TY - JOUR
T1 - Biexciton Resonances Reveal Exciton Localization in Stacked Perovskite Quantum Wells
AU - Elkins, Madeline H.
AU - Pensack, Ryan
AU - Proppe, Andrew H.
AU - Voznyy, Oleksandr
AU - Quan, Li Na
AU - Kelley, Shana O.
AU - Sargent, Edward H.
AU - Scholes, Gregory D.
N1 - Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/8/17
Y1 - 2017/8/17
N2 - Quasi-two-dimensional lead halide perovskites, MAn-1PbnX3n+1, are quantum confined materials with an ever-developing range of optoelectronic device applications. Like other semiconductors, the correlated motion of electrons and holes dominates the material's response to optical excitation influencing its electrical and optical properties such as charge formation and mobility. However, the effects of many-particle correlation have been relatively unexplored in perovskite because of the difficultly of probing these states directly. Here, we use double quantum coherence spectroscopy to explore the formation and localization of multiexciton states in these materials. Between the most confined domains, we demonstrate the presence of an interwell, two-exciton excited state. This demonstrates that the four-body Coulomb interaction electronically couples neighboring wells despite weak electron/hole hybridization in these materials. Additionally, in contrast with inorganic semiconductor quantum wells, we demonstrate a rapid decrease in the dephasing time as wells become thicker, indicating that exciton delocalization is not limited by structural inhomogeneity in low-dimensional perovskite.
AB - Quasi-two-dimensional lead halide perovskites, MAn-1PbnX3n+1, are quantum confined materials with an ever-developing range of optoelectronic device applications. Like other semiconductors, the correlated motion of electrons and holes dominates the material's response to optical excitation influencing its electrical and optical properties such as charge formation and mobility. However, the effects of many-particle correlation have been relatively unexplored in perovskite because of the difficultly of probing these states directly. Here, we use double quantum coherence spectroscopy to explore the formation and localization of multiexciton states in these materials. Between the most confined domains, we demonstrate the presence of an interwell, two-exciton excited state. This demonstrates that the four-body Coulomb interaction electronically couples neighboring wells despite weak electron/hole hybridization in these materials. Additionally, in contrast with inorganic semiconductor quantum wells, we demonstrate a rapid decrease in the dephasing time as wells become thicker, indicating that exciton delocalization is not limited by structural inhomogeneity in low-dimensional perovskite.
UR - http://www.scopus.com/inward/record.url?scp=85027456072&partnerID=8YFLogxK
U2 - 10.1021/acs.jpclett.7b01621
DO - 10.1021/acs.jpclett.7b01621
M3 - Article
C2 - 28767258
AN - SCOPUS:85027456072
VL - 8
SP - 3895
EP - 3901
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 16
ER -