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.