The knowledge of the exact nature of the electronic and optical excitations of Ruddlesden-Popper organic-inorganic halide perovskites (RPPs) is particularly relevant in view of their usage in optoelectronic devices. By means of parameter-free quantum-mechanical simulations, we unambiguously demonstrate the dominant role of many-body Coulomb interaction, as recently proposed by Blancon et al. Indeed, focusing on the first two terms ( n = 1,2) of the Pb-based buthylammonium series, in the form of both isolated nanosheet and repeated bulk-like quantum well, we observe large band gap renormalization and strongly bound excitons with binding energies up to ∼1 eV in the thinnest isolated nanosheet. Notably, taking into account electronic correlation beyond density functional theory, we obtain exciton reduced masses similar to the corresponding 3D bulk counterpart and large Rashba splitting of the same order of the value reported by Zhai et al. in a recent experimental work.
Giorgi, G., Yamashita, K., Palummo, M. (2018). Nature of the Electronic and Optical Excitations of Ruddlesden-Popper Hybrid Organic-Inorganic Perovskites: The Role of the Many-Body Interactions. THE JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 9(19), 5891-5896 [10.1021/acs.jpclett.8b02653].
Nature of the Electronic and Optical Excitations of Ruddlesden-Popper Hybrid Organic-Inorganic Perovskites: The Role of the Many-Body Interactions
Palummo M.
2018-01-01
Abstract
The knowledge of the exact nature of the electronic and optical excitations of Ruddlesden-Popper organic-inorganic halide perovskites (RPPs) is particularly relevant in view of their usage in optoelectronic devices. By means of parameter-free quantum-mechanical simulations, we unambiguously demonstrate the dominant role of many-body Coulomb interaction, as recently proposed by Blancon et al. Indeed, focusing on the first two terms ( n = 1,2) of the Pb-based buthylammonium series, in the form of both isolated nanosheet and repeated bulk-like quantum well, we observe large band gap renormalization and strongly bound excitons with binding energies up to ∼1 eV in the thinnest isolated nanosheet. Notably, taking into account electronic correlation beyond density functional theory, we obtain exciton reduced masses similar to the corresponding 3D bulk counterpart and large Rashba splitting of the same order of the value reported by Zhai et al. in a recent experimental work.File | Dimensione | Formato | |
---|---|---|---|
_system_appendPDF_proof_hi_JPCL.pdf
solo utenti autorizzati
Licenza:
Non specificato
Dimensione
3.93 MB
Formato
Adobe PDF
|
3.93 MB | Adobe PDF | Visualizza/Apri Richiedi una copia |
I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.