We theoretically study femtosecond pulse generation by passive mode-locking of semiconductor disk lasers operating in the blue spectral range using metal nanocomposites as slow saturable absorbers. By using the relation for the nonlinear dielectric response of a layer of silica glass doped with spherical silver nanoparticles and the master equation for mode-locking, we investigate the dynamics of pulse formation and the achievable pulse parameters and predict the generation of pulses as short as 50 fs at 420 nm in such lasers.
© 2012 OSA
Metal nanocomposites exhibit saturable absorption most prominently in the visible spectral range (see e.g. [1,2]). The recovery time of such materials is in the range of a few picoseconds [3,4]. A prospective application of this type of absorbers is passive mode-locking. In comparison with other well-established mode-locking elements such as semiconductor saturable absorber mirrors (SESAMs) , quantum dots  and carbon nanotubes [7,8], its operation range can be extended to much shorter wavelengths, down to the blue spectral range and exhibit several additional advantages. In the early works of mode-locking, saturable absorbers in the visible spectral range consisted of dyes dissolved in different solvents . The disadvantages of such saturable dyes, such as maintaining a constant stream in the dye jet, temperature sensitivity and long-term instability restricted their versatility.
Semiconductor disk lasers (SDLs) are compact and low cost devices covering a wide spectral range extending from the blue to the mid-IR ). In combination with a fast saturable absorber, mode-locked pulses can be achieved, typically at high pulse repetition rates larger than 1 GHz , which are attractive, e.g., for frequency comb generation . Mode-locking of SDLs was demonstrated at different wavelengths in the infrared spectral range using SESAMs [11,13]. The shortest pulses to date were generated at around 1 µm with 107 fs and 198 fs in the fundamentally and harmonically mode-locked regime, respectively . Theoretical studies of SDLs mode-locked by SESAMs have been published in [14,15]. Recently, several continuous-wave SDLs emitting in the blue spectral range were realized [16,17]. Special applications of femtosecond optical pulses in the blue spectral range are in bio-imaging or in the next generation of high-density optical storage , but the present laser sources are rather complex and expensive. Therefore, blue femtosecond mode-locked SDLs would be an attractive alternative source. In order to attain passive mode-locking of SDLs, composite materials doped with metal nanoparticles (NPs) are a promising candidate because of their distinguished saturable absorption properties in the visible range. In particular, compared to the wide-spread semiconductor-based saturable absorbers, NP-based saturable absorbers can be fabricated much simpler and more cost-effectively. In , the authors have theoretically studied passive mode-locking of dielectric solid-state lasers emitting in the green spectral range by using metal nanocomposites as slow saturable absorbers and predicted pulse generation with a duration as short as 100 fs in a Ho:YLF laser at 545 nm. Unlike dielectric solid-state gain media, semiconductor gain materials dynamically respond with a much shorter response time, which is in the order of a few nanoseconds, and the mode-locked dynamics differ by this reason.
In this paper, we analyze passive mode-locking of SDLs in the blue spectral range with metal nanocomposites as slow saturable absorbers from a theoretical point of view. To utilize the strong saturable absorption of NPs one has to ensure that the surface plasmon resonance (SPR) is located at the central lasing wavelength of the gain medium. In general, this is accomplished by tailoring the size and shape of metal NPs and choosing an appropriated embedding medium. Here we study passive mode-locking of a GaN-based SDL operating at a central wavelength of 420 nm. As will be shown, such laser can be mode-locked by a thin layer of silica glass doped with spherical silver NPs. The plasmon resonance of the latter is located at 414 nm.
2. Theoretical fundamentals
In metal NPs, the absorption near the plasmon resonance becomes saturated with increasing intensity [1,2] corresponding to a saturation intensity in the range of 10 MW/cm2. The physical reason for this effect is related to the intensity-dependent dielectric function of metals leading to a nonlinear shift of the plasmon resonance . The transient nonlinear response of the NPs is determined by the electron thermalization and the cooling of the hot electrons through the thermal exchange with the lattices in the metal. These processes can be described by the semiclassical two-temperature model for the electron temperature and the lattice temperature .
For a moderate pump fluence the change of the dielectric function of the metal is proportional to the change of the temperature of the electrons in the metal NPs. Based on these facts, an equation for the transient dielectric function of the metal NPs can be derived, which is given by 
The effective dielectric function of metal nanocomposites can be directly calculated by using the Maxwell-Garnett model for nanospheres smaller than 10 nm, given by19]).
To study the lasing dynamics of SDLs containing a metal nanocomposite as a slow saturable absorber in the laser cavity, we apply the following standard master equation14,15,17].). In the above equation, the gain coefficient is given by
3. Numerical results
Figure 1(a) shows the transient transmittance of a 1-µm thin silica glass layer doped with Ag nanospheres smaller than 10 nm for different pump pulse fluences at 430 nm. The pump pulse duration is 50 fs and and were chosen to be 100 fs and 1 ps, respectively. The dielectric functions of silver and silica have been taken from  and from . The calculated recovery time of the NP-nanocomposite yields 3 ps and compiles with the needed requirements of an absorber recovery time of few ps for femtosecond SDLs .
Here we study a mode-locked semiconductor disk laser containing GaN as gain material as an example [16,17]. The laser is operating at a central wavelength of 420 nm and the length of the resonator is set to 20 cm. The small signal gain is chosen to be , the gain linewidth THz, and the linewidth enhancement factor [16,17]. The gain recovery time is approximately 1 ns [22,23] and the saturation energy of the gain medium 0.6 nJ. As a saturable absorber we have chosen a 1-µm thin silica glass film doped with Ag nanospheres smaller than 10 nm. In this case, the SPR is located at 414 nm and the composite exhibits strong saturated absorption at the lasing wavelength of 420 nm. The main contribution to nonsaturable loss of NP-SAs is related to scattering. For the estimation of the latter we refer to the precise calculations for gold NPs of . For NP diameters smaller than 20 nm scattering loss is negligible in the visible spectral range . Therefore, applying metal nanoparticles smaller than 10 nm, as in our case, we can approximately neglect nonsaturable loss caused by scattering. Additionally, loss related to NP size distributions are not relevant for such small NPs. The substrate itself is also silica glass and only the 1-µm thick surface layer is doped with Ag NPs. The substrate thickness can be chosen to adjust the positive dispersion in the cavity when required.
In Figs. 1(b)-1(d), we present calculated results and properties of the passively mode-locked laser operation of this laser with a group delay dispersion (GDD) of fs2 and a beam area on the metal nanocomposite of 0.002 mm2. Figure 1(b) demonstrates the mechanism of mode-locking. Pulse shortening and stability is explained by the combined action of the dynamics of saturable gain and saturable loss. This can be seen in Fig. 1(b) because the net gain is negative both at the leading and the trailing fronts of the generated pulse. The leading edge of the pulse is suppressed by the action of the absorber, until the pulse energy has reached a value at which the absorption is greatly diminished due to saturation. On the other hand, the trailing edge is suppressed as well because above a certain pulse energy the amplification is decreased due to the depletion of the population inversion in the gain medium. This mechanism is similar as in passively mode-locked dye lasers. In Fig. 1(c) the evolution of the pulse energy is presented. The formation of a pulse containing the highest pulse energy occurs at the very beginning of the process (~20 ns) while the pulse stabilization with the formation of a cw regime takes place on a much longer timescale (200 ns) because of the energy-depending dynamic of the pulse build-up with increasing round-trip numbers. After reaching the cw-regime, the resultant pulse duration is 83 fs. Figure 1(d) shows the intensity profile and the chirp of the pulse. The pulse is positively chirped which can be explained by the nonlinear index of gain and absorber.
Figure 2 shows the dependencies of pulse duration and energy on the GDD. The other parameters are the same as in Fig. 1. Pulse shaping is unstable only for a small dispersion range between −150 fs2 and 40 fs2. This is attributed to the imbalance between the dispersion-induced pulse broadening and compression by the dynamic gain and loss due to the slow response of the gain and the metal NP-nanocomposite. The pulse duration in the positive and negative GDD ranges attain similar values. However, for the same pulse duration the absolute value of negative GDD is larger than those for positive GDD value which can be interpreted by the fact that the pulse broadening effect is stronger for positive GDD because of the positive chirp of the pulses. As Fig. 2(a) indicates the shortest pulse duration of about 54 fs is achieved for a negative dispersion parameter of fs2, while the shortest duration in the positive GDD range is very similar, about 55 fs for D = 50 fs2. In Fig. 2(b), the dependence of the pulse energy on the GDD parameter is presented. A remarkable point is the larger pulse energy in the positive GDD range than in the negative GDD range, which can be explained by the advancement of the pulse due to the negative GDD and the positive chirp leading to strong suppression in the leading part of the pulse by the absorber loss. Since the shortest pulse durations are very similar, the positive GDD range is more favorable due to the higher pulse energy.
Passive mode-locking by NP-composites is possible only in a small interval of filling factors. For filling factors smaller than the mode-locked operation becomes unstable due to the excessive dynamic range of saturable loss. For filling factors larger than , lasing itself becomes impossible due to the negative small signal net gain. For and , the resultant pulse durations and pulse energies are and fs, and and nJ, respectively. These values are calculated for fs2. Other parameters were taken to be the same as in Fig. 2.
In Fig. 3 we show the dependencies of pulse duration and energy on the beam area on the metal nanocomposite absorbers for the same absolute values of the pump power for GDD parameters fs2 and fs2. The other parameters are the same as in Fig. 1. The figure shows that the pulse duration has a shortest value for an optimum beam area (or correspondingly for an optimum pump fluence) but is not altered significantly when changing the beam area. This is in contrast to the case of dielectric solid-state lasers mode-locked by metal NP-nanocomposites, where the pulse duration depends much stronger on the beam area . With the above given parameters, the fluence on the silver NP saturable absorber is in the range from ~15 to ~45 µJ/cm2.
To conclude, we have theoretically studied passive mode-locking of semiconductor disk lasers with metal nanocomposites as saturable absorbers in blue spectral range. For a GaN-based semiconductor disk laser operating at 420 nm and 1µm thick layer of silica glass doped with silver NPs, we studied the dependence of pulse parameters on the absorber and laser parameters and predicted a shortest pulse duration of about 50 fs. Compared with other saturable absorbers, the application of composites containing metal NPs offers several advantages. It allows the development of very compact and cheap mode-locking devices with tunable operation regions, extending from IR down to the blue spectral range.
References and links
1. R. A. Ganeev, A. I. Ryasnyansky, A. L. Stepanov, and T. Usmanov, “Saturated absorption and nonlinear refraction of silicate glasses doped with silver nanoparticles at 532 nm,” Opt. Quantum Electron. 36(10), 949–960 (2004). [CrossRef]
3. V. Halté, J. Guille, J.-C. Merle, I. Perakis, and J.-Y. Bigot, “Electron dynamics in silver nanoparticles: comparison between thin films and glass embedded nanoparticles,” Phys. Rev. B 60(16), 11738–11746 (1999). [CrossRef]
4. J. S. Melinger, V. D. Kleiman, D. McMorrow, F. Gröhn, B. J. Bauer, and E. Amis, “Ultrafast dynamics of gold-based nanocomposite materials,” J. Phys. Chem. B 107(18), 3424–3431 (2003). [CrossRef]
5. U. Keller, K. J. Weingarten, F. X. Kartner, D. Kopf, B. Braun, I. D. Jung, R. Fluck, C. Honninger, N. Matuschek, and J. Aus der Au, “Semiconductor saturable absorber mirrors (SESAMs) for femtosecond to nanosecond pulse generation in solid-state lasers,” IEEE J. Sel. Top. Quantum Electron. 2(3), 435–453 (1996). [CrossRef]
6. K. Wundke, S. Pötting, J. Auxier, A. Schülzgen, N. Peyghambarian, and N. F. Borrelli, “PbS quantum-dot doped glasses for ultrashort-pulse generation,” Appl. Phys. Lett. 76(1), 10–12 (2000). [CrossRef]
7. A. Schmidt, S. Rivier, G. Steinmeyer, J. H. Yim, W. B. Cho, S. Lee, F. Rotermund, M. C. Pujol, X. Mateos, M. Aguiló, F. Díaz, V. Petrov, and U. Griebner, “Passive mode locking of Yb:KLuW using a single-walled carbon nanotube saturable absorber,” Opt. Lett. 33(7), 729–731 (2008). [CrossRef] [PubMed]
8. S. Y. Set, H. Yaguchi, Y. Tanaka, and M. Jablonski, “Laser mode locking using a saturable absorber incorporating carbon nanotubes,” J. Lightwave Technol. 22(1), 51–56 (2004). [CrossRef]
9. J.-C. Diels and W. Rudolph, Ultrashort Laser Pulse Phenomena, 2nd ed. (Elsevier, Amsterdam, 2006).
10. O. G. Okhotnikov, Semiconductor Disk Laser (Wiley-VHC, Weinheim, 2010).
11. U. Keller and A. C. Tropper, “Passively mode-locked surface-emitting semiconductor lasers,” Phys. Rep. 429(2), 67–120 (2006). [CrossRef]
12. F. Quinlan, G. Ycas, S. Osterman, and S. A. Diddams, “A 12.5 GHz-spaced optical frequency comb spanning >400 nm for near-infrared astronomical spectrograph calibration,” Rev. Sci. Instrum. 81(6), 063105 (2010). [CrossRef] [PubMed]
13. P. Klopp, U. Griebner, M. Zorn, and M. Weyers, “Pulse repetition rate up to 92 GHz or pulse duration shorter than 110 fs from a mode-locked semiconductor disk laser,” Appl. Phys. Lett. 98(7), 071103 (2011). [CrossRef]
14. E. J. Saarinen, R. Herda, and O. G. Okhotnikov, “Dynamics of pulse formation in mode-locked semiconductor disk lasers,” J. Opt. Soc. Am. B 24(11), 2784–2790 (2007). [CrossRef]
15. R. Paschotta, R. Häring, A. Garnache, S. Hoogland, A. Tropper, and U. Keller, “Soliton-like pulse-shaping mechanism in passively mode-locked surface-emitting semiconductor lasers,” Appl. Phys. B 75(4-5), 445–451 (2002). [CrossRef]
16. T.-C. Lu, J.-T. Chu, S.-W. Chen, B.-S. Cheng, H.-C. Kuo, and S.-C. Wang, “Lasing behavior, gain property, and strong coupling effects in GaN-based vertical-cavity surface-emitting lasers,” Jpn. J. Appl. Phys. 47(8), 6655–6659 (2008). [CrossRef]
17. T.-C. Lu, B.-S. Cheng, and M.-C. Liu, “Temperature dependent gain characteristics in GaN-based vertical-cavity surface-emitting lasers,” Opt. Express 17(22), 20149–20154 (2009). [CrossRef] [PubMed]
19. K.-H. Kim, U. Griebner, and J. Herrmann, “Theory of passive mode locking of solid-state lasers using metal nanocomposites as slow saturable absorbers,” Opt. Lett. 37(9), 1490–1492 (2012). [CrossRef] [PubMed]
20. W. D. Lynch and W. R. Hunter, “Comments on the optical constants of metals and an introduction to the data for several metals,” in Handbook of Optical Constants of Solids, E. D. Palik, ed. (Academic, Orlando, Fla., 1985).
21. E. L. Falcão-Filho, C. B. de Araujo, A. Galembeck, M. M. Oliveira, and A. J. G. Zarbin, “Nonlinear susceptibility of colloids consisting of silver nanoparticles in carbon disulfide,” J. Opt. Soc. Am. B 22(11), 2444–2449 (2005). [CrossRef]
22. Y.-K. Song, H. Zhou, M. Diagne, A. V. Nurmikko, R. P. Schneider, C. P. Kuo, M. R. Krames, R. S. Kern, C. Carter-Coman, and F. A. Kish, “A quasicontinuous wave, optically pumped violet vertical cavity surface emitting laser,” Appl. Phys. Lett. 76(13), 1662–1664 (2000). [CrossRef]
24. P. K. Jain, K. S. Lee, I. H. El-Sayed, and M. A. El-Sayed, “Calculated absorption and scattering properties of gold nanoparticles of different size, shape, and composition: applications in biological imaging and biomedicine,” J. Phys. Chem. B 110(14), 7238–7248 (2006). [CrossRef] [PubMed]