An efficient and green method has been developed for the synthesis of 2H-indazolo[2,1-b]phthalazinetriones derivatives by employing 15 mol%β-cyclodextrinvia a one-pot multicomponent reaction of aldehyde,dimedone,hydr...An efficient and green method has been developed for the synthesis of 2H-indazolo[2,1-b]phthalazinetriones derivatives by employing 15 mol%β-cyclodextrinvia a one-pot multicomponent reaction of aldehyde,dimedone,hydrazine hydrate with succinic anhydride/phthalic anhydride in water at 80 ℃ for first time.The catalyst could be recovered and reused for four consecutive cycles without appreciable loss in catalytic activity and evaluated for in vitro antimicrobial activity against different Gram-positive and Gram-negative bacterial strains.The outcome of the screening study showed that compound 6d,6f and7 n exhibited excellent activity against E.coil.Whereas,compound 6f and 6h exhibited excellent activity against P.aeurginosa,and compound 6c,and 6e displayed again excellent activity against Staphylococcus aureus whereas compound 7o shows excellent activity against S.aureus and B.subtilis when compared with Ampicillin（standard control）.The results indicated that maximum compounds are moderately effective against bacterial growth and their effectiveness is highest against standard drugs.展开更多
Monolayer group VI transition metal dichalcogenides(TMDs)have recently emerged as promising candidates for photonic and opto-valleytronic applications.The optoelectronic properties of these atomically-thin semiconduct...Monolayer group VI transition metal dichalcogenides(TMDs)have recently emerged as promising candidates for photonic and opto-valleytronic applications.The optoelectronic properties of these atomically-thin semiconducting crystals are strongly governed by the tightly bound electron-hole pairs such as excitons and trions(charged excitons).The anomalous spin and valley configurations at the conduction band edges in monolayer WS_(2)give rise to even more fascinating valley many-body complexes.Here we find that the indirect Q valley in the first Brillouin zone of monolayer WS_(2)plays a critical role in the formation of a new excitonic state,which has not been well studied.By employing a high-quality h-BN encapsulated WS_(2)field-effect transistor,we are able to switch the electron concentration within K-Q valleys at conduction band edges.Consequently,a distinct emission feature could be excited at the high electron doping region.Such feature has a competing population with the K valley trion,and experiences nonlinear power-law response and lifetime dynamics under doping.Our findings open up a new avenue for the study of valley many-body physics and quantum optics in semiconducting 2D materials,as well as provide a promising way of valley manipulation for next-generation entangled photonic devices.展开更多
Light-harvesters with long-lived excited states are desired for efficient solar energy conversion systems. Many solar-to-fuel conversion reactions, such as H2 evolution and CO2 reduction, require multiple sequential e...Light-harvesters with long-lived excited states are desired for efficient solar energy conversion systems. Many solar-to-fuel conversion reactions, such as H2 evolution and CO2 reduction, require multiple sequential electron transfer processes, which leads to a complicated situation that excited states involves not only excitons （electron-hole pairs） but also multi-excitons and charged excitons. While long-lived excitons can be obtained in various systems （e.g., semiconductor nanocrystals）, multi-excitons and charged excitons are typically shorted-lived due to nonradiative Auger recombination pathways whereby the recombination energy of an exciton is quickly transferred to the third carrier on a few to hundreds of picoseconds timescale. In this work, we report a study of excitons, trions （an exciton plus an additional charge）, and biexcitons in CdSe/CdTe colloidal quantum wells or nanoplatelets. The type- II band alignment effectively separates electrons and holes in space, leading to a single exciton lifetime of 340 ns which is -2 order of magnitudes longer than that in plane CdSe nanoplatelets. More importantly, the electron-hole separation also dramatically slows down Auger decay, giving rise to a trion lifetime of 70 ns and a biexciton lifetime of 11 ns, among the longest values ever reported for colloidal nanocrystals. The long-lived exciton, trion, and biexciton states, combined with the intrinsically strong light-absorption capability of two-dimensional systems, enable the CdSe/CdTe type-II nanoplatelets as promising light harvesters for efficient solar-to-fuel conversion reactions.展开更多
In this paper, a negatively charged exciton trapped by a spherical parabolic quantum dot has been investigated. The energy spectra of low-lying states are calculated by means of matrix diagonalization. The important f...In this paper, a negatively charged exciton trapped by a spherical parabolic quantum dot has been investigated. The energy spectra of low-lying states are calculated by means of matrix diagonalization. The important feature of the low-lying states of the negatively charged excitons in a spherical quantum dot is obtained via an analysis of the energy spectra.展开更多
The achievement of efficient continuous-wave(CW)solid-state lasers has been intensively pursued in fields like spectroscopy,data communication,and sensing.However,the realization of CW lasers has been hampered by incr...The achievement of efficient continuous-wave(CW)solid-state lasers has been intensively pursued in fields like spectroscopy,data communication,and sensing.However,the realization of CW lasers has been hampered by increased nonradiative recombi-nation losses under intense photoexcitation.Here,we demonstrate trion-ignited CW lasing in lithium ion(Li^(+))-doped cuboidal perovskite microcrystals(MCs)with impeded Auger decay.Incorporating Li^(+)into perovskite MCs populates the conduction band with permanent charges,which subsequently bind with excitons through Coulomb interaction to create trions.These generated trions significantly prolong optical gain lifetime as their radiative decay prevails over Auger recombination,facilitating the achieve-ment of population inversion.As a result,the promi-nent emission of trion over exciton and suppression of Auger recombination at low temperatures contrib-ute to the achievement of CW lasing action in such doped MCs.Our work provides a general approach to suppressing nonradiative recombination losses that restrict the implementation of CW and electrically pumped lasers.展开更多
Moirésuperlattices in twisted two-dimensional(2D)van der Waals materials offer a versatile platform for engineering quantum states,leading to breakthroughs in correlated insulating phases,superconductivity,and fl...Moirésuperlattices in twisted two-dimensional(2D)van der Waals materials offer a versatile platform for engineering quantum states,leading to breakthroughs in correlated insulating phases,superconductivity,and flat-band physics.In particular,the Moirépotential in twisted transition metal dichalcogenides(TMDs)can trap excitons and trions,resulting in quantized energy levels and emergent many-body interactions.However,methods for precisely modulating excitonic complexes in these systems remain insufficiently explored.Here,we fabricate 1.3°-twisted R-stacked MoSe_(2)homobilayers on prepatterned substrates and investigate strain-engineered Moirétrions using spectroscopic techniques at variable temperatures and magnetic fields.In strained twisted MoSe_(2),we observe a significant increase in Moirétrion emission multiplicity,accompanied by a 65%reduction in linewidth.Raman spectroscopy,second-harmonic generation(SHG)analysis,and density functional theory(DFT)calculations reveal that the enhanced splitting and localization of Moirétrion emissions are due to broken symmetry and stronger lattice reconfiguration induced by uniaxial strain,which lifts the degeneracy of flat bands and spatially confines the Moirépotential.This work advances the understanding of strain-coupled Moiréphysics and paves the way for developing quantum light sources and information devices based on Moiré superlattices.展开更多
Mixed dimensional van der Waals(VdW)heterostructures constructed by one-dimensional(1D)and two-dimensional(2D)materials exhibit extra degree of freedom to modulate the electronic and optical properties due to the comb...Mixed dimensional van der Waals(VdW)heterostructures constructed by one-dimensional(1D)and two-dimensional(2D)materials exhibit extra degree of freedom to modulate the electronic and optical properties due to the combination of difterent dimensionalities.The charge transfer at the intertace between 1D and 2D materials plays a crucial role in the optoelectronic properties and performance of the heterostructure-based devices.Here,we stacked single-walled carbon nanotubes(SWNTs)on monolayer WS2 for a mixed dimensional vdW heterostructure,and investigated the local modulation of excitions and trions in WS2 by SWNTs.Different directions of charge transfer between SWNTs and WSz are evidenced by the photoluminescence(PL)spectra of WS2.The PL intensity can be either enhanced or weakened by individual SWNTs.In our work,the PL intensity of WS2 is enhanced and the exciton peak position heterostructure is red-shifted about 3 meV due to the charge transfer from WS2 to an individual SWNT(SWNT#1).The change of PL by another SWNT(SWNT#2)can not be well-resolved in far fild,but scanning near field optical microscope(SNOM)measurements show that the PL intensity of WS2 is weakened by the SWNT.The peak position of exciton is blue-shifted by^1 meV while that of trion is redshifted by^1 meV due to the charge transfer from the SWNT to WS2,These results give insight into the charge transfer at the interface of SWNTWS2 heterostructure,and can be useful for design of optoelectronic devices based on mixed dimensional vdW heterostructures.展开更多
Strain-engineered silicon nanocrystals(SiNCs)have recently been shown to possess direct bandgap.Here,we report the observation of a rich structure in the single-nanocrystal photoluminescence spectra of strain-engineer...Strain-engineered silicon nanocrystals(SiNCs)have recently been shown to possess direct bandgap.Here,we report the observation of a rich structure in the single-nanocrystal photoluminescence spectra of strain-engineered direct-bandgap SiNCs in the temperature range of 9–300 K.The relationship between individual types of spectra is discussed,and the numerical modeling of spectral diffusion of the experimentally acquired spectra reveals a common origin for most types.The intrinsic spectral shape is shown to be a structure that contains three peaks,approximately 150 meV apart,each of which possesses a Si phonon substructure.Narrow spectral lines,reaching ≤ meV at 20 K,are detected.The observed temperature dependence of the spectral structure can be assigned to the radiative recombination of positively charged trions,in contrast to several previous reports linking a very similar shape to phonons in the surface capping layers.Our result serves as strong additional support for the direct-bandgap nature of the investigated SiNCs.展开更多
A convenient,economical and green approach to the synthesis of 1H-indazolo[1,2-b]phthalazine-1,6,11-trione derivatives has been achieved via a one-pot protocol using phthalhydrazide,a cyclic-β-diketone and an aldehyd...A convenient,economical and green approach to the synthesis of 1H-indazolo[1,2-b]phthalazine-1,6,11-trione derivatives has been achieved via a one-pot protocol using phthalhydrazide,a cyclic-β-diketone and an aldehyde in the presence of a ceric ammonium nitrate catalyst in polyethylene glycol.The simple work up,mild conditions,excellent yields,inexpensive and non-toxic catalyst and simple solvent recyclability render this protocol both attractive and economically viable.展开更多
基金supported by Special Assistance Programme SAP,University Grants Commission,New Delhi,India
文摘An efficient and green method has been developed for the synthesis of 2H-indazolo[2,1-b]phthalazinetriones derivatives by employing 15 mol%β-cyclodextrinvia a one-pot multicomponent reaction of aldehyde,dimedone,hydrazine hydrate with succinic anhydride/phthalic anhydride in water at 80 ℃ for first time.The catalyst could be recovered and reused for four consecutive cycles without appreciable loss in catalytic activity and evaluated for in vitro antimicrobial activity against different Gram-positive and Gram-negative bacterial strains.The outcome of the screening study showed that compound 6d,6f and7 n exhibited excellent activity against E.coil.Whereas,compound 6f and 6h exhibited excellent activity against P.aeurginosa,and compound 6c,and 6e displayed again excellent activity against Staphylococcus aureus whereas compound 7o shows excellent activity against S.aureus and B.subtilis when compared with Ampicillin（standard control）.The results indicated that maximum compounds are moderately effective against bacterial growth and their effectiveness is highest against standard drugs.
基金the strong support from Singapore Ministry of Education via AcRF Tier 3 Programme “Geometrical Quantum Materials” (MOE2018-T3-1-002)AcRF Tier 2 grants (MOE2017-T2-1040)+7 种基金the National Natural Science Foundation of China (Grant No. 61435010)the National Natural Science Foundation of China (Grant No. 61905156)the National Natural Science Foundation of China (Grant No. 61575010)the China Postdoctoral Science Foundation (Grant No. 2017M622764)the Natural Science Foundation of Fujian Province (Grant No. 2022J01555)the Beijing Municipal Natural Science Foundation (Grant No. 4162016)the financial support of the Presidential Postdoctoral Fellowship program of the Nanyang Technological Universitysupport from the Elemental Strategy Initiative conducted by the MEXT, Japan and the CREST (JPMJCR15F3), JST
文摘Monolayer group VI transition metal dichalcogenides(TMDs)have recently emerged as promising candidates for photonic and opto-valleytronic applications.The optoelectronic properties of these atomically-thin semiconducting crystals are strongly governed by the tightly bound electron-hole pairs such as excitons and trions(charged excitons).The anomalous spin and valley configurations at the conduction band edges in monolayer WS_(2)give rise to even more fascinating valley many-body complexes.Here we find that the indirect Q valley in the first Brillouin zone of monolayer WS_(2)plays a critical role in the formation of a new excitonic state,which has not been well studied.By employing a high-quality h-BN encapsulated WS_(2)field-effect transistor,we are able to switch the electron concentration within K-Q valleys at conduction band edges.Consequently,a distinct emission feature could be excited at the high electron doping region.Such feature has a competing population with the K valley trion,and experiences nonlinear power-law response and lifetime dynamics under doping.Our findings open up a new avenue for the study of valley many-body physics and quantum optics in semiconducting 2D materials,as well as provide a promising way of valley manipulation for next-generation entangled photonic devices.
文摘Light-harvesters with long-lived excited states are desired for efficient solar energy conversion systems. Many solar-to-fuel conversion reactions, such as H2 evolution and CO2 reduction, require multiple sequential electron transfer processes, which leads to a complicated situation that excited states involves not only excitons （electron-hole pairs） but also multi-excitons and charged excitons. While long-lived excitons can be obtained in various systems （e.g., semiconductor nanocrystals）, multi-excitons and charged excitons are typically shorted-lived due to nonradiative Auger recombination pathways whereby the recombination energy of an exciton is quickly transferred to the third carrier on a few to hundreds of picoseconds timescale. In this work, we report a study of excitons, trions （an exciton plus an additional charge）, and biexcitons in CdSe/CdTe colloidal quantum wells or nanoplatelets. The type- II band alignment effectively separates electrons and holes in space, leading to a single exciton lifetime of 340 ns which is -2 order of magnitudes longer than that in plane CdSe nanoplatelets. More importantly, the electron-hole separation also dramatically slows down Auger decay, giving rise to a trion lifetime of 70 ns and a biexciton lifetime of 11 ns, among the longest values ever reported for colloidal nanocrystals. The long-lived exciton, trion, and biexciton states, combined with the intrinsically strong light-absorption capability of two-dimensional systems, enable the CdSe/CdTe type-II nanoplatelets as promising light harvesters for efficient solar-to-fuel conversion reactions.
基金The project supported by National Natural Science Foundation of China under Grant No. 10475021 and the Natured Science Foundation of Guangdong Province of China under Grant No. 04009519
文摘In this paper, a negatively charged exciton trapped by a spherical parabolic quantum dot has been investigated. The energy spectra of low-lying states are calculated by means of matrix diagonalization. The important feature of the low-lying states of the negatively charged excitons in a spherical quantum dot is obtained via an analysis of the energy spectra.
基金supported financially by the Ministry of Science and Technology of China(grant no.2022YFA1204403,2020YFA0714601,2018YFA0704802)the National Natural Science Foundation of China(grant no.22090023)+1 种基金the Chinese Academy of Sciences(grant no.XDB0520203)the Beijing National Laboratory for Molecular Sciences(grant no.BNLMS-CXXM-202405).
文摘The achievement of efficient continuous-wave(CW)solid-state lasers has been intensively pursued in fields like spectroscopy,data communication,and sensing.However,the realization of CW lasers has been hampered by increased nonradiative recombi-nation losses under intense photoexcitation.Here,we demonstrate trion-ignited CW lasing in lithium ion(Li^(+))-doped cuboidal perovskite microcrystals(MCs)with impeded Auger decay.Incorporating Li^(+)into perovskite MCs populates the conduction band with permanent charges,which subsequently bind with excitons through Coulomb interaction to create trions.These generated trions significantly prolong optical gain lifetime as their radiative decay prevails over Auger recombination,facilitating the achieve-ment of population inversion.As a result,the promi-nent emission of trion over exciton and suppression of Auger recombination at low temperatures contrib-ute to the achievement of CW lasing action in such doped MCs.Our work provides a general approach to suppressing nonradiative recombination losses that restrict the implementation of CW and electrically pumped lasers.
基金support of the National Natural Science Foundation of China(Nos.52373311 and 62274151)the Innovation Programme for Quantum Science and Technology(No.2021ZD0301605)+4 种基金the High-Performance Complex Manufacturing Key State Laboratory Project at Central South University(No.ZZYJKT2020-12)for their significant contributionsthe Australian Research Council(ARC Discovery Project,DP180102976)for its pivotal role in advancing this researchsupport from the National Natural Science Foundation of China(Nos.92263202 and 11974387)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB33000000)the National Key Research and Development Program of China(No.2020YFA0711502).
文摘Moirésuperlattices in twisted two-dimensional(2D)van der Waals materials offer a versatile platform for engineering quantum states,leading to breakthroughs in correlated insulating phases,superconductivity,and flat-band physics.In particular,the Moirépotential in twisted transition metal dichalcogenides(TMDs)can trap excitons and trions,resulting in quantized energy levels and emergent many-body interactions.However,methods for precisely modulating excitonic complexes in these systems remain insufficiently explored.Here,we fabricate 1.3°-twisted R-stacked MoSe_(2)homobilayers on prepatterned substrates and investigate strain-engineered Moirétrions using spectroscopic techniques at variable temperatures and magnetic fields.In strained twisted MoSe_(2),we observe a significant increase in Moirétrion emission multiplicity,accompanied by a 65%reduction in linewidth.Raman spectroscopy,second-harmonic generation(SHG)analysis,and density functional theory(DFT)calculations reveal that the enhanced splitting and localization of Moirétrion emissions are due to broken symmetry and stronger lattice reconfiguration induced by uniaxial strain,which lifts the degeneracy of flat bands and spatially confines the Moirépotential.This work advances the understanding of strain-coupled Moiréphysics and paves the way for developing quantum light sources and information devices based on Moiré superlattices.
基金the National Basic Research Program of China(Nos.2018YFA0703502 and 2016YFA0200104)the National Natural Science Foundation of China(Nos.51720105003,21790052,21573004 and 21974004).
文摘Mixed dimensional van der Waals(VdW)heterostructures constructed by one-dimensional(1D)and two-dimensional(2D)materials exhibit extra degree of freedom to modulate the electronic and optical properties due to the combination of difterent dimensionalities.The charge transfer at the intertace between 1D and 2D materials plays a crucial role in the optoelectronic properties and performance of the heterostructure-based devices.Here,we stacked single-walled carbon nanotubes(SWNTs)on monolayer WS2 for a mixed dimensional vdW heterostructure,and investigated the local modulation of excitions and trions in WS2 by SWNTs.Different directions of charge transfer between SWNTs and WSz are evidenced by the photoluminescence(PL)spectra of WS2.The PL intensity can be either enhanced or weakened by individual SWNTs.In our work,the PL intensity of WS2 is enhanced and the exciton peak position heterostructure is red-shifted about 3 meV due to the charge transfer from WS2 to an individual SWNT(SWNT#1).The change of PL by another SWNT(SWNT#2)can not be well-resolved in far fild,but scanning near field optical microscope(SNOM)measurements show that the PL intensity of WS2 is weakened by the SWNT.The peak position of exciton is blue-shifted by^1 meV while that of trion is redshifted by^1 meV due to the charge transfer from the SWNT to WS2,These results give insight into the charge transfer at the interface of SWNTWS2 heterostructure,and can be useful for design of optoelectronic devices based on mixed dimensional vdW heterostructures.
基金Czech Science Foundation Funding(Grant Nos.GPP204/12/P235(Katerina Kusova)and P108/12/G108(Ivan Pelant))and a L’Oreal-UNESCO for Women in Science scholarship(Katerina Kusova)are gratefully acknowledgedPart of this work was supported by the Czech-Japan collaborative project LG14246(Jan Valenta).
文摘Strain-engineered silicon nanocrystals(SiNCs)have recently been shown to possess direct bandgap.Here,we report the observation of a rich structure in the single-nanocrystal photoluminescence spectra of strain-engineered direct-bandgap SiNCs in the temperature range of 9–300 K.The relationship between individual types of spectra is discussed,and the numerical modeling of spectral diffusion of the experimentally acquired spectra reveals a common origin for most types.The intrinsic spectral shape is shown to be a structure that contains three peaks,approximately 150 meV apart,each of which possesses a Si phonon substructure.Narrow spectral lines,reaching ≤ meV at 20 K,are detected.The observed temperature dependence of the spectral structure can be assigned to the radiative recombination of positively charged trions,in contrast to several previous reports linking a very similar shape to phonons in the surface capping layers.Our result serves as strong additional support for the direct-bandgap nature of the investigated SiNCs.
文摘A convenient,economical and green approach to the synthesis of 1H-indazolo[1,2-b]phthalazine-1,6,11-trione derivatives has been achieved via a one-pot protocol using phthalhydrazide,a cyclic-β-diketone and an aldehyde in the presence of a ceric ammonium nitrate catalyst in polyethylene glycol.The simple work up,mild conditions,excellent yields,inexpensive and non-toxic catalyst and simple solvent recyclability render this protocol both attractive and economically viable.
