Determining Out-of-Plane Hole Mobility in CuSCN via the Time-of-Flight Technique To Elucidate Its Function in Perovskite Solar Cells

• Published in: ACS applied materials & interfaces 2021-08, Vol.13 (32), p.38499-38507
• Main Authors: Mohan, Lokeshwari, Ratnasingham, Sinclair R, Panidi, Julianna, Daboczi, Matyas, Kim, Ji-Seon, Anthopoulos, Thomas D, Briscoe, Joe, McLachlan, Martyn A, Kreouzis, Theo
• Format: Article
• Language: English
• Subjects: Functional Inorganic Materials and Devices
• ISSN: 1944-8244; 1944-8252
• DOI: 10.1021/acsami.1c09750

Copper­(I) thiocyanate (CuSCN) is a stable, low-cost, solution-processable p-type inorganic semiconductor used in numerous optoelectronic applications. Here, for the first time, we employ the time-of-flight (ToF) technique to measure the out-of-plane hole mobility of CuSCN films, enabled by the deposition of 4 μm-thick films using aerosol-assisted chemical vapor deposition (AACVD). A hole mobility of ∼10–3 cm2/V s was measured with a weak electric field dependence of 0.005 cm/V1/2. Additionally, by measuring several 1.5 μm CuSCN films, we show that the mobility is independent of thickness. To further validate the suitability of our AACVD-prepared 1.5 μm-thick CuSCN film in device applications, we demonstrate its incorporation as a hole transport layer (HTL) in methylammonium lead iodide (MAPbI3) perovskite solar cells (PSCs). Our AACVD films result in devices with measured power conversion efficiencies of 10.4%, which compares favorably with devices prepared using spin-coated CuSCN HTLs (12.6%), despite the AACVD HTLs being an order of magnitude thicker than their spin-coated analogues. Improved reproducibility and decreased hysteresis were observed, owing to a combination of excellent film quality, high charge-carrier mobility, and favorable interface energetics. In addition to providing a fundamental insight into charge-carrier mobility in CuSCN, our work highlights the AACVD methodology as a scalable, versatile tool suitable for film deposition for use in optoelectronic devices.