Abstract

The saturable optical absorption properties of PbSe core nanocrystals (NCs), and their corresponding PbSePbS coreshell and PbSePbSexS1-x core∕alloyed-shell NCs, were examined at λ=1.54μm. Saturation intensities of approximately 100MWcm2 were obtained. The NCs act as passive Q switches in near-infrared pulsed lasers. Q-switched output pulse energies up to 3   mJ, with a pulse duration of 40–55 ns were demonstrated. Analysis of the optical transmission versus pulse light intensity was carried out according to a model that includes ground-state as well as excited-state absorption. For pulses 10  ns long, the NCs act as fast saturable absorbers. The theoretical fits yield a ground-state absorption cross section of 10161015cm2, an excited-state absorption cross section of σes1016cm2, and an effective lifetime of τeff5×1012  s.

© 2006 Optical Society of America

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    [Crossref]

2005 (6)

S. A. Zolotovskaya, K. V. Yumashev, N. V. Kuleshov, and A. V. Sandulenko, "Diode-pumped Yb, Er:glass laser passively Q switched with a V3+:YAG crystal," Appl. Opt. 44, 1704-1708 (2005).
[Crossref]

H. C. Lai, A. Li, D. W. Su, M. L. Ku, Y. F. Chen, and D. F. Huang, "InAs/GaAs quantum dot saturable absorbers for diode-pumped passively Q-switched Nd-doped 1.3 μm lasers," Opt. Lett. 30, 480-482 (2005).
[Crossref]

R. J. Ellingson, M. C. Beard, J. C. Johnson, P. Yu, O. I. Micic, A. J. Nozik, A. Shabaev, and A. L. Efros, "Highly efficient multiple exciton generation in colloidal PbSe and PbS quantum dots," Nano. Lett. 5, 865-871 (2005).
[Crossref]

M. Brumer, A. Kigel, L. Amirav, A. Sashchiuk, O. Solomesch, N. Tessler, and E. Lifshitz, "PbSe/PbS and PbSe/PbSexS1-x core/shell nanocrystals," Adv. Funct. Mater. 15, 1111-1116 (2005).
[Crossref]

R. D. Schaller, M. A. Petruska, and V. I. Klimov, "Effect of electronic structure on carrier multiplication efficiency: comparative study of PbSe and CdSe nanocrystals," Appl. Phys. Lett. 87, 253101 (2005).
[Crossref]

J. M. Harbold, H. Du, T. D. Krauss, K. S. Cho, C. B. Murray, and F. W. Wise, "Time-resolved intraband relaxation of strongly confined electrons and holes in colloidal PbSe nanocrystals," Phys. Rev. B 72, 195312 (2005).
[Crossref]

2004 (8)

G. Allan and C. Delerue, "Confinement effects in PbSe quantum wells and nanocrystals," Phys. Rev. B 70, 245321 (2004).
[Crossref]

J. S. Steckel, J. P. Zimmer, S. Coe-Sullivan, N. E. Stott, V. Bulovic, and M. G. Bawendi, "Blue luminescence from (CdS)ZnS core-shell nanocrystals," Angew. Chem. Int. Ed. Engl. 43, 2154-2158 (2004).
[Crossref]

M. Sirota, E. Galun, V. Krupkin, A. Glushko, A. Kigel, M. Brumer, A. Sachshiuk, L. Amirav, and E. Lifsthiz, "IV-VI semiconductors nanocrystals for passive Q-switch in IR," in Nanophotonic Materials, D. L. Andrews, G. C. Cao, and Z. Gaburro, eds., Proc. SPIE 5510, 9-16 (2004).
[Crossref]

R. D. Schaller and V. I. Klimov, "High efficiency carrier multiplication in PbSe nanocrystals: implication for solar energy conversion," Phys. Rev. Lett. 92, 186601 (2004).
[Crossref]

K. Kang, K. Daneshvar, and R. Tsu, "Size dependence saturation and absorption of PbS quantum dots," Microelectron. J. 35, 629-633 (2004).
[Crossref]

R. P. Prasankumar, I. Hartl, J. T. Gopinath, E. P. Ippen, J. G. Fujimoto, P. Mak, and M. F. Ruane, "Design and characterization of semiconductor-doped silica film saturable absorbers," J. Opt. Soc. Am. B 21, 851-857 (2004).
[Crossref]

V. G. Savitski, A. M. Malyarevich, K. V. Yumashev, V. L. Kalashnikov, B. D. Sinclair, H. Raaben, and A. A. Zhilin, "Experiment and modeling of a diode-pumped 1.3 μm Nd:YVO4 laser passively Q-switched with PbS-doped glass," Appl. Phys. B 79, 315-319 (2004).
[Crossref]

A. A. Lagatsky, C. G. Leburn, C. T. A. Brown, W. Sibbett, A. M. Mayarevich, V. G. Savitski, K. V. Yumashev, E. L. Raaben, and A. A. Zhilin, "Passive mode locking of a Cr4+:YAG laser by PbS quantum dot doped glass saturable absorber," Opt. Commun. 241, 449-454 (2004).
[Crossref]

2003 (5)

U. Keller, "Recent developments in compact ultrafast lasers," Nature 424, 831-838 (2003).
[Crossref]

R. D. Schaller, M. A. Petruska, and V. I. Klimov, "Tunable near-infrared optical gain and amplified spontaneous emission using PbSe nanocrystals," J. Phys. Chem. 107, 13765-13768 (2003).

J. S. Steckel, S. Coe-Sullivan, V. Bulovic, and M. G. Bawendi, "1.3 μm to 1.55 μm tunable electroluminescence from PbSe quantum dots embedded within an organic device," Adv. Mater. 15, 1862-1866 (2003).
[Crossref]

N. Gaponik, I. L. Radtchenko, M. R. Gerstenberger, Y. A. Fedutik, G. B. Sukhorukov, and A. L. Rogach, "Labeling of biocompatible polymer microcapsules with near-infrared emitting nanocrystals," Nano. Lett. 3, 369-372 (2003).
[Crossref]

A. V. Podlipensky, K. V. Yumashev, N. V. Kuleshov, H. M. Kretschmann, and G. Huber, "Passive Q-switching of 1.44 μm and 1.34 μm diode-pumped Nd:YAG lasers with a V:YAG saturable absorber," Appl. Phys. B 76, 245-247 (2003).
[Crossref]

2002 (3)

V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdatle, H. J. Eisler, and M. G. Bawendi, "Optical gain and stimulated emission in nanocrystals quantum dots," Science 290, 314-317 (2002).
[Crossref]

H. Du, C. Chen, R. Krishnan, T. D. Krauss, J. M. Harbold, F. W. Wise, M. G. Thomas, and J. Silcox, "Optical properties of colloidal PbSe nanocrystals," Nano. Lett. 2, 1321-1324 (2002).
[Crossref]

B. L. Wehrenberg, C. Wang, and P. Guyot-Sionnest, "Interband and intraband optical studies of PbSe colloidal quantum dots," J. Phys. Chem. B 106, 10634-10640 (2002).
[Crossref]

2001 (4)

A. M. Malyarevich, P. V. Prokoshin, M. I. Demchuk, K. V. Yumashev, and A. A. Lipovskii, "Passively Q-switched Ho3+:Y3Al5O12 laser using a PbSe-doped glass," Appl. Phys. Lett. 78, 572-573 (2001).
[Crossref]

J. F. Philipps, T. Töpfer, H. Ebendorff-Heidepriem, D. Ehrt, R. Sauerbrey, and N. F. Borrelli, "Diode-pumped erbium-ytterbium-glass laser passively Q-switched with a PbS semiconductor quantum-dot doped glass," Appl. Phys. B 72, 175-178 (2001).

A. M. Malyarevich, V. G. Savitsky, I. A. Denisov, P. V. Prokoshin, K. V. Yumashev, E. Raaben, A. A. Zhilin, and A. A. Lipovskii, "PbS(Se) quantum dot doped glass applications as laser passive Q-switches," Phys. Status Solidi B 224, 253-256 (2001).
[Crossref]

Z. Burshtein, Y. Shimony, R. Feldman, V. Krupkin, A. Glushko, and E. Galun, "Excited state absorption at 1.57 mm in U2+:CaF2 and Co2+:ZnSe saturable absorbers," Opt. Mater. 15, 285-291 (2001).
[Crossref]

2000 (4)

K. V. Yumashev, I. A. Denisov, N. N. Posnov, P. V. Prokoshin, and V. P. Mikhailov, "Nonlinear absorption properties of Co2+:MgAl2O4 crystal," Appl. Phys. B 70, 179-184 (2000).
[Crossref]

T. Y. Tsai and M. Birnbaum, "Co2+:ZnS and Co2+:ZnSe saturable absorber Q switches," J. Appl. Phys. 87, 25-29 (2000).
[Crossref]

R. G. Neuhauser, K. T. Shimizu, W. K. Woo, S. A. Empedocles, and M. G. Bawendi, "Correlation between fluorescence intermittency and spectral diffusion in single semiconductor quantum dots," Phys. Rev. Lett. 85, 3301-3304 (2000).
[Crossref]

O. I. Micic, B. B. Smith, and A. J. Nozik, "Core-shell quantum dots of lattice-matched ZnCdSe2 shells on InP cores: experiment and theory," J. Phys. Chem. B 104, 12149-12156 (2000).
[Crossref]

1999 (5)

J. C. de Mello, H. F. Wittmann, and R. H. Friend, "An improved experimental determination of external photoluminescence quantum efficiency," Adv. Mater. 9, 230-232 (1999).
[Crossref]

E. Poles, D. C. Selmarten, O. I. Micic, and A. J. Nozik, "Anti-Stokes photoluminescence in colloidal semiconductor quantum dots," Appl. Phys. Lett. 75, 971-973 (1999).
[Crossref]

A. D. Andreev and A. A. Lipovskii, "Anisotropy-induced optical transitions in PbSe and PbS spherical quantum dots," Phys. Rev. B 59, 15402-15404 (1999).
[Crossref]

K. V. Yumashev, I. A. Denisov, N. N. Posnov, V. P. Mikhailov, R. Moncorge, D. Vivien, B. Ferrand, and Y. Guyot, "Nonlinear spectroscopy and passive Q-switching operation of a Co2+:LaMgAl11O19 crystal," J. Opt. Soc. Am. B 16, 2189-2194 (1999).

A. V. Podlipensky, V. G. Shcherbitsky, N. V. Kuleshov, V. P. Mikhailov, V. I. Levchenko, and V. N. Yakimovich, "Cr2+ ZnSe and Co2+ ZnSe saturable-absorber Q switches for 1.54-μm Er glass lasers," Opt. Lett. 24, 960-962 (1999).

1998 (3)

A. M. Malyarevich, I. A. Denisov, K. V. Yumashev, V. P. Mikhailov, R. S. Conroy, and B. D. Sinclair, "V:YAG--a new passive Q-switch for diode-pumped solid-state lasers," Appl. Phys. B 67, 555-558 (1998).
[Crossref]

Z. Burshtein, P. Blau, Y. Kalisky, Y. Shimony, and M. R. Kokta, "Excited-state absorption studies of Cr4+ ions in several garnet host crystals," IEEE J. Quantum Electron. 34, 292-299 (1998).
[Crossref]

I. P. Bilinsky, J. G. Fujimoto, J. N. Walpole, and L. J. Missaggia, "Semiconductor-doped-silica saturable-absorber films for solid-state laser mode locking," Opt. Lett. 23, 1766-1768 (1998).

1997 (3)

P. T. Guerreiro, S. Ten, N. F. Borrelli, J. Butty, G. E. Gabbour, and N. Peyghambarian, "PbS quantum-dot doped glasses as saturable absorbers for mode locking of a Cr:forsterite laser," Appl. Phys. Lett. 71, 1595-1597 (1997).
[Crossref]

I. Kang and F. W. Wise, "Electronic structure and optical properties of PbS and PbSe quantum dots," J. Opt. Soc. Am. B 14, 1632-1646 (1997).

S. H. Wei and A. Zunger, "Electronic and structural anomalies in lead chalcogenides," Phys. Rev. B 55, 13605-13610 (1997).
[Crossref]

1996 (1)

S. Tsuda, W. H. Knox, S. T. Cundiff, W. Y. Jan, and J. E. Cunningham, "Mode-locking ultrafast solid-state lasers with saturable Bragg reflectors," IEEE J. Sel. Top. Quantum Electron. 2, 454-464 (1996).
[Crossref]

1995 (3)

R. D. Stultz, M. B. Camargo, and M. Birnbaum, "Passive Q-switch at 1.53 μm using divalent uranium ions in calcium fluoride," J. Appl. Phys. 78, 2959-2961 (1995).
[Crossref]

M. B. Camargo, R. D. Stultz, M. Birnbaum, and M. Kokta, "Co2+:YSGG saturable absorber Q switch for infrared erbium lasers," Opt. Lett. 20, 339-341 (1995).

Y. Shimony, Z. Burshtein, and Y. Kalisky, "Cr4+:YAG as passive Q-switch and Brewster plate in a pulsed Nd:YAG laser," IEEE J. Quantum Electron. 31, 1738-1741 (1995).
[Crossref]

1992 (1)

A. Santoni, G. Paolucci, G. Santoro, K. C. Prince, and N. E. Christensen, "Band structure of lead sulphide," J. Phys. Condens. Matter 4, 6759-6768 (1992).
[Crossref]

1962 (1)

S. J. Strickler and R. A. Berg, "Relationship between absorption and fluorescence lifetime of molecules," J. Chem. Phys. 37, 814-822 (1962).
[Crossref]

Allan, G.

G. Allan and C. Delerue, "Confinement effects in PbSe quantum wells and nanocrystals," Phys. Rev. B 70, 245321 (2004).
[Crossref]

Amirav, L.

M. Brumer, A. Kigel, L. Amirav, A. Sashchiuk, O. Solomesch, N. Tessler, and E. Lifshitz, "PbSe/PbS and PbSe/PbSexS1-x core/shell nanocrystals," Adv. Funct. Mater. 15, 1111-1116 (2005).
[Crossref]

M. Sirota, E. Galun, V. Krupkin, A. Glushko, A. Kigel, M. Brumer, A. Sachshiuk, L. Amirav, and E. Lifsthiz, "IV-VI semiconductors nanocrystals for passive Q-switch in IR," in Nanophotonic Materials, D. L. Andrews, G. C. Cao, and Z. Gaburro, eds., Proc. SPIE 5510, 9-16 (2004).
[Crossref]

Andreev, A. D.

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V. G. Savitski, A. M. Malyarevich, K. V. Yumashev, V. L. Kalashnikov, B. D. Sinclair, H. Raaben, and A. A. Zhilin, "Experiment and modeling of a diode-pumped 1.3 μm Nd:YVO4 laser passively Q-switched with PbS-doped glass," Appl. Phys. B 79, 315-319 (2004).
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A. M. Malyarevich, P. V. Prokoshin, M. I. Demchuk, K. V. Yumashev, and A. A. Lipovskii, "Passively Q-switched Ho3+:Y3Al5O12 laser using a PbSe-doped glass," Appl. Phys. Lett. 78, 572-573 (2001).
[Crossref]

A. M. Malyarevich, V. G. Savitsky, I. A. Denisov, P. V. Prokoshin, K. V. Yumashev, E. Raaben, A. A. Zhilin, and A. A. Lipovskii, "PbS(Se) quantum dot doped glass applications as laser passive Q-switches," Phys. Status Solidi B 224, 253-256 (2001).
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A. Santoni, G. Paolucci, G. Santoro, K. C. Prince, and N. E. Christensen, "Band structure of lead sulphide," J. Phys. Condens. Matter 4, 6759-6768 (1992).
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J. F. Philipps, T. Töpfer, H. Ebendorff-Heidepriem, D. Ehrt, R. Sauerbrey, and N. F. Borrelli, "Diode-pumped erbium-ytterbium-glass laser passively Q-switched with a PbS semiconductor quantum-dot doped glass," Appl. Phys. B 72, 175-178 (2001).

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A. A. Lagatsky, C. G. Leburn, C. T. A. Brown, W. Sibbett, A. M. Mayarevich, V. G. Savitski, K. V. Yumashev, E. L. Raaben, and A. A. Zhilin, "Passive mode locking of a Cr4+:YAG laser by PbS quantum dot doped glass saturable absorber," Opt. Commun. 241, 449-454 (2004).
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E. Poles, D. C. Selmarten, O. I. Micic, and A. J. Nozik, "Anti-Stokes photoluminescence in colloidal semiconductor quantum dots," Appl. Phys. Lett. 75, 971-973 (1999).
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Figures (8)

Fig. 1
Fig. 1

Schematic of an Er:glass laser cavity, including a passive Q switch. For details, see text.

Fig. 2
Fig. 2

(a) HR-TEM image of a 6.1 nm PbSe PbS core∕shell NC with a 4.8   nm core using 1:1:1.5 Pb:Se:S molar ratio in the mother solution; (b) HR-TEM image of a 6.1   nm PbSe PbSe x S 1− x core∕alloyed-shell NC with Pb:Se:S molar ratio similar to the sample in (a). Bar scales in (a) and (b) are 5.0   nm . (c) SAED picture of the sample in (a); (d) TEM image of 6.7   nm PbSe PbSe x S 1− x core∕alloyed-shell NCs , arranged in an ordered assembly on a TEM grid. Bar scale is 20.0   nm .

Fig. 3
Fig. 3

(Color online) (a) Absorbance (dashed curves) and PL (bold curves) spectra of PbSe PbS core∕shell NCs with 4.9   nm PbSe core and n MLs of a PbS shell ( n = 0 , 1 , 3 ) ; (b) three-dimensional plot of the 1S-exciton emission energy versus PbSe core diameter and versus number of PbS MLs.

Fig. 4
Fig. 4

Schematic of the ground and excited states in PbSe NCs . σ gs and σ es correspond to the ground-state and excited-state absorption cross sections, respectively. τ i ( i = 1 4 ) refers to the nonradiative decay times between the designated states, while τ R corresponds to the radiative emission lifetime.

Fig. 5
Fig. 5

(a) Absorbance (dashed curves) and PL spectra (solid curves) of PbSe PbSe x S 1− x core∕alloyed-shell NCs , with a gradual increase of the S content, the molar fraction x varying between 1.0 and 0.5 with approximately −0.1 steps from bottom to top. (b) Absorbance (dashed curves) and PL spectra (solid curves) of PbSe core NCs , with a diameter D ranging between 4.0 and 6.0   nm , with 0.25   nm steps from bottom to top.

Fig. 6
Fig. 6

Transmission versus laser intensity of 5.6   nm PbSe NCs (top), 5.8   nm PbSe PbS 1.5 monolayered core∕shell NCs (middle), and 6.0   nm PbSe PbSe x S 1− x core∕alloyed-shell NCs (bottom), all suspended in chloroform. The dots represent the experimental data; solid curves correspond to the simulation, utilizing Eq. (2).

Fig. 7
Fig. 7

Oscilloscope trace of a single output pulse of an Er:glass laser cavity (plot of intensity versus time) using PbSe NCs colloidal solution as a Q switch.

Fig. 8
Fig. 8

Output versus input pump energies of an Er:glass laser under free-running and under passive Q-switching conditions. Solid squares, free-running; open circles, PbSe PbS NCs in PMMA; solid circles, PbSe PbS NCs in chloroform. Scale for the Q-switched output is on the right.

Tables (4)

Tables Icon

Table 1 Fluorescence Quantum Yields η, Radiative Lifetimes τ R , and Fluorescence Lifetimes τ f for Several Representative NC Samples a

Tables Icon

Table 2 Best Fit Values of σ gs , σ es , τ eff , and I S , Using Eq. (2) for Several Representative NCs' Samples a

Tables Icon

Table 3 Results of Q -Switching Performance Tests

Tables Icon

Table 4 Spectroscopic Characteristics Summary of Various Saturable Absorber Q Switches Demonstrated for Er:Glass Lasers

Equations (2)

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

τ R     1 = 8 π n 2 N c 2 0 ν 2 α ( ν ) d ν ,
I 0 = S [ 1 ( T 0 / T ) 1 / D ] ( T 0 / T ) 1 / D T ,

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