Lithography-Free Broadband Ultrathin-Film Absorbers with Gap

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Lithography-Free Broadband Ultrathin Film Absorbers with Gap Plasmon Resonance for Organic Photovoltaics Minjung Choi, Gumin Kang, Dongheok Shin, Nilesh Barange, Chang-Won Lee, Doo-Hyun Ko, and Kyoungsik Kim ACS Appl. Mater. Interfaces, Just Accepted Manuscript • DOI: 10.1021/acsami.6b02340 • Publication Date (Web): 10 May 2016 Downloaded from http://pubs.acs.org on May 13, 2016

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ACS Applied Materials & Interfaces

Lithography-Free Broadband Ultrathin Film Absorbers with Gap Plasmon Resonance for Organic Photovoltaics Minjung Choi1, Gumin Kang1, Dongheok Shin1, Nilesh Barange2, Chang-Won Lee3, Doo-Hyun Ko4*, and Kyoungsik Kim1* 1

School of Mechanical Engineering, Yonsei University, 50 Yonsei-ro, Seodaemun-gu, Seoul 03722, Republic of Korea. 2

Korea Institute of Science and Technology, Hwarangno 14-gil, Seongbuk-gu, Seoul 02792, Republic of Korea.

3

Samsung Advanced Institute of Technology, Suwon-si, Gyeonggi-do 16678, Republic of Korea.

4

Department of Applied Chemistry, Kyung Hee University, Yongin, Gyeonggi 17104, Republic of Korea.

* email: [email protected], [email protected].

ACS Paragon Plus Environment

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ABSTRACT Strategies to confine electromagnetic field within ultrathin film emerge as essential technologies for applications from thin-film solar cells to imaging and sensing devices. We demonstrate lithography-free, low-cost, large-scale method to realize broadband ultrathin film metal-dielectric-metal (MDM) absorbers, by exploiting gap-plasmon-resonances for strongly confined electromagnetic field. Two steps method, firstly organizing Au nanoparticles via thermal dewetting then transferring the nanoparticles to a spacer-reflector substrate, is used to achieve broader absorption bandwidth by manipulating geometric shapes of top metallic layer into hemiellipsoids. Fast-deposited nominal Au film, instead of conventional slow one, is employed in Ostwald ripening process to attain hemiellipsoidal nanoparticles. Polymer supported transferring step allows a wider range of dewetting temperature to manipulate the nanoparticles’ shape. By incorporating circularity with ImageJ software, the geometries of hemiellipsoidal nanoparticles are quantitatively characterized. Controlling the top geometry of MDM structure from hemisphere to hemiellipsoid increases the average absorption at 500-900 nm from 23.1% to 43.5% in the ultrathin film and full-width at half-maximum 132 nm to 324 nm, which is consistently explained by finite-difference time-domain simulation. The structural advantages of our scheme are easily applicable to thin-film photovoltaic devices because metal electrodes can act as metal reflectors and semiconductor layers as dielectric spacers.

KEYWORDS ultrathin film absorber, gap surface plasmons, broadband absorption, thermal dewetting, nanoparticles.


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1. INTRODUCTION Thin film light absorbers have been extensively researched for their versatile applications by strongly confining light into subwavelength dimension: thin-film solar cells,1 flammable gas sensing,2 biosensing,3,4 imaging,5 thermal emitters,6 and even future optical switch based on nonlinear bistability.7 In addition, thin film photovoltaic (PV) technologies attract us for the cost competitiveness and the feasibility of large-area deposition.8–11 There are various kinds of thin film active materials, including organic12 and inorganic semiconductors.13 The PV cells have very short carrier diffusion length of 1–20 nm12,14 for organic materials and = {'$

results were paired: (1) ./0 , the referential reflectance from the spacer-reflector layer without Au NPs, and (2) 12./. , the reflectance of the absorber which consists of Au NP on top of spacer-reflector layer. Through the equation ( = 1 ) between simulated transmissions (T) and reflections (R) and zero transmission characteristic, we acquired normalized absorption by subtracting the absorption of the reference from the absorption of absorber according to 32.4 = ./0 12./. . 4.2. Measurement of Total Reflectance and Normalized Absorption. We performed total reflectance measurements on absorber samples using UV-vis-NIR spectrophotometer (UV3600, Shimadzu Scientific Instruments, Inc., Kyoto, Japan) with an integrating sphere (MPC-3100 unit, equipped with an integrating sphere of 60 mm diameter). Through a monochromator coupled to a halogen lamp, unpolarized light source was illuminated onto the samples at an incidence angle of 8˚ from the surface normal. The beam spot size was about 25 mm2 which was sufficiently large


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for measuring the ensemble results of nanoscale MDM absorber units. Two measurements were paired to normalize the absorption data: (1) ./0 , the referential total reflectance of the spacerreflector layer without transferring Au NPs, and (2) 12./. , the total reflectance of the absorber which consists of Au NPs-spacer-reflector substrate. Because the Au reflector was thick enough not to allow light transmission, the transmittance (T) of our samples did not need to be considered. We attribute normalized absorption spectra through background correction of the measured

absorption

by

subtracting

the

reference

spectrum

by

(32.4 λ = 61 12./. 7 81 ./0 9 = ./0 λ 12./. ). In this way, we produce normalized absorption comparable among absorber samples with different spacer thicknesses independent of the interband transition property of Au reflector. 4.3. Material and OPV device fabrication. The blend with 1:1.5 ratio of poly[[4,8-bis[(2ethylhexyl)oxy]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl][3-fluoro-2-[(2ethylhexyl)carbonyl]thieno[3,4-b]thiophenediyl]] (PTB7) (from 1-Material) and phenyl-C70butyric acid methyl ester (PC70BM) (1-Material) is dissolved in 1-2 dichlorobenzene. For the zinc oxide (ZnO) sol-gel synthesis, we followed the literature method,59 and the Zinc acetate (0.1g) was mixed with 5ml of 2-methoxyethanol, and 30 µl ethanolamine as a stabilizer was added. An ITO-coated glass was cleaned with acetone, isopropyl alcohol and deionized water, followed by treatment with UV ozone. For the OPV device with Au NPs, the PMMA-Au NPs film was simply transferred to the ITO-coated glass substrate. The prepared ZnO sol-gel was spin coated on ITO-coated glass substrate with and without Au NPs, and annealed at 150 ºC for 45 min (see Figure S11 in the supporting information for the SEM image of the prepared ZnO film). The blend solution is then spin coated, and subsequently molybdenum oxide (MoO3) was deposited using thermal evaporator. Finally, a 100 nm silver (Ag) was evaporated under high


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vacuum (10-6 Torr). The completed OPVs were sealed using an encapsulation glass prior to further characterization. The active area of the developed PV cells was 0.11 cm2.


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AUTHOR INFORMATION Corresponding Author * Correspondence and requests for materials should be addressed to K.K. (email: [email protected]), and D.H.K. (email: [email protected]).

Author Contributions K.K. conceived the idea of this study. M.C. designed, fabricated the samples, performed experiments, and collected the data. M.C., and G.K. conducted numerical simulations. C.W.L. and D.H.K. made theoretical analysis. N.B fabricated the OPV devices, and performed experiments. M.C., G.K., D.S., and K.K. edited manuscript. K.K. supervised the project. ACKNOWLEDGMENT This research was supported by Basic Science Research Program and the Pioneer Research Center Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT and Future Planning (NRF-2015R1A2A2A11001112, NRF2013M3C1A3065045) and the Low Observable Technology Research Center program of the Defense Acquisition Program Administration and Agency for Defense Development.

Supporting Information Available: SEM images before and after transferring process. Defined angle of orientation according to the major axis of the nanoparticles. Major and minor axes diameters of S-700. Circularity and particle diameter analysis results of F-500. Normalized absorption spectra of S-700 and F-600. Error bar included FWHM of measured absorption


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spectra of absorber samples. External quantum efficiency of reference and Au NPs OPV device for active layer thickness of ~80 nm. Characteristics of both bare and with Au NP OPV devices. Calculated solar photon flux-weighted absorption for HENP ans HSNP absorbers. Simulated Ezfield For the HENP and HSNP absorbers. SEM image of the ZnO film on the Au nanoparticles. This material is available free of charge via the Internet at http://pubs.acs.org.

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