Revealing the factors that affect the vibrational frequency of Stark probe at interface is a pre-requirement for evaluating the absolute interfacial electric field.Here using surface-enhanced infrared absorption(SEIRA...Revealing the factors that affect the vibrational frequency of Stark probe at interface is a pre-requirement for evaluating the absolute interfacial electric field.Here using surface-enhanced infrared absorption(SEIRA)spectroscopy,attenuated total reflection(ATR)spectroscopy and molecular dynamics(MD),we reveal the assembled C≡N at gold nanofilm exhibits a reduced Stark tuning rate(STR)referring to the vibrational frequency shift in response to electric field comparing with the bulk which was regulated by the electron transfer between S and Au.These findings lead to a deeper understanding of the vibrational Stark effect at the interface and provide guidance for improving the interface electric field theory.展开更多
Semiconductor moirésuperlattices provide great platforms for exploring exotic collective excitations.Optical Stark effect,a shift of the electronic transition in the presence of a light field,provides an ultrafas...Semiconductor moirésuperlattices provide great platforms for exploring exotic collective excitations.Optical Stark effect,a shift of the electronic transition in the presence of a light field,provides an ultrafast and coherent method of manipulating matter states,which,however,has not been demonstrated in moirématerials.Here,we report the valleyselective optical Stark effect of moiréexcitons in the WSe_(2)/WS_(2)superlattice by using transient reflection spectroscopy.Prominent valley-selective energy shifts up to 7.8 meV have been observed for moiréexcitons,corresponding to pseudomagnetic fields as large as 34 T.Our results provide a route to coherently manipulate exotic states in moirésuperlattices.展开更多
Optical temperature sensing based on the fluorescence intensity ratio(FIR)of red emission for lanthanide ions holds significant relevance in non-contact temperature measurement for biological application.In this study...Optical temperature sensing based on the fluorescence intensity ratio(FIR)of red emission for lanthanide ions holds significant relevance in non-contact temperature measurement for biological application.In this study,the perovskite-structured KZnF_(3)is utilized as a host material for Er^(3+)to achieve a high-purity upconversion(UC)red emission.The observed Stark splitting of the red emission peak provides evidence of the energy level splitting of Er^(3+).Group theory is employed to decompose the spectral branching of Er^(3+)under the point group symmetry of KZnF_(3),allowing for the derivation of Stark splitting energy levels induced by the crystal field effect.The optical temperature-sensing behavior of the red UC luminescence was investigated,specifically examining the FIR of the splitting sub-peaks,which exhibited an exponential relationship with temperature.The KZnF_(3):Yb^(3+),Er^(3+)demonstrated a relative sensitivity(S_(r))of 0.00182%·K^(-1)at 298 K,highlighting its excellent response to temperature.Ex vivo bio-thermometry experiments conducted on chicken breast validated the material's ability to penetrate biological tissues and showed its significant sensitivity of the FIR to temperature.These results establish KZnF_(3):Yb^(3+),Er^(3+)as a promising material for optical thermometry in various biological applications.展开更多
This study investigates the properties of exciton-polaritons in a two-dimensional(2D)hybrid organic-inorganic perovskite microcavity in the presence of optical Stark effect.Through both steady and dynamic state analys...This study investigates the properties of exciton-polaritons in a two-dimensional(2D)hybrid organic-inorganic perovskite microcavity in the presence of optical Stark effect.Through both steady and dynamic state analyses,strong coupling between excitons of perovskite and cavity photons is revealed,indicating the formation of polaritons in the perovskite microcavity.Besides,it is found that an external optical Stark pulse can induce energy shifts of excitons proportional to the pulse intensity,which modifies the dispersion characteristics of the polaritons.展开更多
Defects can strongly affect the lattice,strain,and electronic structures of nanomaterials photocatalysts,like a double-edged sword of both positive significance and negative influence on photocatalytic performances.To...Defects can strongly affect the lattice,strain,and electronic structures of nanomaterials photocatalysts,like a double-edged sword of both positive significance and negative influence on photocatalytic performances.To date,most studies into defects only partially elucidated their beneficial or detrimental roles in photocatalysis.However,a quantitative understanding of the photocatalytic performances modulated by defect concentration still needs to be discovered.Here,a series of TiO_(2-X)mesoporous spheres(MS)with different oxygen vacancy concentrations for photocatalytic applications were prepared by hightemperature chemical reduction.The link between oxygen vacancy concentration and photocatalytic performance was successfully established.The localization of carriers dominated by the Stark effect is first enhanced and then weakened with increasing oxygen vacancy concentration,which is a crucial factor in explaining the double-edged sword role of defect concentration in photocatalysis.As the reduction temperature rises to 300℃,carrier localization dominated by the quantum-confined Stark effect maximizes the separation ability of photo generated electron hole pairs,thus exhibiting the best catalytic performance for photocatalytic hydrogen production and the degradation of organic pollutants,as demonstrated by a hydrogen evolution rate of 523.7μmol g^(-1)h^(-1)and a ninefold higher RhB photodegradation rate compared to TiO_(2)MS.The work offers excellent flexibility for precisely constructing high-performance photocatalysts by understanding vacancy engineering.展开更多
基金The National Key R&D Program of China(No.2022YFE0113000)the National Science Fund for Distinguished Young Scholars(No.22025406)+1 种基金the National Natural Science Foundation of China(Nos.22074138,12174457)the Youth Innovation Promotion Association of CAS(No.2020233)for financial support。
文摘Revealing the factors that affect the vibrational frequency of Stark probe at interface is a pre-requirement for evaluating the absolute interfacial electric field.Here using surface-enhanced infrared absorption(SEIRA)spectroscopy,attenuated total reflection(ATR)spectroscopy and molecular dynamics(MD),we reveal the assembled C≡N at gold nanofilm exhibits a reduced Stark tuning rate(STR)referring to the vibrational frequency shift in response to electric field comparing with the bulk which was regulated by the electron transfer between S and Au.These findings lead to a deeper understanding of the vibrational Stark effect at the interface and provide guidance for improving the interface electric field theory.
基金Project supported by the National Key R&D Program of China(Grant Nos.2022YFA1402400 and 2022YFA1405400)the National Natural Science Foundation of China(Grant Nos.11934011 and 12274365)+3 种基金Zhejiang Provincial Natural Science Foundation of China(Grant No.LR24A040001)Open project of Key Laboratory of Artificial Structures and Quantum Control(Ministry of Education)of Shanghai Jiao Tong Universitysupport from the JSPS KAKENHI(Grant Nos.20H00354 and 23H02052)World Premier International Research Center Initiative(WPI),MEXT,Japan。
文摘Semiconductor moirésuperlattices provide great platforms for exploring exotic collective excitations.Optical Stark effect,a shift of the electronic transition in the presence of a light field,provides an ultrafast and coherent method of manipulating matter states,which,however,has not been demonstrated in moirématerials.Here,we report the valleyselective optical Stark effect of moiréexcitons in the WSe_(2)/WS_(2)superlattice by using transient reflection spectroscopy.Prominent valley-selective energy shifts up to 7.8 meV have been observed for moiréexcitons,corresponding to pseudomagnetic fields as large as 34 T.Our results provide a route to coherently manipulate exotic states in moirésuperlattices.
基金financially supported by Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)"Qinglan Project"Young and Middle-aged Academic Leaders Program of Jiangsu Province。
文摘Optical temperature sensing based on the fluorescence intensity ratio(FIR)of red emission for lanthanide ions holds significant relevance in non-contact temperature measurement for biological application.In this study,the perovskite-structured KZnF_(3)is utilized as a host material for Er^(3+)to achieve a high-purity upconversion(UC)red emission.The observed Stark splitting of the red emission peak provides evidence of the energy level splitting of Er^(3+).Group theory is employed to decompose the spectral branching of Er^(3+)under the point group symmetry of KZnF_(3),allowing for the derivation of Stark splitting energy levels induced by the crystal field effect.The optical temperature-sensing behavior of the red UC luminescence was investigated,specifically examining the FIR of the splitting sub-peaks,which exhibited an exponential relationship with temperature.The KZnF_(3):Yb^(3+),Er^(3+)demonstrated a relative sensitivity(S_(r))of 0.00182%·K^(-1)at 298 K,highlighting its excellent response to temperature.Ex vivo bio-thermometry experiments conducted on chicken breast validated the material's ability to penetrate biological tissues and showed its significant sensitivity of the FIR to temperature.These results establish KZnF_(3):Yb^(3+),Er^(3+)as a promising material for optical thermometry in various biological applications.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11974071 and 62375040)the Sichuan Science and Technology Program(Grant Nos.2022ZYD0108 and 2023JDRC0030).
文摘This study investigates the properties of exciton-polaritons in a two-dimensional(2D)hybrid organic-inorganic perovskite microcavity in the presence of optical Stark effect.Through both steady and dynamic state analyses,strong coupling between excitons of perovskite and cavity photons is revealed,indicating the formation of polaritons in the perovskite microcavity.Besides,it is found that an external optical Stark pulse can induce energy shifts of excitons proportional to the pulse intensity,which modifies the dispersion characteristics of the polaritons.
基金supported by the National Key Research and Development Program of China,(No.2019YFA0705201)the National Natural Science Foundation of China(No.U2032129)。
文摘Defects can strongly affect the lattice,strain,and electronic structures of nanomaterials photocatalysts,like a double-edged sword of both positive significance and negative influence on photocatalytic performances.To date,most studies into defects only partially elucidated their beneficial or detrimental roles in photocatalysis.However,a quantitative understanding of the photocatalytic performances modulated by defect concentration still needs to be discovered.Here,a series of TiO_(2-X)mesoporous spheres(MS)with different oxygen vacancy concentrations for photocatalytic applications were prepared by hightemperature chemical reduction.The link between oxygen vacancy concentration and photocatalytic performance was successfully established.The localization of carriers dominated by the Stark effect is first enhanced and then weakened with increasing oxygen vacancy concentration,which is a crucial factor in explaining the double-edged sword role of defect concentration in photocatalysis.As the reduction temperature rises to 300℃,carrier localization dominated by the quantum-confined Stark effect maximizes the separation ability of photo generated electron hole pairs,thus exhibiting the best catalytic performance for photocatalytic hydrogen production and the degradation of organic pollutants,as demonstrated by a hydrogen evolution rate of 523.7μmol g^(-1)h^(-1)and a ninefold higher RhB photodegradation rate compared to TiO_(2)MS.The work offers excellent flexibility for precisely constructing high-performance photocatalysts by understanding vacancy engineering.
