Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite
Liang Luo,Long Men,Zhaoyu Liu,Yaroslav Mudryk,Xin Zhao,Yongxin Yao,Joong M. Park,Ruth Shinar,Joseph Shinar,Kai-Ming Ho,Ilias E. Perakis,Javier Vela,Jigang Wang +12 more
TLDR
Exitonic Rydberg states with distinct formation pathways are revealed by observing the multiple resonant, internal quantum transitions using ultrafast terahertz quasi-particle transport in the hybrid perovskite system.Abstract:
How photoexcitations evolve into Coulomb-bound electron and hole pairs, called excitons, and unbound charge carriers is a key cross-cutting issue in photovoltaics and optoelectronics Until now, the initial quantum dynamics following photoexcitation remains elusive in the hybrid perovskite system Here we reveal excitonic Rydberg states with distinct formation pathways by observing the multiple resonant, internal quantum transitions using ultrafast terahertz quasi-particle transport Nonequilibrium emergent states evolve with a complex co-existence of excitons, carriers and phonons, where a delayed buildup of excitons under on- and off-resonant pumping conditions allows us to distinguish between the loss of electronic coherence and hot state cooling processes The nearly ∼1 ps dephasing time, efficient electron scattering with discrete terahertz phonons and intermediate binding energy of ∼135 meV in perovskites are distinct from conventional photovoltaic semiconductors In addition to providing implications for coherent energy conversion, these are potentially relevant to the development of light-harvesting and electron-transport devices The generation of bound electron and hole pairs—excitons—is a key process in photovoltaic technologies, yet it is challenging to follow their initial dynamics Here, Luoet al probe the Rydberg eigenstates that characterize the excitonic transport and coherent conversion in a perovskite materialread more
Citations
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Bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process.
Chris Davies,Marina R. Filip,Jay B. Patel,Timothy W. Crothers,Carla Verdi,Adam D. Wright,Rebecca L. Milot,Feliciano Giustino,Michael B. Johnston,Laura M. Herz +9 more
TL;DR: It is shown that the sharpening of photon, electron and hole distribution functions significantly enhances bimolecular charge recombination as the temperature is lowered, mirroring trends in transient spectroscopy.
Journal ArticleDOI
From Ultrafast to Ultraslow: Charge-Carrier Dynamics of Perovskite Solar Cells
TL;DR: In this paper, the charge-carrier dynamics of a perovskite solar cell in a wide time span are summarized and discussed to provide a comprehensive understanding of the optoelectronic processes of the perovsite material and devices.
Journal ArticleDOI
Ultrafast transition between exciton phases in van der Waals heterostructures
Philipp Merkl,Fabian Mooshammer,Philipp Steinleitner,Anna Girnghuber,Kai-Qiang Lin,Philipp Nagler,Johannes Holler,Christian Schüller,John M. Lupton,Tobias Korn,Tobias Korn,Simon Ovesen,Samuel Brem,Ermin Malic,Rupert Huber +14 more
TL;DR: In this article, a femtosecond pump-probe measurements of Coulomb correlations in WS2/WSe2/WS2 heterostructures reveal the interlayer exciton binding energy, determined from the 1s-2p resonance, as well as the dynamics of the conversion of intra-to inter-layer excitons.
Journal ArticleDOI
Slow Cooling of Hot Polarons in Halide Perovskite Solar Cells
TL;DR: In this article, the authors calculate the initial thermalization rate of a perovskite from the scattering time in the Frohlich polaron model to be 78 meV ps-1 for CH3NH3PbI3.
Journal ArticleDOI
Ultrafast transition between exciton phases in van der Waals heterostructures
Philipp Merkl,Fabian Mooshammer,Philipp Steinleitner,Anna Girnghuber,Kai-Qiang Lin,Philipp Nagler,Johannes Holler,Christian Schüller,John M. Lupton,Tobias Korn,Tobias Korn,Simon Ovesen,Samuel Brem,Ermin Malic,Rupert Huber +14 more
TL;DR: A direct ultrafast access to Coulomb correlations between monolayers is introduced, where phase-locked mid-infrared pulses allow to measure the binding energy of interlayer excitons in WSe2/WS2 hetero-bilayers by revealing a novel 1s–2p resonance, explained by a fully quantum mechanical model.
References
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Electron-hole diffusion lengths exceeding 1 micrometer in an organometal trihalide perovskite absorber.
Samuel D. Stranks,Giles E. Eperon,Giulia Grancini,Christopher Menelaou,Marcelo J. P. Alcocer,Tomas Leijtens,Laura M. Herz,Annamaria Petrozza,Henry J. Snaith +8 more
TL;DR: In this article, transient absorption and photoluminescence-quenching measurements were performed to determine the electron-hole diffusion lengths, diffusion constants, and lifetimes in mixed halide and triiodide perovskite absorbers.
Journal Article
Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber
Samuel D. Stranks,Giles E. Eperon,Giulia Grancini,Christopher Menelaou,Marcelo J. P. Alcocer,Tomas Leijtens,Laura M. Herz,Annamaria Petrozza,Henry J. Snaith +8 more
TL;DR: In this paper, transient absorption and photoluminescence-quenching measurements were performed to determine the electron-hole diffusion lengths, diffusion constants, and lifetimes in mixed halide and triiodide perovskite absorbers.
Journal ArticleDOI
Long-Range Balanced Electron- and Hole-Transport Lengths in Organic-Inorganic CH3NH3PbI3
Guichuan Xing,Nripan Mathews,Shuangyong Sun,Swee Sien Lim,Yeng Ming Lam,Michael Grätzel,Michael Grätzel,Subodh Mhaisalkar,Tze Chien Sum +8 more
TL;DR: Two studies show, using a variety of time-resolved absorption and emission spectroscopic techniques, that perovskite materials manifest relatively long diffusion paths for charge carriers energized by light absorption, highlighting effective carrier diffusion as a fruitful parameter for further optimization.
Journal ArticleDOI
The emergence of perovskite solar cells
TL;DR: In this article, a review describes the rapid progress that has been made in hybrid organic-inorganic perovskite solar cells and their applications in the photovoltaic sector.
Journal ArticleDOI
High-performance photovoltaic perovskite layers fabricated through intramolecular exchange
Woon Seok Yang,Jun Hong Noh,Nam Joong Jeon,Young Chan Kim,Seungchan Ryu,Jangwon Seo,Sang Il Seok +6 more
TL;DR: An approach for depositing high-quality FAPbI3 films, involving FAP bI3 crystallization by the direct intramolecular exchange of dimethylsulfoxide (DMSO) molecules intercalated in PbI2 with formamidinium iodide is reported.