Abstract

Optical sectioning is performed by collecting the fluorescent emission of two-exciton states in colloidal quantum dots. The two-exciton state is created by two consecutive resonant absorption events, thus requiring unprecedented low excitation energy and peak powers as low as 105Wcm2. The depth resolution is shown to be equivalent to that of standard multiphoton microscopy, and it was found to deteriorate only slowly as saturation of the two-exciton state is approached, owing to signal contribution from higher excitonic states.

© 2008 Optical Society of America

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    [CrossRef] [PubMed]
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2008 (2)

B. Mahler, P. Spinicelli, S. Buil, X. Quelin, J. P. Hermier, and B. Dubertret, Nat. Mater. 7, 612 (2008).
[CrossRef]

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, J. Am. Chem. Soc. 130, 5026 (2008).
[CrossRef] [PubMed]

2007 (1)

D. Oron, M. Kazes, and U. Banin, Phys. Rev. B 75, 035330 (2007).
[CrossRef]

2006 (3)

I. A. Akimov, J. T. Andrews, and F. Henneberger, Phys. Rev. Lett. 96, 067401 (2006).
[CrossRef] [PubMed]

M. Wimmer, S. V. Nair, and J. Shumway, Phys. Rev. B 73, 165305 (2006).
[CrossRef]

G. A. Narvaez, G. Bester, A. Franceschetti, and A. Zunger, Phys. Rev. B 74, 205422 (2006).
[CrossRef]

2005 (2)

B. Fisher, J.-M. Caruge, Y.-T. Chan, J. Halpert, and M. G. Bawendi, Chem. Phys. 318, 71 (2005).
[CrossRef]

A. F. van Driel, G. Allan, C. Delerue, P. Lodahl, W. L. Vos, and D. Vanmaekelbergh, Phys. Rev. Lett. 95, 236804 (2005).
[CrossRef] [PubMed]

2003 (4)

S. Kim, B. Fisher, H.-J. Eisler, and M. Bawendi, J. Am. Chem. Soc. 125, 11466 (2003).
[CrossRef] [PubMed]

W. W. Yu, L. Qu, W. Guo, and X. Peng, Chem. Mater. 15, 2854 (2003).
[CrossRef]

W. R. Zipfel, R. M. Williams, and W. W. Webb, Nat. Biotechnol. 21, 1369 (2003).
[CrossRef] [PubMed]

D. R. Larson, W. R. Zipfel, R. M. Williams, S. W. Clark, M. P. Bruchez, F. W. Wise, and W. W. Webb, Science 300, 1434 (2003).
[CrossRef] [PubMed]

2000 (1)

V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, Science 287, 1011 (2000).
[CrossRef] [PubMed]

1999 (2)

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

L. Ventelon, M. Blanchard-Desce, L. Moreaux, and J. Mertz, Chem. Commun. (Cambridge) 20, 2055 (1999).
[CrossRef]

1997 (2)

Y. Barad, H. Eizenberg, M. Horowitz, and Y. Silberberg, Appl. Phys. Lett. 70, 922 (1997).
[CrossRef]

S. Maiti, J. B. Shear, R. M. Williams, W. R. Zipfel, and W. W. Webb, Science 275, 530 (1997).
[CrossRef] [PubMed]

1990 (1)

W. Denk, J. H. Strickler, and W. W. Webb, Science 248, 73 (1990).
[CrossRef] [PubMed]

1978 (1)

J. Gannaway and C. J. R. Sheppard, Opt. Quantum Electron. 10, 435 (1978).
[CrossRef]

Akimov, I. A.

I. A. Akimov, J. T. Andrews, and F. Henneberger, Phys. Rev. Lett. 96, 067401 (2006).
[CrossRef] [PubMed]

Allan, G.

A. F. van Driel, G. Allan, C. Delerue, P. Lodahl, W. L. Vos, and D. Vanmaekelbergh, Phys. Rev. Lett. 95, 236804 (2005).
[CrossRef] [PubMed]

Andrews, J. T.

I. A. Akimov, J. T. Andrews, and F. Henneberger, Phys. Rev. Lett. 96, 067401 (2006).
[CrossRef] [PubMed]

Banin, U.

D. Oron, M. Kazes, and U. Banin, Phys. Rev. B 75, 035330 (2007).
[CrossRef]

Barad, Y.

Y. Barad, H. Eizenberg, M. Horowitz, and Y. Silberberg, Appl. Phys. Lett. 70, 922 (1997).
[CrossRef]

Bawendi, M.

S. Kim, B. Fisher, H.-J. Eisler, and M. Bawendi, J. Am. Chem. Soc. 125, 11466 (2003).
[CrossRef] [PubMed]

Bawendi, M. G.

B. Fisher, J.-M. Caruge, Y.-T. Chan, J. Halpert, and M. G. Bawendi, Chem. Phys. 318, 71 (2005).
[CrossRef]

V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, Science 287, 1011 (2000).
[CrossRef] [PubMed]

Bester, G.

G. A. Narvaez, G. Bester, A. Franceschetti, and A. Zunger, Phys. Rev. B 74, 205422 (2006).
[CrossRef]

Blanchard-Desce, M.

L. Ventelon, M. Blanchard-Desce, L. Moreaux, and J. Mertz, Chem. Commun. (Cambridge) 20, 2055 (1999).
[CrossRef]

Bruchez, M. P.

D. R. Larson, W. R. Zipfel, R. M. Williams, S. W. Clark, M. P. Bruchez, F. W. Wise, and W. W. Webb, Science 300, 1434 (2003).
[CrossRef] [PubMed]

Buil, S.

B. Mahler, P. Spinicelli, S. Buil, X. Quelin, J. P. Hermier, and B. Dubertret, Nat. Mater. 7, 612 (2008).
[CrossRef]

Bussian, D. A.

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, J. Am. Chem. Soc. 130, 5026 (2008).
[CrossRef] [PubMed]

Caruge, J.-M.

B. Fisher, J.-M. Caruge, Y.-T. Chan, J. Halpert, and M. G. Bawendi, Chem. Phys. 318, 71 (2005).
[CrossRef]

Casson, J. L.

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, J. Am. Chem. Soc. 130, 5026 (2008).
[CrossRef] [PubMed]

Chan, Y.-T.

B. Fisher, J.-M. Caruge, Y.-T. Chan, J. Halpert, and M. G. Bawendi, Chem. Phys. 318, 71 (2005).
[CrossRef]

Chen, Y.

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, J. Am. Chem. Soc. 130, 5026 (2008).
[CrossRef] [PubMed]

Clark, S. W.

D. R. Larson, W. R. Zipfel, R. M. Williams, S. W. Clark, M. P. Bruchez, F. W. Wise, and W. W. Webb, Science 300, 1434 (2003).
[CrossRef] [PubMed]

Delerue, C.

A. F. van Driel, G. Allan, C. Delerue, P. Lodahl, W. L. Vos, and D. Vanmaekelbergh, Phys. Rev. Lett. 95, 236804 (2005).
[CrossRef] [PubMed]

Denk, W.

W. Denk, J. H. Strickler, and W. W. Webb, Science 248, 73 (1990).
[CrossRef] [PubMed]

Dubertret, B.

B. Mahler, P. Spinicelli, S. Buil, X. Quelin, J. P. Hermier, and B. Dubertret, Nat. Mater. 7, 612 (2008).
[CrossRef]

Eisler, H.-J.

S. Kim, B. Fisher, H.-J. Eisler, and M. Bawendi, J. Am. Chem. Soc. 125, 11466 (2003).
[CrossRef] [PubMed]

Eizenberg, H.

Y. Barad, H. Eizenberg, M. Horowitz, and Y. Silberberg, Appl. Phys. Lett. 70, 922 (1997).
[CrossRef]

Fisher, B.

B. Fisher, J.-M. Caruge, Y.-T. Chan, J. Halpert, and M. G. Bawendi, Chem. Phys. 318, 71 (2005).
[CrossRef]

S. Kim, B. Fisher, H.-J. Eisler, and M. Bawendi, J. Am. Chem. Soc. 125, 11466 (2003).
[CrossRef] [PubMed]

Franceschetti, A.

G. A. Narvaez, G. Bester, A. Franceschetti, and A. Zunger, Phys. Rev. B 74, 205422 (2006).
[CrossRef]

Gannaway, J.

J. Gannaway and C. J. R. Sheppard, Opt. Quantum Electron. 10, 435 (1978).
[CrossRef]

Guo, W.

W. W. Yu, L. Qu, W. Guo, and X. Peng, Chem. Mater. 15, 2854 (2003).
[CrossRef]

Halpert, J.

B. Fisher, J.-M. Caruge, Y.-T. Chan, J. Halpert, and M. G. Bawendi, Chem. Phys. 318, 71 (2005).
[CrossRef]

Henneberger, F.

I. A. Akimov, J. T. Andrews, and F. Henneberger, Phys. Rev. Lett. 96, 067401 (2006).
[CrossRef] [PubMed]

Hermier, J. P.

B. Mahler, P. Spinicelli, S. Buil, X. Quelin, J. P. Hermier, and B. Dubertret, Nat. Mater. 7, 612 (2008).
[CrossRef]

Hollingsworth, J. A.

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, J. Am. Chem. Soc. 130, 5026 (2008).
[CrossRef] [PubMed]

Holtom, G. R.

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

Horowitz, M.

Y. Barad, H. Eizenberg, M. Horowitz, and Y. Silberberg, Appl. Phys. Lett. 70, 922 (1997).
[CrossRef]

Htoon, H.

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, J. Am. Chem. Soc. 130, 5026 (2008).
[CrossRef] [PubMed]

Kazes, M.

D. Oron, M. Kazes, and U. Banin, Phys. Rev. B 75, 035330 (2007).
[CrossRef]

Kim, S.

S. Kim, B. Fisher, H.-J. Eisler, and M. Bawendi, J. Am. Chem. Soc. 125, 11466 (2003).
[CrossRef] [PubMed]

Klimov, V. I.

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, J. Am. Chem. Soc. 130, 5026 (2008).
[CrossRef] [PubMed]

V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, Science 287, 1011 (2000).
[CrossRef] [PubMed]

Larson, D. R.

D. R. Larson, W. R. Zipfel, R. M. Williams, S. W. Clark, M. P. Bruchez, F. W. Wise, and W. W. Webb, Science 300, 1434 (2003).
[CrossRef] [PubMed]

Leatherdale, C. A.

V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, Science 287, 1011 (2000).
[CrossRef] [PubMed]

Lodahl, P.

A. F. van Driel, G. Allan, C. Delerue, P. Lodahl, W. L. Vos, and D. Vanmaekelbergh, Phys. Rev. Lett. 95, 236804 (2005).
[CrossRef] [PubMed]

Mahler, B.

B. Mahler, P. Spinicelli, S. Buil, X. Quelin, J. P. Hermier, and B. Dubertret, Nat. Mater. 7, 612 (2008).
[CrossRef]

Maiti, S.

S. Maiti, J. B. Shear, R. M. Williams, W. R. Zipfel, and W. W. Webb, Science 275, 530 (1997).
[CrossRef] [PubMed]

McBranch, D. W.

V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, Science 287, 1011 (2000).
[CrossRef] [PubMed]

Mertz, J.

L. Ventelon, M. Blanchard-Desce, L. Moreaux, and J. Mertz, Chem. Commun. (Cambridge) 20, 2055 (1999).
[CrossRef]

Mikhailovsky, A. A.

V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, Science 287, 1011 (2000).
[CrossRef] [PubMed]

Moreaux, L.

L. Ventelon, M. Blanchard-Desce, L. Moreaux, and J. Mertz, Chem. Commun. (Cambridge) 20, 2055 (1999).
[CrossRef]

Nair, S. V.

M. Wimmer, S. V. Nair, and J. Shumway, Phys. Rev. B 73, 165305 (2006).
[CrossRef]

Narvaez, G. A.

G. A. Narvaez, G. Bester, A. Franceschetti, and A. Zunger, Phys. Rev. B 74, 205422 (2006).
[CrossRef]

Oron, D.

D. Oron, M. Kazes, and U. Banin, Phys. Rev. B 75, 035330 (2007).
[CrossRef]

Peng, X.

W. W. Yu, L. Qu, W. Guo, and X. Peng, Chem. Mater. 15, 2854 (2003).
[CrossRef]

Qu, L.

W. W. Yu, L. Qu, W. Guo, and X. Peng, Chem. Mater. 15, 2854 (2003).
[CrossRef]

Quelin, X.

B. Mahler, P. Spinicelli, S. Buil, X. Quelin, J. P. Hermier, and B. Dubertret, Nat. Mater. 7, 612 (2008).
[CrossRef]

Shear, J. B.

S. Maiti, J. B. Shear, R. M. Williams, W. R. Zipfel, and W. W. Webb, Science 275, 530 (1997).
[CrossRef] [PubMed]

Sheppard, C. J. R.

J. Gannaway and C. J. R. Sheppard, Opt. Quantum Electron. 10, 435 (1978).
[CrossRef]

Shumway, J.

M. Wimmer, S. V. Nair, and J. Shumway, Phys. Rev. B 73, 165305 (2006).
[CrossRef]

Silberberg, Y.

Y. Barad, H. Eizenberg, M. Horowitz, and Y. Silberberg, Appl. Phys. Lett. 70, 922 (1997).
[CrossRef]

Spinicelli, P.

B. Mahler, P. Spinicelli, S. Buil, X. Quelin, J. P. Hermier, and B. Dubertret, Nat. Mater. 7, 612 (2008).
[CrossRef]

Strickler, J. H.

W. Denk, J. H. Strickler, and W. W. Webb, Science 248, 73 (1990).
[CrossRef] [PubMed]

van Driel, A. F.

A. F. van Driel, G. Allan, C. Delerue, P. Lodahl, W. L. Vos, and D. Vanmaekelbergh, Phys. Rev. Lett. 95, 236804 (2005).
[CrossRef] [PubMed]

Vanmaekelbergh, D.

A. F. van Driel, G. Allan, C. Delerue, P. Lodahl, W. L. Vos, and D. Vanmaekelbergh, Phys. Rev. Lett. 95, 236804 (2005).
[CrossRef] [PubMed]

Vela, J.

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, J. Am. Chem. Soc. 130, 5026 (2008).
[CrossRef] [PubMed]

Ventelon, L.

L. Ventelon, M. Blanchard-Desce, L. Moreaux, and J. Mertz, Chem. Commun. (Cambridge) 20, 2055 (1999).
[CrossRef]

Vos, W. L.

A. F. van Driel, G. Allan, C. Delerue, P. Lodahl, W. L. Vos, and D. Vanmaekelbergh, Phys. Rev. Lett. 95, 236804 (2005).
[CrossRef] [PubMed]

Webb, W. W.

D. R. Larson, W. R. Zipfel, R. M. Williams, S. W. Clark, M. P. Bruchez, F. W. Wise, and W. W. Webb, Science 300, 1434 (2003).
[CrossRef] [PubMed]

W. R. Zipfel, R. M. Williams, and W. W. Webb, Nat. Biotechnol. 21, 1369 (2003).
[CrossRef] [PubMed]

S. Maiti, J. B. Shear, R. M. Williams, W. R. Zipfel, and W. W. Webb, Science 275, 530 (1997).
[CrossRef] [PubMed]

W. Denk, J. H. Strickler, and W. W. Webb, Science 248, 73 (1990).
[CrossRef] [PubMed]

Werder, D. J.

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, J. Am. Chem. Soc. 130, 5026 (2008).
[CrossRef] [PubMed]

Williams, R. M.

W. R. Zipfel, R. M. Williams, and W. W. Webb, Nat. Biotechnol. 21, 1369 (2003).
[CrossRef] [PubMed]

D. R. Larson, W. R. Zipfel, R. M. Williams, S. W. Clark, M. P. Bruchez, F. W. Wise, and W. W. Webb, Science 300, 1434 (2003).
[CrossRef] [PubMed]

S. Maiti, J. B. Shear, R. M. Williams, W. R. Zipfel, and W. W. Webb, Science 275, 530 (1997).
[CrossRef] [PubMed]

Wimmer, M.

M. Wimmer, S. V. Nair, and J. Shumway, Phys. Rev. B 73, 165305 (2006).
[CrossRef]

Wise, F. W.

D. R. Larson, W. R. Zipfel, R. M. Williams, S. W. Clark, M. P. Bruchez, F. W. Wise, and W. W. Webb, Science 300, 1434 (2003).
[CrossRef] [PubMed]

Xie, X. S.

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

Yu, W. W.

W. W. Yu, L. Qu, W. Guo, and X. Peng, Chem. Mater. 15, 2854 (2003).
[CrossRef]

Zipfel, W. R.

D. R. Larson, W. R. Zipfel, R. M. Williams, S. W. Clark, M. P. Bruchez, F. W. Wise, and W. W. Webb, Science 300, 1434 (2003).
[CrossRef] [PubMed]

W. R. Zipfel, R. M. Williams, and W. W. Webb, Nat. Biotechnol. 21, 1369 (2003).
[CrossRef] [PubMed]

S. Maiti, J. B. Shear, R. M. Williams, W. R. Zipfel, and W. W. Webb, Science 275, 530 (1997).
[CrossRef] [PubMed]

Zumbusch, A.

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

Zunger, A.

G. A. Narvaez, G. Bester, A. Franceschetti, and A. Zunger, Phys. Rev. B 74, 205422 (2006).
[CrossRef]

Appl. Phys. Lett. (1)

Y. Barad, H. Eizenberg, M. Horowitz, and Y. Silberberg, Appl. Phys. Lett. 70, 922 (1997).
[CrossRef]

Chem. Commun. (Cambridge) (1)

L. Ventelon, M. Blanchard-Desce, L. Moreaux, and J. Mertz, Chem. Commun. (Cambridge) 20, 2055 (1999).
[CrossRef]

Chem. Mater. (1)

W. W. Yu, L. Qu, W. Guo, and X. Peng, Chem. Mater. 15, 2854 (2003).
[CrossRef]

Chem. Phys. (1)

B. Fisher, J.-M. Caruge, Y.-T. Chan, J. Halpert, and M. G. Bawendi, Chem. Phys. 318, 71 (2005).
[CrossRef]

J. Am. Chem. Soc. (2)

S. Kim, B. Fisher, H.-J. Eisler, and M. Bawendi, J. Am. Chem. Soc. 125, 11466 (2003).
[CrossRef] [PubMed]

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, J. Am. Chem. Soc. 130, 5026 (2008).
[CrossRef] [PubMed]

Nat. Biotechnol. (1)

W. R. Zipfel, R. M. Williams, and W. W. Webb, Nat. Biotechnol. 21, 1369 (2003).
[CrossRef] [PubMed]

Nat. Mater. (1)

B. Mahler, P. Spinicelli, S. Buil, X. Quelin, J. P. Hermier, and B. Dubertret, Nat. Mater. 7, 612 (2008).
[CrossRef]

Opt. Quantum Electron. (1)

J. Gannaway and C. J. R. Sheppard, Opt. Quantum Electron. 10, 435 (1978).
[CrossRef]

Phys. Rev. B (3)

D. Oron, M. Kazes, and U. Banin, Phys. Rev. B 75, 035330 (2007).
[CrossRef]

M. Wimmer, S. V. Nair, and J. Shumway, Phys. Rev. B 73, 165305 (2006).
[CrossRef]

G. A. Narvaez, G. Bester, A. Franceschetti, and A. Zunger, Phys. Rev. B 74, 205422 (2006).
[CrossRef]

Phys. Rev. Lett. (3)

A. F. van Driel, G. Allan, C. Delerue, P. Lodahl, W. L. Vos, and D. Vanmaekelbergh, Phys. Rev. Lett. 95, 236804 (2005).
[CrossRef] [PubMed]

A. Zumbusch, G. R. Holtom, and X. S. Xie, Phys. Rev. Lett. 82, 4142 (1999).
[CrossRef]

I. A. Akimov, J. T. Andrews, and F. Henneberger, Phys. Rev. Lett. 96, 067401 (2006).
[CrossRef] [PubMed]

Science (4)

D. R. Larson, W. R. Zipfel, R. M. Williams, S. W. Clark, M. P. Bruchez, F. W. Wise, and W. W. Webb, Science 300, 1434 (2003).
[CrossRef] [PubMed]

W. Denk, J. H. Strickler, and W. W. Webb, Science 248, 73 (1990).
[CrossRef] [PubMed]

S. Maiti, J. B. Shear, R. M. Williams, W. R. Zipfel, and W. W. Webb, Science 275, 530 (1997).
[CrossRef] [PubMed]

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[CrossRef] [PubMed]

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Figures (3)

Fig. 1
Fig. 1

(a) Schematic description of the two available recombination channels for the BX state. (b) Schematic of the experimental setup.

Fig. 2
Fig. 2

(a) Measured histograms (plots are shifted for clarity) at 0.25 photons/dot/pulse for z positions (measured from the objective focal plane) of 0, 0.75, 1.5, and 3 μ m , top to bottom. (b) Decomposition of the time traces to slow (crosses) and fast (dots) normalized components accompanied by model calculation (solid curves).

Fig. 3
Fig. 3

Saturation properties of the doubly resonant scheme. (a) FWHM of the fast transient component as a function of excitation intensity. Measurements (stars) are well fitted by the model, shown for the BX alone (solid curve) or corrected for the TX emission (dashed curve). (b) Amplitude ratio of the fast to the slow component at t = 0 as a function of the excitation intensity. Measurements (stars) exhibit delayed saturation relative to the model taking into account only the BX (solid curve) and are well fitted by correcting for the TX (dashed curve).

Equations (2)

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N BX N X = 1 ( 1 + n ) e n 1 e n .
I ( t ) = N X ( t ) τ X rad + N BX ( t ) τ BX rad = N tot ( t ) τ X rad + ( r 1 ) N BX ( t ) τ X rad ,

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