A Phonon Scattering Bottleneck for Carrier Cooling in Lead-Chalcogenide Nanocrystals

ABSTRACTThe cooling dynamics of hot charge carriers in colloidal lead chalcogenide nanocrystals is studied by white light transient absorption spectroscopy. We demonstrate a transient accumulation of charge carriers at a high-energy critical point in the Brillouin zone. Using a theoretical study of the cooling rate in lead chalcogenides, we attribute this slowing down of charge carrier cooling to a phonon scattering bottleneck around this critical point. Our approach allows for the first ever determination of hot carrier cooling rates, relevant in e.g. modeling of multiple exciton generation.

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Manipulation of hot carrier cooling dynamics in two-dimensional Dion–Jacobson hybrid perovskites via Rashba band splitting

Nature Communications ◽

10.1038/s41467-021-24258-7 ◽

2021 ◽

Vol 12 (1) ◽

Author(s):

Jun Yin ◽

Rounak Naphade ◽

Partha Maity ◽

Luis Gutiérrez-Arzaluz ◽

Dhaifallah Almalawi ◽

...

Keyword(s):

Transient Absorption ◽

Phonon Scattering ◽

Transient Absorption Spectroscopy ◽

Band Model ◽

Two Dimensional ◽

Spintronic Devices ◽

Hot Carrier ◽

Band Splitting ◽

Perovskite Materials ◽

Spin Polarized

AbstractHot-carrier cooling processes of perovskite materials are typically described by a single parabolic band model that includes the effects of carrier-phonon scattering, hot phonon bottleneck, and Auger heating. However, little is known (if anything) about the cooling processes in which the spin-degenerate parabolic band splits into two spin-polarized bands, i.e., the Rashba band splitting effect. Here, we investigated the hot-carrier cooling processes for two slightly different compositions of two-dimensional Dion–Jacobson hybrid perovskites, namely, (3AMP)PbI4 and (4AMP)PbI4 (3AMP = 3-(aminomethyl)piperidinium; 4AMP = 4-(aminomethyl)piperidinium), using a combination of ultrafast transient absorption spectroscopy and first-principles calculations. In (4AMP)PbI4, upon Rashba band splitting, the spin-dependent scattering of hot electrons is responsible for accelerating hot-carrier cooling at longer delays. Importantly, the hot-carrier cooling of (4AMP)PbI4 can be extended by manipulating the spin state of the hot carriers. Our findings suggest a new approach for prolonging hot-carrier cooling in hybrid perovskites, which is conducive to further improving the performance of hot-carrier-based optoelectronic and spintronic devices.

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Ultrafast hot-carrier relaxation in silicon monitored by phase-resolved transient absorption spectroscopy

Physical Review B ◽

10.1103/physrevb.104.l041201 ◽

2021 ◽

Vol 104 (4) ◽

Author(s):

Martin Wörle ◽

Alexander W. Holleitner ◽

Reinhard Kienberger ◽

Hristo Iglev

Keyword(s):

Absorption Spectroscopy ◽

Transient Absorption ◽

Transient Absorption Spectroscopy ◽

Carrier Relaxation ◽

Hot Carrier

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Interfacial charge separation in Cu2O/RuOx as a visible light driven CO2 reduction catalyst

Physical Chemistry Chemical Physics ◽

10.1039/c4cp00102h ◽

2014 ◽

Vol 16 (13) ◽

pp. 5922-5926 ◽

Cited By ~ 36

Author(s):

Ernest Pastor ◽

Federico M. Pesci ◽

Anna Reynal ◽

Albertus D. Handoko ◽

Mingjia Guo ◽

...

Keyword(s):

Visible Light ◽

Absorption Spectroscopy ◽

Charge Separation ◽

Transient Absorption ◽

Co2 Reduction ◽

Charge Carriers ◽

Transient Absorption Spectroscopy ◽

Visible Light Driven ◽

Interfacial Charge

Transient absorption spectroscopy as a tool to monitor charge carriers in Cu2O–RuOx photocathodes for CO2 reduction.

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High energy, low repetition rate, photonic crystal fiber generated supercontinuum for nanosecond to millisecond transient absorption spectroscopy

Optics Communications ◽

10.1016/j.optcom.2012.12.070 ◽

2013 ◽

Vol 294 ◽

pp. 250-254 ◽

Cited By ~ 3

Author(s):

Julie L.H. Kho ◽

Charles A. Rohde ◽

Frédérique Vanholsbeeck ◽

M. Cather Simpson

Keyword(s):

Photonic Crystal ◽

Photonic Crystal Fiber ◽

Absorption Spectroscopy ◽

Repetition Rate ◽

Transient Absorption ◽

High Energy ◽

Transient Absorption Spectroscopy ◽

Crystal Fiber

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Hot carrier dynamics in HfN and ZrN measured by transient absorption spectroscopy

Solar Energy Materials and Solar Cells ◽

10.1016/j.solmat.2016.01.026 ◽

2016 ◽

Vol 150 ◽

pp. 51-56 ◽

Cited By ~ 8

Author(s):

Hongze Xia ◽

Xiaoming Wen ◽

Yu Feng ◽

Robert Patterson ◽

Simon Chung ◽

...

Keyword(s):

Absorption Spectroscopy ◽

Transient Absorption ◽

Carrier Dynamics ◽

Transient Absorption Spectroscopy ◽

Hot Carrier

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Charge-transfer biexciton annihilation in a donor–acceptor co-crystal yields high-energy long-lived charge carriers

Chemical Science ◽

10.1039/d0sc03301d ◽

2020 ◽

Vol 11 (35) ◽

pp. 9532-9541

Author(s):

Itai Schlesinger ◽

Natalia E. Powers-Riggs ◽

Jenna L. Logsdon ◽

Yue Qi ◽

Stephen A. Miller ◽

...

Keyword(s):

Charge Transfer ◽

Transient Absorption ◽

High Energy ◽

Charge Carriers ◽

One Dimensional ◽

Femtosecond Transient Absorption ◽

Donor Acceptor ◽

Charge Transfer Excitons

Femtosecond transient absorption microscopy of donor–acceptor single co-crystals shows that photogenerated charge transfer excitons in one-dimensional donor–acceptor π stacks annihilate to produce high-energy, long-lived electrons and holes.

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Bottleneck-Free Hot Hole Cooling in CH3NH3PbI3 Revealed by Femtosecond XUV Absorption

10.26434/chemrxiv.8323289 ◽

2019 ◽

Author(s):

Max A. Verkamp ◽

Joshua Leveillee ◽

Aastha Sharma ◽

André Schleife ◽

Josh Vura-Weis

Keyword(s):

Quantitative Measurement ◽

Transient Absorption ◽

Extreme Ultraviolet ◽

Transient Absorption Spectroscopy ◽

Electron Dynamics ◽

Hot Carrier ◽

Phonon Bottleneck ◽

Conduction Bands ◽

Band Signal ◽

Optical Transient

Femtosecond carrier cooling in the organohalide perovskite semiconductor CH3NH3PbI3 is measured using extreme ultraviolet (XUV) and optical transient absorption spectroscopy. XUV absorption between 44 eV and 58 eV measures transitions from the I 4d core to the valence and conduction bands and gives distinct signals for hole and electron dynamics. The core-to-valence-band signal directly maps the photoexcited hole distribution and provides a quantitative measurement of the hole temperature. The combination of XUV and optical probes reveals that upon excitation at 400 nm, the initial hole distribution is 3.5 times hotter than the electron distribution. At an initial carrier density of 1.4×1020 cm-3 both carriers are subject to a hot phonon bottleneck, but at 4.2×1019 cm-3 the holes cool to less than 1000 K within 400 fs. This result places significant constraints on the use of organohalide perovskites in hot-carrier photovoltaics.

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Highly Selective Photocatalytic Reduction of o-Dinitrobenzene to o-Phenylenediamine over Non-Metal-Doped TiO2 under Simulated Solar Light Irradiation

Catalysts ◽

10.3390/catal8120641 ◽

2018 ◽

Vol 8 (12) ◽

pp. 641 ◽

Cited By ~ 5

Author(s):

Hamza El-Hosainy ◽

Said El-Sheikh ◽

Adel Ismail ◽

Amer Hakki ◽

Ralf Dillert ◽

...

Keyword(s):

Fluorescence Lifetime ◽

Transient Absorption ◽

Charge Carriers ◽

Photocatalytic Reduction ◽

Transient Absorption Spectroscopy ◽

Solar Light ◽

High Yield ◽

Tio2 Photocatalysts ◽

Doped Tio2 ◽

Metal Doped

Photocatalytic reduction and hydrogenation reaction of o-dinitrobenzene in the presence of oxalic acid over anatase-brookite biphasic TiO2 and non-metal-doped anatase-brookite biphasic TiO2 photocatalysts under solar simulated light was investigated. Compared with commercial P25 TiO2, the prepared un-doped and doped anatase-brookite biphasic TiO2 exhibited a high selectivity towards the formation of o-nitroaniline (85.5%) and o-phenylenediamine ~97%, respectively. The doped anatase-brookite biphasic TiO2 has promoted photocatalytic reduction of the two-nitro groups of o-dinitrobenzene to the corresponding o-phenylenediamine with very high yield ~97%. Electron paramagnetic resonance analysis, Transient Absorption Spectroscopy (TAS) and Photoluminescence analysis (PL) were performed to determine the distribution of defects and the fluorescence lifetime of the charge carriers for un-doped and doped photocatalysts. The superiority of the doped TiO2 photocatalysts is accredited to the creation of new dopants (C, N, and S) as hole traps, the formation of long-lived Ti3+ defects which leads to an increase in the fluorescence lifetime of the formed charge carriers. The schematic diagram of the photocatalytic reduction of o-dinitrobenzene using the doped TiO2 under solar light was also illustrated in detail.

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