LLF is a crystal isomorph to LiYF
4 (YLF), being a tetragonal crystal with the structure of the scheelite (CaWO
4). Its lattice constants are
and
[
20]. It was preferred over YLF due to its better thermomechanical properties [
21]. In this host, praseodymium absorption transition
is located at 444
and its absorption cross section is about
, allowing efficient diode-based optical pumping [
2]. Its fluorescence spectrum in the 600–750
is composed by four main transitions. The one with the greater emission cross section is the
, corresponding to an emission wavelength of 640
in
polarization (E//a). At the same wavelength, two peaks of low intensity (639
and 645
) are present for
polarization (E//c). For
polarization, three other peaks are present:
(604
),
(698
),
(721
). For sigma polarization, a strong emission is present at 607
and minor peaks are present in correspondence of the other transitions listed before. Polarized absorption and fluorescence spectra are reported in
Figure 1.
High quality LLF:Pr single crystals have been grown from high purity powders (LiF, LuF
3 and PrF
3 powders from AC materials, Tarpon Springs, FL, USA), by a Czochralski furnace at the University of Pisa. The dopant concentration in the melt was of 1%. Using X-ray diffraction [
3], the crystallographic axes have been identified and the boule oriented. Subsequently, two oriented samples have been carved from the boule. A known effect in growing Pr:LLF is dopant segregation [
3]. This reflects in lower concentrations of Pr
3+ ions in the grown material with respect to the nominal doping in the melt. The real dopant concentration has been estimated from absorption measurements, realized with a CARY 5000 spectrophotometer, by knowing the absorption cross section [
2]. The Pr
3+ concentration results equal to 0.2% for both samples. This value is in agreement with the one obtained by ICP analysis in [
3]. Samples have been polished to obtain laser quality facets. The final dimensions of the samples are 4
(a) × 4
(c) × 8
(a) for sample 1 and 4
(a) × 4
(c) × 9
(a) for sample 2. The waveguides were written parallel to an a-axis in both samples, resulting in a 8
long waveguide for sample 1 and 9
long for sample 2.
2.1. Waveguide Fabrication
The waveguides were fabricated in the Pr:LLF samples by using an amplified femtosecond laser system (Spitfire ACE, Spectra Physics, Milpitas, USA) that delivered 60 pulses with a central wavelength of 800 , at a repetition rate of 5 . The beam profile has a nearly Gaussian shape with and it is linearly polarized perpendicularly to the scanning direction. The pulse energy was finely tuned by using a set of half-wave plate and linear polarizer, and a calibrated neutral density filter. Then, the beam was focused through a 40X microscope objective (0.65 NA) inside the crystal to produce localized damage tracks by non-linear (multiphoton) absorption. To inscribe each of the designed waveguides, the sample was moved at constant velocity with a motorized XYZ micropositioning stage (HPL-170, PiMicos, PImiCos GmbH, Karlsruhe, Germany).
In crystalline materials, the fabrication of optical waveguides by femtosecond laser irradiation is not as easy as in glasses [
7] because, in many cases, it is not possible to produce a refractive index increase, able to directly confine and guide light along a certain trajectory. On the contrary, the most typical situation is that the refractive index of the crystal is decreased by the effect of the high intensity of the laser, but even in those cases it can be used anyway to design efficient waveguides [
22].
In our study, we designed and fabricated waveguides with different configurations and geometries in the search for the best performance, helping us to understand the confinement mechanisms in Pr:LLF. The following waveguide types were tested:
Circular cladding (CC): this waveguide type consists of a cladding with a reduced refractive index that is produced by multiple parallel laser damage tracks following the desired circular geometry [
8]. The scanning velocity was varied between 600
/
and 1200
/
, the pulse energy between 70
and 100
and the separation between adjacent tracks was set to 2
. With these parameters CCs were inscribed with different radius.
Circular cladding “with ears” (CC-E): in certain circumstances, propagation loss of CC waveguides is reduced by designing a more complex structure of damage tracks at the side of the claddings (“ears”) that may minimize leakage from the waveguide [
10]. Same parameters as CC were tested for CC-E waveguide fabrication.
Hexagonal cladding (HC): cladding waveguides with a hexagonal geometry [
23]. The separation between tracks of the cladding was set to 7
, and the pulse energy and scanning velocity were varied as for CC waveguides.
Stress-induced double-line (DL): stress-induced waveguides make use of the compressive stress created at the side of the damage tracks to produce a region with increased refractive index [
24]. Our design consisted of two parallel tracks with a separation of 3
, and two other identical tracks with a separation of 14, 16 or 20
. The pulse energy was varied between 90–120
and the scanning velocity was set to 100
/
.
Stress-induced double-line with rhombic cladding (DL-RC): same structure as DL but adding some tracks above or below the waveguide region to improve confinement [
14]. DL tracks were fabricated with the same parameters as DLs and the cladding tracks with a pulse energy of 100
and a scanning velocity of 100 or 500
/
.
Single line (SL): it consists of a single laser scan that acts as waveguide in the cases where a refractive index increase could be produced at the damage track [
24]. We have tested these structures in Pr:LLF with pulse energies between 50 and 100
, and scanning velocities between 150 and 500
/
.
As an example, images of the cross-sections of some waveguides are shown in
Figure 2.
2.2. Waveguide Analysis
To characterize the waveguides, we initially performed coupling and transmission measurements at
, employing an unpolarized He-Ne laser as the source and a Glan–Thompson polarizer to control the polarization of the incident beam. The measurements were carried out both for
-polarization and for
-polarization due to the birefringence of the host material, which could lead to a different behavior of the waveguides for different polarizations. The laser beam was focused with several lenses, obtaining the best performance with an achromatic lens of 30
focal length. The corresponding beam diameter at the waist was
. The light exiting from the waveguide has been collected with an OLYMPUS PLN20× microscope objective (N.A. of 0.4, manufactured by Olympus Corporation, Japan), forming an image of the confined mode on a beam profiler (BP, DataRay WinCamD-UCD15, DataRay Inc., USA). For all those measurements, the sample was placed in a custom made copper holder, which allows active temperature stabilization of the sample through a thermoelectric cooler. The whole system was placed on a 3-axes goniometer as well as a translation stage to optimize the beam coupling. The positions of both coupling and collection optics have been controlled by placing each of them on a 3D precision translation stage (THORLABS MBT616D/M, manufactured by Thorlabs Inc.). Some of the measured intensity profiles with the corresponding microscope images of the waveguide cross-sections are shown in
Figure 3. Measuring the transmission efficiency of the waveguide, an upper limit for the propagation losses can be set, subtracting the effect of Fresnel losses and assuming the complete coupling of the laser beam in the waveguide. The best results for each type of waveguide are shown in
Table 1 and
Table 2. There, the presence of confined modes, their characteristics and the upper limit on the propagation losses are reported. In the tables, the writing parameters for each waveguide are also listed. The complete data of waveguide parameters are included in
Appendix B.
Some of the SL waveguides written on sample 2 (WG15-WG16 of c-cut facet and WG15, WG17-WG20 of a-cut facet) showed confinement only for
polarization while none of the SL waveguides confine
polarization. For DL waveguides (WG15-WG20 of sample 1), no confinement has been observed for both polarizations. Better results have been achieved from DL-RC waveguides, which confine
polarization in the core. No confinement of the
polarization has been observed in these waveguides. A different behavior has been observed in depressed cladding waveguides, where
polarization is confined in the core and
in the cladding. This behavior can be explained in terms of a refractive index increase at the damage tracks for
polarization, opposed to the refractive index decrease observed for
polarization. It means that the modification produced by the femtosecond laser irradiation is highly anysotropic, as it has been reported for other crystalline material such as LiTaO
3 [
25]. In this case, the multiple tracks that compose the waveguide act as a set of parallel waveguides (see
Figure 3c), coupling a total power comparable or greater than the one confined in the core, but with a modal profile that resembles the cladding shape, which is not useful for the construction of a laser device. The waveguide design which demonstrates the lower propagation losses is the CC-E design. Except for WG10 of sample 1, those waveguides possess propagation losses lower than
/
for
-polarization, a value lower than those previously reported for femtosecond-laser-written waveguides on fluorides [
14,
15]. In particular, waveguide WG8 of sample 1 shows an upper limit for the propagation losses of
/
, a value comparable to the one observed for ultra-large area waveguides realized by helical inscription technique [
16].
To estimate the refractive index reduction in the irradiated area for
-polarization, a measurement of the numerical aperture of the waveguide has been performed. The waveguide chosen was WG8 of sample 1, due to the greater transmission efficiency and thus, less scattered light on the beam profiler. Through the step index waveguide approximation [
11], it is possible to connect the numerical aperture to the refractive index difference between core and cladding. The obtained value for
is 2 ×
.
To identify the waveguides suitable for lasing, coupling and transmission measurements have been performed also at 444 . The chosen source was an InGaN-based laser diode tuned to emit at 444 in order to match the absorption peak of Pr3+ ions. A collimation lens was used to collect the beam exiting from the laser diode and then a couple of cylindrical lenses (Schäfter+Kirchhoff 5 AN-3-V-35) was used to reduce the beam astigmatism. Since the laser diode emission is mainly polarized, a half wavelength plate and a polarizing beam splitter were used to control the pump power, keeping constant the emission wavelength of the diode. A second half wavelength plate was employed to control the beam polarization, in order to study both and polarization at this wavelength. The maximum available power before the focusing lens was about . The best performance has been observed employing as coupling lens the same achromatic lens of 30 focal length employed for the wavelength. The focused beam has been studied with the BP. The beam had a diameter of 60 with a corresponding value of of 20 in the horizontal direction and a diameter of 40 with an of 1.7 for the vertical direction. The definition of and is the one reported in the ISO 11146-1:2021 standard. The choice of a pump beam wider than the average dimension of the waveguide is due to the numerical aperture of the waveguides (about 0.04), which limits the divergence of the input beam. The chosen lens was found to be the best compromise between beam diameter and divergence.
SL waveguides do not show any confinement for both polarizations, while DL waveguides and DL-RC waveguides confine only
polarization at the pump wavelength, with a transmission efficiency of a few percent, once the praseodymium absorption is subtracted. Waveguides which shows the best performance are the depressed cladding ones. These waveguides confine
polarization in the core and for some designs (CC-E and HC structures),
polarization is also confined in the core but with transmission efficiencies of about 1–4%. All the waveguides which confine the radiation were found to be multimodal. As already observed at
, the best results were achieved with the CC-E waveguides. A summary of the transmission efficiencies measured for these waveguides is reported in
Table 3. Observing the results of the coupling measurements, we expected
-polarized lasing from the waveguides given the lower propagation losses of this polarization with respect to
polarization.
A phenomenon noted during the measurements is the increase in the transmission efficiency when increasing the incident power on the waveguide. A possible explanation of this effect is related to the presence of praseodymium ions whose absorption spectrum has a peak at 444.0
for
polarization, as reported in
Figure 1. The transition involved in the absorption process is the
. This last manifold quickly decays via phonon-assisted transition to the
, a metastable level with a mean lifetime of about 45
[
3]. The high pump power together with the spatial confinement induced by the presence of the waveguide leads to a radiation intensity of approx. 100
, and saturation of the absorption of the active medium in the waveguide can occur, due to the depletion of the ground state. The same effect has been reported for femtosecond-laser-written waveguides in Tm:KLu(WO
)
[
11]. A simple modelization of this effect can be achieved with a rate equation system and it is reported in
Appendix A. The obtained relation between the incident power on the waveguide facet (
) and the output power (
) is given by:
where
is the Wright omega function, and
and
are the Fresnel losses at the two interfaces between air and LLF.
This model has three parameters:
is the coupling efficiency of the waveguide for the pump beam,
is an effective saturation power and
Q is connected to the low-intensity absorption coefficient, directly measured by transmission measurement with the unfocused laser diode light through the bulk crystal, subtracting the effect of the Fresnel losses. In this case, no violations of the linear trend are observed, due to the larger beam diameter, about 1
, with respect to the waveguide diameter. The values of the other two parameters are derived from the best fit of the transmission data. The measurements have been carried out on three waveguides of different diameters, WG3, WG7 and WG8 of sample 1, in order to study this effect with waveguides of different diameter, namely 20
, 36
and 40
. A best fit with the model reported in Equation (
1) has been performed. The results of the best fit for the three waveguides are reported in
Table 4, while the data and the best fit plot are reported in
Figure 4a–c. In the figures,
is the incident power while
is the output power from the waveguide.
As expected, the value of
is greater for larger waveguides. To exploit the dependence on the area of the waveguide, a linear fit is performed between the area of the waveguide (
A) and the saturation power obtained from the best fit. The model used is:
where
is an additional parameter to compensate the effect of the approximations made.
The obtained result is
= 50
and
. Data and best fit are presented in
Figure 4d. The assumed linear trend is found in the experimental data. The expected value for
can be derived from Equation (
A9), assuming as value for the absorption cross section the one reported in [
2], obtaining thus a value of 1.0
. This value differs by a factor of two from the experimental one, but this is acceptable since the simplicity of the rate equation model considered and the approximations made, similar to the uniform distribution of the power in the core of the waveguide, not satisfied by the waveguides studied (see
Figure 3f), where the output profile at maximum coupling efficiency is reported. With this method it is possible to isolate the coupling efficiency of the waveguide. The value of
reported in
Table 4 are compatible with the value of
shown in
Table 3, and this corresponds to a low value of propagation losses, as indeed observed with the measurement reported in
Table A2. The values of the coupling efficiency (<50%) are mainly due to the diameter mismatch between the waveguides and the pump beam, namely 20–40
and 60
. Since it is possible to estimate the coupling efficiency, both the threshold power and the slope efficiency of the realized lasers will be given with respect to the power coupled in the waveguide (
). Here
indicates the laser output power.