Abstract

We report on digitally printed distributed feedback lasers on flexible polyethylene terephthalate substrates based on methylammonium lead iodide perovskite gain material. The perovskite lasers are printed with a digital drop-on-demand inkjet printer, providing full freedom in the shape and design of the gain layer. We show that adjusting the perovskite ink increases the potential processing window and decreases the surface roughness of the active layer to less than 7 nm, which is essential for low lasing thresholds. Prototype inkjet-printed perovskite lasers processed on top of nanopatterned rigid as well as flexible substrates are demonstrated. Optimized perovskite gain layers printed on PET substrates demonstrated lasing and showed a linewidth of 0.4 nm and a lasing threshold of 270 kW/cm2. In addition, printing of a distinct shape shows a high level of uniformity, demonstrated by a low spatial resolved full width half maximum variation over the whole printing area. These results reveal the possibilities of digital printed perovskite layers towards large-scale and low-cost laser applications of arbitrary shape.

© 2018 Optical Society of America

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2017 (8)

A. S. D. Sandanayaka, T. Matsushima, F. Bencheikh, K. Yoshida, M. Inoue, T. Fujihara, K. Goushi, J.-C. Ribierre, and C. Adachi, “Toward continuous-wave operation of organic semiconductor lasers,” Sci. Adv. 3(4), e1602570 (2017).
[PubMed]

F. Fan, O. Voznyy, R. P. Sabatini, K. T. Bicanic, M. M. Adachi, J. R. McBride, K. R. Reid, Y.-S. Park, X. Li, A. Jain, R. Quintero-Bermudez, M. Saravanapavanantham, M. Liu, M. Korkusinski, P. Hawrylak, V. I. Klimov, S. J. Rosenthal, S. Hoogland, and E. H. Sargent, “Continuous-wave lasing in colloidal quantum dot solids enabled by facet-selective epitaxy,” Nature 544(7648), 75–79 (2017).
[PubMed]

S. Chen, C. Zhang, J. Lee, J. Han, and A. Nurmikko, “High-Q, Low-Threshold Monolithic Perovskite Thin-Film Vertical-Cavity Lasers,” Adv. Mater. 29(16), 1604781 (2017).
[PubMed]

N. Zhang, W. Sun, S. P. Rodrigues, K. Wang, Z. Gu, S. Wang, W. Cai, S. Xiao, and Q. Song, “Highly Reproducible Organometallic Halide Perovskite Microdevices based on Top-Down Lithography,” Adv. Mater. 29(15), 1606205 (2017).
[PubMed]

P. J. Cegielski, S. Neutzner, C. Porschatis, H. Lerch, J. Bolten, S. Suckow, A. R. S. Kandada, B. Chmielak, A. Petrozza, T. Wahlbrink, and A. L. Giesecke, “Integrated perovskite lasers on a silicon nitride waveguide platform by cost-effective high throughput fabrication,” Opt. Express 25(12), 13199–13206 (2017).
[PubMed]

P. Brenner, O. Bar-On, T. Siegle, T. Leonhard, R. Gvishi, C. Eschenbaum, H. Kalt, J. Scheuer, and U. Lemmer, “3D whispering-gallery-mode microlasers by direct laser writing and subsequent soft nanoimprint lithography,” Appl. Opt. 56(13), 3703–3708 (2017).
[PubMed]

N. Pourdavoud, S. Wang, A. Mayer, T. Hu, Y. Chen, A. Marianovich, W. Kowalsky, R. Heiderhoff, H. C. Scheer, and T. Riedl, “Photonic Nanostructures Patterned by Thermal Nanoimprint Directly into Organo-Metal Halide Perovskites,” Adv. Mater. 29(12), 1605003 (2017).
[PubMed]

P. Brenner, T. Glöckler, D. Rueda-Delgado, T. Abzieher, M. Jackoby, B. S. Richards, U. W. Paetzold, I. A. Howard, and U. Lemmer, “Triple cation mixed-halide perovskites for tunable lasers,” Opt. Mater. Express 11, 4082–4094 (2017).

2016 (8)

F. Liu, Q. Dong, M. K. Wong, A. B. Djurišić, A. Ng, Z. Ren, Q. Shen, C. Surya, W. K. Chan, J. Wang, A. M. C. Ng, C. Liao, H. Li, K. Shih, C. Wei, H. Su, and J. Dai, “Is Excess PbI2 Beneficial for Perovskite Solar Cell Performance?” Adv. Energy Mater. 6, 1–9 (2016).

F. Mathies, T. Abzieher, A. Hochstuhl, K. Glaser, A. Colsmann, U. W. Paetzold, G. Hernandez-Sosa, U. Lemmer, and A. Quintilla, “Multipass inkjet printed planar methylammonium lead iodide perovskite solar cells,” J. Mater. Chem. A Mater. Energy Sustain. 4, 19207–19213 (2016).

Y. Jia, R. A. Kerner, A. J. Grede, A. N. Brigeman, B. P. Rand, and N. C. Giebink, “Diode-pumped organo-lead halide perovskite lasing in a metal-clad distributed feedback resonator,” Nano Lett. 16(7), 4624–4629 (2016).
[PubMed]

P. Brenner, M. Stulz, D. Kapp, T. Abzieher, U. W. Paetzold, A. Quintilla, I. A. Howard, H. Kalt, and U. Lemmer, “Highly stable solution processed metal-halide perovskite lasers on nanoimprinted distributed feedback structures,” Appl. Phys. Lett. 109, 141106 (2016).

G. L. Whitworth, J. R. Harwell, D. N. Miller, G. J. Hedley, W. Zhang, H. J. Snaith, G. A. Turnbull, and I. D. W. Samuel, “Nanoimprinted distributed feedback lasers of solution processed hybrid perovskites,” Opt. Express 24(21), 23677–23684 (2016).
[PubMed]

B. R. Sutherland and E. H. Sargent, “Perovskite photonic sources,” Nat. Photonics 10, 295–302 (2016).

G. Li, M. Price, and F. Deschler, “Research Update: Challenges for high-efficiency hybrid lead-halide perovskite LEDs and the path towards electrically pumped lasing,” APL Mater. 4, 91507 (2016).

A. J. C. Kuehne and M. C. Gather, “Organic Lasers: Recent Developments on Materials, Device Geometries, and Fabrication Techniques,” Chem. Rev. 116(21), 12823–12864 (2016).
[PubMed]

2015 (6)

P. Brenner, L. M. Fleig, X. Liu, A. Welle, S. Bräse, and U. Lemmer, “Degradation mechanisms of polyfluorene-based organic semiconductor lasers under ambient and oxygen-free conditions,” J. Polym. Sci. Part B Polym. Phys. 53, 1029–1034 (2015).

S. Yakunin, L. Protesescu, F. Krieg, M. I. Bodnarchuk, G. Nedelcu, M. Humer, G. De Luca, M. Fiebig, W. Heiss, and M. V. Kovalenko, “Low-threshold amplified spontaneous emission and lasing from colloidal nanocrystals of caesium lead halide perovskites,” Nat. Commun. 6, 8056 (2015).
[PubMed]

L. Qin, L. Lv, Y. Ning, C. Li, Q. Lu, L. Zhu, Y. Hu, Z. Lou, F. Teng, and Y. Hou, “Enhanced amplified spontaneous emission from morphology-controlled organic–inorganic halide perovskite films,” RSC Advances 5, 103674 (2015).

Q. Xia and R. F. Pease, “Nanoimprint lithography 20 years on,” Nanotechnology 26(18), 182501 (2015).
[PubMed]

U. W. Paetzold, W. Qiu, F. Finger, J. Poortmans, and D. Cheyns, “Nanophotonic front electrodes for perovskite solar cells,” Appl. Phys. Lett. 106, 173101 (2015).

P. Löper, M. Stuckelberger, B. Niesen, J. Werner, M. Filipič, S.-J. Moon, J.-H. Yum, M. Topič, S. De Wolf, and C. Ballif, “Complex Refractive Index Spectra of CH3NH3PbI3 Perovskite Thin Films Determined by Spectroscopic Ellipsometry and Spectrophotometry,” J. Phys. Chem. Lett. 6(1), 66–71 (2015).
[PubMed]

2014 (6)

N. J. Jeon, J. H. Noh, Y. C. Kim, W. S. Yang, S. Ryu, and S. I. Seok, “Solvent engineering for high-performance inorganic-organic hybrid perovskite solar cells,” Nat. Mater. 13(9), 897–903 (2014).
[PubMed]

S. Z. Bisri, T. Takenobu, and Y. Iwasa, “The pursuit of electrically-driven organic semiconductor lasers,” J. Mater. Chem. C Mater. Opt. Electron. Devices 2, 2827 (2014).

G. Xing, N. Mathews, S. S. Lim, N. Yantara, X. Liu, D. Sabba, M. Grätzel, S. Mhaisalkar, and T. C. Sum, “Low-temperature solution-processed wavelength-tunable perovskites for lasing,” Nat. Mater. 13(5), 476–480 (2014).
[PubMed]

F. Deschler, M. Price, S. Pathak, L. E. Klintberg, D. D. Jarausch, R. Higler, S. Hüttner, T. Leijtens, S. D. Stranks, H. J. Snaith, M. Atatüre, R. T. Phillips, and R. H. Friend, “High Photoluminescence Efficiency and Optically Pumped Lasing in Solution-Processed Mixed Halide Perovskite Semiconductors,” J. Phys. Chem. Lett. 5(8), 1421–1426 (2014).
[PubMed]

R. Dhanker, A. N. Brigeman, A. V. Larsen, R. J. Stewart, J. B. Asbury, and N. C. Giebink, “Random lasing in organo-lead halide perovskite microcrystal networks,” Appl. Phys. Lett. 105, 151112 (2014).

Q. Zhang, S. T. Ha, X. Liu, T. C. Sum, and Q. Xiong, “Room-Temperature Near-Infrared High-Q Perovskite Whispering-Gallery Planar Nano lasers,” Nano Lett. 14(10), 5995–6001 (2014).
[PubMed]

2013 (1)

2012 (1)

S. Chénais and S. Forget, “Recent advances in solid-state organic lasers,” Polym. Int. 61, 390–406 (2012).

2011 (1)

2010 (1)

J. Clark and G. Lanzani, “Organic photonics for communications,” Nat. Photonics 4, 438–446 (2010).

2009 (2)

S. H. Ahn and L. J. Guo, “Large-Area Roll-to-Roll and Roll-to-Plate Nanoimprint Lithography: A Step toward High-Throughput Application of Continuous Nanoimprinting,” ACS Nano 3(8), 2304–2310 (2009).
[PubMed]

I. D. W. Samuel, E. B. Namdas, and G. A. Turnbull, “How to recognize lasing,” Nat. Photonics 3, 546–549 (2009).

2005 (1)

A. Rose, Z. Zhu, C. F. Madigan, T. M. Swager, and V. Bulović, “Sensitivity gains in chemosensing by lasing action in organic polymers,” Nature 434(7035), 876–879 (2005).
[PubMed]

2002 (1)

H.-J. Eisler, V. C. Sundar, M. G. Bawendi, M. Walsh, H. I. Smith, and V. Klimov, “Color-selective semiconductor nanocrystal laser,” Appl. Phys. Lett. 80, 4614–4616 (2002).

2000 (1)

B. Hu and W. C. Chew, “Fast inhomogeneous plane wave algorithm for electromagnetic solutions in layered medium structures: Two-dimensional case,” Radio Sci. 35, 31–43 (2000).

1997 (1)

W. Plass, R. Maestle, K. Wittig, A. Voss, and A. Giesen, “High-resolution knife-edge laser beam profiling,” Opt. Commun. 134, 21–24 (1997).

1996 (1)

N. Tessler, G. J. Denton, and R. H. Friend, “Lasing from conjugated-polymer microcavities,” Nature 382, 695–697 (1996).

Abzieher, T.

P. Brenner, T. Glöckler, D. Rueda-Delgado, T. Abzieher, M. Jackoby, B. S. Richards, U. W. Paetzold, I. A. Howard, and U. Lemmer, “Triple cation mixed-halide perovskites for tunable lasers,” Opt. Mater. Express 11, 4082–4094 (2017).

P. Brenner, M. Stulz, D. Kapp, T. Abzieher, U. W. Paetzold, A. Quintilla, I. A. Howard, H. Kalt, and U. Lemmer, “Highly stable solution processed metal-halide perovskite lasers on nanoimprinted distributed feedback structures,” Appl. Phys. Lett. 109, 141106 (2016).

F. Mathies, T. Abzieher, A. Hochstuhl, K. Glaser, A. Colsmann, U. W. Paetzold, G. Hernandez-Sosa, U. Lemmer, and A. Quintilla, “Multipass inkjet printed planar methylammonium lead iodide perovskite solar cells,” J. Mater. Chem. A Mater. Energy Sustain. 4, 19207–19213 (2016).

Adachi, C.

A. S. D. Sandanayaka, T. Matsushima, F. Bencheikh, K. Yoshida, M. Inoue, T. Fujihara, K. Goushi, J.-C. Ribierre, and C. Adachi, “Toward continuous-wave operation of organic semiconductor lasers,” Sci. Adv. 3(4), e1602570 (2017).
[PubMed]

Adachi, M. M.

F. Fan, O. Voznyy, R. P. Sabatini, K. T. Bicanic, M. M. Adachi, J. R. McBride, K. R. Reid, Y.-S. Park, X. Li, A. Jain, R. Quintero-Bermudez, M. Saravanapavanantham, M. Liu, M. Korkusinski, P. Hawrylak, V. I. Klimov, S. J. Rosenthal, S. Hoogland, and E. H. Sargent, “Continuous-wave lasing in colloidal quantum dot solids enabled by facet-selective epitaxy,” Nature 544(7648), 75–79 (2017).
[PubMed]

Ahn, S. H.

S. H. Ahn and L. J. Guo, “Large-Area Roll-to-Roll and Roll-to-Plate Nanoimprint Lithography: A Step toward High-Throughput Application of Continuous Nanoimprinting,” ACS Nano 3(8), 2304–2310 (2009).
[PubMed]

Asbury, J. B.

R. Dhanker, A. N. Brigeman, A. V. Larsen, R. J. Stewart, J. B. Asbury, and N. C. Giebink, “Random lasing in organo-lead halide perovskite microcrystal networks,” Appl. Phys. Lett. 105, 151112 (2014).

Atatüre, M.

F. Deschler, M. Price, S. Pathak, L. E. Klintberg, D. D. Jarausch, R. Higler, S. Hüttner, T. Leijtens, S. D. Stranks, H. J. Snaith, M. Atatüre, R. T. Phillips, and R. H. Friend, “High Photoluminescence Efficiency and Optically Pumped Lasing in Solution-Processed Mixed Halide Perovskite Semiconductors,” J. Phys. Chem. Lett. 5(8), 1421–1426 (2014).
[PubMed]

Ballif, C.

P. Löper, M. Stuckelberger, B. Niesen, J. Werner, M. Filipič, S.-J. Moon, J.-H. Yum, M. Topič, S. De Wolf, and C. Ballif, “Complex Refractive Index Spectra of CH3NH3PbI3 Perovskite Thin Films Determined by Spectroscopic Ellipsometry and Spectrophotometry,” J. Phys. Chem. Lett. 6(1), 66–71 (2015).
[PubMed]

Bar-On, O.

Bawendi, M. G.

H.-J. Eisler, V. C. Sundar, M. G. Bawendi, M. Walsh, H. I. Smith, and V. Klimov, “Color-selective semiconductor nanocrystal laser,” Appl. Phys. Lett. 80, 4614–4616 (2002).

Bencheikh, F.

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Figures (6)

Fig. 1
Fig. 1 (a) Schematic of the replication and the inkjet printing process. The grating period was 380 nm and a grating height z of 80 nm was used. Drop diameter ~80 µm are indicated. (b) Photography of a Flexible PET foil with the nanoimprinted pattern. (c) Image of a perovskite layer on PET structured as the logo of our university.
Fig. 2
Fig. 2 (a) Surface roughness of printed CH3NH3PbI3 inks on rigid glass substrate in dependency of ink concentration, ink composition and vacuum drying time calculated from white light interferometer images (b) shows corresponding atomic force microscopy images of CH3NH3PbI3 underlining the improved process control for low surface roughness of polycrystalline perovskite films. Values on the bottom left are the extracted root mean square (rms) values.
Fig. 3
Fig. 3 Inkjet-printed CH3NH3PbI3 laser on a flexible PET substrate with nanoimprinted grating and planar regions. (a) Photoluminescence, amplified spontaneous emission (on planar regions) and lasing (on structured regions) spectra. (b) Emission intensity at the peak wavelength as a function of the pump laser pulse fluence. The lasing threshold is 270 kW/cm2. The lasing threshold of an inkjet-printed gain layer on top of a rigid SiO2 layer shows a similar threshold of 235 kW/cm2. (c) High resolution spectrum of the laser peak on a grating with 380 nm period, showing a full width at half maximum of only 0.4 nm. (d) Signal strength detected for lasing emission as a function of the rotation angle of a linear polarizer placed between the sample and detector.
Fig. 4
Fig. 4 (a) Spatially resolved full width at half maximum (FWHM) of an inkjet-printed KIT-Logo on a glass substrate. Photoluminescence is seen between 10 and 50 nm (blue to green). Amplified spontaneous emission below 10 nm (dark blue). (b) Normalized intensity distribution of the printed layer. Red indicates high intensities with strong ASE signal. (c) Large area white light interferometer image stitched together from 72 single images. Layer is inhomogeneous at the edges of the printed areas is attributed to the coffee-ring-effect.
Fig. 5
Fig. 5 Atomic force microscopy images of CH3NH3PbI3 on electron-beam structured SiO2 grating and on Nanoimprinted OrmoComp® substrate respectively. The calculated rms values are 27 nm on SiO2 and 32 nm on PET, using a 1.4M CH3NH3PbI3 ink and a 180s vacuum annealing step.
Fig. 6
Fig. 6 Emission intensity stability of the inkjet-printed CH3NH3PbI3 laser on a flexible PET substrate with a nanoimprinted grating in N2 atmosphere. The intensity drops to half of its initial value after 0.7 x 107 pulses. The samples were excited with a repetition rate of 5 kHz and an excitation density of 480 kW/cm2.

Equations (1)

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λ l a s i n g   λ b r a g g =   2 Λ n e f f m

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