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Oct 14, 2024

Low-threshold distributed feedback laser based on holographic polymer dispersed liquid crystals through the oriented organic semiconductor films | Scientific Reports

Scientific Reports volume 14, Article number: 17790 (2024) Cite this article 507 Accesses Metrics details A specific optimized configuration for low threshold organic semiconductor laser based on a

Scientific Reports volume 14, Article number: 17790 (2024) Cite this article

507 Accesses

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A specific optimized configuration for low threshold organic semiconductor laser based on a holographic polymer dispersed liquid crystal (HPDLC) transmission grating was demonstrated. Here the organic semiconductor films and phase separated liquid crystal (LC) molecules were oriented along the direction of the HPDLC grating grooves. The influence of the organic semiconductor chain orientation and the excitation polarization on the optical properties of the materials has been investigated. Especially, when polymer chain orientation, LC molecules and pump light polarization are consistent with the direction of the grating grooves, the performance of the outgoing laser is greatly improved. Up to 9.78% conversion efficiency with a threshold lower to 0.12 μJ/pulse can be obtained, indicating their potential for high-performance organic optoelectronics.

Organic semiconductors can be easily and large-area integrated by solution or evaporation to form a variety of optoelectronic devices1,2,3,4,5,6. They exhibit broad gain range, chemically tuneable structure and strong optical transitions, making them attractive candidates as laser materials7,8,9,10,11,12. Until now, the majority of research on organic semiconductor lasers (OSLs) has relied on laser pumping13,14,15, a method that is complex and costly. Therefore, the use of electrical pumping for OSLs is recommended for widespread use. Conversely, the process of electrical pumping, which entails the injection of a current to induce a population inversion and consequent light amplification, proves to be challenging to implement in OSLs13,16. By improving optical design to reduce threshold, utilizing indirect electrical pumping through an LED is a highly efficient method for achieving compact and cost-effective electrically driven OSLs17. Distributed feedback (DFB) structures possess favorable resonator geometries characterized by low thresholds and emission of a single longitudinal mode. These properties arise from their extended gain path and strong wavelength selectivity10. A holographic polymer dispersed liquid crystal (HPDLC) grating is utilized as DFB cavity due to its ease of preparation18,19, low scattering loss20,21 and electrical tunability22,23. Furthermore, we have been able to independently control the parameters of the organic semiconductor (gain medium) layer and HPDLC grating (feedback) separately. This enables us to control the laser output performance more effectively.

Researchers carried out extensive research to lower the threshold of the OSLs based on HPDLC gratings. Low-functionality acrylate-based monomers can reduce the crosslinking degree caused by the polymerization process, which coupled with the application of narrower gratings, enables the alignment of liquid crystal (LC) molecules along the grating grooves. This alignment resulted in improved lasing feedback performance, leading to a significant reduction in the lasing output threshold to 0.18 μJ24. The effect of organic semiconductor annealing on the output performance of lasers has also been reported. Single mode laser emission was realized by thermal annealing at 120 °C, and the threshold was reduced to 0.2 μJ /pulse25. The dissolution solvents of the laser gain layer also had an impact on the output laser threshold. The arrangement of organic semiconductor side chains using non-aromatic organic solvents suppressed the occurrence of photophysical aggregation, reduced fluorescence quenching, and thus lowered the threshold26. The pump polarization dependency was also studied. The laser threshold under p polarization and s polarization pump light were measured as 0.22 μJ/pulse and 0.15 μJ/pulse, respectively27. However, previous studies have either only focused on the gain layer or the grating layer, and there has been little research on the relationships between the layers. According to reports, oriented polymer films makes it easier to create high gain devices28. Nevertheless, there is a scarcity of quantitative data about the impact of chain alignment on the performance of lasing. Considering the anisotropy of the phase separated LC molecules in the grating, the optimal arrangement of LC molecules and polymer chains can definitely reduce the threshold. However, the relationship between the two has not been reported, and the specific optimized configuration of the laser is not shown.

In this work, the semiconducting polymer poly(2-methoxy-5-(20-ethylhexyloxy) p-phenyl-enevinylene) (MEH-PPV) chain alignment effect on lasing performance was performed in OSLs. The gain film absorption, net gain and loss were investigated. The output performance of lasers under different polarized light pumping conditions has also been studied. We analyzed the relationship between the layers of the laser, and identified the specific optimized configuration for low threshold. Theoretically and experimentally, the polymer chain orientation, LC molecules and pump light polarization are consistent with the direction of the grating groove arrangement, resulting in the best laser output performance. The DFB laser in this instance exhibits bright laser emission, characterized by a reduced threshold of 0.12 μJ/pulse and an enhanced conversion efficiency of 9.78%.

The structure of the laser is shown in Fig. 1(a). MEH-PPV (Mw ~ 1.2 \(\times\) 105, Xi’an P-OLED Material Tech.) is utilized as a gain medium layer, while the HPDLC grating is employed as feedback layer. Contrary to earlier studies, polyimide (PI) was applied to the bottom glass substrate. As seen in Fig. 1(b), different films were prepared. The PI layer on the bottom glass substrate of one sample was not processed, while the PI layer of another sample was mechanically rubbed in a unidirectional manner using a velvet cloth along the y-axis. Then homogeneous spin-coating and orientated thin films were obtained by spin-coating (2200 rpm; 30 s) the MEH-PPV solution in xylene solvent (7 mg/ml) onto the two PI-coated glass substrates mentioned above, followed by 120 °C annealing in a vacuum oven. After annealing, the thickness of MEH-PPV layer shrank from 85 to 80 nm. An empty cell was formed by merging the MEH-PPV coated glass substrate with a bare glass substrate. Mylar spacers was used to control the cell gap at 6 μm.

Schematic of (a) the OSLs; (b) spin-coating and oriented MEH-PPV film; (c) MEH-PPV molecule being excited; (d) absorption, PL and ASE spectra of MEH-PPV films drying at room temperature and annealed at 120 °C, respectively, the inset indicates the molecular formula for MEH-PPV.

A UV–Visible spectrophotometer (PerkinElmer, LAMBDA 1050) combined with a polarizer was used to measure the absorption of MEH-PPV layers. The photoluminescence (PL) spectra were measured by Edinburgh, FLS-1000 equipped with a monochromatized 150 W Xenon lamp as an excitation source. The absorption and fluorescence intensity of PI were negligibly weak in comparison to those of MEH-PPV. The photoluminescence quantum yield (PLQY) of MEH-PPV thin films has been measured by a fluorescence spectrometer with integrating sphere (FL920; Edinburgh instruments, China). Schematic structure of MEH-PPV molecule being excited was shown in Fig. 1(c). The PI film did not exhibit any optical dichroism. Figure 1(d) exhibited the intensity for absorption and PL spectra of spin-coating MEH-PPV films before (room temperature) and after (120 °C) annealing. It was worth noting that there was a significant improvement in absorption and PL intensity of MEH-PPV films after annealing, especially in PL intensity, we will discuss this more in Section "Optical properties of the MEH-PPV films".

The HPDLC pre-polymer syrup was made by mixing bifunctionality light-sensitive monomer, nematic LC (\(n_{o}\) = 1.522, \(n_{e}\) = 1.692), chain extender, co-initiator and photo-initiator, their proportions were 60%, 28%, 10%, 1.5% and 0.5%, respectively. (See the supporting materials for more details). The mixture was subsequently dripped into the cell and exposed to the holographic optical field to generate HPDLC gratings. The period \(\Lambda\) of grating is determined by \(\Lambda { = }\frac{{\lambda_{532} }}{2\sin (\theta /2)}\) , and \(\theta\) was the intersection angle of the two curing beams from a CW Nd:YAG laser (532 nm, 6 mW/cm2). Gratings with a period of 395 nm were chosen for this study. The duration of exposure was 5 min, resulting in a grating area measuring 8 mm* 8 mm. The amplified spontaneous emission (ASE) measurement involved exposing the sample to a uniform laser beam of 12 mW/cm2 for 8 min. By illuminating the polymer matrix, the LC molecules would be evenly distributed throughout, forming a polymer dispersed liquid crystal (PDLC).

In order to assess the characteristics of HPDLC gratings, the real time diffraction efficiency and scattering loss were quantified using two circular polarization He–Ne lasers, as described in a previous study29. Diffraction efficiency refers to the proportion of the intensity of diffracted light in the first order to the intensity of the incident light. The scattering loss is determined by \(L = (I_{t} - I_{d} )/I_{t}\) through a rotating polarizer. Here \(I_{t}\) and \(I_{d}\) represent the intensity of He–Ne laser traversing the sample before grating exposing and in real time, respectively. More details and optical setup see support material Fig. S1.

We utilized a Q-switched Nd:YAG pulsed laser (532 nm, 1 Hz, 8 ns) for pumping (Fig. 2) . The polarization of the pump source was controlled by rotating polarizer. A cylindrical lens (focal length: 20 cm) was employed together with an adjustable slit to modify the strip beam into a slender rectangular shape measuring 5 mm*0.1 mm. Then two rectangular beams of equal intensity were obtained by a beam splitter. One rectangular beam was pointed into an energy meter, while the other was used to pump the sample surface at a 45° angle. The output lasing was collected using a spectrometer (LabMax-TOP; Coherent Inc.) connected to a fiber pigtail detector.

Schematic setup for pumping lasing measurement.

The real-time diffraction efficiencies of s and p polarization states are illustrated in Fig. 3(a). Previous studies have shown that the variation of diffraction efficiency in different polarization state was mostly influenced by the alignment of the phase-separated LC molecules29. The s-polarization diffraction efficiencies of 57.1% is higher than 1.6% for p-polarization, which indicates that the LC molecules are aligned with the grating grooves (y-axis, Fig. 1(a)). The inset illustrates the atomic force microscopy (AFM, Nanosurf) image of the HPDLC grating with a period of 395 nm. The grating has good periodicity and a flat surface. Figure 3(b) shows that the p-polarization scattering loss is around 2.3%, in sharp contrast, the s polarization is close to 5.0%. This is because the difference in refractive index (RI) between the polymer layer and the LC layer is greater for s-polarized light, which also reveals the alignment of LC molecules along grating grooves. The orientation of the LCs is due to the low functional monomers used in this work, which produce fewer polymer filaments in the LC rich region, therefore, the grating groove can more effectively anchor the LC molecules. For TE light, the RI modulation is the highest in this case, and the grating feedback ability is the strongest. We will discuss this more in Section "Lasing performance".

(a) Real time diffraction efficiency and (b) evolution of the scattering loss for s polarization (sphere) and p polarization (square) for the sample. The inset illustrates the AFM image of the grating.

Polarized UV–vis absorption spectroscopy measurements are commonly frequently employed to evaluate orientation intensities. As illustrated in Fig. 4(a), an oriented MEH-PPV film is placed between the light source and detector. The magnitude of absorbance varies with an alteration in the angle of the polarizer. The absorption spectrum has its highest intensity when the polarized light oscillates in parallel with the orientation of MEH-PPV film, and absorption spectrum reaches its lowest intensity when light source oscillates perpendicular. The dichroic ratio at the absorption peak wavelength is ~ 5, as illustrated in Fig. 4(b). In contrast, the absorption spectra of the spin-coating sample exhibited no dependence on the polarization of the incident light, indicating that MEH-PPV molecules were randomly aligned within the plane of the substrate (Fig. 4c). Annealing is an essential component in determining the orientation of MEH-PPV molecules. The fabrication circumstances have a significant impact on the crystallinity and crystal arrangement of solution-processed organic films because of the weak van der Waals interaction between molecules30,31,32,33. According to Time–temperature equivalence principle, polymer chains can move more freely and eliminate internal stress at higher temperatures, which improves the \(\pi \)-conjugate delocalization and changes the twist angle of the adjacent rings by rearranging the chains to make them coplanar. At the same time, annealing has another effect, that is to improve the PLQY of MEH-PPV. After annealing, the PLQY of MEH-PPV rose from 22 to 35%.

(a) A schematic of polarized absorption; the polarized absorption spectra of (b) oriented and (c) spin-coating MEH-PPV film, respectively.

Figure 5(a) shows the emission intensity at 624 nm as a function of excitation stripe length for spin-coating and oriented MEH-PPV films. S-polarized light with an intensity of 3.5 kW/cm2 is used for pumping, and emission intensity satisfies the following Eq. 34.

where \(A(\lambda )\) represents a constant associated to spontaneous emission cross section, \(I_{P}\) denotes the pump intensity, \(g(\lambda )\) is the net gain coefficient, and \(l\) indicates the length of the pump stripe. The exponential subset of the corresponding data is fitted to the solid lines utilizing Eq. (1). For the spin coating sample, the gain coefficient was 45 cm−1. For the oriented sample, the gain coefficient was observed at 65.8 cm−1 (32.2 cm−1) when the polarization of the pump source was parallel to its orientation (perpendicular).

Dependence of the output intensity on the (a) pump length and (b) distance x between the sample edge and the pump stripe.

In order to further understand the waveguide losses of conjugated polymers, we conducted an experiment where we maintained a constant length for the pump stripe and shifted it farther from the edge of the samples. As demonstrated in Fig. 5(b), constant intensity is maintained by the emitted end of the pump stripe, while the ASE intensity should decrease in accordance with

where \(x\) denotes the distance in unpumped region from the edge of the sample to the end of the pump stripe, \(\alpha (\lambda )\) represents the absorption and scattering losses, and \(I_{0} (\lambda )\) is the intensity at the end of the pump stripe. We calculated the loss coefficient for the spin coating sample to be 8.7 cm−1 through fitting these data to Eq. (2). It is important to mention that when the polarization of the pump light was aligned either parallel or perpendicular to the orientation of the MEH-PPV film, the losses were measured to be 3.7 cm−1 and 5.2 cm−1, respectively. These were lower than the losses observed in the spin coating sample. This occurs because less scattering arises as a result of the neat arrangement of the chains caused by the molecular orientation of MEH-PPV.

Laser emission was produced by the device when it was optically pumped. The output lasing wavelength \(\lambda_{las}\) satisfies Bragg condition: \(m\lambda_{las} = 2n_{eff} \Lambda\), where \(n_{eff}\) is the effective RI, \(m\) denotes the Bragg order, which was specifically chosen as 2 for this study. The spectra at a 2 × threshold s-polarized pump energy is displayed in Fig. 6(a). The thickness of MEH-PPV is very thin, and the waveguide structure allows for only one mode of oscillation. As a result, the laser emitted from it is single mode. The laser beam was emitted perpendicular to the glass substrate, as depicted in the inset. The spin coating sample and the oriented sample emit laser with wavelength of 629.7 nm and 631.1 nm respectively regardless of whether it is pumped by s-polarized or p-polarized light. This is because the effective RI of the sample is independent of the polarization of the pump light.

(a) Output lasing spectra and (b) the variation of output laser intensity with polarization angle of polarizer for spin-coating and oriented DFB laser under s and p polarization pump light, respectively, the inset shows the vertical laser emission.

We analyzed the relationship between the polarization angle and the intensity of the three lasing peaks when the light passes through a linear polarizer (Fig. 6b). It is clear that the laser emitted from both spin coated and oriented samples is TE polarized. For TE polarized light, MEH-PPV layer has a RI of 1.90 at 630 nm, while for TM light, it is 1.5235. The inability to attain gain amplification in the TM mode is due to the fact that the RI of TM light in MEH-PPV layer is lower than that of the external grating substrate layer (1.54) and the glass substrate (1.516). For orientated samples, the main chain of the MEH-PPV polymer is parallel to the TE light, causing the TE light to have a higher RI, resulting in a larger \(n_{eff}\) and an increase in the wavelength of the produced laser. In addition, the alignment of LC in the grating caused by phase separation is along the y-axis, for TE polarized light, \(n_{e}\) of LC and the polymer contributes to the RI difference in the vector direction of the grating. At this time, the RI difference is maximum and the laser feedback performance is best. This is also the reason why we prepared the above-mentioned grating.

Keep the pump light path and the position of the sample unchanged, and rotate the polarizer to change the polarization of the pump light. Figure 7(a) shows the variation of laser energy emitted from spin coating sample with pump energy under different polarization pumping conditions. The straight line represents the linear fitting of the corresponding experimental data. when the pump light is p-polarized, the maximum threshold is 0.25 μJ/pulse, the corresponding minimum energy efficiency is 4.71%; When the pump light is polarized at 45°, the threshold is slightly lower at 0.22 μJ/pulse, the corresponding energy efficiency is relatively high at 5.75%. When the pump light is s-polarized, the minimum threshold is 0.17 μJ/pulse, the highest energy efficiency at this time is 6.30%. That is to say, with all device parameters being the same, simply changing the pump light from the p state to the s state can increase energy efficiency by approximately 38%.

Dependence of lasing output intensity on pump intensity for (a) the spin-coating DFB laser under different polarization pump light; (b) the oriented DFB laser under s and p polarization pump light.

Although the light absorption of spin coating sample is insensitive to polarization direction (Fig. 4c), when pumped with s light, molecules organized in the y direction are more excited, whereas molecules in other directions are less stimulated (Fig. 1c). The anisotropy of this excited state molecule results in enhanced TE directional polarization luminescence. As mentioned earlier, the feedback cavity only supports TE mode oscillation, which means the threshold of output lasing will be lower and energy efficiency will be higher. Similarly, p-polarized light raises the laser threshold and lowers energy efficiency. Because of the disordered distribution of luminous chains in the plane, even under S-polarized pumping, there are a substantial number of excited state molecules in other directions, resulting in a significant energy loss. Figure 7(b) shows that orienting MEH-PPV along the y-axis can further increase output lasing performance. S-polarized light pumped parallel to the orientation gives the MEH-PPV layer the most absorption and TE polarization gain. Meanwhile, TE polarized light can obtain the strongest feedback in the grating. Here, we can achieve an energy efficiency of 9.78% and lower the laser threshold to 0.12 μJ/pulse. The most inefficient operation occurs when the polarization of pump light is orthogonal (p-polarized light)to the orientation of MEH-PPV molecule. The current laser threshold is 0.28 μJ/pulse and the conversion efficiency is represented as 4.35%.

In conclusion, we have obtained a low threshold OSL based on HPDLC grating. We showed that the output lasing performance are strongly dependent on the excitation polarization, anisotropic arrangement of polymer chains and the orientation of LC molecules in HPDLC gratings. We analyzed the relationship between the layers of the laser, and the specific optimized configuration for low threshold was identified. The results indicate that the polymer chain orientation, LC molecules and pump light polarization all followed the direction of the grating grooves, resulting in the best laser output performance. Our research provides an effective choice for the fabrication of low threshold, highly efficient OSLs that may eventually allow for electrically driven.

The datasets used and/or analysed during the current study available from the corresponding author on reasonable request.

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This work was financially supported by the National Natural Science Foundation of China (NSFC) (grant numbers 62241505).

College of Electrical and Information Engineering, Quzhou University, Quzhou, 324000, China

Lijuan Liu, Hanmin Hu, Feng Zhang & Xiaobo Kong

Laser Institute, Qilu University of Technology (Shandong Academy of Sciences), Qingdao, 266000, China

Minzhe Liu

State Key Laboratory of Applied Optics, Fine Mechanics and Physics, Changchun Institute of Optics, Chinese Academy of Sciences, Changchun, 130033, China

Qidong Wang

School of Physics and Physical Engineering, Shandong Provincial Key Laboratory of Laser Polarization and Information Technology, Qufu Normal University, Qufu, 273165, China

Lijuan Liu

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Lijuan Liu: Methodology, Writing – original draft. Minzhe Liu: formal analysis, data curation. Qidong Wang: Validation, Methodology. Hanmin Hu: Data curation. Feng Zhang: Data curation. Xiaobo Kong: Writing – review & editing. All authors have read and agreed to the published version of the manuscript.

Correspondence to Xiaobo Kong.

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Liu, L., Liu, M., Wang, Q. et al. Low-threshold distributed feedback laser based on holographic polymer dispersed liquid crystals through the oriented organic semiconductor films. Sci Rep 14, 17790 (2024). https://doi.org/10.1038/s41598-024-68896-5

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Received: 03 April 2024

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DOI: https://doi.org/10.1038/s41598-024-68896-5

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