Wavelength Tunable Random Laser E.Tikhonov 1, Vasil P.Yashchuk 2, O.Prygodjuk 2, V.Bezrodny 1

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1 Solid State Phenomena Vol. 06 (005) pp 87-9 Online available since 005/Sep/5 at (005) Trans Tech Publications, Switzerland doi:0.408/ Wavelength Tunable Random Laser E.Tikhonov, Vasil P.Yashchuk, O.Prygodjuk, V.Bezrodny Physics Institute of the Ukrainian Academy of Science; 46, Nauky av., 0650 Kyiv, Ukraine, Physics Department of Kyiv Taras Shevchenko University; 6,Glushkov av., Kyiv, Ukraine Keywords: tunable random laser, multiple scattering, lasing, wedge, active media, dye, rhodamine 6G, polymer. Abstract. Continuously tunable random laser basing on rhodamine 6G was achieved. Wavelength tuning was implemented by wedge-shaped sample shift relatively to the pump beam. The physical base of the tuning method is gain band shift caused by reabsorption. We ascertained that two medium thickness ranges of significantly different tune efficiency exist. The lasing characteristics of the laser were investigated depending on active medium and pump beam parameters. The feedback formation mechanisms in the random lasers of different thickness were analyzed. Introduction Random lasers are principally new sources of stimulated emission where positive feedback is due to multiple light scattering. The random laser is itself the active light-scattering medium without any cavity and other optical elements. These lasers are characterized by a small lasing volume and arbitrary shape. Currently two different random laser types are known: based on a liquid or solid dye solution [,] and on semiconductor powder [3]. Whereas probable application of such a laser is relatively clear [4] its practical use is not yet known, because the physical processes and their influence on lasing of random lasers have not been adequately investigated. Development of the tuning method can promote practical use of the lasers. Since this type of laser is practically deprived of any external optical element, the only spectraldepending element is the gain band. In [5] we demonstrated that the gain band maximum wavelength of the dye-based random laser depends on reabsorption-affecting the medium parameters: dye molecule concentration, concentration and refractive index of scattering particles and sample thickness. To tune the continuously lasing wavelength we have proposed changing the thickness of the active region by a wedge-shaped sample shift respective to the pump beam. This paper is devoted both to practical realization of the method mentioned above and to the investigation of such tunable random laser characteristics. Experimental Investigations were made using wedge-shaped samples made from solid R6G polyvinyl acetate solutions with embedded particles of silica (diameter d~µm) and synthetic diamond (d~7µm). The weight concentration of the particles was 30% for silica and 5% for diamond (particle concentrations were C part =0 and 0 9 cm -3 respectively). The solid solutions were prepared by careful mixing solutions of polyvinyl acetate in alcohol and R6G with the scattering powder. The alcohol was slowly evaporated from the mixture. The wedges All rights reserved. No part of contents of this paper may be reproduced or transmitted in any form or by any means without the written permission of TTP, (ID: , Pennsylvania State University, University Park, United States of America-03/06/4,9:0:4)

2 88 From Nanopowders to Functional Materials were cut from the blanks obtained. The dihedral angle of the wedges was α~4 0, wedge heights (maximum side thickness) were 0.45mm for wedges with silica particles and 0.65mm for wedges with diamond particles. Fig. Schematic representation of experimental setup where - focusing lens; wedge-like shaped active medium, 3 microscope objective; 4 spectrograph; 5 CCD-camera. These wedges were set alternately on the adjustable table to gradually move them across the pump beam (Fig.). Thus the wedge thickness at the incidence spot of the focused pump beam was changed from 50 to 450 (650)µm while the wedge was being moved within 6 (8) mm. The wedge thickness in the spot of pumping was controlled by a measuring microscope accurate to 50µm. The focused pump beam diameter at the incidence spot was 30µm. The difference in wedge thickness within the pump spot was h~µm: thus the effective (mean) wedge thickness h eff is important. The active medium was pumped with the second harmonic of quasi single-mode Q- switched Nd +3 :YAG (λ=53nm, τ~5ns). The focused beam diameter d was estimated as the The intensity bandwidth of the beam intensity distribution at 0.5 of its maximum intensity. distribution in the pump beam cross-section registered by CCD-cam was near-gaussian. The lasing spectra of random laser were registered by CCD-cam in one pump impulse according to experimental scheme in Fig.. To study the lasing energy parameters we used a similar registration scheme where spectrograph and CCD-cam were displaced with a monochromator and a photomultiplier. The lasing radiation was registered backward to the pump incidence direction. The pump intensity was stabilized. The results obtained were used to calculate the h eff -dependencies of the energy spectral density ρ max =(de e /dλ) max at the spectrum peak and the radiation energy E e integrated over the lasing spectrum. To determine the pump energy distribution through the sample depth we investigated h eff - dependence of the sample transmission. In this case the passed pump radiation was directed to monochromator (tuned to λ=53nm) and registered with a photomultiplier. Results and discussion The method of continuous lasing wavelength λ m tuning for the random laser was achieved by using a wedge-shaped scattering sample being displaced relative to the pump beam. The realised tuning range is over a δλ m ~8nm for the wedge with silica and ~4nm for that with diamond scattering particles. The tuning characteristic λ m (h eff ) (Fig.a) is essentially non-linear; and the lasing spectrum bandwidth λ depends on h eff (Fig.b). Both dependencies f =λ m (h eff ) and f = λ(h eff ) consist of two ranges with essentially different efficiencies γ=df i /dh eff, i={,} of the parameters changes. Over the h eff <00µm range both dependencies quickly increase as h eff increases and effective wavelength tuning is accompanied by significant spectrum bandwidth changes. Over the h eff >00µm range both curves slightly depend on the h eff and the tuning is ineffective.

3 Solid State Phenomena Vol λ m, nm λ, nm de/dλ, arb.un b) h eff, mm 0,0 0, 0, 0,3 0,4 0,5 0,6,0 c) 3 0,5 a) 0,0 0, 0, 0,3 0,4 0,5 λ m, nm 0, Fig. Peak wavelength (a) and bandwidth (b) of the lasing spectrum of wedge-shaped random laser with silica (), diamond () particles as a function of the wedge effective thickness; c) luminescence spectra of the thickest side of the wedges with silica (), diamond () particles, and the spectrum of optically thin homogeneous sample (3). h eff, mm Fig.3 demonstrate the dependence of radiation energy E e (h eff ) integrated over the lasing spectrum. It is shown that E e (h eff ) dependence has a maximum at h eff =50 00µm (the h eff -dependence of the spectral density ρ max =(de e /dλ) max at the lasing spectrum peak is the same). Such behaviour of λ m (h eff ), λ(h eff ), E e (h eff ) and ρ(h eff ) dependencies testifies to the difference between the lasing-rise condition in thin (h eff <00µm) and thick (h eff >00µm) random media. According to transmission measurements, the main part of the pump energy (about 90%) is absorbed within the near-surface layer of 00µm thick. It confirms that active region of the sample is approximately 00µm thick. So the lasing condition dependence on the sample thickness resulted from the fact that the thin sample is whole-depth active in contrast to the thick sample containing an inactive (absorbing) part as well as an active one. Active and inactive sample regions act differently in lasing rise. Light amplification occurs in the active part of the sample []. Multiple scattering within the active part provides positive feedback for lasing rise (the scattering type of feedback) [5]. The inactive region does not amplify the light. It only scatters multiply and reabsorbs the light radiated within the active region. Multiple scattering causes partial return of the light to the active region, hence the inactive layer acts as a diffusion reflector [6] taking part in the scattering type of feedback formation (Fig.4). The reflector efficiency is wavelength-dependent owing to the spectral selectivity of reabsorption. Thus scattering feedback 0,9 type is wavelength-dependent as well: its efficiency rapidly increases as λ grows within the reabsorption spectral region. E, relat.units 0,6 0,3 h eff, µm Fig. 3 Radiated energy of the tunable random laser versus the wedge effective thickness. Apart from the scattering type of feedback, there is the other, due to light reflection at the sample surfaces (reflection feedback). In the plane and wedge-shaped samples the transverse sizes exceed sample thickness, thus only two sample surfaces, i.e. front (incident) and back (opposite to the incident), take part in the feedback formation [5] (Fig.4). Thus this feedback is wavelength-independent.

4 90 From Nanopowders to Functional Materials Thinning of the inactive layer causes a decrease in its efficiency as a diffusion reflector. However, the thinning increases the contribution of back surface reflection. Thus wavelength-dependent (scattering) feedback is displaced with wavelength independent (reflection). It leads to the shortwave shift of the lasing spectrum under sample thinning. The lasing wavelength tuning is accompanied with lasing energy and spectrum bandwidth changes. It is conditioned by different efficiency of the mentioned types of feedback. The reflection feedback is formed due to reflection, both by the boundary particles, and at the polymer-air surface. The boundary particles reflection is more effective than scattering by the particles inside the sample because the relative refractive index of particle-air interface is evidently higher than that of the particle polymer interface. Thus reflection feedback is more effective than the scattering feedback. Fig. 4 Schematic representation of feedback formation in the random laser. In the thick sample, the contribution of the back surface reflection is low due to high attenuation of the light in the inactive region. Thinning of the sample decreases the thickness of the inactive region and gradually displaces the scattering feedback of the inactive region by the more effective reflection feedback at back surface (Fig.4). Thus the total feedback efficiency grows that results in the increase of radiation energy (Fig.3). The energy achieves the maximum when the sample thickness is equal to the thickness of the active layer (h eff 00µm). In the thin sample the inactive layer is absent. Scattering occurs in the active layer only and reflection at both surfaces forms the total feedback. The reflection feedback contribution is essential. This was proved by disappearance of lasing if the surface reflection was suppressed by immersing the sample into glycerol [5]. At h eff < 00µm the lasing energy E decreases due to the active volume reduction. Nevertheless the spectrum narrows under h eff <00µm (Fig.b) which confirms the increase of effective amplification along the photon trajectories. It occurs because the photon trajectories are located entirely within the active region. Moreover the total feedback efficiency grows because scattering feedback is partially substituted for the more effective feedback formed by back surface reflection. However, it is noticeable that scattering is of fundamental importance for lasing rise, because lasing does not arise in the homogeneous samples.

5 Solid State Phenomena Vol According to Fig. 3 a random laser of fixed thickness (without wavelength tuning) can be characterized with an optimal thickness value. This value corresponds to the maximum radiation energy and depends on the dye, particle material and its concentration. Significantly different tuning efficiencies for the thin (h eff <00µm) and thick (h eff >00µm) sample are interrelated. The thin sample is characterized with significant overlapping of luminescence and absorption spectra that results in rapid growth of the probability of reabsorption under increases of h eff. It leads to an effective shift of the gain band and high efficiency of lasing spectra tuning. The thick sample is characterized with the long-wave shifted luminescence spectrum to be slightly overlapped by the absorption one. Thus reabsorption probability changes slowly under increases of h eff. It results in slow tuning efficiency. The tuning spectral range depends on the range of sample thickness changes and medium parameters influencing the light scattering and reabsorption probability (particle concentration and refractive index). The increasing of these parameters shifts the luminescence spectrum and effective gain band to the long-wave region [5,6]. The relation between the tuning ranges (8nm and 4nm, Fig.a) of random lasers with different light scattering efficiency correlate with the relative shift (0nm and 0nm, Fig c) of luminescence spectra of the thickest wedge part and unabsorbed luminescence spectrum. Increasing the wedge height can at least double the tuning range [5]. But the tuning range is confined by the overlapping region of the luminescence and absorption spectra (~50nm for R6G). Threshold intensity, arb.un Pump beam area, mm 0,0 0,04 0,06 0,08 Fig. 5 Lasing threshold as a function of pump beam cross-section area at two effective wedge thickness - 00µm, - 450µm. The accuracy of lasing tuning increases as the pump beam diameter d reduces. When d<00µm (the cross-section area is 0.05mm ) the lasing threshold becomes h eff dependent (Fig.5). At d>00µm the dependence is negligible. These results testify to inapplicability of harder focusing for the laser parameter stabilization. The h eff dependency of the lasing threshold is conditioned by dependence of effective gain coefficient on the relation between active region diameter determined by pump beam diameter d and mean dimension D of photon trajectory location. If D>d a significant part of the photon trajectory passes out the active region (Fig.4) causing a reduction in the gain coefficient and increases in the lasing threshold. Conclusions Continuous tuning of random laser spectrum is realized by wedge-shaped sample displasment across the pump beam. The tuning range is defined by the wedge height and by the parameters influencing the reabsorption probability of luminescence (the light scattering parameters). Significant differences between the tuning efficiency and the other lasing characteristics at a small (h eff <00µ) and large (h eff >00µ) effective thickness of the wedge are conditioned by different influences of the active and inactive sample regions on the reabsorption probability and feedback formation.

6 9 From Nanopowders to Functional Materials A random laser of fixed thickness is characterized with an optimal thickness value and optimal focusing of the pump beam. References [] N. M. Lawandy, R. M. Balachandran, A. S. L. Gomes & E. Sauvain Laser action in strongly scattering media, Nature, 368, p (994); [] E.O.Tikhonov, Vasil P.Yashchuk, O.A.Prygodjuk, V.I.Bezrodny, Solid State Phenomena, 94, p.95-98(003); [3] H. Cao, Y.G. Zhao, H.C. Ong, S.T. Ho, J.Y. Dai, J.Y. Wu, and R.P.H. Chang: Appl.Phys.Lett. 73, p.3656(998); [4] H. Cao, Waves Random Media, 3, p.r R39(003); [5] E.O.Tikhonov, Vasil P.Yashchuk, O.A.Prygodjuk, V.I.Bezrodny, Solid State Phenomena, 99, p.77-8(004); [6] E.O.Tikhonov, Vasil P.Yashchuk, O.A.Prygodjuk, V.I.Bezrodny, Semiconductors, Quantum Electronics and Optoelectronics, 7, p.77-8(004).

7 From Nanopowders to Functional Materials 0.408/ Wavelength Tunable Random Laser 0.408/

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