Inorganic Cs_(2)SnI_(6) perovskite has exhibited substantial potential for light harvesting due to its exceptional optoelectronic properties and remarkable stability in ambient conditions.The charge transport characte...Inorganic Cs_(2)SnI_(6) perovskite has exhibited substantial potential for light harvesting due to its exceptional optoelectronic properties and remarkable stability in ambient conditions.The charge transport characteristics within perovskite films are subject to modulation by various factors,including crystalline orientation,morphology,and crystalline quality.Achieving preferred crystalline orientation and film morphology via a solution-based process is challenging for Cs_(2)SnI_(6) films.In this work,we employed thiourea as an additive to optimize crystal orientation,enhance film morphology,promote crystallization,and achieve phase purity.Thiourea lowers the surface energy of the(222)plane along the(111)direction,confirmed by x-ray diffraction,x-ray photoelectron spectroscopy,ultraviolet photoelectron spectroscopy studies,and density functional theory calculations.Varying thiourea concentration enables a bandgap tuning of Cs_(2)SnI_(6) from 1.52 eV to1.07 eV.This approach provides a novel method for utilizing Cs_(2)SnI_(6) films in high-performance optoelectronic devices.展开更多
A large database is desired for machine learning(ML) technology to make accurate predictions of materials physicochemical properties based on their molecular structure.When a large database is not available,the develo...A large database is desired for machine learning(ML) technology to make accurate predictions of materials physicochemical properties based on their molecular structure.When a large database is not available,the development of proper featurization method based on physicochemical nature of target proprieties can improve the predictive power of ML models with a smaller database.In this work,we show that two new featurization methods,volume occupation spatial matrix and heat contribution spatial matrix,can improve the accuracy in predicting energetic materials' crystal density(ρ_(crystal)) and solid phase enthalpy of formation(H_(f,solid)) using a database containing 451 energetic molecules.Their mean absolute errors are reduced from 0.048 g/cm~3 and 24.67 kcal/mol to 0.035 g/cm~3 and 9.66 kcal/mol,respectively.By leave-one-out-cross-validation,the newly developed ML models can be used to determine the performance of most kinds of energetic materials except cubanes.Our ML models are applied to predict ρ_(crystal) and H_(f,solid) of CHON-based molecules of the 150 million sized PubChem database,and screened out 56 candidates with competitive detonation performance and reasonable chemical structures.With further improvement in future,spatial matrices have the potential of becoming multifunctional ML simulation tools that could provide even better predictions in wider fields of materials science.展开更多
1. Introduction The increasing global demand for sustainable energy sources and emerging environmental issues have pushed the development of energy conversion and storage technologies to the forefront of chemical rese...1. Introduction The increasing global demand for sustainable energy sources and emerging environmental issues have pushed the development of energy conversion and storage technologies to the forefront of chemical research [1,2]. In particular, electrochemical CO_(2) reduction(CO_(2) R) to value-added fuels and chemicals presents a feasible pathway for renewable energy storage and could help mitigate the ever-increasing CO_(2) emissions [3].展开更多
The thermal expansion coefficient(TEC)and thermal conductivity(k)of thermal fillers are key factors for designing thermal management and thermal protection composite materials.Due to its unique advantages,hexagonal bo...The thermal expansion coefficient(TEC)and thermal conductivity(k)of thermal fillers are key factors for designing thermal management and thermal protection composite materials.Due to its unique advantages,hexagonal boron nitride(h-BN)is one of the most commonly used thermal fillers.However,its TEC and k values are still unclear due to the inconsistency of characterization techniques and sample preparations.In this work,these disputes were addressed using the quasi-harmonic approximation(QHA)method and phonon Boltzmann transport equation(BTE)theory based on the density functional theory(DFT),respectively.The accuracy of our calculated TEC and k values was confirmed by previously reported experimental results,and the underlying physical principles were analyzed from the phonon behaviors.Our TEC results show that the h-BN has small in-plane negative value and large cross-plane positive value,which are-2.4×10^(-6) and 36.4×10^(-6) K^(-1) at 300 K,respectively.And the anisotropic TEC is mainly determined by the anisotropic isothermal bulk modulus and the low-frequency out-of-plane longitudinal phonon modes.We found that the convergence of cutoff radius and q-grid size have significant effect on the accuracy of k of h-BN.Our results show that the in-plane k is much higher than the cross-plane k,and the values at 300 K are 286.6 and 2.7 W m^(-1) K^(-1),respectively.The anisotropic phonon group velocity arising from the vibration behaviors of acoustic phonon modes should be primarily responsible for the anisotropic k.Our calculated TEC and k values will provide important references for the design of h-BN composite materials.展开更多
基金Project supported by the National Natural Science Foundation of China (Grant Nos.12174275,62174113,61874139,61904201,and 11875088)Guangdong Basic and Applied Basic Research Foundation (Grant No.2019B1515120057)。
文摘Inorganic Cs_(2)SnI_(6) perovskite has exhibited substantial potential for light harvesting due to its exceptional optoelectronic properties and remarkable stability in ambient conditions.The charge transport characteristics within perovskite films are subject to modulation by various factors,including crystalline orientation,morphology,and crystalline quality.Achieving preferred crystalline orientation and film morphology via a solution-based process is challenging for Cs_(2)SnI_(6) films.In this work,we employed thiourea as an additive to optimize crystal orientation,enhance film morphology,promote crystallization,and achieve phase purity.Thiourea lowers the surface energy of the(222)plane along the(111)direction,confirmed by x-ray diffraction,x-ray photoelectron spectroscopy,ultraviolet photoelectron spectroscopy studies,and density functional theory calculations.Varying thiourea concentration enables a bandgap tuning of Cs_(2)SnI_(6) from 1.52 eV to1.07 eV.This approach provides a novel method for utilizing Cs_(2)SnI_(6) films in high-performance optoelectronic devices.
基金support from the Ministry of Education(MOE) Singapore Tier 1 (RG8/20)。
文摘A large database is desired for machine learning(ML) technology to make accurate predictions of materials physicochemical properties based on their molecular structure.When a large database is not available,the development of proper featurization method based on physicochemical nature of target proprieties can improve the predictive power of ML models with a smaller database.In this work,we show that two new featurization methods,volume occupation spatial matrix and heat contribution spatial matrix,can improve the accuracy in predicting energetic materials' crystal density(ρ_(crystal)) and solid phase enthalpy of formation(H_(f,solid)) using a database containing 451 energetic molecules.Their mean absolute errors are reduced from 0.048 g/cm~3 and 24.67 kcal/mol to 0.035 g/cm~3 and 9.66 kcal/mol,respectively.By leave-one-out-cross-validation,the newly developed ML models can be used to determine the performance of most kinds of energetic materials except cubanes.Our ML models are applied to predict ρ_(crystal) and H_(f,solid) of CHON-based molecules of the 150 million sized PubChem database,and screened out 56 candidates with competitive detonation performance and reasonable chemical structures.With further improvement in future,spatial matrices have the potential of becoming multifunctional ML simulation tools that could provide even better predictions in wider fields of materials science.
基金supported by the National Natural Science Foundation of China(Grants 21872039,22072030 and 52025023)the Science and Technology Commission of Shanghai Municipality(Grants 18JC1411700 and 19DZ2270100)+3 种基金the Key R&D Program of Guangdong Province(Grant 2020B010189001)funding support from the original personalized project of Hehai Universityfunding support from China Postdoctoral Science Foundation(2021M700810)。
文摘1. Introduction The increasing global demand for sustainable energy sources and emerging environmental issues have pushed the development of energy conversion and storage technologies to the forefront of chemical research [1,2]. In particular, electrochemical CO_(2) reduction(CO_(2) R) to value-added fuels and chemicals presents a feasible pathway for renewable energy storage and could help mitigate the ever-increasing CO_(2) emissions [3].
基金the National Natural Science Foundation of China(51621091,51225203,and 51672060)the National Key Research and Development Program of China(2017YFB0310400)。
文摘The thermal expansion coefficient(TEC)and thermal conductivity(k)of thermal fillers are key factors for designing thermal management and thermal protection composite materials.Due to its unique advantages,hexagonal boron nitride(h-BN)is one of the most commonly used thermal fillers.However,its TEC and k values are still unclear due to the inconsistency of characterization techniques and sample preparations.In this work,these disputes were addressed using the quasi-harmonic approximation(QHA)method and phonon Boltzmann transport equation(BTE)theory based on the density functional theory(DFT),respectively.The accuracy of our calculated TEC and k values was confirmed by previously reported experimental results,and the underlying physical principles were analyzed from the phonon behaviors.Our TEC results show that the h-BN has small in-plane negative value and large cross-plane positive value,which are-2.4×10^(-6) and 36.4×10^(-6) K^(-1) at 300 K,respectively.And the anisotropic TEC is mainly determined by the anisotropic isothermal bulk modulus and the low-frequency out-of-plane longitudinal phonon modes.We found that the convergence of cutoff radius and q-grid size have significant effect on the accuracy of k of h-BN.Our results show that the in-plane k is much higher than the cross-plane k,and the values at 300 K are 286.6 and 2.7 W m^(-1) K^(-1),respectively.The anisotropic phonon group velocity arising from the vibration behaviors of acoustic phonon modes should be primarily responsible for the anisotropic k.Our calculated TEC and k values will provide important references for the design of h-BN composite materials.
