Two-dimensional(2D)materials attract considerable attention due to their remarkable electronic,mechanical and optical properties.Despite their use in combination with substrates in practical applications,computational...Two-dimensional(2D)materials attract considerable attention due to their remarkable electronic,mechanical and optical properties.Despite their use in combination with substrates in practical applications,computational studies often neglect the effects of substrate interactions for simplicity.This study presents a novel method for predicting the atomic structure of 2D materials on substrates by combining an evolutionary algorithm,a lattice-matching technique,an automated machinelearning interatomic potentials training protocol,and the ab initio thermodynamics approach.Using the molybdenum-sulfur system on a sapphire substrate as a case study,we reveal several new stable and metastable structures,including previously known 1H-MoS_(2)and newly found Pmma Mo_(3)S_(2),P1^(-)Mo_(2)S,P2_(1)m Mo_(5)S_(3),and P_(4)mm Mo_(4)S,where the Mo_(4)S structure is specifically stabilized by interaction with the substrate.Finally,we use the ab initio thermodynamics approach to predict the synthesis conditions of the discovered structures in the parameter space of the commonly used chemical vapor deposition technique.展开更多
Thanks to their record high refractive index and giant optical anisotropy,van der Waals(vdW)materials have accelerated the development of nanophotonics.However,traditional high refractive index materials,such as titan...Thanks to their record high refractive index and giant optical anisotropy,van der Waals(vdW)materials have accelerated the development of nanophotonics.However,traditional high refractive index materials,such as titanium dioxide(TiO_(2)),still dominate in the most important visible range.This is due to the current lack of transparent vdW materials across the entire visible spectrum.In this context,we propose that germanium disulfide(GeS_(2))could offer a significant breakthrough.With its high refractive index,negligible losses,and biaxial optical anisotropy across the whole visible range,GeS_(2)has the potential to complement TiO2 and close the application gap of vdW materials in the visible spectrum.The addition of GeS_(2)could have a profound impact on the design of van der Waals nanophotonic circuits for any operation wavelength from ultraviolet to infrared,emphasizing the significance of the potential impact of GeS_(2)on the field of nanophotonics.展开更多
The emergence of van der Waals(vdW)materials resulted in the discovery of their high optical,mechanical,and electronic anisotropic properties,immediately enabling countless novel phenomena and applications.Such succes...The emergence of van der Waals(vdW)materials resulted in the discovery of their high optical,mechanical,and electronic anisotropic properties,immediately enabling countless novel phenomena and applications.Such success inspired an intensive search for the highest possible anisotropic properties among vdW materials.Furthermore,the identification of the most promising among the huge family of vdW materials is a challenging quest requiring innovative approaches.Here,we suggest an easy-to-use method for such a survey based on the crystallographic geometrical perspective of vdW materials followed by their optical characterization.Using our approach,we found As2S3 as a highly anisotropic vdW material.It demonstrates high in-plane optical anisotropy that is~20%larger than for rutile and over two times as large as calcite,high refractive index,and transparency in the visible range,overcoming the century-long record set by rutile.Given these benefits,As2S3 opens a pathway towards nextgeneration nanophotonics as demonstrated by an ultrathin true zero-order quarter-wave plate that combines classical and the Fabry–Pérot optical phase accumulations.Hence,our approach provides an effective and easy-to-use method to find vdW materials with the utmost anisotropic properties.展开更多
基金RSF No.24-73-10055 for financial support of the development of ML interatomic potential for Mo-S system and calculation of dynamical properties of newly found materialsA.V.A.is supported by the Ministry of Science and Higher Education(FSMG-2025-0005)+3 种基金D.G.K.acknowledges financial support from the federal budget of the Russian Ministry of Science and Higher Education(No.125020401357-4)A.R.O.gratefully acknowledges support from Russian Science Foundation(grant 24-43-00162)K.S.N acknowledges support from the Ministry of Education,Singapore under Research Centre of Excellence award to the Institute for Functional Intelligent Materials,I-FIM(project No.EDUNC-33-18-279-V12)and under the Tier 3 program(MOE-MOET32024-0001)the National Research Foundation,Singapore under its AI Singapore Programme(AISG Award No:AISG3-RP-2022-028).
文摘Two-dimensional(2D)materials attract considerable attention due to their remarkable electronic,mechanical and optical properties.Despite their use in combination with substrates in practical applications,computational studies often neglect the effects of substrate interactions for simplicity.This study presents a novel method for predicting the atomic structure of 2D materials on substrates by combining an evolutionary algorithm,a lattice-matching technique,an automated machinelearning interatomic potentials training protocol,and the ab initio thermodynamics approach.Using the molybdenum-sulfur system on a sapphire substrate as a case study,we reveal several new stable and metastable structures,including previously known 1H-MoS_(2)and newly found Pmma Mo_(3)S_(2),P1^(-)Mo_(2)S,P2_(1)m Mo_(5)S_(3),and P_(4)mm Mo_(4)S,where the Mo_(4)S structure is specifically stabilized by interaction with the substrate.Finally,we use the ab initio thermodynamics approach to predict the synthesis conditions of the discovered structures in the parameter space of the commonly used chemical vapor deposition technique.
基金K.S.N.acknowledges support from the Ministry of Education,Singapore(Research Centre of Excellence award to the Institute for Functional Intelligent Materials,I-FIM,project No.EDUNC-33-18-279-V12)the National Research Foundation,Singapore under its AI Singapore Programme(AISG Award No:AISG3-RP-2022-028)the Royal Society(UK,grant number RSRP\R\190000).
文摘Thanks to their record high refractive index and giant optical anisotropy,van der Waals(vdW)materials have accelerated the development of nanophotonics.However,traditional high refractive index materials,such as titanium dioxide(TiO_(2)),still dominate in the most important visible range.This is due to the current lack of transparent vdW materials across the entire visible spectrum.In this context,we propose that germanium disulfide(GeS_(2))could offer a significant breakthrough.With its high refractive index,negligible losses,and biaxial optical anisotropy across the whole visible range,GeS_(2)has the potential to complement TiO2 and close the application gap of vdW materials in the visible spectrum.The addition of GeS_(2)could have a profound impact on the design of van der Waals nanophotonic circuits for any operation wavelength from ultraviolet to infrared,emphasizing the significance of the potential impact of GeS_(2)on the field of nanophotonics.
基金financially supported by the National Key Research and Development Program of China(2021YFB3601502)the Key Research Program of Frontier Sciences,CAS(ZDBS-LY-SLH035)+6 种基金the National Natural Science Foundation of China(22193044,61835014,51972336)the West Light Foundation of CAS(2019-YDYLTD-002)the Natural Science Foundation of Xinjiang(2021D01E05)the CAS Project for Young Scientists in Basic Research(YSBR-024)Xinjiang Major Science and Technology Project(2021A01001)the CAS President’s International Fellowship Initiative(PIFI,2020PM0046)Tianshan Basic Research Talents(2022TSYCJU0001)。
基金K.S.N.acknowledges support from the Ministry of Education,Singapore(Research Centre of Excellence award to the Institute for Functional Intelligent Materials,I-FIM,project No.EDUNC-33-18-279-V12)and from the Royal Society(UK,grant number RSRP\R\190000).S.M.N.acknowledges the financial support from the Ministry of Science and Higher Education(agreement No.075-15-2022-1150)+2 种基金A.S.S.and A.N.T.gratefully acknowledge the financial support from the RSF(grant No.22-19-00558)D.A.G.,A.V.A.,and V.S.V.acknowledge support from the Higher Education and Science Committee of the Ministry of Education,Science,Culture,and Sport of the Republic of Armenia Project No.23RL-2A031D.M.T.acknowledges support from the M.V.Lomonosov Moscow State University Program of Development.
文摘The emergence of van der Waals(vdW)materials resulted in the discovery of their high optical,mechanical,and electronic anisotropic properties,immediately enabling countless novel phenomena and applications.Such success inspired an intensive search for the highest possible anisotropic properties among vdW materials.Furthermore,the identification of the most promising among the huge family of vdW materials is a challenging quest requiring innovative approaches.Here,we suggest an easy-to-use method for such a survey based on the crystallographic geometrical perspective of vdW materials followed by their optical characterization.Using our approach,we found As2S3 as a highly anisotropic vdW material.It demonstrates high in-plane optical anisotropy that is~20%larger than for rutile and over two times as large as calcite,high refractive index,and transparency in the visible range,overcoming the century-long record set by rutile.Given these benefits,As2S3 opens a pathway towards nextgeneration nanophotonics as demonstrated by an ultrathin true zero-order quarter-wave plate that combines classical and the Fabry–Pérot optical phase accumulations.Hence,our approach provides an effective and easy-to-use method to find vdW materials with the utmost anisotropic properties.
