The origin of broadband blue emission in zero-dimensional organic lead iodine perovskites: A first-principles study DOI
Jieyao Tan, Xingxing Jiang, Dongyu Liu

и другие.

The Journal of Chemical Physics, Год журнала: 2024, Номер 161(14)

Опубликована: Окт. 8, 2024

Broadband blue emission in zero-dimensional perovskites has received considerable attention, which is very important for the realization of stable blue-light emitters; however, underlying formation mechanism remains unclear. Based on first-principles calculations, we have systematically studied self-trapped excitons (STEs) behavior and luminescence properties 0D-(DMA)4PbI6 perovskite. Our calculations show that there a significant difference between intrinsic STE (∼2.51 eV) experimental observations (∼2.70 eV). In contrast, found iodine vacancy (VI) energetically accessible exhibits shallow charge transition level at ∼2.69 eV (0/+1) above valence band maximum, provides initial local well STEs formation. Moreover, low electronic dimension synergistic Jahn–Teller distortion facilitates extrinsic self-trapping. Further excited state structure analysis configuration coordinate diagram confirmed broadband origin VI-induced instead STEs. Therefore, our simulation results rationalize phenomena provide insights into low-dimensional perovskite systems.

Язык: Английский

Origins of the Accelerated Decomposition in Inorganic Tin Perovskites Contaminated by Oxygen: Ab Initio and Quantum Dynamics Study DOI

Akang Li,

Qi Liu, WanZhen Liang

и другие.

The Journal of Physical Chemistry C, Год журнала: 2023, Номер 127(33), С. 16721 - 16731

Опубликована: Авг. 10, 2023

Tin-based perovskites are one of the most promising candidates for development lead-free perovskite solar cells (PSCs) and have attracted lots attention. Despite extensive research efforts, performance tin-based PSCs (Sn-PSCs) still lags far behind lead containing counterparts due to poor stability self-p-doping. Here, we perform first-principles density functional theory calculations combined with non-adiabatic molecular dynamics simulations unveil origins instability tin iodine when exposed O2. It is found that O2 more thermally favorable be adsorbed on iodine-vacancy (VI) defect sites in defective surface rather than pristine surface, generation peroxide species VI dramatically accelerates structural decomposition. The presence defects CsSnI3 decreases band gap by inducing a local shallow state around conduction minimum, significantly accelerating electron–hole recombination. adsorption site slightly increases compared influence surface's optoelectronic properties recombination rate but decomposition weakening tolerance ability [SnI6]4– octahedra as well carriers' relaxation. increased points passivation main optimization scheme efficient stable Sn-PSCs.

Язык: Английский

Процитировано

2
Lessons Learned from Catalysis to Qubits: General Strategies to Build Accessible and Accurate First-Principles Models of Point Defects DOI Creative Commons
Gil M. Repa, Lisa A. Fredin

The Journal of Physical Chemistry C, Год журнала: 2023, Номер 127(45), С. 21930 - 21939

Опубликована: Ноя. 8, 2023

Defects and dopants play critical roles in defining the properties of a material. Achieving mechanistic understanding how such arise is challenging with current experimental methods, computational approaches suffer from significant modeling limitations that frequently require posteriori fitting. Consequently, pace dopant discovery as means tuning material for particular application has been slow. However, recent advances computation have enabled researchers to move away semiempirical schemes reposition density functional theory predictive tool improve accessibility highly accurate first-principles methods all researchers. This Perspective discusses some these achievements provide more geometric, thermodynamic, optical, electronic simultaneously. Advancements related supercells, basis sets, functionals, optimization protocols, well suggestions evaluating quality model through comparison data, are discussed. Moreover, results fields energy materials, heterogeneous catalysis, quantum informatics reviewed along an evaluation frontiers opportunities field materials chemistry.

Язык: Английский

Процитировано

1
The Effective Prolongation of the Excited-State Carrier Lifetime of CsPbI2Br with Applying Strain DOI
Chang Liu, Chundan Lin, Yuhong Xia

и другие.

Physical Chemistry Chemical Physics, Год журнала: 2024, Номер 26(26), С. 18006 - 18015

Опубликована: Янв. 1, 2024

Applying 2% tensile and compressive strains to the all-inorganic perovskite CsPbI 2 Br extends excited-state carrier lifetimes by 4.7 1.6 times, respectively.

Язык: Английский

Процитировано

0
The origin of broadband blue emission in zero-dimensional organic lead iodine perovskites: A first-principles study DOI
Jieyao Tan, Xingxing Jiang, Dongyu Liu

и другие.

The Journal of Chemical Physics, Год журнала: 2024, Номер 161(14)

Опубликована: Окт. 8, 2024

Broadband blue emission in zero-dimensional perovskites has received considerable attention, which is very important for the realization of stable blue-light emitters; however, underlying formation mechanism remains unclear. Based on first-principles calculations, we have systematically studied self-trapped excitons (STEs) behavior and luminescence properties 0D-(DMA)4PbI6 perovskite. Our calculations show that there a significant difference between intrinsic STE (∼2.51 eV) experimental observations (∼2.70 eV). In contrast, found iodine vacancy (VI) energetically accessible exhibits shallow charge transition level at ∼2.69 eV (0/+1) above valence band maximum, provides initial local well STEs formation. Moreover, low electronic dimension synergistic Jahn–Teller distortion facilitates extrinsic self-trapping. Further excited state structure analysis configuration coordinate diagram confirmed broadband origin VI-induced instead STEs. Therefore, our simulation results rationalize phenomena provide insights into low-dimensional perovskite systems.

Язык: Английский

Процитировано

0