. Kulzer and M. Orrit, Single-Molecule Optics, Annu. Rev. Phys. Chem. 55, 585-611 (2004).
[CrossRef] [PubMed]

2003

B. Alen, F. Bickel, K. Karrai, R. J. Warburton, and P. M. Petroff, "Stark-shift modulation absorption spectroscopy of single quantum dots," Appl. Phys. Lett. 83, 2235-2237 (2003).
[CrossRef]

A. A. Mikhailovsky, M. A. Petruska, M. I. Stockman, and V. I. Klimov, "Broadband near-field interference spectroscopy of metal nanoparticles using a femtosecond white-light continuum," Opt. Lett. 28, 1686-1688 (2003).
[CrossRef] [PubMed]

2002

T. Plakhotnik, "Absorption and coherent emission of single molecules," J. Lumin. 98, 57-62 (2002).
[CrossRef]

2001

T. Plakhotnik and V. Palm, "Interferometric signatures of single molecules," Phys. Rev. Lett. 87, 183602 (2001).
[CrossRef]

2000

S. Schultz, D. R. Smith, J. J. Mock, and D. A. Schultz, "Single-target molecule detection with nonbleaching multicolor optical immunolabels," PNAS 97, 996-1001 (2000).
[CrossRef] [PubMed]

C. Sonnichsen, S. Geier, N. E. Hecker, G. von Plessen, J. Feldmann, H. Ditlbacher, b. Lamprecht, J. R. Krenn, F. R. Aussenegg, V. Z.-H. Chan, J. P. Spatz, and M. M¨oller, "Spectroscopy of single metallic nanoparticles using total internal reflection microscopy," Appl. Phys. Lett. 77, 2949-2951 (2000).
[CrossRef]

1994

S. Nie, D. T. Chiu, and R. N. Zare, "Probing Individual Molecules with Confocal Fluorescence Microscopy," Science 266, 1018-1021 (1994).
[CrossRef] [PubMed]

W. E. Moerner, "Examining Nanoenvironments in Solids on the Scale of a Single, Isolated Impurity Molecule," Science 265, 46-53 (1994).
[CrossRef] [PubMed]

1993

E. Betzig and R. J. Chichester, "Single Molecules Observed by Near-Field Scanning Optical Microscopy," Science 262, 1422-1425 (1993).
[CrossRef] [PubMed]

1990

M. Orrit and J. Bernard, "Single Pentacene Molecules Detected by Fluorescence Excitation in a p-Terphenyl Crystal," Phys. Rev. Lett. 65, 2716-2719 (1990).
[CrossRef] [PubMed]

E. Shera, N. Seitzinger, L. Davis, R. Keller, and S. Soper, "Detection of single fluorescent molecules," Chem. Phys. Lett. 174, 553-557 (1990).
[CrossRef]

1989

W. E. Moerner and L. Kador, "Optical Detection and Spectroscopy of Single Molecules in a Solid," Phys. Rev. Lett. 62, 2535-2538 (1989).
[CrossRef] [PubMed]

1983

Agio, M.

G. Zumofen, N. M. Mojarad, V. Sandoghdar, and M. Agio, "Perfect Reflection of Light by an Oscillating Dipole," Phys. Rev. Lett. (to appear), http://arxiv.org/abs/0805.3231v2 (2008).
[CrossRef] [PubMed]

I. Gerhardt, G. Wrigge, P. Bushev, G. Zumofen, M. Agio, R. Pfab, and V. Sandoghdar, "Strong extinction of a laser beam by a single molecule," Phys. Rev. Lett. 98, 033601 (2007).
[CrossRef] [PubMed]

I. Gerhardt, G. Wrigge, M. Agio, P. Bushev, G. Zumofen, and V. Sandoghdar, "Scanning Near-Field Optical Coherent Spectroscopy of Single Molecules at 1.4 Kelvin," Opt. Lett. 32, 1420-1422 (2007).
[CrossRef] [PubMed]

Alen, B.

B. Alen, F. Bickel, K. Karrai, R. J. Warburton, and P. M. Petroff, "Stark-shift modulation absorption spectroscopy of single quantum dots," Appl. Phys. Lett. 83, 2235-2237 (2003).
[CrossRef]

Arbouet, A.

A. Arbouet, D. Christofilos, N. D. Fatti, F. Vall�??ee, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, "Direct measurement of the single-metal-cluster optical absorption," Phys. Rev. Lett. 93, 127401 (2004).
[CrossRef] [PubMed]

Arnaud, L.

A. Arbouet, D. Christofilos, N. D. Fatti, F. Vall�??ee, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, "Direct measurement of the single-metal-cluster optical absorption," Phys. Rev. Lett. 93, 127401 (2004).
[CrossRef] [PubMed]

Atature, M.

A. N. Vamivakas, M. Atature, J. Dreiser, S. T. Yilmaz, A. Badolato, A. K. Swan, B. B. Goldberg, A. Imamoglu, and M. S. Unlu, "Strong extinction of a far-field laser beam by a single quantum dot," Nano Lett. 7, 2892-2896 (2007).
[CrossRef] [PubMed]

Badolato, A.

A. N. Vamivakas, M. Atature, J. Dreiser, S. T. Yilmaz, A. Badolato, A. K. Swan, B. B. Goldberg, A. Imamoglu, and M. S. Unlu, "Strong extinction of a far-field laser beam by a single quantum dot," Nano Lett. 7, 2892-2896 (2007).
[CrossRef] [PubMed]

Bernard, J.

M. Orrit and J. Bernard, "Single Pentacene Molecules Detected by Fluorescence Excitation in a p-Terphenyl Crystal," Phys. Rev. Lett. 65, 2716-2719 (1990).
[CrossRef] [PubMed]

Betzig, E.

E. Betzig and R. J. Chichester, "Single Molecules Observed by Near-Field Scanning Optical Microscopy," Science 262, 1422-1425 (1993).
[CrossRef] [PubMed]

Bickel, F.

B. Alen, F. Bickel, K. Karrai, R. J. Warburton, and P. M. Petroff, "Stark-shift modulation absorption spectroscopy of single quantum dots," Appl. Phys. Lett. 83, 2235-2237 (2003).
[CrossRef]

Billaud, P.

A. Arbouet, D. Christofilos, N. D. Fatti, F. Vall�??ee, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, "Direct measurement of the single-metal-cluster optical absorption," Phys. Rev. Lett. 93, 127401 (2004).
[CrossRef] [PubMed]

Broyer, M.

A. Arbouet, D. Christofilos, N. D. Fatti, F. Vall�??ee, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, "Direct measurement of the single-metal-cluster optical absorption," Phys. Rev. Lett. 93, 127401 (2004).
[CrossRef] [PubMed]

Brunner, C.

Bushev, P.

I. Gerhardt, G. Wrigge, P. Bushev, G. Zumofen, M. Agio, R. Pfab, and V. Sandoghdar, "Strong extinction of a laser beam by a single molecule," Phys. Rev. Lett. 98, 033601 (2007).
[CrossRef] [PubMed]

I. Gerhardt, G. Wrigge, M. Agio, P. Bushev, G. Zumofen, and V. Sandoghdar, "Scanning Near-Field Optical Coherent Spectroscopy of Single Molecules at 1.4 Kelvin," Opt. Lett. 32, 1420-1422 (2007).
[CrossRef] [PubMed]

Celebrano, M.

P. Kukura, M. Celebrano, A. Renn, and V. Sandoghdar, "Seeing a single quantum emitter in its bright and dark states," Nano Lett. (DOI: 10.1021/nl801735y), http://arxiv.org/abs/0802.1206 (2008).
[PubMed]

Chan, V. W. S.

Chichester, R. J.

E. Betzig and R. J. Chichester, "Single Molecules Observed by Near-Field Scanning Optical Microscopy," Science 262, 1422-1425 (1993).
[CrossRef] [PubMed]

Chiu, D. T.

S. Nie, D. T. Chiu, and R. N. Zare, "Probing Individual Molecules with Confocal Fluorescence Microscopy," Science 266, 1018-1021 (1994).
[CrossRef] [PubMed]

Christofilos, D.

A. Arbouet, D. Christofilos, N. D. Fatti, F. Vall�??ee, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, "Direct measurement of the single-metal-cluster optical absorption," Phys. Rev. Lett. 93, 127401 (2004).
[CrossRef] [PubMed]

Davis, L.

E. Shera, N. Seitzinger, L. Davis, R. Keller, and S. Soper, "Detection of single fluorescent molecules," Chem. Phys. Lett. 174, 553-557 (1990).
[CrossRef]

Ditlbacher, H.

C. Sonnichsen, S. Geier, N. E. Hecker, G. von Plessen, J. Feldmann, H. Ditlbacher, b. Lamprecht, J. R. Krenn, F. R. Aussenegg, V. Z.-H. Chan, J. P. Spatz, and M. M¨oller, "Spectroscopy of single metallic nanoparticles using total internal reflection microscopy," Appl. Phys. Lett. 77, 2949-2951 (2000).
[CrossRef]

Dreiser, J.

A. N. Vamivakas, M. Atature, J. Dreiser, S. T. Yilmaz, A. Badolato, A. K. Swan, B. B. Goldberg, A. Imamoglu, and M. S. Unlu, "Strong extinction of a far-field laser beam by a single quantum dot," Nano Lett. 7, 2892-2896 (2007).
[CrossRef] [PubMed]

Ewers, H.

H. Ewers, V. Jacobsen, E. Klotzsch, A. E. Smith, A. Helenius, and V. Sandoghdar, "Label-free Optical Detection and Tracking of Single Virions Bound to their Receptor in Supported Membrane Bilayers," Nano Lett. 7, 2263-2266 (2007).
[CrossRef] [PubMed]

Fatti, N. D.

A. Arbouet, D. Christofilos, N. D. Fatti, F. Vall�??ee, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, "Direct measurement of the single-metal-cluster optical absorption," Phys. Rev. Lett. 93, 127401 (2004).
[CrossRef] [PubMed]

Feldmann, J.

C. Sonnichsen, S. Geier, N. E. Hecker, G. von Plessen, J. Feldmann, H. Ditlbacher, b. Lamprecht, J. R. Krenn, F. R. Aussenegg, V. Z.-H. Chan, J. P. Spatz, and M. M¨oller, "Spectroscopy of single metallic nanoparticles using total internal reflection microscopy," Appl. Phys. Lett. 77, 2949-2951 (2000).
[CrossRef]

Geier, S.

C. Sonnichsen, S. Geier, N. E. Hecker, G. von Plessen, J. Feldmann, H. Ditlbacher, b. Lamprecht, J. R. Krenn, F. R. Aussenegg, V. Z.-H. Chan, J. P. Spatz, and M. M¨oller, "Spectroscopy of single metallic nanoparticles using total internal reflection microscopy," Appl. Phys. Lett. 77, 2949-2951 (2000).
[CrossRef]

Gerhardt, I.

G. Wrigge, I. Gerhardt, J. Hwang, G. Zumofen, and V. Sandoghdar, "Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence," Nature Phys. 4, 60-66 (2008).
[CrossRef]

I. Gerhardt, G. Wrigge, M. Agio, P. Bushev, G. Zumofen, and V. Sandoghdar, "Scanning Near-Field Optical Coherent Spectroscopy of Single Molecules at 1.4 Kelvin," Opt. Lett. 32, 1420-1422 (2007).
[CrossRef] [PubMed]

I. Gerhardt, G. Wrigge, P. Bushev, G. Zumofen, M. Agio, R. Pfab, and V. Sandoghdar, "Strong extinction of a laser beam by a single molecule," Phys. Rev. Lett. 98, 033601 (2007).
[CrossRef] [PubMed]

Goldberg, B. B.

A. N. Vamivakas, M. Atature, J. Dreiser, S. T. Yilmaz, A. Badolato, A. K. Swan, B. B. Goldberg, A. Imamoglu, and M. S. Unlu, "Strong extinction of a far-field laser beam by a single quantum dot," Nano Lett. 7, 2892-2896 (2007).
[CrossRef] [PubMed]

Hecker, N. E.

C. Sonnichsen, S. Geier, N. E. Hecker, G. von Plessen, J. Feldmann, H. Ditlbacher, b. Lamprecht, J. R. Krenn, F. R. Aussenegg, V. Z.-H. Chan, J. P. Spatz, and M. M¨oller, "Spectroscopy of single metallic nanoparticles using total internal reflection microscopy," Appl. Phys. Lett. 77, 2949-2951 (2000).
[CrossRef]

Helenius, A.

H. Ewers, V. Jacobsen, E. Klotzsch, A. E. Smith, A. Helenius, and V. Sandoghdar, "Label-free Optical Detection and Tracking of Single Virions Bound to their Receptor in Supported Membrane Bilayers," Nano Lett. 7, 2263-2266 (2007).
[CrossRef] [PubMed]

Huntzinger, J. R.

A. Arbouet, D. Christofilos, N. D. Fatti, F. Vall�??ee, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, "Direct measurement of the single-metal-cluster optical absorption," Phys. Rev. Lett. 93, 127401 (2004).
[CrossRef] [PubMed]

Hwang, J.

G. Wrigge, I. Gerhardt, J. Hwang, G. Zumofen, and V. Sandoghdar, "Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence," Nature Phys. 4, 60-66 (2008).
[CrossRef]

Ignatovich, F. V.

F. V. Ignatovich and L. Novotny, "Real-Time and Background-Free Detection of Nanoscale Particles," Phys. Rev. Lett. 96, 013901 (2006).
[CrossRef] [PubMed]

Imamoglu, A.

A. N. Vamivakas, M. Atature, J. Dreiser, S. T. Yilmaz, A. Badolato, A. K. Swan, B. B. Goldberg, A. Imamoglu, and M. S. Unlu, "Strong extinction of a far-field laser beam by a single quantum dot," Nano Lett. 7, 2892-2896 (2007).
[CrossRef] [PubMed]

Jacobsen, V.

H. Ewers, V. Jacobsen, E. Klotzsch, A. E. Smith, A. Helenius, and V. Sandoghdar, "Label-free Optical Detection and Tracking of Single Virions Bound to their Receptor in Supported Membrane Bilayers," Nano Lett. 7, 2263-2266 (2007).
[CrossRef] [PubMed]

V. Jacobsen, P. Stoller, C. Brunner, V. Vogel, and V. Sandoghdar, "Interferometric optical detection and tracking of very small gold nanoparticles at a water-glass interface," Opt. Express 14, 405-414 (2006).
[CrossRef] [PubMed]

Kador, L.

W. E. Moerner and L. Kador, "Optical Detection and Spectroscopy of Single Molecules in a Solid," Phys. Rev. Lett. 62, 2535-2538 (1989).
[CrossRef] [PubMed]

Kalkbrenner, T.

K. Lindfors, T. Kalkbrenner, P. Stoller, and V. Sandoghdar, "Detection and spectroscopy of gold nanoparticle using supercontinuum white light confocal microscopy," Phys. Rev. Lett. 93, 037401 (2004).
[CrossRef] [PubMed]

Karrai, K.

B. Alen, F. Bickel, K. Karrai, R. J. Warburton, and P. M. Petroff, "Stark-shift modulation absorption spectroscopy of single quantum dots," Appl. Phys. Lett. 83, 2235-2237 (2003).
[CrossRef]

Keller, R.

E. Shera, N. Seitzinger, L. Davis, R. Keller, and S. Soper, "Detection of single fluorescent molecules," Chem. Phys. Lett. 174, 553-557 (1990).
[CrossRef]

Klimov, V. I.

Klotzsch, E.

H. Ewers, V. Jacobsen, E. Klotzsch, A. E. Smith, A. Helenius, and V. Sandoghdar, "Label-free Optical Detection and Tracking of Single Virions Bound to their Receptor in Supported Membrane Bilayers," Nano Lett. 7, 2263-2266 (2007).
[CrossRef] [PubMed]

Kukura, P.

P. Kukura, M. Celebrano, A. Renn, and V. Sandoghdar, "Seeing a single quantum emitter in its bright and dark states," Nano Lett. (DOI: 10.1021/nl801735y), http://arxiv.org/abs/0802.1206 (2008).
[PubMed]

Kulzer, F.

F. Kulzer and M. Orrit, Single-Molecule Optics, Annu. Rev. Phys. Chem. 55, 585-611 (2004).
[CrossRef] [PubMed]

Lindfors, K.

K. Lindfors, T. Kalkbrenner, P. Stoller, and V. Sandoghdar, "Detection and spectroscopy of gold nanoparticle using supercontinuum white light confocal microscopy," Phys. Rev. Lett. 93, 037401 (2004).
[CrossRef] [PubMed]

Mikhailovsky, A. A.

Mock, J. J.

S. Schultz, D. R. Smith, J. J. Mock, and D. A. Schultz, "Single-target molecule detection with nonbleaching multicolor optical immunolabels," PNAS 97, 996-1001 (2000).
[CrossRef] [PubMed]

Moerner, W. E.

W. E. Moerner, "Examining Nanoenvironments in Solids on the Scale of a Single, Isolated Impurity Molecule," Science 265, 46-53 (1994).
[CrossRef] [PubMed]

W. E. Moerner and L. Kador, "Optical Detection and Spectroscopy of Single Molecules in a Solid," Phys. Rev. Lett. 62, 2535-2538 (1989).
[CrossRef] [PubMed]

Mojarad, N. M.

G. Zumofen, N. M. Mojarad, V. Sandoghdar, and M. Agio, "Perfect Reflection of Light by an Oscillating Dipole," Phys. Rev. Lett. (to appear), http://arxiv.org/abs/0805.3231v2 (2008).
[CrossRef] [PubMed]

Nie, S.

S. Nie, D. T. Chiu, and R. N. Zare, "Probing Individual Molecules with Confocal Fluorescence Microscopy," Science 266, 1018-1021 (1994).
[CrossRef] [PubMed]

Novotny, L.

F. V. Ignatovich and L. Novotny, "Real-Time and Background-Free Detection of Nanoscale Particles," Phys. Rev. Lett. 96, 013901 (2006).
[CrossRef] [PubMed]

Orrit, M.

F. Kulzer and M. Orrit, Single-Molecule Optics, Annu. Rev. Phys. Chem. 55, 585-611 (2004).
[CrossRef] [PubMed]

M. Orrit and J. Bernard, "Single Pentacene Molecules Detected by Fluorescence Excitation in a p-Terphenyl Crystal," Phys. Rev. Lett. 65, 2716-2719 (1990).
[CrossRef] [PubMed]

Palm, V.

T. Plakhotnik and V. Palm, "Interferometric signatures of single molecules," Phys. Rev. Lett. 87, 183602 (2001).
[CrossRef]

Petroff, P. M.

B. Alen, F. Bickel, K. Karrai, R. J. Warburton, and P. M. Petroff, "Stark-shift modulation absorption spectroscopy of single quantum dots," Appl. Phys. Lett. 83, 2235-2237 (2003).
[CrossRef]

Petruska, M. A.

Pfab, R.

I. Gerhardt, G. Wrigge, P. Bushev, G. Zumofen, M. Agio, R. Pfab, and V. Sandoghdar, "Strong extinction of a laser beam by a single molecule," Phys. Rev. Lett. 98, 033601 (2007).
[CrossRef] [PubMed]

Plakhotnik, T.

T. Plakhotnik, "Absorption and coherent emission of single molecules," J. Lumin. 98, 57-62 (2002).
[CrossRef]

T. Plakhotnik and V. Palm, "Interferometric signatures of single molecules," Phys. Rev. Lett. 87, 183602 (2001).
[CrossRef]

Renn, A.

P. Kukura, M. Celebrano, A. Renn, and V. Sandoghdar, "Seeing a single quantum emitter in its bright and dark states," Nano Lett. (DOI: 10.1021/nl801735y), http://arxiv.org/abs/0802.1206 (2008).
[PubMed]

Sandoghdar, V.

P. Kukura, M. Celebrano, A. Renn, and V. Sandoghdar, "Seeing a single quantum emitter in its bright and dark states," Nano Lett. (DOI: 10.1021/nl801735y), http://arxiv.org/abs/0802.1206 (2008).
[PubMed]

G. Zumofen, N. M. Mojarad, V. Sandoghdar, and M. Agio, "Perfect Reflection of Light by an Oscillating Dipole," Phys. Rev. Lett. (to appear), http://arxiv.org/abs/0805.3231v2 (2008).
[CrossRef] [PubMed]

G. Wrigge, I. Gerhardt, J. Hwang, G. Zumofen, and V. Sandoghdar, "Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence," Nature Phys. 4, 60-66 (2008).
[CrossRef]

I. Gerhardt, G. Wrigge, P. Bushev, G. Zumofen, M. Agio, R. Pfab, and V. Sandoghdar, "Strong extinction of a laser beam by a single molecule," Phys. Rev. Lett. 98, 033601 (2007).
[CrossRef] [PubMed]

I. Gerhardt, G. Wrigge, M. Agio, P. Bushev, G. Zumofen, and V. Sandoghdar, "Scanning Near-Field Optical Coherent Spectroscopy of Single Molecules at 1.4 Kelvin," Opt. Lett. 32, 1420-1422 (2007).
[CrossRef] [PubMed]

H. Ewers, V. Jacobsen, E. Klotzsch, A. E. Smith, A. Helenius, and V. Sandoghdar, "Label-free Optical Detection and Tracking of Single Virions Bound to their Receptor in Supported Membrane Bilayers," Nano Lett. 7, 2263-2266 (2007).
[CrossRef] [PubMed]

V. Jacobsen, P. Stoller, C. Brunner, V. Vogel, and V. Sandoghdar, "Interferometric optical detection and tracking of very small gold nanoparticles at a water-glass interface," Opt. Express 14, 405-414 (2006).
[CrossRef] [PubMed]

K. Lindfors, T. Kalkbrenner, P. Stoller, and V. Sandoghdar, "Detection and spectroscopy of gold nanoparticle using supercontinuum white light confocal microscopy," Phys. Rev. Lett. 93, 037401 (2004).
[CrossRef] [PubMed]

Schultz, D. A.

S. Schultz, D. R. Smith, J. J. Mock, and D. A. Schultz, "Single-target molecule detection with nonbleaching multicolor optical immunolabels," PNAS 97, 996-1001 (2000).
[CrossRef] [PubMed]

Schultz, S.

S. Schultz, D. R. Smith, J. J. Mock, and D. A. Schultz, "Single-target molecule detection with nonbleaching multicolor optical immunolabels," PNAS 97, 996-1001 (2000).
[CrossRef] [PubMed]

Seitzinger, N.

E. Shera, N. Seitzinger, L. Davis, R. Keller, and S. Soper, "Detection of single fluorescent molecules," Chem. Phys. Lett. 174, 553-557 (1990).
[CrossRef]

Shera, E.

E. Shera, N. Seitzinger, L. Davis, R. Keller, and S. Soper, "Detection of single fluorescent molecules," Chem. Phys. Lett. 174, 553-557 (1990).
[CrossRef]

Smith, A. E.

H. Ewers, V. Jacobsen, E. Klotzsch, A. E. Smith, A. Helenius, and V. Sandoghdar, "Label-free Optical Detection and Tracking of Single Virions Bound to their Receptor in Supported Membrane Bilayers," Nano Lett. 7, 2263-2266 (2007).
[CrossRef] [PubMed]

Smith, D. R.

S. Schultz, D. R. Smith, J. J. Mock, and D. A. Schultz, "Single-target molecule detection with nonbleaching multicolor optical immunolabels," PNAS 97, 996-1001 (2000).
[CrossRef] [PubMed]

Sonnichsen, C.

C. Sonnichsen, S. Geier, N. E. Hecker, G. von Plessen, J. Feldmann, H. Ditlbacher, b. Lamprecht, J. R. Krenn, F. R. Aussenegg, V. Z.-H. Chan, J. P. Spatz, and M. M¨oller, "Spectroscopy of single metallic nanoparticles using total internal reflection microscopy," Appl. Phys. Lett. 77, 2949-2951 (2000).
[CrossRef]

Soper, S.

E. Shera, N. Seitzinger, L. Davis, R. Keller, and S. Soper, "Detection of single fluorescent molecules," Chem. Phys. Lett. 174, 553-557 (1990).
[CrossRef]

Stockman, M. I.

Stoller, P.

V. Jacobsen, P. Stoller, C. Brunner, V. Vogel, and V. Sandoghdar, "Interferometric optical detection and tracking of very small gold nanoparticles at a water-glass interface," Opt. Express 14, 405-414 (2006).
[CrossRef] [PubMed]

K. Lindfors, T. Kalkbrenner, P. Stoller, and V. Sandoghdar, "Detection and spectroscopy of gold nanoparticle using supercontinuum white light confocal microscopy," Phys. Rev. Lett. 93, 037401 (2004).
[CrossRef] [PubMed]

Swan, A. K.

A. N. Vamivakas, M. Atature, J. Dreiser, S. T. Yilmaz, A. Badolato, A. K. Swan, B. B. Goldberg, A. Imamoglu, and M. S. Unlu, "Strong extinction of a far-field laser beam by a single quantum dot," Nano Lett. 7, 2892-2896 (2007).
[CrossRef] [PubMed]

Vall???ee, F.

A. Arbouet, D. Christofilos, N. D. Fatti, F. Vall�??ee, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, "Direct measurement of the single-metal-cluster optical absorption," Phys. Rev. Lett. 93, 127401 (2004).
[CrossRef] [PubMed]

Vamivakas, A. N.

A. N. Vamivakas, M. Atature, J. Dreiser, S. T. Yilmaz, A. Badolato, A. K. Swan, B. B. Goldberg, A. Imamoglu, and M. S. Unlu, "Strong extinction of a far-field laser beam by a single quantum dot," Nano Lett. 7, 2892-2896 (2007).
[CrossRef] [PubMed]

Vogel, V.

von Plessen, G.

C. Sonnichsen, S. Geier, N. E. Hecker, G. von Plessen, J. Feldmann, H. Ditlbacher, b. Lamprecht, J. R. Krenn, F. R. Aussenegg, V. Z.-H. Chan, J. P. Spatz, and M. M¨oller, "Spectroscopy of single metallic nanoparticles using total internal reflection microscopy," Appl. Phys. Lett. 77, 2949-2951 (2000).
[CrossRef]

Warburton, R. J.

B. Alen, F. Bickel, K. Karrai, R. J. Warburton, and P. M. Petroff, "Stark-shift modulation absorption spectroscopy of single quantum dots," Appl. Phys. Lett. 83, 2235-2237 (2003).
[CrossRef]

Wrigge, G.

G. Wrigge, I. Gerhardt, J. Hwang, G. Zumofen, and V. Sandoghdar, "Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence," Nature Phys. 4, 60-66 (2008).
[CrossRef]

I. Gerhardt, G. Wrigge, M. Agio, P. Bushev, G. Zumofen, and V. Sandoghdar, "Scanning Near-Field Optical Coherent Spectroscopy of Single Molecules at 1.4 Kelvin," Opt. Lett. 32, 1420-1422 (2007).
[CrossRef] [PubMed]

I. Gerhardt, G. Wrigge, P. Bushev, G. Zumofen, M. Agio, R. Pfab, and V. Sandoghdar, "Strong extinction of a laser beam by a single molecule," Phys. Rev. Lett. 98, 033601 (2007).
[CrossRef] [PubMed]

Yilmaz, S. T.

A. N. Vamivakas, M. Atature, J. Dreiser, S. T. Yilmaz, A. Badolato, A. K. Swan, B. B. Goldberg, A. Imamoglu, and M. S. Unlu, "Strong extinction of a far-field laser beam by a single quantum dot," Nano Lett. 7, 2892-2896 (2007).
[CrossRef] [PubMed]

Yuen, H. P.

Zare, R. N.

S. Nie, D. T. Chiu, and R. N. Zare, "Probing Individual Molecules with Confocal Fluorescence Microscopy," Science 266, 1018-1021 (1994).
[CrossRef] [PubMed]

Zumofen, G.

G. Wrigge, I. Gerhardt, J. Hwang, G. Zumofen, and V. Sandoghdar, "Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence," Nature Phys. 4, 60-66 (2008).
[CrossRef]

G. Zumofen, N. M. Mojarad, V. Sandoghdar, and M. Agio, "Perfect Reflection of Light by an Oscillating Dipole," Phys. Rev. Lett. (to appear), http://arxiv.org/abs/0805.3231v2 (2008).
[CrossRef] [PubMed]

I. Gerhardt, G. Wrigge, P. Bushev, G. Zumofen, M. Agio, R. Pfab, and V. Sandoghdar, "Strong extinction of a laser beam by a single molecule," Phys. Rev. Lett. 98, 033601 (2007).
[CrossRef] [PubMed]

I. Gerhardt, G. Wrigge, M. Agio, P. Bushev, G. Zumofen, and V. Sandoghdar, "Scanning Near-Field Optical Coherent Spectroscopy of Single Molecules at 1.4 Kelvin," Opt. Lett. 32, 1420-1422 (2007).
[CrossRef] [PubMed]

Annu. Rev. Phys. Chem.

F. Kulzer and M. Orrit, Single-Molecule Optics, Annu. Rev. Phys. Chem. 55, 585-611 (2004).
[CrossRef] [PubMed]

Appl. Phys. Lett.

B. Alen, F. Bickel, K. Karrai, R. J. Warburton, and P. M. Petroff, "Stark-shift modulation absorption spectroscopy of single quantum dots," Appl. Phys. Lett. 83, 2235-2237 (2003).
[CrossRef]

C. Sonnichsen, S. Geier, N. E. Hecker, G. von Plessen, J. Feldmann, H. Ditlbacher, b. Lamprecht, J. R. Krenn, F. R. Aussenegg, V. Z.-H. Chan, J. P. Spatz, and M. M¨oller, "Spectroscopy of single metallic nanoparticles using total internal reflection microscopy," Appl. Phys. Lett. 77, 2949-2951 (2000).
[CrossRef]

Chem. Phys. Lett.

E. Shera, N. Seitzinger, L. Davis, R. Keller, and S. Soper, "Detection of single fluorescent molecules," Chem. Phys. Lett. 174, 553-557 (1990).
[CrossRef]

J. Lumin.

T. Plakhotnik, "Absorption and coherent emission of single molecules," J. Lumin. 98, 57-62 (2002).
[CrossRef]

Nano Lett.

A. N. Vamivakas, M. Atature, J. Dreiser, S. T. Yilmaz, A. Badolato, A. K. Swan, B. B. Goldberg, A. Imamoglu, and M. S. Unlu, "Strong extinction of a far-field laser beam by a single quantum dot," Nano Lett. 7, 2892-2896 (2007).
[CrossRef] [PubMed]

P. Kukura, M. Celebrano, A. Renn, and V. Sandoghdar, "Seeing a single quantum emitter in its bright and dark states," Nano Lett. (DOI: 10.1021/nl801735y), http://arxiv.org/abs/0802.1206 (2008).
[PubMed]

H. Ewers, V. Jacobsen, E. Klotzsch, A. E. Smith, A. Helenius, and V. Sandoghdar, "Label-free Optical Detection and Tracking of Single Virions Bound to their Receptor in Supported Membrane Bilayers," Nano Lett. 7, 2263-2266 (2007).
[CrossRef] [PubMed]

Nature Phys.

G. Wrigge, I. Gerhardt, J. Hwang, G. Zumofen, and V. Sandoghdar, "Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence," Nature Phys. 4, 60-66 (2008).
[CrossRef]

Opt. Express

Opt. Lett.

Phys. Rev. Lett.

G. Zumofen, N. M. Mojarad, V. Sandoghdar, and M. Agio, "Perfect Reflection of Light by an Oscillating Dipole," Phys. Rev. Lett. (to appear), http://arxiv.org/abs/0805.3231v2 (2008).
[CrossRef] [PubMed]

I. Gerhardt, G. Wrigge, P. Bushev, G. Zumofen, M. Agio, R. Pfab, and V. Sandoghdar, "Strong extinction of a laser beam by a single molecule," Phys. Rev. Lett. 98, 033601 (2007).
[CrossRef] [PubMed]

W. E. Moerner and L. Kador, "Optical Detection and Spectroscopy of Single Molecules in a Solid," Phys. Rev. Lett. 62, 2535-2538 (1989).
[CrossRef] [PubMed]

M. Orrit and J. Bernard, "Single Pentacene Molecules Detected by Fluorescence Excitation in a p-Terphenyl Crystal," Phys. Rev. Lett. 65, 2716-2719 (1990).
[CrossRef] [PubMed]

T. Plakhotnik and V. Palm, "Interferometric signatures of single molecules," Phys. Rev. Lett. 87, 183602 (2001).
[CrossRef]

K. Lindfors, T. Kalkbrenner, P. Stoller, and V. Sandoghdar, "Detection and spectroscopy of gold nanoparticle using supercontinuum white light confocal microscopy," Phys. Rev. Lett. 93, 037401 (2004).
[CrossRef] [PubMed]

A. Arbouet, D. Christofilos, N. D. Fatti, F. Vall�??ee, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, "Direct measurement of the single-metal-cluster optical absorption," Phys. Rev. Lett. 93, 127401 (2004).
[CrossRef] [PubMed]

F. V. Ignatovich and L. Novotny, "Real-Time and Background-Free Detection of Nanoscale Particles," Phys. Rev. Lett. 96, 013901 (2006).
[CrossRef] [PubMed]

PNAS

S. Schultz, D. R. Smith, J. J. Mock, and D. A. Schultz, "Single-target molecule detection with nonbleaching multicolor optical immunolabels," PNAS 97, 996-1001 (2000).
[CrossRef] [PubMed]

Science

E. Betzig and R. J. Chichester, "Single Molecules Observed by Near-Field Scanning Optical Microscopy," Science 262, 1422-1425 (1993).
[CrossRef] [PubMed]

S. Nie, D. T. Chiu, and R. N. Zare, "Probing Individual Molecules with Confocal Fluorescence Microscopy," Science 266, 1018-1021 (1994).
[CrossRef] [PubMed]

W. E. Moerner, "Examining Nanoenvironments in Solids on the Scale of a Single, Isolated Impurity Molecule," Science 265, 46-53 (1994).
[CrossRef] [PubMed]

Other

C. Cohen-Tannoudji, J. Dupont-Roc, and G. Grynberg, Atom-Photon Interactions (John Wiley & Sons, Inc., 1992).

D. Jackson, Classical Electrodynamics (Wiley and Sons, 1999).

H. A. Haus, Electromagnetic Noise and Quantum Optical Measurements (Springer-Verlag, Heidelberg, 2000).

T. Basche, W. E. Moerner, M. Orrit, and U. Wild, Single Molecule Spectroscopy (John Wiley and Sons, 1999).

J. R. Guest, T. H. Stievater, X. Li, J. Cheng, D. G. Steel, D. Gammon, D. S. Katzer, D. Park, C. Ell, A. Thranhardt, G. Khitrova, and H. M. Gibbs, "Measurement of optical absorption by a single quantum dot exciton," Phys. Rev. B. 65, 241310(R) (2002).
[CrossRef]

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Figures (4)

Fig. 1.
Fig. 1.

(a) The level scheme of a dye molecule. (b) The schematics of our experimental setup. A laser beam is focused onto the sample using an aspheric lens (AL) and a hemispherical solid-immersion lens (SIL). A second aspherical lens is used to collect the transmitted laser beam as well as the forward emitted fluorescence of the molecule. LP: long pass filter, SP: short pass filter, PD: photodetector.

Fig. 2.
Fig. 2.

a), c), e) Extinction spectra recorded from a single molecule in transmission at three different detected laser powers of 106, 3×104, 2×103 cps as measured on the detector. b), d), f) Fluorescence excitation spectra recorded under same conditions as spectra a), c), and e), respectively.

Fig. 3.
Fig. 3.

The signal-to-noise ratios of the resonant transmission (circles, green lines) and fluorescence (triangles, red lines) signals as a function of the excitation power and saturation parameter for two different definitions of noise: (a) noise determined from the fluctuations of the signal on resonance, (b) noise evaluated from the fluctuations of the off-resonant background. Symbols display the experimental data and the lines denote the theoretical behavior.

Fig. 4.
Fig. 4.

The SNR for a resonant transmission detection of emitters with different radiative decay rates. Here we have assumed α=µ=1, P drk=20 cps, and K=0.5. Γ1 is given in units of rad/sec.

Equations (14)

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

P = ε 0 c r 2 2 h ̄ ω Ω ( E ̂ las · E ̂ las + + E ̂ m · E ̂ m + + 2 R e E ̂ las · E ̂ m + ) d Ω
= P las + P m Ω P ext ,
P las = ε 0 c r 2 2 h ̄ ω Ω E ̂ las · E ̂ las + d Ω
P m 4 π = ε 0 c r 2 2 h ̄ ω 4 π E ̂ m · E ̂ m + d Ω = Γ 1 ρ 22 = Γ 1 2 S 1 + S
P m Ω = ζ P m 4 π
P m res = α P m Ω
P m red = ( 1 α ) P m Ω = ζ ( 1 α ) Γ 1 2 S 1 + S
P ext = ε 0 c r 2 2 h ̄ ω Ω 2 R e E ̂ las · E ̂ m + d Ω .
S = V 2 Γ 1 Γ 2 ,
S = α Γ 2 K P las ,
SNR red = μ P m red N red = { μ ζ ( 1 α ) Γ 1 2 P drk S 1 + S , μ P red P drk μ ζ ( 1 α ) Γ 1 2 S 1 + S , μ P red P drk ,
P dip res = P ext P m res = P m 4 π P m res = ( 1 α ζ ) Γ 1 2 S 1 + S .
N res = μ ( P las P dip res ) + μ 2 κ 2 ( P las P dip res ) 2 + P drk ,
SNR res = μ P dip res N res ( 1 ζ α ) Γ 1 2 μ α K Γ 2 S 1 + S .

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