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Zigzag edged nanographenes such as peri-acenoacenes are promising materials for organic lasers, but the effects of heteroatom doping on the electronic properties and gain medium performance remain unclear. Herein, the facile synthesis of a new 1,2-oxaborine (BO) doped peri-tetracenotetracene derivative, the bis(1,2-oxaborine)peri-tetracenotetracene (BOTT-Mes), is reported. X-ray crystallographic analysis confirms the BO-doped planar structure and the nonexistence of intermolecular π–π stacking in solid state. Compared with the all-carbon peri-tetracenotetracene derivative (TT-Ar), the BO-doped BOTT-Mes exhibits more disrupted π-conjugation at the BO sites, a lower-lying highest occupied molecular orbital, and a larger energy gap. Due to its rigid skeleton and nonaggregative feature, it displays well-resolved absorption and emission spectra with a small Stokes shift (8 nm) and high photoluminescence quantum yield (80%) when it is dispersed in a polystyrene (PS) thin film. Notably, 1,2-oxaborine doping improves the film amplified spontaneous emission (ASE) performance, with a lower ASE threshold (Eth-ASE = 66 µJ cm–2) as compared to the TT-Ar doped PS film (Eth-ASE = 100 µJ cm–2). Furthermore, a low threshold (22 µJ cm–2) solution-processed distributed feedback laser is fabricated, indicating the feasibility of using BOTT-Mes as gain medium for practical laser applications. J.W. acknowledges financial support from A*STAR Advanced Manufacturing and Engineering grant (A20E5c0089) and National Research Foundation Investigatorship Award (NRF-NRFI05-2019-0005). The group at the University of Alicante acknowledges financial support from the “Ministerio de Ciencia e Innovación” of Spain, European Regional Development Fund and European Social Funds (PID2019-106114GB-I00 and BES-2016-077681) and from the Conselleria de Innovación, Universidades y Sociedad Digital de la Comunidad Valenciana (Grant No. AICO/2021/093).

A naphtho[2,1-b:6,5-b′]difuran derivative was found to serve as an effective violet-emitting laser dye. It showed amplified spontaneous emission at 413 nm with the threshold of 1.1–2.9 mJ cm−2 using 0.1–0.5 wt% in polystyrene film. Lasing was also demonstrated using all-polymeric distributed-feedback lasers emitting at 411–417 nm with the threshold of 2.0–2.9 mJ cm−2. This work was supported by JSPS KAKENHI grant JP19H05716 (to H. T.) and by the “Ministerio de Ciencia, Innovación y Universidades” of Spain, via grants MAT2015-66586-R and PID2020-119124RB-I00 and by the “Generalitat Valenciana” through grant AICO/2021/093.

The molecule N,N′-bis(3-methylphenyl)-N,N′-dyphenylbenzidine (TPD) has been widely used in optoelectronic applications, mainly for its hole-transporting properties, but also for its capability to emit blue light and amplified spontaneous emission, which is important for the development of organic lasers. Here, we report deep-blue-emitting distributed feedback (DFB) lasers based on TPD dispersed in polystyrene (PS), as active media, and dichromated gelatin layers with holographically engraved relief gratings, as laser resonators. The effect of the device architecture (with the resonator located below or on top of the active layer) is investigated with a dye (TPD) that can be doped into PS at higher rates (up to 60 wt%), than with previously used dyes (&lt, 5 wt%). This has enabled changing the index contrast between film and resonator, which has an important effect on the laser performance. With regards to thresholds, both architectures behave similarly for TPD concentrations above 20 wt%, while for lower concentrations, top-layer resonator devices show lower values (around half). Remarkably, the operational durability of top-layer resonator devices is larger (in a factor of around 2), independently of the TPD concentration. This is a consequence of the protection offered by the resonator against dye photo-oxidation when the device is illuminated with pulsed UV light.

High-transparency polymers, called optical polymers (OPs), are used in many thin-film devices, for which the knowledge of film thickness (h) and refractive index (n) is generally required. Spectrophotometry is a cost-effective, simple and fast non-destructive method often used to determine these parameters simultaneously, but its application is limited to films where h > 500 nm. Here, a simple spectrophotometric method is reported to obtain simultaneously the n and h of a sub-micron OP film (down to values of a few tenths of a nm) from its transmission spectrum. The method is valid for any OP where the n dispersion curve follows a two-coefficient Cauchy function and complies with a certain equation involving n at two different wavelengths. Remarkably, such an equation is determined through the analysis of n data for a wide set of commercial OPs, and its general validity is demonstrated. Films of various OPs (pristine or doped with fluorescent compounds), typically used in applications such as thin-film organic lasers, are prepared, and n and h are simultaneously determined with the proposed procedure. The success of the method is confirmed with variable-angle spectroscopic ellipsometry. Spanish Ministry of Economy and Competitivity (MINECO) and European Community (FEDER) through grant no. MAT2015-66586-R.

The search of compounds emitting in the near-infrared (NIR) has been accelerated owing to their use in biomedical and telecommunications applications. In this regard, nanographenes (NGs) are attractive materials adequate for integration with other technologies, which have recently demonstrated amplified spontaneous emission (ASE) and lasing across the visible spectrum. Here, the optical and ASE properties of four-zigzag edged NGs of the [m,n]peri-acenoacene family are reported, whose size is increased through conjugation extension by varying n (from 3 to 5) while keeping m = 2. Results show that such 1D conjugation extension method is more efficient in terms of shifting the photoluminescence (PL) to the infrared (PL at 710 nm in the larger compound, PP-Ar) than through 2D conjugation extension as in previously reported NGs (PL at 676 nm with the largest compound FZ3, with n = 3 and m = 4). Additionally, PP-Ar shows dual-ASE (at 726 and 787 nm), whose origin is elucidated through Raman and transient absorption spectroscopies. These compounds’ potential for red and NIR lasing is demonstrated through the fabrication of distributed feedback lasers with top-layer resonators. This study paves the way towards the development of stable low-cost all-plastic NIR lasers. The authors acknowledge financial support from the “Ministerio de Ciencia, Innovación y Universidades” of Spain, European Regional Development Fund and European Social Funds (MAT2015-66586-R, PDI2019-106114GB-I00, BES-2016-077681, PGC2018-098533-B-100 and RED2018-102815-T). J.C. thanks the Junta de Andalucía of Spain (UMA18FEDERJA057). The authors also thank the Research Central Services (SCAI) of the University of Málaga. F.G. acknowledges the Spanish Government for an FPI grant. G.M.P. thanks Fondazione Cariplo (grant no 2018-0979) for the financial support. J.W. acknowledges the “Agency for Science, Technology and Research of Singapore” for financial support from A*STAR AME grant (A20E5c0089). A.M.R. and F.S. have received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (grant agreement No. [816313]).

All‐solution processed surface‐emitting organic distributed feedback lasers are attractive devices for low‐cost applications. Here, lasers emitting in the spectral region between 375 and 475 nm, in which both active material and resonator (1D relief gratings) are based on solution‐processable polymer films, are reported. Ten different organic compounds dispersed in polystyrene are used as active layers of the prepared devices. They include various carbon‐bridged oligo(p‐phenylenevinylene) (COPVn, with n = 1,2) derivatives and two terfluorene compounds. The synthesis and complete optical and amplified spontaneous emission properties of one of the COPV1 compounds, COPV1(Me)‐t‐Bu, designed for deep‐blue emission, are also included. The feasibility of the resonator fabrication, performed by holographic lithography with a dichromated gelatine photoresist over the active film, is successfully demonstrated for all devices. Remarkably, no resolution limitations are found even for the lowest grating period (235 nm) required for the fabrication of the laser based on COPV1(Me)‐t‐Bu. It is also demonstrated that the rectangular grating profile with duty cycle 0.75:0.25 (hill:valley) is very convenient to optimize the resonator efficacy. The Spanish team acknowledges support from the Spanish Government (MINECO) and the European Community (FEDER) through Grant No. MAT2015-66586-R. H.T. and E.N. thank the financial support from MEXT (JP19H05716 for H.T. and JP19H0549 for E.N.).

Surface-emitting distributed feedback (DFB) lasers with both, resonator and active material based on solution-processable polymers, are attractive light sources for a variety of low-cost applications. Besides, the lasers should have competitive characteristics compared to devices based on high-quality inorganic resonators. Here, we report high performing all-solution-processed organic DFB lasers, consisting of water-processed photoresist layers with surface relief gratings located over the active films, whose emission properties can be finely tuned through resonator design. Their laser threshold and efficiency are simultaneously optimized by proper selection of residual resist thickness and grating depth, d. Lowest thresholds and largest efficiencies are obtained when there is no residual layer, while a trade-off between threshold and efficiency is found in relation to d, because both parameters decrease with decreasing d. This behaviour is successfully explained in terms of an overlap factor r, defined to quantify the interaction strength between the grating and the light emitted by the active film and traveling along it, via the evanescent field. It is found that optimal grating depths are in the range 100–130 nm (r ~ 0.5−0.4). Overall, this study provides comprehensive design rules towards an accurate control of the emission properties of the reported lasers.

The design, synthesis and evaluation of the amplified spontaneous emission (ASE) properties of a series of arylalkynyl-benzo[c][1,2,5]thiadiazole (BTD) and [1,2,5]thiadiazolo[3,4-g]quinoxaline (TDQ) derivatives are described. The synthetic strategy entailed the use of Sonogashira and Stille reactions based on the different aromatic natures of the two cores. The ASE properties were measured in thin polystyrene (PS) films doped with different concentrations of the synthesised compounds. BTD derivatives showed narrowing of the photoluminescence spectra (PL), thus revealing their potential laser applications. Only one TDQ derivative showed ASE. X-ray diffraction analysis was carried out to understand the observed results and to establish structure–property relationships. Molecules that showed strong molecular packing quenched the PL emission, thus giving rise to higher ASE thresholds. This is the first study in which ASE has been studied in BTD and TDQ derivatives and it represents a step forward in understanding this class of compounds for laser applications. The Alicante team acknowledges support from Ministerio de Ciencia, Innovación y Universidades, Spain, under projects MAT2015-66586-R (MINECO/FEDER), FIS2017-82919-R (MINECO/AEI/FEDER,UE) and FIS2015-66570-P (MINECO/FEDER). The authors acknowledge financial support from the Junta de Comunidades de Castilla-La Mancha (JCCM-FEDER) (project SBPLY/17/180501/000189), the Spanish Ministry of Economy and Competitiveness (CTQ2013-45415P) and Gobierno Vasco-Eusko Jaularitza (IT-673-13). R. Martı´n is grateful to the MEC for an FPU studentship.

Two-dimensional (2D) distributed feedback (DFB) lasers with gratings imprinted by thermal nanoimprint lithography on the active film are reported. They show thresholds for lasing of ∼10 kW/cm2, similar to the most efficient imprinted DFB lasers reported; and long operational lifetimes (under ambient conditions) of ∼12 × 104 pump pulses. The key for their successful operation has been the selection of a highly efficient and stable dye, perylene orange (PDI-O), and a proper matrix to host it, the fluoro-modified thermoplastic resist mr-I7030R, which has enabled 2D imprinting while preserving the dye optical properties. The use of the UV-curable resist SU8 as an alternative matrix for PDI-O to be imprinted by combined nanoimprint and photolithography was also investigated, and was concluded to be unsuccessful due to severe photoluminescence quenching. By replacing PDI-O with Rhodamine 6G, lasers with reasonable thresholds, but with significantly inferior operational lifetimes in comparison to PDI-O/mr-I7030R devices, were obtained., We thank support from the Spanish Government (MINECO) and the European Community (FEDER) through Grants MAT2011-28167-C02 and MAT2015-66586-R, as well as to the University of Alicante. M.M-V. has been partly supported by a MINECO FPI fellowship (no. BES-2009-020747) and by a Junta de Castilla y León grant (no. SA046U16).

Amplified spontaneous emission (ASE) in dye-doped mesostructured silica films, deposited directly over fused silica substrates, is demonstrated with low thresholds. Due to functionalization of the silica network with phenyl groups, the refractive index of the active layer is sufficiently increased to impart waveguiding properties that lead to highly efficient ASE. Such functionalization eliminates the need for a separate low-refractive-index layer between the active film and the substrate, as is often used to achieve waveguiding properties with silica mesostructured materials, though which is typically accompanied by significant optical losses that reduce overall ASE performance. By forming a high-quality waveguide without the need for a separate low-refractive-index layer, significantly improved properties are obtained, with ASE thresholds as low as 8 kW cm−2. Solid-state 2D NMR spectroscopy measurements establish the compositions and structures of the active mesostructured film at a molecular level, in particular that phenyl functionalization of the mesochannel surfaces promotes the homogeneous dispersion of the laser dye species over nanoscale dimensions in the materials. The authors thank support from the Spanish Government through the “Ministerio de Economía y Competitividad” (MINECO) and the European Community (FEDER) through grant nos. MAT2008–06648-C02 and MAT2011–28167-C02. M.G.R. has been supported by a CSIC fellowship within the program JAE. M.A.D.G. acknowledges funding received from the “Ministerio de Educación y Ciencia, MEC” (reference no. PR2009–0456) to perform a research stay at UCSB to initiate the collaboration between the two teams contributing to this work. M.J.N.J. acknowledges financial support from the Alexander von Humboldt-Foundation through a Feodor Lynen Research Fellowship. The NMR experiments were conducted in the Central Facilities of the UCSB Materials Research Laboratory supported by the MRSEC program of the U.S. NSF under award no. DMR-1121053. The work at UCSB was supported by the USARO through the Institute for Collaborative Biotechnologies through W911NF-09-D-0001.

Thin film organic lasers represent a new generation of inexpensive, mechanically flexible devices for spectroscopy, optical communications and sensing. For this purpose, it is desired to develop highly efficient, stable, wavelength-tunable and solution-processable organic laser materials. Here we report that carbon-bridged oligo(p-phenylenevinylene)s serve as optimal materials combining all these properties simultaneously at the level required for applications by demonstrating amplified spontaneous emission and distributed feedback laser devices. A series of six compounds, with the repeating unit from 1 to 6, doped into polystyrene films undergo amplified spontaneous emission from 385 to 585 nm with remarkably low threshold and high net gain coefficients, as well as high photostability. The fabricated lasers show narrow linewidth (105 pump pulses for oligomers with three to six repeating units) and wavelength tunability across the visible spectrum (408–591 nm)., Thin film organic solid-state lasers are low-cost flexible devices which require efficient, stable, colour-tunable, solution-processable materials. Here, the authors show that oligo(p-phenylenevinylene)s simultaneously possess all such properties, as demonstrated by their use in laser devices.

The refractive index sensing capabilitity of distributed feedback (DFB) lasers based on highly photostable (under ambient conditions) perylenediimide-based active films, are reported. The sensor bulk sensitivity is determined from changes in the laser emission wavelength upon exposure to different liquids. The role of the active film thickness (hf) on the sensor sensitivity and on the laser parameters is studied. Sensors based on very thin films (hf = 160 nm) show the highest sensitivities, but their laser thresholds are relatively high and their operational durabilities moderate. The use of thicker films (hf = 850 nm) allows reducing the laser threshold and increasing the durability by two orders of magnitude. In this case, a higher sensitivity is achieved when the sensor operates at the wavelength corresponding to the first-order TE1 mode, instead of at the TE0 one. Finally, it is also shown that the inclusion of a high refractive index TiO2 layer on top of the sensor structure improves the sensitivity by around two times. This work was supported by the Spanish Government (MINECO) and the European Community (FEDER) through grant no. MAT-2011–28167-C02. This work was partially funded by the Basque Government within the framework of the Etortek Program (Grant No. IE13-360). M. Morales-Vidal has been partly supported by a MINECO FPI fellowship (no. BES-2009-020747).

Thin film organic lasers (TFOLs) represent a new generation of inexpensive, mechanically flexible devices with demonstrated applicability in numerous applications in the fields of spectroscopy, optical communications and sensing requiring an organic, efficient, stable, wavelength-tunable and solution-processable laser material. A distributed feedback (DFB) laser is a particularly attractive TFOL because it shows single mode emission, low pump energy, easy integration with other devices, mechanical flexibility and potentially low production cost. Here, amplified spontaneous emission (ASE) and DFB laser applications of novel high performing perylene dyes and p-phenylenevinylene (PV) oligomers, both dispersed in thermoplastic polymers, used as passive matrixes, are reported. Second-order DFB lasers based on these materials show single mode emission, wavelength tunability across the visible spectrum, operational lifetimes of >105 pump pulses, larger than previously reported PV oligomers or polymers, and thresholds close to pumping requirements with light-emitting diodes. This work was supported by the Spanish Government (MINECO) and the European Community (FEDER) through grant no. MAT-2011–28167-C02. M. Morales-Vidal has been partly supported by a MINECO FPI fellowship (no. BES-2009-020747).

Amplified spontaneous emission sASEd in optically pumped polystyrene sPSd films doped with two different oligo-sp-phenylenevinylened derivatives sOPVsd, with three s3-OPVd and five s5-OPVd monomer units is reported. It is observed that there is a maximum content of oligomer s25 wt. % for 3-OPV and 20 wt. % for 5-OPVd that can be introduced in the films, due to degradation sin 3-OPVd and ASE quenching sin 5-OPVd. Optimal concentrations swith minimum pump-intensity thresholds for the observation of ASEd of 15 wt. % and 9 wt. % are measured for the trimer and the pentamer, respectively. The concentration dependence of the ASE threshold is discussed in terms of the optical absorption spectra. Gain coefficients are obtained by analyzing the dependence of the ASE with the length of the pump stripe. The results show that films based on 5-OPV appear to be more efficient and stable than those based on 3-OPV