Intrinsic Defect Tolerance in Inorganic Tin–Lead Perovskites DOI
Jiajia Zhang,

Xinhao Duan,

Zhuang Hu

и другие.

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер unknown, С. 5208 - 5212

Опубликована: Май 15, 2025

Experimentally, inorganic tin-lead (Sn-Pb) perovskites exhibit an extremely short carrier lifetime of mere nanoseconds, primarily attributed to strong nonradiative recombination induced by high-density defects. This has led the belief that they are highly defect-sensitive. Here, we argue Sn-Pb intrinsically defect-tolerant. We substantiate this claim performing rigorous first-principles calculations for a prototypical composition CsSn0.5Pb0.5I3. Our results show material possesses ultralong 10 μs, even under assumption high defect concentration 1016 cm-3. The alteration in band edge energies arising from mixing CsSnI3 and CsPbI3 is proven contribute remarkable tolerance. ascribe poor photoelectric performance observed inadequate miscibility their components. study reveals inherent superior properties have thus far remained unrecognized research community suggests achieving phase-pure systems crucial fully exploit untapped potential.

Язык: Английский

Extending Carrier Lifetimes of Metal Halide Perovskites by Defect Passivation with Alkaline Earth Metals: A Time-Domain Study DOI
Xue Tian, Run Long

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер 16(9), С. 2438 - 2444

Опубликована: Фев. 27, 2025

Intrinsic defects that serve as non-radiative recombination centers significantly accelerate charge and energy losses in hybrid organic-inorganic perovskites. The defect IMA, formed by replacing an MA with I MAPbI3 (MA = CH3NH3+), creates trimer produces a deep electron trap state. Non-adiabatic (NA) molecular dynamics simulations demonstrate excited conduction band is rapidly captured this within 100 ps, followed valence hole 1 ns, which 3 times faster than the pristine system. Doping interstitial Sr Ba eliminates state breaking trimer, thereby restoring electron-hole across bandgap to durations up 3.20 4.36 respectively. delayed attributed decreased NA coupling shortened decoherence time. These findings provide critical insights into perovskite passivation strategies alkaline earth metals.

Язык: Английский

Процитировано

1
Nuclear Quantum Effects Accelerate Hot Carrier Relaxation but Slow Down Recombination in Metal Halide Perovskites DOI
Yulong Liu, Shiying Shen, Oleg V. Prezhdo

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Март 19, 2025

Inorganic semiconductors are composed of heavy elements whose vibrational motions well described by classical mechanics. Heavy elements, such as Pb and I, support charge carriers in metal halide perovskites. Nevertheless, the soft structure strong coupling between organic inorganic components create conditions which nuclear quantum effects (NQEs) can play important roles. By combining ab initio, ring-polymer, nonadiabatic molecular dynamics approaches with time-domain density functional theory, we demonstrate how NQEs influence structural electronic properties electron-vibrational hybrid organic-inorganic (MAPbI3) all-inorganic (CsPbI3) Quantum zero-point fluctuations enhance disorder, reduce band gap, accelerate elastic scattering responsible for coherence loss. have opposite influences on intraband carrier relaxation interband recombination. These inelastic events governed product overlap-like electron-phonon matrix element atomic velocity. overlap increases The involves many states. Reduction some states is offset other pathways, while an increased velocity makes faster. Electron-hole band-edge plays a key role recombination, its reduction NQEs-enhanced disorder recombination slower. This phenomenon seen both MAPbI3 CsPbI3 much more pronounced when light component present. study offers detailed understanding processes perovskites, offering theoretical insights into hot that govern performance solar cells optoelectronic devices.

Язык: Английский

Процитировано

1
Strain Engineering of Two-Dimensional Hybrid Perovskites with Band Edge Modulation and Charge Separation DOI

Jiali Liao,

Xi-Meng Tang,

Long Zhang

и другие.

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер unknown, С. 4401 - 4409

Опубликована: Апрель 24, 2025

Strain engineering in two-dimensional (2D) perovskites has been widely explored recent years. In this study, first-principles and nonadiabatic molecular dynamics simulations reveal that biaxial strain (exceeding 6%) introduces an abnormal transition of the conduction band minimum (CBM) from inorganic to organic contributions 2D Dion-Jacobson perovskite (3AMPY)PbI4 (3AMPY, 3-(aminomethyl)pyridinium). Further research demonstrates such CBM transitions under tensile compressive are primarily attributed competition between Pb-I interaction organic-inorganic hydrogen bonding interaction. The reconfiguration effectively promotes charge separation, which shortens quantum coherence time suppresses coupling, so it enhances carrier lifetime, particularly 6% strain. findings highlight a novel strain-engineering strategy for optimizing edge modulation transport perovskites, providing valuable insights design high-performance solar cells.

Язык: Английский

Процитировано

0
Intrinsic Defect Tolerance in Inorganic Tin–Lead Perovskites DOI
Jiajia Zhang,

Xinhao Duan,

Zhuang Hu

и другие.

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер unknown, С. 5208 - 5212

Опубликована: Май 15, 2025

Experimentally, inorganic tin-lead (Sn-Pb) perovskites exhibit an extremely short carrier lifetime of mere nanoseconds, primarily attributed to strong nonradiative recombination induced by high-density defects. This has led the belief that they are highly defect-sensitive. Here, we argue Sn-Pb intrinsically defect-tolerant. We substantiate this claim performing rigorous first-principles calculations for a prototypical composition CsSn0.5Pb0.5I3. Our results show material possesses ultralong 10 μs, even under assumption high defect concentration 1016 cm-3. The alteration in band edge energies arising from mixing CsSnI3 and CsPbI3 is proven contribute remarkable tolerance. ascribe poor photoelectric performance observed inadequate miscibility their components. study reveals inherent superior properties have thus far remained unrecognized research community suggests achieving phase-pure systems crucial fully exploit untapped potential.

Язык: Английский

Процитировано

0