Abstract

In organic photovoltaics many key ultrafast processes occur at the interface between electron donor and acceptor molecules. Traditional ultrafast spectroscopies, such as pump–probe or time-resolved fluorescence, are not ideal for studying the interface because most of their signal is from the bulk material. Time-resolved second-harmonic generation (TRSHG) spectroscopy solves this problem by only generating signal from the interface. We demonstrate an optically heterodyned TRSHG to reduce the impact of stray light, enhance sensitivity, and detect the full complex signal field.

© 2014 Optical Society of America

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  1. N. Giebink, G. Wiederrecht, M. Wasielewski, and S. Forrest, Phys. Rev. B 82, 155305 (2010).
    [CrossRef]
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    [CrossRef]
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    [CrossRef]
  4. S. Singh and Z. Vardeny, Materials 6, 897 (2013).
    [CrossRef]
  5. A. R. S. Kandada, G. Grancini, A. Petrozza, S. Perissinotto, D. Fazzi, S. S. K. Raavi, and G. Lanzani, Sci. Rep. 3, 2073 (2013).
    [CrossRef]
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2014 (1)

B. Bernardo, D. Cheyns, B. Verreet, R. D. Schaller, B. P. Rand, and N. C. Giebink, Nat. Commun. 5, 3245 (2014).
[CrossRef]

2013 (3)

S. Singh and Z. Vardeny, Materials 6, 897 (2013).
[CrossRef]

A. R. S. Kandada, G. Grancini, A. Petrozza, S. Perissinotto, D. Fazzi, S. S. K. Raavi, and G. Lanzani, Sci. Rep. 3, 2073 (2013).
[CrossRef]

A. E. Jailaubekov, A. P. Willard, J. R. Tritsch, W.-L. Chan, N. Sai, R. Gearba, L. G. Kaake, K. J. Williams, K. Leung, P. J. Rossky, and X.-Y. Zhu, Nat. Mater. 12, 66 (2013).
[CrossRef]

2012 (1)

F. Etzold, I. A. Howard, N. Forler, D. M. Cho, M. Meister, H. Mangold, J. Shu, M. R. Hansen, K. Müllen, and F. Laquai, J. Am. Chem. Soc. 134, 10569 (2012).
[CrossRef]

2011 (2)

L. G. Kaake, A. Jailaubekov, K. J. Williams, and X.-Y. Zhu, Appl. Phys. Lett. 99, 083307 (2011).
[CrossRef]

J. Kirkpatrick, P. E. Keivanidis, A. Bruno, F. Ma, S. A. Haque, A. Yarstev, V. Sundstrom, and J. Nelson, J. Phys. Chem. B 115, 15174 (2011).
[CrossRef]

2010 (1)

N. Giebink, G. Wiederrecht, M. Wasielewski, and S. Forrest, Phys. Rev. B 82, 155305 (2010).
[CrossRef]

2003 (1)

2000 (1)

E. Riedle, M. Beutter, S. Lochbrunner, J. Piel, S. Schenkl, S. Spörlein, and W. Zinth, Appl. Phys. B 71, 457 (2000).
[CrossRef]

1999 (1)

1998 (1)

K. J. Veenstra, A. V. Petukhov, A. P. de Boer, and T. Rasing, Phys. Rev. B 58, R16020 (1998).
[CrossRef]

1996 (1)

X. Shi, E. Borguet, A. Tarnovsky, and K. Eisenthal, Chem. Phys. 205, 167 (1996).
[CrossRef]

1995 (1)

1994 (1)

J. M. Lantz and R. M. Corn, J. Phys. Chem. 98, 9387 (1994).
[CrossRef]

1986 (1)

K. Kemnitz, K. Bhattacharyya, J. Hicks, G. Pinto, B. Eisenthal, and T. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[CrossRef]

1983 (1)

C. V. Shank, R. Yen, and C. Hirlimann, Phys. Rev. Lett. 51, 900 (1983).
[CrossRef]

1979 (1)

M. D. Levenson and G. L. Eesley, Appl. Phys. 19, 1 (1979).
[CrossRef]

1965 (1)

R. Chang, J. Ducuing, and N. Bloembergen, Phys. Rev. Lett. 15, 6 (1965).
[CrossRef]

Aktsipetrov, O. A.

Bernardo, B.

B. Bernardo, D. Cheyns, B. Verreet, R. D. Schaller, B. P. Rand, and N. C. Giebink, Nat. Commun. 5, 3245 (2014).
[CrossRef]

Beutter, M.

E. Riedle, M. Beutter, S. Lochbrunner, J. Piel, S. Schenkl, S. Spörlein, and W. Zinth, Appl. Phys. B 71, 457 (2000).
[CrossRef]

Bhattacharyya, K.

K. Kemnitz, K. Bhattacharyya, J. Hicks, G. Pinto, B. Eisenthal, and T. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[CrossRef]

Bloembergen, N.

R. Chang, J. Ducuing, and N. Bloembergen, Phys. Rev. Lett. 15, 6 (1965).
[CrossRef]

Borguet, E.

X. Shi, E. Borguet, A. Tarnovsky, and K. Eisenthal, Chem. Phys. 205, 167 (1996).
[CrossRef]

Boyd, R. W.

R. W. Boyd, Nonlinear Optics, 3rd ed. (Academic, 2008).

Bruno, A.

J. Kirkpatrick, P. E. Keivanidis, A. Bruno, F. Ma, S. A. Haque, A. Yarstev, V. Sundstrom, and J. Nelson, J. Phys. Chem. B 115, 15174 (2011).
[CrossRef]

Carriles, R.

Chan, W.-L.

A. E. Jailaubekov, A. P. Willard, J. R. Tritsch, W.-L. Chan, N. Sai, R. Gearba, L. G. Kaake, K. J. Williams, K. Leung, P. J. Rossky, and X.-Y. Zhu, Nat. Mater. 12, 66 (2013).
[CrossRef]

Chang, R.

R. Chang, J. Ducuing, and N. Bloembergen, Phys. Rev. Lett. 15, 6 (1965).
[CrossRef]

Chériaux, G.

Cheyns, D.

B. Bernardo, D. Cheyns, B. Verreet, R. D. Schaller, B. P. Rand, and N. C. Giebink, Nat. Commun. 5, 3245 (2014).
[CrossRef]

Cho, D. M.

F. Etzold, I. A. Howard, N. Forler, D. M. Cho, M. Meister, H. Mangold, J. Shu, M. R. Hansen, K. Müllen, and F. Laquai, J. Am. Chem. Soc. 134, 10569 (2012).
[CrossRef]

Corn, R. M.

J. M. Lantz and R. M. Corn, J. Phys. Chem. 98, 9387 (1994).
[CrossRef]

de Boer, A. P.

K. J. Veenstra, A. V. Petukhov, A. P. de Boer, and T. Rasing, Phys. Rev. B 58, R16020 (1998).
[CrossRef]

Downer, M. C.

Ducuing, J.

R. Chang, J. Ducuing, and N. Bloembergen, Phys. Rev. Lett. 15, 6 (1965).
[CrossRef]

Eesley, G. L.

M. D. Levenson and G. L. Eesley, Appl. Phys. 19, 1 (1979).
[CrossRef]

Eisenthal, B.

K. Kemnitz, K. Bhattacharyya, J. Hicks, G. Pinto, B. Eisenthal, and T. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[CrossRef]

Eisenthal, K.

X. Shi, E. Borguet, A. Tarnovsky, and K. Eisenthal, Chem. Phys. 205, 167 (1996).
[CrossRef]

Etzold, F.

F. Etzold, I. A. Howard, N. Forler, D. M. Cho, M. Meister, H. Mangold, J. Shu, M. R. Hansen, K. Müllen, and F. Laquai, J. Am. Chem. Soc. 134, 10569 (2012).
[CrossRef]

Fazzi, D.

A. R. S. Kandada, G. Grancini, A. Petrozza, S. Perissinotto, D. Fazzi, S. S. K. Raavi, and G. Lanzani, Sci. Rep. 3, 2073 (2013).
[CrossRef]

Forler, N.

F. Etzold, I. A. Howard, N. Forler, D. M. Cho, M. Meister, H. Mangold, J. Shu, M. R. Hansen, K. Müllen, and F. Laquai, J. Am. Chem. Soc. 134, 10569 (2012).
[CrossRef]

Forrest, S.

N. Giebink, G. Wiederrecht, M. Wasielewski, and S. Forrest, Phys. Rev. B 82, 155305 (2010).
[CrossRef]

Gearba, R.

A. E. Jailaubekov, A. P. Willard, J. R. Tritsch, W.-L. Chan, N. Sai, R. Gearba, L. G. Kaake, K. J. Williams, K. Leung, P. J. Rossky, and X.-Y. Zhu, Nat. Mater. 12, 66 (2013).
[CrossRef]

Gedik, N.

J. McIver, C. Lee, D. Torchinsky, and N. Gedik, in APS March Meeting (2013), paper BAPS.2013.MAR.Z23.10.

Giebink, N.

N. Giebink, G. Wiederrecht, M. Wasielewski, and S. Forrest, Phys. Rev. B 82, 155305 (2010).
[CrossRef]

Giebink, N. C.

B. Bernardo, D. Cheyns, B. Verreet, R. D. Schaller, B. P. Rand, and N. C. Giebink, Nat. Commun. 5, 3245 (2014).
[CrossRef]

Grancini, G.

A. R. S. Kandada, G. Grancini, A. Petrozza, S. Perissinotto, D. Fazzi, S. S. K. Raavi, and G. Lanzani, Sci. Rep. 3, 2073 (2013).
[CrossRef]

Hansen, M. R.

F. Etzold, I. A. Howard, N. Forler, D. M. Cho, M. Meister, H. Mangold, J. Shu, M. R. Hansen, K. Müllen, and F. Laquai, J. Am. Chem. Soc. 134, 10569 (2012).
[CrossRef]

Haque, S. A.

J. Kirkpatrick, P. E. Keivanidis, A. Bruno, F. Ma, S. A. Haque, A. Yarstev, V. Sundstrom, and J. Nelson, J. Phys. Chem. B 115, 15174 (2011).
[CrossRef]

Heinz, T.

K. Kemnitz, K. Bhattacharyya, J. Hicks, G. Pinto, B. Eisenthal, and T. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[CrossRef]

Hicks, J.

K. Kemnitz, K. Bhattacharyya, J. Hicks, G. Pinto, B. Eisenthal, and T. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[CrossRef]

Hirlimann, C.

C. V. Shank, R. Yen, and C. Hirlimann, Phys. Rev. Lett. 51, 900 (1983).
[CrossRef]

Howard, I. A.

F. Etzold, I. A. Howard, N. Forler, D. M. Cho, M. Meister, H. Mangold, J. Shu, M. R. Hansen, K. Müllen, and F. Laquai, J. Am. Chem. Soc. 134, 10569 (2012).
[CrossRef]

Jailaubekov, A.

L. G. Kaake, A. Jailaubekov, K. J. Williams, and X.-Y. Zhu, Appl. Phys. Lett. 99, 083307 (2011).
[CrossRef]

Jailaubekov, A. E.

A. E. Jailaubekov, A. P. Willard, J. R. Tritsch, W.-L. Chan, N. Sai, R. Gearba, L. G. Kaake, K. J. Williams, K. Leung, P. J. Rossky, and X.-Y. Zhu, Nat. Mater. 12, 66 (2013).
[CrossRef]

Jiang, Y.

Joffre, M.

Kaake, L. G.

A. E. Jailaubekov, A. P. Willard, J. R. Tritsch, W.-L. Chan, N. Sai, R. Gearba, L. G. Kaake, K. J. Williams, K. Leung, P. J. Rossky, and X.-Y. Zhu, Nat. Mater. 12, 66 (2013).
[CrossRef]

L. G. Kaake, A. Jailaubekov, K. J. Williams, and X.-Y. Zhu, Appl. Phys. Lett. 99, 083307 (2011).
[CrossRef]

Kandada, A. R. S.

A. R. S. Kandada, G. Grancini, A. Petrozza, S. Perissinotto, D. Fazzi, S. S. K. Raavi, and G. Lanzani, Sci. Rep. 3, 2073 (2013).
[CrossRef]

Keivanidis, P. E.

J. Kirkpatrick, P. E. Keivanidis, A. Bruno, F. Ma, S. A. Haque, A. Yarstev, V. Sundstrom, and J. Nelson, J. Phys. Chem. B 115, 15174 (2011).
[CrossRef]

Kemnitz, K.

K. Kemnitz, K. Bhattacharyya, J. Hicks, G. Pinto, B. Eisenthal, and T. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[CrossRef]

Kirkpatrick, J.

J. Kirkpatrick, P. E. Keivanidis, A. Bruno, F. Ma, S. A. Haque, A. Yarstev, V. Sundstrom, and J. Nelson, J. Phys. Chem. B 115, 15174 (2011).
[CrossRef]

Lantz, J. M.

J. M. Lantz and R. M. Corn, J. Phys. Chem. 98, 9387 (1994).
[CrossRef]

Lanzani, G.

A. R. S. Kandada, G. Grancini, A. Petrozza, S. Perissinotto, D. Fazzi, S. S. K. Raavi, and G. Lanzani, Sci. Rep. 3, 2073 (2013).
[CrossRef]

Laquai, F.

F. Etzold, I. A. Howard, N. Forler, D. M. Cho, M. Meister, H. Mangold, J. Shu, M. R. Hansen, K. Müllen, and F. Laquai, J. Am. Chem. Soc. 134, 10569 (2012).
[CrossRef]

Lee, C.

J. McIver, C. Lee, D. Torchinsky, and N. Gedik, in APS March Meeting (2013), paper BAPS.2013.MAR.Z23.10.

Lepetit, L.

Leung, K.

A. E. Jailaubekov, A. P. Willard, J. R. Tritsch, W.-L. Chan, N. Sai, R. Gearba, L. G. Kaake, K. J. Williams, K. Leung, P. J. Rossky, and X.-Y. Zhu, Nat. Mater. 12, 66 (2013).
[CrossRef]

Levenson, M. D.

M. D. Levenson and G. L. Eesley, Appl. Phys. 19, 1 (1979).
[CrossRef]

Lochbrunner, S.

E. Riedle, M. Beutter, S. Lochbrunner, J. Piel, S. Schenkl, S. Spörlein, and W. Zinth, Appl. Phys. B 71, 457 (2000).
[CrossRef]

Ma, F.

J. Kirkpatrick, P. E. Keivanidis, A. Bruno, F. Ma, S. A. Haque, A. Yarstev, V. Sundstrom, and J. Nelson, J. Phys. Chem. B 115, 15174 (2011).
[CrossRef]

Mangold, H.

F. Etzold, I. A. Howard, N. Forler, D. M. Cho, M. Meister, H. Mangold, J. Shu, M. R. Hansen, K. Müllen, and F. Laquai, J. Am. Chem. Soc. 134, 10569 (2012).
[CrossRef]

McIver, J.

J. McIver, C. Lee, D. Torchinsky, and N. Gedik, in APS March Meeting (2013), paper BAPS.2013.MAR.Z23.10.

Meister, M.

F. Etzold, I. A. Howard, N. Forler, D. M. Cho, M. Meister, H. Mangold, J. Shu, M. R. Hansen, K. Müllen, and F. Laquai, J. Am. Chem. Soc. 134, 10569 (2012).
[CrossRef]

Mishina, E. D.

Müllen, K.

F. Etzold, I. A. Howard, N. Forler, D. M. Cho, M. Meister, H. Mangold, J. Shu, M. R. Hansen, K. Müllen, and F. Laquai, J. Am. Chem. Soc. 134, 10569 (2012).
[CrossRef]

Nelson, J.

J. Kirkpatrick, P. E. Keivanidis, A. Bruno, F. Ma, S. A. Haque, A. Yarstev, V. Sundstrom, and J. Nelson, J. Phys. Chem. B 115, 15174 (2011).
[CrossRef]

Perissinotto, S.

A. R. S. Kandada, G. Grancini, A. Petrozza, S. Perissinotto, D. Fazzi, S. S. K. Raavi, and G. Lanzani, Sci. Rep. 3, 2073 (2013).
[CrossRef]

Petrozza, A.

A. R. S. Kandada, G. Grancini, A. Petrozza, S. Perissinotto, D. Fazzi, S. S. K. Raavi, and G. Lanzani, Sci. Rep. 3, 2073 (2013).
[CrossRef]

Petukhov, A. V.

K. J. Veenstra, A. V. Petukhov, A. P. de Boer, and T. Rasing, Phys. Rev. B 58, R16020 (1998).
[CrossRef]

Piel, J.

E. Riedle, M. Beutter, S. Lochbrunner, J. Piel, S. Schenkl, S. Spörlein, and W. Zinth, Appl. Phys. B 71, 457 (2000).
[CrossRef]

Pinto, G.

K. Kemnitz, K. Bhattacharyya, J. Hicks, G. Pinto, B. Eisenthal, and T. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[CrossRef]

Raavi, S. S. K.

A. R. S. Kandada, G. Grancini, A. Petrozza, S. Perissinotto, D. Fazzi, S. S. K. Raavi, and G. Lanzani, Sci. Rep. 3, 2073 (2013).
[CrossRef]

Rand, B. P.

B. Bernardo, D. Cheyns, B. Verreet, R. D. Schaller, B. P. Rand, and N. C. Giebink, Nat. Commun. 5, 3245 (2014).
[CrossRef]

Rasing, T.

K. J. Veenstra, A. V. Petukhov, A. P. de Boer, and T. Rasing, Phys. Rev. B 58, R16020 (1998).
[CrossRef]

Riedle, E.

E. Riedle, M. Beutter, S. Lochbrunner, J. Piel, S. Schenkl, S. Spörlein, and W. Zinth, Appl. Phys. B 71, 457 (2000).
[CrossRef]

Rossky, P. J.

A. E. Jailaubekov, A. P. Willard, J. R. Tritsch, W.-L. Chan, N. Sai, R. Gearba, L. G. Kaake, K. J. Williams, K. Leung, P. J. Rossky, and X.-Y. Zhu, Nat. Mater. 12, 66 (2013).
[CrossRef]

Sai, N.

A. E. Jailaubekov, A. P. Willard, J. R. Tritsch, W.-L. Chan, N. Sai, R. Gearba, L. G. Kaake, K. J. Williams, K. Leung, P. J. Rossky, and X.-Y. Zhu, Nat. Mater. 12, 66 (2013).
[CrossRef]

Schaller, R. D.

B. Bernardo, D. Cheyns, B. Verreet, R. D. Schaller, B. P. Rand, and N. C. Giebink, Nat. Commun. 5, 3245 (2014).
[CrossRef]

Schenkl, S.

E. Riedle, M. Beutter, S. Lochbrunner, J. Piel, S. Schenkl, S. Spörlein, and W. Zinth, Appl. Phys. B 71, 457 (2000).
[CrossRef]

Shank, C. V.

C. V. Shank, R. Yen, and C. Hirlimann, Phys. Rev. Lett. 51, 900 (1983).
[CrossRef]

Shi, X.

X. Shi, E. Borguet, A. Tarnovsky, and K. Eisenthal, Chem. Phys. 205, 167 (1996).
[CrossRef]

Shu, J.

F. Etzold, I. A. Howard, N. Forler, D. M. Cho, M. Meister, H. Mangold, J. Shu, M. R. Hansen, K. Müllen, and F. Laquai, J. Am. Chem. Soc. 134, 10569 (2012).
[CrossRef]

Singh, S.

S. Singh and Z. Vardeny, Materials 6, 897 (2013).
[CrossRef]

Spörlein, S.

E. Riedle, M. Beutter, S. Lochbrunner, J. Piel, S. Schenkl, S. Spörlein, and W. Zinth, Appl. Phys. B 71, 457 (2000).
[CrossRef]

Sundstrom, V.

J. Kirkpatrick, P. E. Keivanidis, A. Bruno, F. Ma, S. A. Haque, A. Yarstev, V. Sundstrom, and J. Nelson, J. Phys. Chem. B 115, 15174 (2011).
[CrossRef]

Tarnovsky, A.

X. Shi, E. Borguet, A. Tarnovsky, and K. Eisenthal, Chem. Phys. 205, 167 (1996).
[CrossRef]

Torchinsky, D.

J. McIver, C. Lee, D. Torchinsky, and N. Gedik, in APS March Meeting (2013), paper BAPS.2013.MAR.Z23.10.

Tritsch, J. R.

A. E. Jailaubekov, A. P. Willard, J. R. Tritsch, W.-L. Chan, N. Sai, R. Gearba, L. G. Kaake, K. J. Williams, K. Leung, P. J. Rossky, and X.-Y. Zhu, Nat. Mater. 12, 66 (2013).
[CrossRef]

Vardeny, Z.

S. Singh and Z. Vardeny, Materials 6, 897 (2013).
[CrossRef]

Veenstra, K. J.

K. J. Veenstra, A. V. Petukhov, A. P. de Boer, and T. Rasing, Phys. Rev. B 58, R16020 (1998).
[CrossRef]

Verreet, B.

B. Bernardo, D. Cheyns, B. Verreet, R. D. Schaller, B. P. Rand, and N. C. Giebink, Nat. Commun. 5, 3245 (2014).
[CrossRef]

Wasielewski, M.

N. Giebink, G. Wiederrecht, M. Wasielewski, and S. Forrest, Phys. Rev. B 82, 155305 (2010).
[CrossRef]

Wiederrecht, G.

N. Giebink, G. Wiederrecht, M. Wasielewski, and S. Forrest, Phys. Rev. B 82, 155305 (2010).
[CrossRef]

Willard, A. P.

A. E. Jailaubekov, A. P. Willard, J. R. Tritsch, W.-L. Chan, N. Sai, R. Gearba, L. G. Kaake, K. J. Williams, K. Leung, P. J. Rossky, and X.-Y. Zhu, Nat. Mater. 12, 66 (2013).
[CrossRef]

Williams, K. J.

A. E. Jailaubekov, A. P. Willard, J. R. Tritsch, W.-L. Chan, N. Sai, R. Gearba, L. G. Kaake, K. J. Williams, K. Leung, P. J. Rossky, and X.-Y. Zhu, Nat. Mater. 12, 66 (2013).
[CrossRef]

L. G. Kaake, A. Jailaubekov, K. J. Williams, and X.-Y. Zhu, Appl. Phys. Lett. 99, 083307 (2011).
[CrossRef]

Wilson, P. T.

Yarstev, A.

J. Kirkpatrick, P. E. Keivanidis, A. Bruno, F. Ma, S. A. Haque, A. Yarstev, V. Sundstrom, and J. Nelson, J. Phys. Chem. B 115, 15174 (2011).
[CrossRef]

Yen, R.

C. V. Shank, R. Yen, and C. Hirlimann, Phys. Rev. Lett. 51, 900 (1983).
[CrossRef]

Zhu, X.-Y.

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Figures (3)

Fig. 1.
Fig. 1.

Diagram of the heterodyne-detected TRSHG setup. Collinear beams are visually offset for clarity. The visible pump beam (yellow) is time-delayed relative to the 800 nm NIR probe beam (red) with a hollow retroreflector on a motor-controlled stage. The combined beams interact with the sample, generating a 400 nm signal (blue). A second 400 nm beam, the LO (blue), is generated in a nonlinear crystal. The pump and probe are filtered out before the spectrometer. NOPA, noncollinear optical parametric amplifier. BBWP, broadband (achromatic) half-wave plate designed for 400–700 nm. WP, half-wave plate for 800 nm. BBP, broadband wire grid polarizer. DM, ultrafast dichroic mirror reflecting 800 nm and transmitting 550–700 nm. LP, long-pass filter with 500 nm cutoff. S, sample oriented 45 deg to the pump and probe beams. G, removable glass to introduce variable time delay between signal and LO. DBWP, dual-band wave plate with full-wave retardance at 400 nm and half-wave retardance at 800 nm. BBO, 10-μm-thick beta barium borate crystal, oriented to prevent phase-matching. P, dielectric thin-film polarizer for 400 nm. BPF, bandpass filter centered at 400 nm.

Fig. 2.
Fig. 2.

Comparison of S/N with respect to LO strength on a log–log plot. Blue dots, measured S/N for different LO strengths; green solid line, fitted curve to the measured data based on equation 17 of [13]; red dashed line, theoretical S/N of 2.7 for a similar experiment without a LO and without stray light. Left side of measured data, read-noise-dominated regime; middle of measured data, shot-noise-dominated regime; right side of measured data, onset of 1/f-noise-dominated regime. Compare to Fig. 1 of [13].

Fig. 3.
Fig. 3.

Typical measured TRSHG trace S(t), measured relative to the second-harmonic field in the absence of a pump. Top, absolute value; bottom, relative phase in degrees. Blue dots, measured data; green solid line, fitted bi-exponential curve. Fractional noise in absolute signal is less than 1%, and relative noise in measured phase is less than 1 deg.

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