Dynamic lattice disorder in two-dimensional
(2D) halide perovskites
can play an important role in their optical properties through carrier/exciton–lattice
interactions. Previously, the 2D halide–pseudohalide perovskite
(MA)2Pb(SCN)2I2 (MA+ =
methylammonium) was demonstrated to have a dynamically inhomogeneous
lattice with structural evolution occurring on a picosecond time scale.
Here, we have investigated two purely inorganic 2D perovskites, Cs2Pb(SCN)2X2 (X = Br or I). 2D infrared
(2D IR) and polarization-selective pump–probe (PSPP) experiments
were used to study dynamics and the effects of changing the halide
anions. The 12CN stretching mode was used as the vibrational
probe. The films were isotopically doped, ∼99% 13CN, to avoid excessive IR absorption, heating, and vibrational excitation
transfer. PSPP measurements were performed on thin films using the
reflection geometry to improve the signal-to-noise ratio. The results
showed that the 12CN vibrational lifetime in Cs2Pb(SCN)2X2 is significantly longer than that
in (MA)2Pb(SCN)2I2, and the lifetimes
were essentially the same for Br and I analogues of Cs2Pb(SCN)2X2. 2D IR spectroscopy is carried out
to measure both spectral diffusion (structural evolution) and homogeneous
dephasing of the inhomogeneously broadened CN stretch absorption line.
The Cs2Pb(SCN)2X2 2D perovskites
displayed substantially slower structural evolution compared to (MA)2Pb(SCN)2I2. The spectral diffusion is
independent of the halide anion. There is also significant homogeneous
dephasing caused by the coupling of the CN stretch to lattice phonons.
Our findings provide insights into lattice dynamics of inorganic 2D
perovskites and lay a foundation for studies on their complex carrier/exciton–lattice
interactions, of importance for applications in optoelectronic devices.