TY - JOUR
T1 - Crystal Orientation Drives the Interface Physics at Two/Three-Dimensional Hybrid Perovskites
AU - Bouduban, Marine E.F.
AU - Queloz, Valentin I.E.
AU - Caselli, Valentina M.
AU - Cho, Kyung Taek
AU - Kirmani, Ahmad R.
AU - Paek, Sanghyun
AU - Roldan-Carmona, Cristina
AU - Richter, Lee J.
AU - Savenije, Tom J.
PY - 2019
Y1 - 2019
N2 - Combining halide perovskites with tailored dimensionality into two/three-dimensional (2D/3D) systems has revealed a powerful strategy to boost the performances of perovskite photovoltaics (PVs). Despite recent advances, a clear understanding of the intimate link between interface structure and physics is still missing, leading so far to a blind optimization of the 2D/3D PVs. Here, we reveal the impact of 2D/3D crystal alignment in driving interface charge-recombination dynamics. The 2D crystal growth and orientation are manipulated by specific fluorination of phenethylammonium (PEA), used here as the organic cation backbone of the 2D component. By means of time-resolved optoelectronic analysis from the femto- to microsecond regions, we demonstrate a static function of the 2D layer as an electron barrier and homogeneous surface passivant, together with a dynamic role in retarding back charge recombination. Our results reveal a crucial dependence of such beneficial effects with the 2D layer, leading to an enhanced open-circuit voltage (Voc), mostly attributed to the 2D phase which orients parallel on the 3D layer. Such findings provide a deep understanding and delineate precise guidelines for the smart design of multidimensional perovskite interfaces for advanced PVs and beyond.
AB - Combining halide perovskites with tailored dimensionality into two/three-dimensional (2D/3D) systems has revealed a powerful strategy to boost the performances of perovskite photovoltaics (PVs). Despite recent advances, a clear understanding of the intimate link between interface structure and physics is still missing, leading so far to a blind optimization of the 2D/3D PVs. Here, we reveal the impact of 2D/3D crystal alignment in driving interface charge-recombination dynamics. The 2D crystal growth and orientation are manipulated by specific fluorination of phenethylammonium (PEA), used here as the organic cation backbone of the 2D component. By means of time-resolved optoelectronic analysis from the femto- to microsecond regions, we demonstrate a static function of the 2D layer as an electron barrier and homogeneous surface passivant, together with a dynamic role in retarding back charge recombination. Our results reveal a crucial dependence of such beneficial effects with the 2D layer, leading to an enhanced open-circuit voltage (Voc), mostly attributed to the 2D phase which orients parallel on the 3D layer. Such findings provide a deep understanding and delineate precise guidelines for the smart design of multidimensional perovskite interfaces for advanced PVs and beyond.
UR - http://www.scopus.com/inward/record.url?scp=85072879681&partnerID=8YFLogxK
U2 - 10.1021/acs.jpclett.9b02224
DO - 10.1021/acs.jpclett.9b02224
M3 - Article
C2 - 31497955
SN - 1948-7185
VL - 10
SP - 5713
EP - 5720
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 19
ER -