Perovskite Layers with Additives

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Energy Conversion and Storage; Plasmonics and Optoelectronics

Diffusion Enhancement in Highly Excited MAPbI Perovskite Layers with Additives 3

Patrik Scajev, Chuanjiang Qin, Ramunas Aleksiejunas, Paulius Baronas, Saulius Miasojedovas, Takashi Fujihara, Toshinori Matsushima, Chihaya Adachi, and Saulius Jursenas J. Phys. Chem. Lett., Just Accepted Manuscript • Publication Date (Web): 28 May 2018 Downloaded from http://pubs.acs.org on May 28, 2018

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Diffusion Enhancement in Highly Excited MAPbI3 Perovskite Layers with Additives

Patrik Ščajev1, Chuanjiang Qin2,3, Ramūnas Aleksiejūnas1, Paulius Baronas1, Saulius Miasojedovas1, Takashi Fujihara4, Toshinori Matsushima2,3,5, Chihaya Adachi2,3,5, and Saulius Juršėnas1

1

Institute of Photonics and Nanotechnology, Vilnius University, Sauletekio Ave. 3, LT 10257,

Vilnius, Lithuania 2

Center for Organic Photonics and Electronics Research (OPERA), Kyushu University 744,

Motooka, Nishi, Fukuoka 819-0395, Japan 3

Adachi Molecular Exciton Engineering Project, Japan Science and Technology Agency (JST),

ERATO, 744 Motooka, Nishi, Fukuoka 819-0395, Japan 4

Innovative Organic Device Laboratory, Institute of Systems, Information Technologies and

Nanotechnologies (ISIT), Fukuoka Industry-Academia Symphonicity (FiaS) 2-110, 4-1 Kyudaishinmachi, Nishi, Fukuoka 819-0388, Japan 5

International Institute for Carbon Neutral Energy Research (WPI-I2CNER), Kyushu University,

744 Motooka, Nishi, Fukuoka 819-0395, Japan

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Abstract Carrier mobility is one of the crucial parameters determining the electronic device performance. Here, we apply the light induced transient grating technique to measure independently the carrier diffusion coefficient and lifetime and to reveal the impact of additives on carrier transport properties in wet-cast CH3NH3PbI3 (MAPbI3) perovskite films. We use the high excitation regime where diffusion length of carriers is controlled purely by carrier diffusion and not by the lifetime. We demonstrate a four-fold increase in diffusion coefficient due to reduction of localization center density by additives; however, the density dependence analysis shows the dominance of localization-limited diffusion regime. The presented approach allows to estimate the limits of technological improvement – carrier diffusion coefficient in wet-cast layers can be expected to enhance up to one order of magnitude.

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Metal halide perovskites are an attractive candidate for cheap and efficient solar cells.1 Also, they are considered for other applications as well, including light emitting diodes,2 lasers,3 photodetectors,4 and transistors.5 One of the major advantages of perovskites is that they can be produced from solution, which offers cheap and scalable manufacturing of devices. Unfortunately, the quality of wet-cast perovskite layers is usually worse than that of crystals, which shows in vastly scattered electrical parameters. For example, the reported diffusion coefficient in spin-coated CH3NH3PbI3 (MAPbI3) varies from ~10-5 cm2/s to 2.7 cm2/s,6–20 while in MAPbI3 single crystals the hole diffusion coefficient varies only within 1.7–2.3 cm2/s range,21,22 the effective or ambipolar diffusion coefficient – within 0.4–2.4 cm2/s range.23–25 One way to improve the electrical characteristics of the wet-cast perovskite layers is to use additives during the layer formation. Additives are effective in controlling the film morphology, surface uniformity, and crystallite size.26 In particular, it has been demonstrated that benzoquinone improves the structural quality of MAPbI3 spin-coated layers and increases the efficiency of solar cells.27 It can be anticipated that the additives can have a positive effect on carrier dynamics as well, although this aspect has not been sufficiently studied and remains unclear. An important factor defining the limits of how much the carrier mobility (diffusivity) can be improved by optimizing the growth technology is the dominant diffusion regime in a layer. In our recent study, two diffusion regimes were identified in perovskites: band-like and localization-limited diffusion.28 Band-like diffusion with typical ambipolar diffusion coefficient (D) of ~1 cm2/s is determined by fundamental material properties and is limited by polar-optical electron-phonon and screened electron-hole scattering.29,30 Localization-limited diffusion, on the other hand, is characterized by D value from 1018 cm-3), which enables establishment of the intrinsic recombination regime when the variation in the carrier diffusion length is controlled solely by 12


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the diffusivity changes. We demonstrate that the localization-limited diffusion regime takes place in our samples, at least up to the carrier densities of 2×1019 cm-3. We show that the correct choice of additives can have a considerable positive effect on both electrical and optical properties. The diffusion coefficient increases up to 4 times in the sample with tetracyanoquinodimethane, which results in 2–2.5 times longer diffusion length of carriers as compared to the reference sample with no additives. Also, the threshold of amplified spontaneous emission drops from 75 µJ/cm2 in pure layer down to 50 µJ/cm2 due to increased layer quality. On the other hand, carrier diffusion remains in the localization-limited regime, the highest value ranging with excitation from 0.1 cm2/s to 1 cm2/s. Therefore, a tenfold increase of the diffusion coefficient (at low carrier densities) can still be anticipated by improving the growth technology of spin-coated MAPbI3 films.

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Experimental Methods

Perovskite film preparation. Four spin-coated MAPbI3 layers of ~400 nm thickness were produced for this study. One sample was prepared without additives, while others where modified using benzoquinone, hydroquinone, and tetracyanoquinodimethane. The samples were encapsulated with glass caps and UV-curing epoxy resin in the glove box in order to prevent degradation caused by atmospheric water and oxygen. The additive-containing perovskites were synthesized by adding different additive at a 2.5% molar ratio into a MAPbI3 precursor solution. The mixtures were then spin-coated on the fused silica at 3000 rpm for 45 s. During spin coating, 0.3 mL of toluene was dropped onto the perovskite precursor layer. The precursor layer was baked on a hotplate at 100 °C for 15 min. More details of sample preparation can be found in Ref27. Optical measurements. LITG experiments were carried out using 10 ps duration pulses from Nd:YLF laser (PL2243 Ekspla) operating at 10 Hz. For transient grating probing and recording, the pulses at fundamental laser wavelength (1054 nm) and its second harmonics (527 nm) were used, respectively. The probe pulses were delayed with respect to the pump pulses using a positioning stage (Aerotech). The transient gratings were recorded using the holographic beam splitter and 4f imaging telescope system. Excitation dependent measurements were performed by attenuating excitation with neutral density (ND) filters. Time-resolved PL measurements were performed in a standard back-scattering geometry using Hamamatsu streak camera and Acton monochromator. For excitation 680 nm and 527 nm 160 fs duration laser pulses from Orpheus (Light Conversion) optical parametric amplifier (OPA) pumped by PHAROS (Light Conversion) laser, operating at 10 kHz repetition rate, were used. Excitation dependent measurements were performed attenuating excitation by ND filters. 14


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For PL, the average carrier density was obtained by additionally averaging over the radial Gaussian pulse, providing the averaging factor. This procedure provided ∆NPL = αI0(1 + exp(– 2αd))/(4hνexc); here d is the sample thickness, hνexc – quantum energy of the pump photons. Thus, ∆NPL = ∆N/2. Stationary absorption coefficient in the layers was measured using a Perkin Elmer spectrometer for the wavelengths 527 nm and 680 nm and was equal to 1.16×105 cm-1 and 2.7×104 cm-1, respectively.

Acknowledgements Vilnius University team acknowledges the financial support provided by Research Council of Lithuania under the project No. S-MIP-17-71. This work was supported by the Japan Science and Technology Agency (JST), ERATO, Adachi Molecular Exciton Engineering Project, under JST ERATO Grant Number JPMJER1305, Japan, the International Institute for Carbon Neutral Energy Research (WPI-I2CNER) sponsored by the Ministry of Education, Culture, Sports, Science and Technology (MEXT), JSPS KAKENHI, grant numbers JP15K14149 and JP16H04192, and Canon Foundation.

Supporting Information Available: A detailed description of light induced transient grating (LITG) technique, experimental verification of the perovskite layers stability, SEM images and XRD spectra, calculations of diffusion coefficient dependence on excitation, time-resolved differential transmission and photoluminescence measurements, ASE spectra in BQ sample, quantum yield in the samples.

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Perovskite Layers with Additives

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