In recent years,Janus two-dimensional(2D)materials have received extensive research interests because of their outstanding electronic,mechanical,electromechanical,and optoelectronic properties.In this work,we explore ...In recent years,Janus two-dimensional(2D)materials have received extensive research interests because of their outstanding electronic,mechanical,electromechanical,and optoelectronic properties.In this work,we explore the structural,electromechanical,and optoelectronic properties of a novel hypothesized Janus InGaSSe monolayer by means of first-principles calculations.It is confirmed that the Janus InGaSSe monolayer indeed show extraordinary charge transport properties with intrinsic electron mobility of 48139 cm^(2)/(V·s)and hole mobility of 16311 cm^(2)/(V·s).Both uniaxial and biaxial strains can effectively tune its electronic property.Moreover,the Janus InGaSSe monolayer possesses excellent piezoelectric property along both inplane and out-of-plane directions.The results of this work imply that the Janus InGaSSe monolayer is in fact an efficient photocatalyst candidate,and may provide useful guidelines for the discovery of other new 2D photocatalytic and piezoelectric materials.展开更多
A two-dimensional(2D)MA_(2)Z_(4)family with and phases has been attracting tremendous interest,the MoSi_(2)N_(4)and WSi_(2)N_(4)of which have been successfully fabricated(Science 369,670(2020)).Janus monolayers have b...A two-dimensional(2D)MA_(2)Z_(4)family with and phases has been attracting tremendous interest,the MoSi_(2)N_(4)and WSi_(2)N_(4)of which have been successfully fabricated(Science 369,670(2020)).Janus monolayers have been achieved in many 2D families,so it is interesting to construct a Janus monolayer from the MA_(2)Z_(4)family.In this work,Janus MSiGeN4(M=Zr and Hf)monolayers are predicted from-MA_(2)Z_(4),which exhibit dynamic,mechanical and thermal stabilities.It is found that they are indirect band-gap semiconductors by using generalized gradient approximation(GGA)plus spin-orbit coupling(SOC).With biaxial strain a/a0 from 0.90 to 1.10,the energy band gap shows a nonmonotonic behavior due to a change of conduction band minimum(CBM).A semiconductor to metal transition can be induced by both compressive and tensile strains,and the phase trans-formation point is about 0.96 for compressive strain and 1.10 for tensile strain.The tensile strain can change the positions of CBM and valence band maximum(VBM),and can also induce the weak Rashba-type spin splitting near CBM.For MSiGeN4(M=Zr and Hf)monolayers,both an in-plane and out-of-plane piezoelectric response can be produced,when a uniaxial strain in the basal plane is applied,which reveals the potential as piezoelectric 2D materials.The high absorption coefficients in the visible light region suggest that MSiGeN4(M=Zr and Hf)monolayers have potential photocatalytic applications.Our works provide an idea to achieve a Janus structure from the MA_(2)Z_(4)family,and can hopefully inspire further research exploring Janus MA_(2)Z_(4)monolayers.展开更多
The transition metal dichalcogenides(TMD)monolayers have shown strong second-harmonic generation(SHG)ow-ing to their lack of inversion symmetry.These ultrathin layers then serve as the frequency converters that can be...The transition metal dichalcogenides(TMD)monolayers have shown strong second-harmonic generation(SHG)ow-ing to their lack of inversion symmetry.These ultrathin layers then serve as the frequency converters that can be intergraded on a chip.Here,taking MoSSe as an example,we report the first detailed experimental study of the SHG of Janus TMD monolayer,in which the transition metal layer is sandwiched by the two distinct chalcogen layers.It is shown that the SHG effectively arises from an in-plane second-harmonic polarization under paraxial focusing and detection.Based on this,the orientation-resolved SHG spectroscopy is realized to readily determine the zigzag and armchair axes of the Janus crystal with an accuracy better than±0.6°.Moreover,the SHG intensity is wavelength-dependent and can be greatly enhanced(~60 times)when the two-photon transition is resonant with the C-exciton state.Our findings uncover the SHG properties of Janus MoSSe monolayer,therefore lay the basis for its integrated frequency-doubling applications.展开更多
First-principles calculations are performed to investigate the effect of strain on the electrochemical performance of Janus MoSSe monolayer.The calculation focuses on the specific capacity,intercalation potential,elec...First-principles calculations are performed to investigate the effect of strain on the electrochemical performance of Janus MoSSe monolayer.The calculation focuses on the specific capacity,intercalation potential,electronic structure,and migration behavior of Li-ion under various strains by using the climbing-image nudged elastic band method.The result shows that the specific capacity is nearly unchanged under strain.But interestingly,the tensile strain can cause the intercalation potential and Li-ion migration energy barrier increase in MoSSe monolayer,whereas the compressive strain can lead to the intercalation potential and energy barrier decreasing.Thus,the rate performance of the MoSSe anode is improved.By analyzing the potential energy surface of MoSSe surface and equilibrium adsorption distance of Li-ion,we explain the physical origin of the change in the intercalation potential and migration energy barrier.The increase of MoSSe potential energy surface and the decrease of adsorption distance caused by tensile strain are the main reason that hinders Li-ion migration.展开更多
Janus transition metal dichalcogenides(TMDs)structures,as a new type of two-dimensional layered materials,have drawn increasing research efforts mostly by the Raman characterization technique since their successful sy...Janus transition metal dichalcogenides(TMDs)structures,as a new type of two-dimensional layered materials,have drawn increasing research efforts mostly by the Raman characterization technique since their successful synthesis.First-and second-order resonant Raman spectra(RRS)have been reported by experiments.But,unlike much interest paid to the first-order RRS,there has been so far no much discussion dedicated to the second-order double resonant Raman(DRR)bands and band assignments of Janus TMDs,which nevertheless is indispensable but hampered by the difficulty of calculations.In this work,we calculate the DRR spectra of Janus Mo SSe monolayer within the first-principles framework and succeed in achieving accurate assignments of the DRR bands.The assignments are in agreement with our group theoretical analysis.Moreover,taking advantage of its strain-sensitive feature,we calculate the DRR spectra under biaxial strain,and further verify the rationality of our assignments by analyzing strain-induced shift of the DRR bands.Our present study supplies an efficient strategy for quantitative understanding on the electron-phonon coupling in the Janus structures.展开更多
基金supported by the Fundamental Research Funds for the Central Universities of China(Nos.PA2021KCPY0029 and LEM21A01)。
文摘In recent years,Janus two-dimensional(2D)materials have received extensive research interests because of their outstanding electronic,mechanical,electromechanical,and optoelectronic properties.In this work,we explore the structural,electromechanical,and optoelectronic properties of a novel hypothesized Janus InGaSSe monolayer by means of first-principles calculations.It is confirmed that the Janus InGaSSe monolayer indeed show extraordinary charge transport properties with intrinsic electron mobility of 48139 cm^(2)/(V·s)and hole mobility of 16311 cm^(2)/(V·s).Both uniaxial and biaxial strains can effectively tune its electronic property.Moreover,the Janus InGaSSe monolayer possesses excellent piezoelectric property along both inplane and out-of-plane directions.The results of this work imply that the Janus InGaSSe monolayer is in fact an efficient photocatalyst candidate,and may provide useful guidelines for the discovery of other new 2D photocatalytic and piezoelectric materials.
基金supported by Natural Science Basis Research Plan in Shaanxi Province of China(2021JM-456)。
文摘A two-dimensional(2D)MA_(2)Z_(4)family with and phases has been attracting tremendous interest,the MoSi_(2)N_(4)and WSi_(2)N_(4)of which have been successfully fabricated(Science 369,670(2020)).Janus monolayers have been achieved in many 2D families,so it is interesting to construct a Janus monolayer from the MA_(2)Z_(4)family.In this work,Janus MSiGeN4(M=Zr and Hf)monolayers are predicted from-MA_(2)Z_(4),which exhibit dynamic,mechanical and thermal stabilities.It is found that they are indirect band-gap semiconductors by using generalized gradient approximation(GGA)plus spin-orbit coupling(SOC).With biaxial strain a/a0 from 0.90 to 1.10,the energy band gap shows a nonmonotonic behavior due to a change of conduction band minimum(CBM).A semiconductor to metal transition can be induced by both compressive and tensile strains,and the phase trans-formation point is about 0.96 for compressive strain and 1.10 for tensile strain.The tensile strain can change the positions of CBM and valence band maximum(VBM),and can also induce the weak Rashba-type spin splitting near CBM.For MSiGeN4(M=Zr and Hf)monolayers,both an in-plane and out-of-plane piezoelectric response can be produced,when a uniaxial strain in the basal plane is applied,which reveals the potential as piezoelectric 2D materials.The high absorption coefficients in the visible light region suggest that MSiGeN4(M=Zr and Hf)monolayers have potential photocatalytic applications.Our works provide an idea to achieve a Janus structure from the MA_(2)Z_(4)family,and can hopefully inspire further research exploring Janus MA_(2)Z_(4)monolayers.
基金This work was supported by the National Natural Science Foundation of China(Grant Nos.61888102,51771224,and 62175253)the National Key R&D Program of China(Grant Nos.2018YFA0305803 and 2019YFA0308501)+4 种基金the Chinese Academy of Sciences(Grant Nos.XDB33030100 and XDB30010000)J.S.and X.L.thank the supports from the National Natural Science Foundation of China(Grant Nos.20173025,22073022,and 11874130)the National Key R&D Program of China(Grant No.2017YFA0205004)the Chinese Academy of Sciences(Grant Nos.XDB3600000 and Y950291)the DNL Cooperation Fund(Grant No.DNL202016).
文摘The transition metal dichalcogenides(TMD)monolayers have shown strong second-harmonic generation(SHG)ow-ing to their lack of inversion symmetry.These ultrathin layers then serve as the frequency converters that can be intergraded on a chip.Here,taking MoSSe as an example,we report the first detailed experimental study of the SHG of Janus TMD monolayer,in which the transition metal layer is sandwiched by the two distinct chalcogen layers.It is shown that the SHG effectively arises from an in-plane second-harmonic polarization under paraxial focusing and detection.Based on this,the orientation-resolved SHG spectroscopy is realized to readily determine the zigzag and armchair axes of the Janus crystal with an accuracy better than±0.6°.Moreover,the SHG intensity is wavelength-dependent and can be greatly enhanced(~60 times)when the two-photon transition is resonant with the C-exciton state.Our findings uncover the SHG properties of Janus MoSSe monolayer,therefore lay the basis for its integrated frequency-doubling applications.
基金Project supported by the Education Department of Jiangxi Province,China(Grant No.GJJ160337)。
文摘First-principles calculations are performed to investigate the effect of strain on the electrochemical performance of Janus MoSSe monolayer.The calculation focuses on the specific capacity,intercalation potential,electronic structure,and migration behavior of Li-ion under various strains by using the climbing-image nudged elastic band method.The result shows that the specific capacity is nearly unchanged under strain.But interestingly,the tensile strain can cause the intercalation potential and Li-ion migration energy barrier increase in MoSSe monolayer,whereas the compressive strain can lead to the intercalation potential and energy barrier decreasing.Thus,the rate performance of the MoSSe anode is improved.By analyzing the potential energy surface of MoSSe surface and equilibrium adsorption distance of Li-ion,we explain the physical origin of the change in the intercalation potential and migration energy barrier.The increase of MoSSe potential energy surface and the decrease of adsorption distance caused by tensile strain are the main reason that hinders Li-ion migration.
基金financially supported by the National Natural Science Foundation of China(No.52031014)the National Key R&D Program of China(No.2017YFA0206301)。
文摘Janus transition metal dichalcogenides(TMDs)structures,as a new type of two-dimensional layered materials,have drawn increasing research efforts mostly by the Raman characterization technique since their successful synthesis.First-and second-order resonant Raman spectra(RRS)have been reported by experiments.But,unlike much interest paid to the first-order RRS,there has been so far no much discussion dedicated to the second-order double resonant Raman(DRR)bands and band assignments of Janus TMDs,which nevertheless is indispensable but hampered by the difficulty of calculations.In this work,we calculate the DRR spectra of Janus Mo SSe monolayer within the first-principles framework and succeed in achieving accurate assignments of the DRR bands.The assignments are in agreement with our group theoretical analysis.Moreover,taking advantage of its strain-sensitive feature,we calculate the DRR spectra under biaxial strain,and further verify the rationality of our assignments by analyzing strain-induced shift of the DRR bands.Our present study supplies an efficient strategy for quantitative understanding on the electron-phonon coupling in the Janus structures.