We have demonstrated a laser-pumped, near-infrared solid-state dye laser (SSDL) with a slope efficiency approximately equal to 35%, tunability over approximately equal to 40 nm (from 710 to 750 nm) and M2 < 1.3. This device utilizes a folded three-mirror resonator containing a tight focus for the gain medium and a collimated section for the tuning element. The folded cavity is astigmatically compensated through proper choice of sample thickness and cavity fold angle. We achieved low-threshold operation through the tight intracavity focus and by mounting the sample at Brewster’s angle. Two pump lasers were used in this study: (1.) a flashlamp-pumped dye laser (FPDL) with an output wavelength of 630 nm and a pulse duration of approximately equal to 1 microsecond; and (2.) a pulsed red diode laser with an output wavelength of 671 nm and a pulse duration of approximately equal to 200 ns. The gain medium consists of the near-infrared dye Oxazine 725 in the solid host modified PMMA. With the FPDL as the pump source, slope efficiencies up to approximately equal to 35% were measured at the center of the tuning range. A single-plate birefringent filter (BRF) was used to tune the output from approximately equal to 710 to 750 nm with a single output wavelength. The BRF narrowed the spectral output from approximately equal to 15 to approximately equal to 0.8 nm, and provided smooth, continuous tuning over the 40-nm range. Lasing was observed outside this range, but the output consisted of two wavelengths separated by approximately equal to 50 nm (the free spectral range of the BRF). Time-resolved data showed that, for these cases, the laser switches from the shorter to the longer wavelength during the pulse. Input/output curves were generated as a function of resonator feedback for several output wavelengths. Findlay-Clay analyses were used to determine the round-trip cavity loss at each wavelength. The results correlate well with known losses in the resonator, including dye self-absorption losses. Beam-quality measurements were made near the peak of the tuning curve (lambda approximately equal to 727 nm) with a cavity feedback of 95%. At 1.5x threshold, the laser output had an M2 value of approximately equal to 1.06. At 7x threshold, the beam quality degraded slightly to M2 approximately equal to 1.26. Good temporal tracking was observed between the pump and output pulses, once the SSDL turned on. With design improvements to reduce the threshold, the tunable SSDL was also lased using the diode laser as the pump source. Further characterization of this device under direct diode-pumping is in process.
Tunable solid-state dye lasers operating in the blue-green spectral region are attractive for a variety of applications. An important consideration in assessing the viability of this technology is the service life of the gain medium, which is presently limited by dye photodegradation. In this study, solid polymeric samples consisting of the coumarin dye C540A in modified PMMA were subjected to controlled photodegradation tests. The excitation laser was a flashlamp-pumped dye laser operating at 440 nm with a pulse duration of 1 μs. A complementary set of data was obtained for dye in solution phase for comparison purposes. Photophysical properties of C540A in water solution of polymethacrylic acid (PMAA) have been investigated with a view to assess the suitability of the sequestering polymer (PMAA) as an effective additive to facilitate use of a water medium for highly efficient blue-green dye lasers. Lasing action of C540A in aqueous PMAA has been realized using flashlamp-pumped laser system, yielding excellent laser efficiencies superior to that achieved in ethanolic solutions with the same dye. Laser characterization of dye in media included measurement of laser threshold, slope efficiency, pulse duration and output wavelength.
We report on the laser characteristics of solid-state dye lasers pumped directly by a pulsed red diode laser. A 1.6-mm thick disk of Oxazine 725 in modified PMMA was excited longitudinally in a nearly hemispherical resonator at ≅671 nm. We operated at rep rates up to 1 kHz, with only a modest drop in energy per pulse at the highest rep rates. (The energy at 1 kHz is ≅83% of that measured at 1 Hz.) The spectral output of this solid-state dye laser was centered at ≅740 nm with a bandwidth (FWHM) of ≅10.5 nm. For a pump pulse of 230 ns (FWHM), the dye laser output was ≅155 ns in duration, and tracked the pump pulse well after turn on. The maximum observed efficiency for a sample containing Ox 725 in modified PMMA was 18%. Data on other solid dye media are also presented.
Physical Sciences Inc. has several ongoing programs to develop novel high-damage-threshold solid-state optical limiters. We are using polymer matrices doped with RSA (reverse saturable absorber) chromophores such as metallo-phthalocyanines to create both a tandem optical limiter and a graded-density limiter. Characterization is performed using a novel f/5 optical setup which simultaneously measures spatial and temporal profiles of the transmitted light as well as the conventional average transmission. A Q-switched doubled Nd:YAG is used as the probe laser. In this paper, we present detailed spatial and temporal characterization of solid-state tandem optical-limiter devices. To our knowledge, few such measurements have been conducted on limiting materials. Our initial results indicate that for these materials, damage typically occurs within two nanoseconds of the damaging pulse. In addition, CCD images reveal the spatial evolution of the nonlinear absorption of the pulse as it interacts with the limiting material at energies ranging from microjoules to millijoules. Lastly, time-resolved damage measurements were conducted on PMMA. These results as well as others which elucidate the limiting and damage dynamics will be presented.
We report on the physical and optical characteristics of the laser-hardened, solid-state host material polymer-filled nanoporous glass (PFNPG). PFNPG consists of a nanoporous glass structure (average pore size =~7 - 10 nm and matrix porosity =~38 - 40%) filled with a damage-resistant polymer. We have previously used this material as a host matrix for solid-state dye lasers, and in this study have applied it to nonlinear filters. The objectives were twofold: (1) to fabricate PFNPG samples with a high laser damage threshold under f/5 focusing conditions; and (2) to successfully dope a nonlinear absorbing dye into this matrix at millimolar concentrations. Undoped PFNPG plates showed damage thresholds of =~42 J/cm2, a value significantly higher than that observed for a bulk polymer in the same test bed. PFNPG samples doped with the nonlinear dye Zn-TPP showed even greater damage resistance. Samples with dye concentrations ≥1 mM showed good nonlinear filtering.
For two meso-substituted benzo-fused pyrromethenes (BPMM and F-BPMM), photophysical and lasing properties in liquids and in poly(methyl methacrylate) (PMMA) are reported. Both dyes exhibit high quantum efficiency (0.6-0.9) along with high extinction coefficients, values which are superior to other NIR dyes such as oxazine 1 and rhodamine 800. Lasing efficiencies in the range of 20-30 % have been recorded for the new dyes. Additionally, the dyes can be pumped by a diode or dye laser emitting at 650 nm. Under continuous UV-Vis irradiation, BPMM and F-BPMM demonstrated improved photostability as compared with a previously reported analog, PM-700 (Scheme 1). The survivability of dyes under conditions of radical polymerization has also been investigated.
Direct diode-pumping of dye-based gain media has the potential to produce a very efficient, inexpensive, compact, tunable laser source. The pulsed diode lasers available for exciting dyes, however, have relatively low peak powers (up to a few watts). Therefore, the focusing characteristics of the diode beam are a key factor in reaching dye-laser threshold. In this work, detailed characterization of the output from a single-stripe red diode was done, including input/output characteristics and temporal and spatial profiles. Based on these results, transfer optics were designed to couple the diode beam into the dye-based gain medium with a small spot size. A solid-state dye element was then excited longitudinally in a low-threshold resonator. Laser results are reported, including measurements of threshold, input/output characteristics, temporal profiles, and spectral properties. The data are discussed in detail, and strategies for improving dye-laser performance are identified.
The photophysical and lasing properties of a benzo-fused pyrromethene dye that is capable of being pumped by a diode or dye laser at relatively long wavelengths have been investigated for liquids and for a solid matrix, poly(methyl methacrylate) (PMMA). Fluorescence data, including quantum efficiency and lifetime, have been obtained. The dye emission, that is centered around 690 nm, shows good quantum efficiency as compared to other NIR dyes such as oxazine 1 or rhodamine 800. Photostability in organic solvents as well as the survivability of the dye under conditions of radical polymerization have also been investigated.
We report on a systematic study of the laser threshold and slope efficiency of solid-state dyes lasers operating in the near-IR under microsecond(s) pumping. The excitation source for this work is a flashlamp-pumped dye laser operating at a wavelength of approximately equal to 660 nm with a pulse duration of approximately equal to 1.25 microsecond(s) . A major objective of this work is to demonstrate laser characteristics traceable to direct diode-pumping of a dye- doped solid matrix. Detailed measurements were made for three laser dyes and three different host materials. Dyes evaluated include Rhodamine 700, Rhodamine 800 and Oxazine 725 at various concentrations. The host matrices studied were modified PMMA, polymer-filled nanoporous glass, and organically modified silicate. Laser measurements included output energy and wavelength as functions of input energy and resonator feedback. Findlay-Clay analyses were performed to extract information on the round-trip cavity losses in each case. Temporal waveforms were obtained for the pump and output pulses in order to evaluate the extent of tracking, and to study the mechanisms for loss of tracking. The highest laser efficiency observed was 43 percent for Oxazine 725 in MPMMA for a 2-mm thick sample. This material had a laser wavelength of approximately 690 nm for Roc < 0.70. The value increased to approximately 735 nm, however, for R > 0.80. The longest output wavelength observed in this study was approximately 797 nm for Rhodamine 800 in PFNPG. The highest efficiency observed for this particular sample was 21 percent. Its emission wavelength was relatively insensitive to feedback over the range studied. Measurements of laser threshold are presented and discussed for the materials investigated.
Pyrromethene dyes, particularly PM 567, have been studied in liquid media using various spectroscopic techniques. Photodecomposition of dyes was monitored by absorption and fluorescence spectroscopy. In laser flash photolysis experiments on dyes in liquids, phototransients were observed (microsecond time domain) that included dye triplets and at least one other transient of the radical or radical-ion type. Experiments included product studies that allowed identification of major products of photodegradation; an assessment of the effectiveness of known stabilizing additives such as DABCO and butazate was also conducted. Purposes of the work included definition of the roles of energy and electron transfer mechanisms in dye photodegradation and the effects of oxygen or additives in dye media.
This paper reports on a systematic study ofthe beam quality ofsolid-state dye lasers for different resonator designs. The resonators investigated include: multimode stable, hard-edge unstable, and unstable with a graded-reflectivity mirror (GRM) output coupler. The purpose ofthe work was to investigate the conditions under which good beam quality can be achieved, and to examine the possible trade-off between beam quality and energy extraction efficiency. Beam quality was quantified through conventional M2 measurements. A hard-edge unstable resonator of magnification ?2.5 produced a beam ofM2 ?11 - 12 at a PRF of 2Hz and a pump flux of 5 MW/cm2. The value increased to ? 18 — 19 at a pump flux of2O MW/cm2. This can be compared with an M2 of ? 140 - 150 with the multimode stable resonator. Preliminary measurements with the GRM resulted in M2 values of ? 5 to 6 at 5 MW/cm2.
This paper reports on the laser emission properties of Pyrromethene 580, Pyrromethene 597, Pyrromethene 650 and Rhodamine 11B in the novel matrix polymer-filled microporous glass (PFMPG). This host material combines the advantages of an organic environment for the dye with the superior thermooptical and mechanical properties of an inorganic glass. Laser efficiency was measured as a function of pump flux for different dye concentrations, resonator feedback, and locations on the sample. Service life, defined as the number of pulses for the output to drop to the 70% point, was recorded at 5 Hz for the higher dye concentrations. The highest efficiencies were observed for Pyrromethene 597 (is congruent to 70%), which had a service life of is congruent to 60,000 shots at 25 MW/cm2 and is congruent to 45,000 shots at 50 MW/cm2. The longest service life was measured for Rhodamine 11B (is congruent to 110,000 pulses at 25 MW/cm2), but this dye had somewhat lower efficiency (is congruent to 50 - 55%). Thermal lensing measurements were made for dye-doped PFMPG and MPMMA, and showed that the lensing is much lower in the hybrid matrix. The agreement with the theoretical modeling is very good.
The photophysical and lasing properties of pyrromethene dyes in epoxy resins have been investigated. These resins show a relatively high damage threshold, as well as good lasing efficiency. Fluorescence properties for PM dyes in epoxy hosts, including quantum efficiencies and lifetimes, have been obtained.
Generation of ultrashort pulses (picosecond range duration) in pyrromethene-580 (PM-580) and xanthene 11B dyes doped modified PMMA polymer lasers is reported. Active polymer elements were pumped by second harmonic radiation of the 50 picosecond Nd:YAG laser. A single-pulse and train-pulse laser generation was observed at different conditions (variable optical resonator length and pump energy) with a pulsewidth ranging from 140 ps to 30 ps. The train-pulse generation is attributed to mode-locking of a laser resonator. The lifetime (tau) e, of an excited quantum state of a laser transition of the PM- 580 dye molecules has been estimated ((tau) e equals 200 divided by 250 ps) from the pulse-train duration.
The laser efficiency and service life have been measured for two different dye-doped solid media: a modified PMMA and an optical epoxy. The samples were longitudinally pumped using the output of either a Q-switched, frequency-doubled YAG laser (532 nm; (tau) p approximately equals 8 ns) or a flashlamp- pumped dye laser (490 nm; (tau) p approximately equals 1.5 microsecond(s) ). The much longer pump pulse of the dye laser can lead to significant differences in performance in such areas as optical damage, dye photobleaching, thermo-optical distortion of the gain medium, and the relative importance of triplet absorption. The impact of pump pulse duration on laser performance parameters will be discussed.
Laser-related properties of pyrromethene-580 doped modified polymethyl methacrylate, including conversion efficiency, operational lifetime, laser induced damage resistance of the polymer matrix and photodestruction of the impregnated dye, were studied under short-pulse and long-pulse laser pumping. High efficiency and operational lifetime have been achieved in the short-pulse mode. Effect of a laser resonator feedback on both the conversion efficiency and lifetime was revealed and studied in the long-pulse operation mode.
This paper describes an ongoing study of dye-doped polymer materials as gain media in flashlamp-pumped systems. In this work, we have demonstrated 300 mJ/pulse at 0.4% energy efficiency using PM-597 in modified PMMA. The slope efficiency was maintained at 0.46%, except at the highest input energies. These results are quite comparable to those obtained for the same dye in liquid solution. Two important materials considerations in achieving these results are to keep the bulk transmission losses below 0.5%/cm, and to design the resonator in accord with the static as well as the dynamic lensing of the rod.
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