Abstract

We report on ultralow frequency Stokes and anti-Stokes Raman spectroscopy of single living cells and microsized particles in an aqueous medium with a frequency shift down to 10cm1 by the combination of a hot rubidium (Rb) vapor filter, a confocal pinhole, and optical trapping. A single frequency-stabilized diode laser beam at 780.2 nm is used to optically trap and excite a single living cell or microparticle, and the Rayleigh scattering light from the particle is effectively blocked with a Rb vapor cell and a confocal pinhole. Ultralow frequency Raman spectra of the trapped cells or microparticles in both Stokes and anti-Stokes regions are then measured with a single-stage CCD spectrograph.

© 2013 Optical Society of America

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  1. K. Brown, S. Erfurth, E. Small, and W. Peticolas, Proc. Natl. Acad. Sci. USA 69, 1467 (1972).
    [CrossRef]
  2. A. Lerbet, F. Affouard, P. Bordat, A. Hedoux, Y. Guinet, and M. Descamps, J. Chem. Phys. 131, 245103 (2009).
    [CrossRef]
  3. J. Ibanez, A. Rapaport, C. Boney, R. Oliva, R. Cuscó, A. Bensaoula, and L. Artús, J. Raman Spectrosc. 43, 237 (2012).
    [CrossRef]
  4. A. Puretzky, D. Geohegan, and C. Rouleau, Phys. Rev. B 82, 245402 (2010).
    [CrossRef]
  5. J. Carriere and F. Havermeyer, Proc. SPIE 8219, 821905 (2012).
    [CrossRef]
  6. N. Brandt, A. Chikishev, A. Kargovsky, M. Nazarov, O. Parashchuk, D. Sapozhnikov, I. Smirnova, A. Shkurinov, and N. Sumbatyan, Vib. Spectrosc. 47, 53 (2008).
  7. H. Okajima and H. Hamaguchi, Appl. Spectrosc. 63, 958 (2009).
    [CrossRef]
  8. R. Indralingam, J. Simeonsson, G. Petrucci, B. Smith, and J. Winefordner, Anal. Chem. 64, 964 (1992).
    [CrossRef]
  9. P. Horoyski and M. Thewalt, Appl. Spectrosc. 48, 843 (1994).
    [CrossRef]
  10. R. B. Miles, A. P. Yalin, Z. Tang, S. H. Zaidiand, and J. N. Forkey, Meas. Sci. Technol. 12, 442 (2001).
    [CrossRef]
  11. S. Lebedkin, C. Blum, N. Stürzl, F. Hennrich, and M. M. Kappes, Rev. Sci. Instrum. 82, 013705 (2011).
    [CrossRef]
  12. C. A. Xie, M. A. Dinno, and Y. Q. Li, Opt. Lett. 27, 249 (2002).
    [CrossRef]
  13. L. B. Kong, P. F. Zhang, G. W. Wang, P. Setlow, and Y. Q. Li, Nat. Protoc. 6, 625 (2011).
    [CrossRef]
  14. Y.-H. Lee, R. G. Maus, B. W. Smith, and J. D. Winefordner, Anal. Chem. 66, 4142 (1994).
    [CrossRef]
  15. L. B. Kong, P. Setlow, and Y. Q. Li, Anal. Chem. 85, 7094 (2013).
    [CrossRef]
  16. T. Achibat, A. Boukenter, E. Duval, G. Lorentz, and S. Etienne, J. Chem. Phys. 95, 2949 (1991).
    [CrossRef]
  17. B. Schmid and W. Schirmacher, Phys. Rev. Lett. 100, 137402 (2008).
    [CrossRef]
  18. A. Kalampounias, K. Andrikopoulos, and S. Yannopoulos, J. Chem. Phys. 118, 8460 (2003).
    [CrossRef]

2013 (1)

L. B. Kong, P. Setlow, and Y. Q. Li, Anal. Chem. 85, 7094 (2013).
[CrossRef]

2012 (2)

J. Ibanez, A. Rapaport, C. Boney, R. Oliva, R. Cuscó, A. Bensaoula, and L. Artús, J. Raman Spectrosc. 43, 237 (2012).
[CrossRef]

J. Carriere and F. Havermeyer, Proc. SPIE 8219, 821905 (2012).
[CrossRef]

2011 (2)

L. B. Kong, P. F. Zhang, G. W. Wang, P. Setlow, and Y. Q. Li, Nat. Protoc. 6, 625 (2011).
[CrossRef]

S. Lebedkin, C. Blum, N. Stürzl, F. Hennrich, and M. M. Kappes, Rev. Sci. Instrum. 82, 013705 (2011).
[CrossRef]

2010 (1)

A. Puretzky, D. Geohegan, and C. Rouleau, Phys. Rev. B 82, 245402 (2010).
[CrossRef]

2009 (2)

A. Lerbet, F. Affouard, P. Bordat, A. Hedoux, Y. Guinet, and M. Descamps, J. Chem. Phys. 131, 245103 (2009).
[CrossRef]

H. Okajima and H. Hamaguchi, Appl. Spectrosc. 63, 958 (2009).
[CrossRef]

2008 (2)

N. Brandt, A. Chikishev, A. Kargovsky, M. Nazarov, O. Parashchuk, D. Sapozhnikov, I. Smirnova, A. Shkurinov, and N. Sumbatyan, Vib. Spectrosc. 47, 53 (2008).

B. Schmid and W. Schirmacher, Phys. Rev. Lett. 100, 137402 (2008).
[CrossRef]

2003 (1)

A. Kalampounias, K. Andrikopoulos, and S. Yannopoulos, J. Chem. Phys. 118, 8460 (2003).
[CrossRef]

2002 (1)

2001 (1)

R. B. Miles, A. P. Yalin, Z. Tang, S. H. Zaidiand, and J. N. Forkey, Meas. Sci. Technol. 12, 442 (2001).
[CrossRef]

1994 (2)

P. Horoyski and M. Thewalt, Appl. Spectrosc. 48, 843 (1994).
[CrossRef]

Y.-H. Lee, R. G. Maus, B. W. Smith, and J. D. Winefordner, Anal. Chem. 66, 4142 (1994).
[CrossRef]

1992 (1)

R. Indralingam, J. Simeonsson, G. Petrucci, B. Smith, and J. Winefordner, Anal. Chem. 64, 964 (1992).
[CrossRef]

1991 (1)

T. Achibat, A. Boukenter, E. Duval, G. Lorentz, and S. Etienne, J. Chem. Phys. 95, 2949 (1991).
[CrossRef]

1972 (1)

K. Brown, S. Erfurth, E. Small, and W. Peticolas, Proc. Natl. Acad. Sci. USA 69, 1467 (1972).
[CrossRef]

Achibat, T.

T. Achibat, A. Boukenter, E. Duval, G. Lorentz, and S. Etienne, J. Chem. Phys. 95, 2949 (1991).
[CrossRef]

Affouard, F.

A. Lerbet, F. Affouard, P. Bordat, A. Hedoux, Y. Guinet, and M. Descamps, J. Chem. Phys. 131, 245103 (2009).
[CrossRef]

Andrikopoulos, K.

A. Kalampounias, K. Andrikopoulos, and S. Yannopoulos, J. Chem. Phys. 118, 8460 (2003).
[CrossRef]

Artús, L.

J. Ibanez, A. Rapaport, C. Boney, R. Oliva, R. Cuscó, A. Bensaoula, and L. Artús, J. Raman Spectrosc. 43, 237 (2012).
[CrossRef]

Bensaoula, A.

J. Ibanez, A. Rapaport, C. Boney, R. Oliva, R. Cuscó, A. Bensaoula, and L. Artús, J. Raman Spectrosc. 43, 237 (2012).
[CrossRef]

Blum, C.

S. Lebedkin, C. Blum, N. Stürzl, F. Hennrich, and M. M. Kappes, Rev. Sci. Instrum. 82, 013705 (2011).
[CrossRef]

Boney, C.

J. Ibanez, A. Rapaport, C. Boney, R. Oliva, R. Cuscó, A. Bensaoula, and L. Artús, J. Raman Spectrosc. 43, 237 (2012).
[CrossRef]

Bordat, P.

A. Lerbet, F. Affouard, P. Bordat, A. Hedoux, Y. Guinet, and M. Descamps, J. Chem. Phys. 131, 245103 (2009).
[CrossRef]

Boukenter, A.

T. Achibat, A. Boukenter, E. Duval, G. Lorentz, and S. Etienne, J. Chem. Phys. 95, 2949 (1991).
[CrossRef]

Brandt, N.

N. Brandt, A. Chikishev, A. Kargovsky, M. Nazarov, O. Parashchuk, D. Sapozhnikov, I. Smirnova, A. Shkurinov, and N. Sumbatyan, Vib. Spectrosc. 47, 53 (2008).

Brown, K.

K. Brown, S. Erfurth, E. Small, and W. Peticolas, Proc. Natl. Acad. Sci. USA 69, 1467 (1972).
[CrossRef]

Carriere, J.

J. Carriere and F. Havermeyer, Proc. SPIE 8219, 821905 (2012).
[CrossRef]

Chikishev, A.

N. Brandt, A. Chikishev, A. Kargovsky, M. Nazarov, O. Parashchuk, D. Sapozhnikov, I. Smirnova, A. Shkurinov, and N. Sumbatyan, Vib. Spectrosc. 47, 53 (2008).

Cuscó, R.

J. Ibanez, A. Rapaport, C. Boney, R. Oliva, R. Cuscó, A. Bensaoula, and L. Artús, J. Raman Spectrosc. 43, 237 (2012).
[CrossRef]

Descamps, M.

A. Lerbet, F. Affouard, P. Bordat, A. Hedoux, Y. Guinet, and M. Descamps, J. Chem. Phys. 131, 245103 (2009).
[CrossRef]

Dinno, M. A.

Duval, E.

T. Achibat, A. Boukenter, E. Duval, G. Lorentz, and S. Etienne, J. Chem. Phys. 95, 2949 (1991).
[CrossRef]

Erfurth, S.

K. Brown, S. Erfurth, E. Small, and W. Peticolas, Proc. Natl. Acad. Sci. USA 69, 1467 (1972).
[CrossRef]

Etienne, S.

T. Achibat, A. Boukenter, E. Duval, G. Lorentz, and S. Etienne, J. Chem. Phys. 95, 2949 (1991).
[CrossRef]

Forkey, J. N.

R. B. Miles, A. P. Yalin, Z. Tang, S. H. Zaidiand, and J. N. Forkey, Meas. Sci. Technol. 12, 442 (2001).
[CrossRef]

Geohegan, D.

A. Puretzky, D. Geohegan, and C. Rouleau, Phys. Rev. B 82, 245402 (2010).
[CrossRef]

Guinet, Y.

A. Lerbet, F. Affouard, P. Bordat, A. Hedoux, Y. Guinet, and M. Descamps, J. Chem. Phys. 131, 245103 (2009).
[CrossRef]

Hamaguchi, H.

Havermeyer, F.

J. Carriere and F. Havermeyer, Proc. SPIE 8219, 821905 (2012).
[CrossRef]

Hedoux, A.

A. Lerbet, F. Affouard, P. Bordat, A. Hedoux, Y. Guinet, and M. Descamps, J. Chem. Phys. 131, 245103 (2009).
[CrossRef]

Hennrich, F.

S. Lebedkin, C. Blum, N. Stürzl, F. Hennrich, and M. M. Kappes, Rev. Sci. Instrum. 82, 013705 (2011).
[CrossRef]

Horoyski, P.

Ibanez, J.

J. Ibanez, A. Rapaport, C. Boney, R. Oliva, R. Cuscó, A. Bensaoula, and L. Artús, J. Raman Spectrosc. 43, 237 (2012).
[CrossRef]

Indralingam, R.

R. Indralingam, J. Simeonsson, G. Petrucci, B. Smith, and J. Winefordner, Anal. Chem. 64, 964 (1992).
[CrossRef]

Kalampounias, A.

A. Kalampounias, K. Andrikopoulos, and S. Yannopoulos, J. Chem. Phys. 118, 8460 (2003).
[CrossRef]

Kappes, M. M.

S. Lebedkin, C. Blum, N. Stürzl, F. Hennrich, and M. M. Kappes, Rev. Sci. Instrum. 82, 013705 (2011).
[CrossRef]

Kargovsky, A.

N. Brandt, A. Chikishev, A. Kargovsky, M. Nazarov, O. Parashchuk, D. Sapozhnikov, I. Smirnova, A. Shkurinov, and N. Sumbatyan, Vib. Spectrosc. 47, 53 (2008).

Kong, L. B.

L. B. Kong, P. Setlow, and Y. Q. Li, Anal. Chem. 85, 7094 (2013).
[CrossRef]

L. B. Kong, P. F. Zhang, G. W. Wang, P. Setlow, and Y. Q. Li, Nat. Protoc. 6, 625 (2011).
[CrossRef]

Lebedkin, S.

S. Lebedkin, C. Blum, N. Stürzl, F. Hennrich, and M. M. Kappes, Rev. Sci. Instrum. 82, 013705 (2011).
[CrossRef]

Lee, Y.-H.

Y.-H. Lee, R. G. Maus, B. W. Smith, and J. D. Winefordner, Anal. Chem. 66, 4142 (1994).
[CrossRef]

Lerbet, A.

A. Lerbet, F. Affouard, P. Bordat, A. Hedoux, Y. Guinet, and M. Descamps, J. Chem. Phys. 131, 245103 (2009).
[CrossRef]

Li, Y. Q.

L. B. Kong, P. Setlow, and Y. Q. Li, Anal. Chem. 85, 7094 (2013).
[CrossRef]

L. B. Kong, P. F. Zhang, G. W. Wang, P. Setlow, and Y. Q. Li, Nat. Protoc. 6, 625 (2011).
[CrossRef]

C. A. Xie, M. A. Dinno, and Y. Q. Li, Opt. Lett. 27, 249 (2002).
[CrossRef]

Lorentz, G.

T. Achibat, A. Boukenter, E. Duval, G. Lorentz, and S. Etienne, J. Chem. Phys. 95, 2949 (1991).
[CrossRef]

Maus, R. G.

Y.-H. Lee, R. G. Maus, B. W. Smith, and J. D. Winefordner, Anal. Chem. 66, 4142 (1994).
[CrossRef]

Miles, R. B.

R. B. Miles, A. P. Yalin, Z. Tang, S. H. Zaidiand, and J. N. Forkey, Meas. Sci. Technol. 12, 442 (2001).
[CrossRef]

Nazarov, M.

N. Brandt, A. Chikishev, A. Kargovsky, M. Nazarov, O. Parashchuk, D. Sapozhnikov, I. Smirnova, A. Shkurinov, and N. Sumbatyan, Vib. Spectrosc. 47, 53 (2008).

Okajima, H.

Oliva, R.

J. Ibanez, A. Rapaport, C. Boney, R. Oliva, R. Cuscó, A. Bensaoula, and L. Artús, J. Raman Spectrosc. 43, 237 (2012).
[CrossRef]

Parashchuk, O.

N. Brandt, A. Chikishev, A. Kargovsky, M. Nazarov, O. Parashchuk, D. Sapozhnikov, I. Smirnova, A. Shkurinov, and N. Sumbatyan, Vib. Spectrosc. 47, 53 (2008).

Peticolas, W.

K. Brown, S. Erfurth, E. Small, and W. Peticolas, Proc. Natl. Acad. Sci. USA 69, 1467 (1972).
[CrossRef]

Petrucci, G.

R. Indralingam, J. Simeonsson, G. Petrucci, B. Smith, and J. Winefordner, Anal. Chem. 64, 964 (1992).
[CrossRef]

Puretzky, A.

A. Puretzky, D. Geohegan, and C. Rouleau, Phys. Rev. B 82, 245402 (2010).
[CrossRef]

Rapaport, A.

J. Ibanez, A. Rapaport, C. Boney, R. Oliva, R. Cuscó, A. Bensaoula, and L. Artús, J. Raman Spectrosc. 43, 237 (2012).
[CrossRef]

Rouleau, C.

A. Puretzky, D. Geohegan, and C. Rouleau, Phys. Rev. B 82, 245402 (2010).
[CrossRef]

Sapozhnikov, D.

N. Brandt, A. Chikishev, A. Kargovsky, M. Nazarov, O. Parashchuk, D. Sapozhnikov, I. Smirnova, A. Shkurinov, and N. Sumbatyan, Vib. Spectrosc. 47, 53 (2008).

Schirmacher, W.

B. Schmid and W. Schirmacher, Phys. Rev. Lett. 100, 137402 (2008).
[CrossRef]

Schmid, B.

B. Schmid and W. Schirmacher, Phys. Rev. Lett. 100, 137402 (2008).
[CrossRef]

Setlow, P.

L. B. Kong, P. Setlow, and Y. Q. Li, Anal. Chem. 85, 7094 (2013).
[CrossRef]

L. B. Kong, P. F. Zhang, G. W. Wang, P. Setlow, and Y. Q. Li, Nat. Protoc. 6, 625 (2011).
[CrossRef]

Shkurinov, A.

N. Brandt, A. Chikishev, A. Kargovsky, M. Nazarov, O. Parashchuk, D. Sapozhnikov, I. Smirnova, A. Shkurinov, and N. Sumbatyan, Vib. Spectrosc. 47, 53 (2008).

Simeonsson, J.

R. Indralingam, J. Simeonsson, G. Petrucci, B. Smith, and J. Winefordner, Anal. Chem. 64, 964 (1992).
[CrossRef]

Small, E.

K. Brown, S. Erfurth, E. Small, and W. Peticolas, Proc. Natl. Acad. Sci. USA 69, 1467 (1972).
[CrossRef]

Smirnova, I.

N. Brandt, A. Chikishev, A. Kargovsky, M. Nazarov, O. Parashchuk, D. Sapozhnikov, I. Smirnova, A. Shkurinov, and N. Sumbatyan, Vib. Spectrosc. 47, 53 (2008).

Smith, B.

R. Indralingam, J. Simeonsson, G. Petrucci, B. Smith, and J. Winefordner, Anal. Chem. 64, 964 (1992).
[CrossRef]

Smith, B. W.

Y.-H. Lee, R. G. Maus, B. W. Smith, and J. D. Winefordner, Anal. Chem. 66, 4142 (1994).
[CrossRef]

Stürzl, N.

S. Lebedkin, C. Blum, N. Stürzl, F. Hennrich, and M. M. Kappes, Rev. Sci. Instrum. 82, 013705 (2011).
[CrossRef]

Sumbatyan, N.

N. Brandt, A. Chikishev, A. Kargovsky, M. Nazarov, O. Parashchuk, D. Sapozhnikov, I. Smirnova, A. Shkurinov, and N. Sumbatyan, Vib. Spectrosc. 47, 53 (2008).

Tang, Z.

R. B. Miles, A. P. Yalin, Z. Tang, S. H. Zaidiand, and J. N. Forkey, Meas. Sci. Technol. 12, 442 (2001).
[CrossRef]

Thewalt, M.

Wang, G. W.

L. B. Kong, P. F. Zhang, G. W. Wang, P. Setlow, and Y. Q. Li, Nat. Protoc. 6, 625 (2011).
[CrossRef]

Winefordner, J.

R. Indralingam, J. Simeonsson, G. Petrucci, B. Smith, and J. Winefordner, Anal. Chem. 64, 964 (1992).
[CrossRef]

Winefordner, J. D.

Y.-H. Lee, R. G. Maus, B. W. Smith, and J. D. Winefordner, Anal. Chem. 66, 4142 (1994).
[CrossRef]

Xie, C. A.

Yalin, A. P.

R. B. Miles, A. P. Yalin, Z. Tang, S. H. Zaidiand, and J. N. Forkey, Meas. Sci. Technol. 12, 442 (2001).
[CrossRef]

Yannopoulos, S.

A. Kalampounias, K. Andrikopoulos, and S. Yannopoulos, J. Chem. Phys. 118, 8460 (2003).
[CrossRef]

Zaidiand, S. H.

R. B. Miles, A. P. Yalin, Z. Tang, S. H. Zaidiand, and J. N. Forkey, Meas. Sci. Technol. 12, 442 (2001).
[CrossRef]

Zhang, P. F.

L. B. Kong, P. F. Zhang, G. W. Wang, P. Setlow, and Y. Q. Li, Nat. Protoc. 6, 625 (2011).
[CrossRef]

Anal. Chem. (3)

R. Indralingam, J. Simeonsson, G. Petrucci, B. Smith, and J. Winefordner, Anal. Chem. 64, 964 (1992).
[CrossRef]

Y.-H. Lee, R. G. Maus, B. W. Smith, and J. D. Winefordner, Anal. Chem. 66, 4142 (1994).
[CrossRef]

L. B. Kong, P. Setlow, and Y. Q. Li, Anal. Chem. 85, 7094 (2013).
[CrossRef]

Appl. Spectrosc. (2)

J. Chem. Phys. (3)

A. Lerbet, F. Affouard, P. Bordat, A. Hedoux, Y. Guinet, and M. Descamps, J. Chem. Phys. 131, 245103 (2009).
[CrossRef]

T. Achibat, A. Boukenter, E. Duval, G. Lorentz, and S. Etienne, J. Chem. Phys. 95, 2949 (1991).
[CrossRef]

A. Kalampounias, K. Andrikopoulos, and S. Yannopoulos, J. Chem. Phys. 118, 8460 (2003).
[CrossRef]

J. Raman Spectrosc. (1)

J. Ibanez, A. Rapaport, C. Boney, R. Oliva, R. Cuscó, A. Bensaoula, and L. Artús, J. Raman Spectrosc. 43, 237 (2012).
[CrossRef]

Meas. Sci. Technol. (1)

R. B. Miles, A. P. Yalin, Z. Tang, S. H. Zaidiand, and J. N. Forkey, Meas. Sci. Technol. 12, 442 (2001).
[CrossRef]

Nat. Protoc. (1)

L. B. Kong, P. F. Zhang, G. W. Wang, P. Setlow, and Y. Q. Li, Nat. Protoc. 6, 625 (2011).
[CrossRef]

Opt. Lett. (1)

Phys. Rev. B (1)

A. Puretzky, D. Geohegan, and C. Rouleau, Phys. Rev. B 82, 245402 (2010).
[CrossRef]

Phys. Rev. Lett. (1)

B. Schmid and W. Schirmacher, Phys. Rev. Lett. 100, 137402 (2008).
[CrossRef]

Proc. Natl. Acad. Sci. USA (1)

K. Brown, S. Erfurth, E. Small, and W. Peticolas, Proc. Natl. Acad. Sci. USA 69, 1467 (1972).
[CrossRef]

Proc. SPIE (1)

J. Carriere and F. Havermeyer, Proc. SPIE 8219, 821905 (2012).
[CrossRef]

Rev. Sci. Instrum. (1)

S. Lebedkin, C. Blum, N. Stürzl, F. Hennrich, and M. M. Kappes, Rev. Sci. Instrum. 82, 013705 (2011).
[CrossRef]

Vib. Spectrosc. (1)

N. Brandt, A. Chikishev, A. Kargovsky, M. Nazarov, O. Parashchuk, D. Sapozhnikov, I. Smirnova, A. Shkurinov, and N. Sumbatyan, Vib. Spectrosc. 47, 53 (2008).

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Figures (3)

Fig. 1.
Fig. 1.

(A) The schematic of the experimental setup. BPF, Bragg bandpass filter; BNF, Bragg notch filter; Obj., objective; M, mirror; DM, dichroic mirror; SP, spectrograph. (B) Raman spectrum of an optically trapped B. megaterium spore in distilled water. (C) Raman spectrum of a sulfur particle in the trap. The inset is the bright-field image of the particle with a scale bar of 4 μm.

Fig. 2.
Fig. 2.

(A) Transmission profile of the Rb vapor filter at 25°C and 130°C. (B) Optical absorbance of the Rb vapor filter at different temperatures with a fixed resonance frequency at 780.2 nm. (C) Raman spectra of an optically trapped 2 μm polystyrene sphere 10 μm above (curve a) or close to the bottom surface (curve b), with the background without the particle in the trap (curve c).

Fig. 3.
Fig. 3.

Ultralow frequency Raman spectra of single optically trapped particles of (A) a single red blood cell (RBC), (B) DPA powder, (C) L-cystine, (D) aspirin, (E) acetaminophen, and (F) TiO2. Insets are the images of the particles or clusters with a scale bar of 4 μm. The laser power was 20mW and the acquisition time was typically 1 s (except for 5 s for the RBC).

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