MB2.3 (Invited) 11:30 AM – 11:00 AM Red, Green, and Blue Colloidal Quantum Dot-based Optically Pumped Distributed Feedback Lasers Kwangdong Roh1, Joonhee Lee1, Cuong Dang1, Craig Breen2, Jonathan S. Steckel2, Seth Coe-Sullivan2, and Arto Nurmikko1* 1 School of Engineering, Brown University, Providence, Rhode Island 02912, USA 2 QD Vision Inc., 29 Hartwell Ave., Lexington, Massachusetts 02421, USA Tel: +1 (401) 863-2869; Fax: +1 (401) 863-1387; Email: Arto_Nurmikko@Brown.edu Abstract— Red, green and blue distributed feedback lasers based on dense colloidal CdSe quantum dot thin films were optically pumped in quasi-steady state. The red lasers showed 32% internal quantum efficiency and 400 µW output power. film are main consideration for the design and optimization of the resonant DFB structures. Index Terms – Colloidal quantum dot, RGB, Single exciton gain, DFB lasers, Steady-state I. INTRODUCTION Advanced colloidal synthesis methods are producing colloidal quantum dots (CQD) as high efficient fluorescent materials covering full-visible spectrum for many applications such as solid state lighting [1] and display [2]. High performance projection displays will benefit from full color, high intensity coherent emitters which currently require at least three different materials with distinct technologies. CQDs are emerging as a potential nanomaterial for full color, single material lasers. By enabling single exciton gain mechanism [3] in CdSe/ZnCdS core/shell CQD films, we recently solved the major obstacle of nonradiative multiexciton Auger recombination [4] while maintaining the high quantum efficiency, optical oscilation strength of type-I CQDs. The first CQD vertical cavity surface emitting lasers demonstrated the high performance level of the CQD gain media. Here, we present a major step toward red, green and blue (RGB), practical CQD lasers for high performance display applications. The RGB distributed feedback (DFB) lasers with a compact, quasi-continuous optical pump source and crisp collimated laser beam outputs are demonstrated with this new type CQD gain media. Fig. 1: Configuration of the second order CQD-DFB lasers. (a) Schematic of a CQD-DFB laser in which a densely-packed solid CQD film is deposited on second order quartz gratings. The pump beam direction is vertical (i.e. perpendicular to grating plane). The second order diffraction provides in-plane feedback for the CQD optical gain media while the first order diffraction provides two output coupling channels for the laser, each vertical (perpendicular) to the grating surface. (b) Cross-sectional SEM image of a quartz grating with a pitch of 400 nm. (c) An angled view of a complete CQD-DFB laser structure under SEM. The CQD-DFB structures were pumped through a cylindrical lens in stripe excitation configuration (perpendicularly oriented to the grating grooves). Fig. 2a-f present close-up images of excitation stripe for RGB lasers with pumping levels are below and above threshold, respectively. These visually demonstrate threshold behavior of laser action in CQD-DFB structures whereupon a bright center area suddenly appears on a uniform photoluminescent stripe when increase pumping intensity. The intensity of laser outputs as a function of pumping level in Fig. 2g shows well defined laser threshold for all CQD-DFB lasers. The thresholds are 250 μJ/cm2, 290 μJ/cm2 and 350 μJ/cm2 for the RGB CQD-DFB lasers, respectively. These values present significant reduction from comparison cavityless laser (ASE), as expected for the low loss, resonant high Q cavity of the DFB structures. The spectra of these CQDDFB lasers in the inset of Fig. 2g clearly show the single mode, narrow laser lines. Optimizing DFB gratings to match the optical gain peak (ASE spectra) need to be done carefully to achieve high performance lasers. Unlike earlier CQD (red) laser demonstrations with ultrashort pulse/powerful pump lasers in the literature, our pumping source employed a double frequency (532 nm for red laser) II. EXPERIMENTS AND RESULTS The CQD-DFB lasers were fabricated by spin casting an extra high concentration CQD solution on second order quartz gratings which were designed and made by either holographic interference lithography (adequate for red lasers) or focused ion beam milling (to reach the green and blue). The second order gratings ease the fabrication process (double pitch of first order gratings). The square profile of a typical quartz grating achieved by inductive plasma coupling reactive ion etching technique is shown in cross-sectional scanning electron microscopy image (Fig. 1b). Fig. 1c shows a complete CQD-DFB structure, where an epitaxial like CQD layer conformally covers the grating and also forms an optically smooth top surface. A spin cast film on planar surface showed a densely packed structure with effective refractive index of 1.75-1.8, which implies a filling factor of 50%. This refractive index and the gain spectra of the CQD 978-1-4577-1507-5/13/$26.00 ©2013 IEEE 22 and triple frequency (355 nm for green and blue lasers) from a compact, sub-nanosecond, solid state laser (1064 nm, 1 kHz, PowerChip laser from Teem Photonics). The full width at half maximum of the optical pump pulse is 270 ps, which is 2.25 times longer than perennially inhibitive non-radiative multiexciton Auger recombination (Au = 120 ps), thus enabling access to quasi-steady state regime. This highlights the role of single exciton mechanism for optical gain of our densely packed CQD thin film as elucidated in Ref [3]. performance of the red CQD-DFB lasers is somewhat similar to that of e.g. semiconductor laser pointers in term of power, collimation, and efficiency. Fig. 2: Performance of quasi-steady state CQD-DFB laser. a-f) Micro-photograph images of pumped stripe (400 μm) on the RGB CQD-DFB lasers with below and above threshold pump levels, respectively. e) RGB laser intensities as a function of pump pulse energy density. (Inset) Single mode RGB laser spectra. Fig. 3: Photographic images of RGB quasi-steady state CQD-DFB lasers. a) Direct, vertical blue-laser output on the remote screen with blue CQD photoluminescence background. b) Top view of a red laser beam under bright room light. c-d) Red and green well collimated CQD-DFB laser beams on remote screens when using the second cylindrical lens for collimation. Fig. 3 shows spatially coherent outputs of the RGB CQDDFB lasers where filters were used to remove residue pump laser. Well-defined beams (average power 400 μW at 1 kHz) were observed on remote screens or by direct view e.g. of the red lasers. The laser output is well collimated in horizontal dimension (Fig. 3a) due to the second order DFB laser. Fig. 3b shows a robust red laser output in bright room light. With a cylindrical lens to collimate the laser beam outputs, Fig. 3c-d show well-defined, spatialy coherent red and green laser beams with their laser spots projected on a remote screen, respectively. ACKNOWLEDGMENT The research was funded by NSF (ECCS-1128331) and US. DOE/BES (DE-FG02-07ER46387). We are very grateful to H. Kim, S. Ahn, and Prof. Heonsu Jeon of Seoul National University for the holographic gratings for red lasers. REFERENCES These proof-of-concept red CQD-DFB lasers presently degrade in the order of an hour as we have applied no heat management or encapsulant protection. In the red internal energy conversion is 28% which corresponds to a 32% of quantum efficiency by the single exciton quantum efficiency. The biexciton gain CQD media in past literature with fast nonradiative multiexciton Auger recombination simply cannot produce such high quantum efficiency. The 978-1-4577-1507-5/13/$26.00 ©2013 IEEE 23 [1] C. Dang, J. Lee, Y. Zhang, J. Han, C. Breen, J. S. Steckel, et al., "A Wafer-Level Integrated White-Light-Emitting Diode Incorporating Colloidal Quantum Dots as a Nanocomposite Luminescent Material," Advanced Materials, vol. 24, pp. 5915-5918, 2012. [2] Y. Shirasaki, G. J. Supran, M. G. Bawendi, and V. Bulovic, "Emergence of colloidal quantum-dot light-emitting technologies," Nat Photon, vol. 7, pp. 13-23, 01//print 2013. [3] C. Dang, J. Lee, C. Breen, J. S. Steckel, S. Coe-Sullivan, and A. Nurmikko, "Red, green and blue lasing enabled by single-exciton gain in colloidal quantum dot films," Nat Nano, vol. 7, pp. 335-339, 2012. [4] V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, et al., "Optical Gain and Stimulated Emission in Nanocrystal Quantum Dots," Science, vol. 290, pp. 314317, 2000.