To advance hierarchical equations of motion as a standard theory for quantum dissipative dynamics, we put forward a mixed Heisenberg-SchrSdinger scheme with block-matrix implementation on efficient evaluation of nonli...To advance hierarchical equations of motion as a standard theory for quantum dissipative dynamics, we put forward a mixed Heisenberg-SchrSdinger scheme with block-matrix implementation on efficient evaluation of nonlinear optical response function. The new approach is also integrated with optimized hierarchical theory and numerical filtering algorithm. Different configurations of coherent two-dimensional spectroscopy of model excitonic dimer systems are investigated, with focusing on the effects of intermolecular transfer coupling and bi-exciton interaction.展开更多
As emerging two-dimensional(2D)materials,carbides and nitrides(MXenes)could be solid solutions or organized structures made up of multi-atomic layers.With remarkable and adjustable electrical,optical,mechanical,and el...As emerging two-dimensional(2D)materials,carbides and nitrides(MXenes)could be solid solutions or organized structures made up of multi-atomic layers.With remarkable and adjustable electrical,optical,mechanical,and electrochemical characteristics,MXenes have shown great potential in brain-inspired neuromorphic computing electronics,including neuromorphic gas sensors,pressure sensors and photodetectors.This paper provides a forward-looking review of the research progress regarding MXenes in the neuromorphic sensing domain and discussed the critical challenges that need to be resolved.Key bottlenecks such as insufficient long-term stability under environmental exposure,high costs,scalability limitations in large-scale production,and mechanical mismatch in wearable integration hinder their practical deployment.Furthermore,unresolved issues like interfacial compatibility in heterostructures and energy inefficiency in neu-romorphic signal conversion demand urgent attention.The review offers insights into future research directions enhance the fundamental understanding of MXene properties and promote further integration into neuromorphic computing applications through the convergence with various emerging technologies.展开更多
Two-dimensional conjugated metal-organic framework(2D c-MOF)nanosheets have garnered significant research interest owing to their suite of distinctive properties.Consequently,diverse synthetic methodologies have been ...Two-dimensional conjugated metal-organic framework(2D c-MOF)nanosheets have garnered significant research interest owing to their suite of distinctive properties.Consequently,diverse synthetic methodologies have been established for the fabrication of 2D c-MOFs exhibiting welldefined nanosheet morphology.In addition,the structural engineering of 2D c-MOF nanosheets for energy storage and conversion has emerged as a prominent research focus.This review comprehensively summarizes recent advancements in 2D c-MOF nanosheets.We commence with a concise overview of diverse synthesis strategies for these materials.Subsequently,progress in their utilization as electrode materials or catalysts for batteries,supercapacitors,and electrocatalysis/photocatalysis is systematically examined.Finally,prevailing challenges and prospective research directions are discussed.Collectively,this review aims to stimulate the development of sophisticated 2D c-MOF nanosheets for high-performance energy applications.展开更多
Nanoscale confinement environments often affect the transport mechanisms of nanofluids.Understanding the dynamic behavior of molecules in two-dimensional(2D)confined channels is of great importance in the areas of sen...Nanoscale confinement environments often affect the transport mechanisms of nanofluids.Understanding the dynamic behavior of molecules in two-dimensional(2D)confined channels is of great importance in the areas of sensing,catalysis and energy storage.As a popular candidate for a new type of gas sensing material,MXenes have the problem of nonselectivity towards polar gases with slow responses,which severely limits their applications.Here,we report a study on regulating the confinement effect of 2D channels between MXene layers through annealing treatment and ion(Na^(+))intercalation for high-performance ammonia(NH_(3))sensing.Firstly,the annealing treatment accurately modulates the size of the 2D channels to effectively block the entry of large-size gas molecules and improve the selectivity for NH_(3).Ab initio molecular dynamics(AIMD)also confirms that the modulated channel size has a special"nano-pumping effect",which can accelerate the dynamic behavior of NH_(3) molecules in the 2D confined space.Moreover,the intercalation of Na+ions increases the adsorption capacity of NH_(3).Therefore,the"nano-pumping effect"and theintercalation of Na+ions effectively enhance the response speed and sensitivity of MXene to NH_(3),respectively.The experimental results show that the modified Ti_(3)C_(2) exhibits high sensitivity(0.17),rapid response(181 s),excellent selectivity and stability towards NH_(3).展开更多
To consider the reliability and performance of electronic devices based on polyimide derivatives, dynamic water sorption and diffusion behavior in a polyimide derivative： poly（4＇4 oxydiphenylene pyromellitimide） ...To consider the reliability and performance of electronic devices based on polyimide derivatives, dynamic water sorption and diffusion behavior in a polyimide derivative： poly（4＇4 oxydiphenylene pyromellitimide） （PMDA-ODA）/silica nanocomposite was investigated by two-dimensional ATR-FTIR spectroscopy, by which three states of water molecules owning different H-bonding strength were distinguished. The amounts and strength of H-bonding also played a significant role in determining the diffusion rate of the different states of water molecules. The type of aggregated water molecules which also formed H-bonding with silicic acid （residues） or polyimide system was the last one diffusing to the polymer side in contact with the ATR crystal element because the polymeric matrix blocked their diffusion to a great extent. The diffusion coefficient was also estimated to gain the information of the dynamic diffusion behavior.展开更多
In this study, two-dimensional correlation spectroscopy integrated with synchronous fluorescence and infrared absorption spectroscopy was employed to investigate the interaction between humic acids and aluminum coagul...In this study, two-dimensional correlation spectroscopy integrated with synchronous fluorescence and infrared absorption spectroscopy was employed to investigate the interaction between humic acids and aluminum coagulant at slightly acidic and neutral p H. Higher fluorescence quenching was produced for fulvic-like and humic-like fractions at p H 5. At p H 5, the humic-like fractions originating from the carboxylic acid, carboxyl and polysaccharide compounds were bound to aluminum first, followed by the fulvic-like fractions originating from the carboxyl and polysaccharide compounds. This finding also demonstrated that the activated functional groups of HA were involved in forming the Al-HA complex, which was accompanied by the removal of other groups by co-precipitation.Meanwhile, at p H 7, almost no fluorescence quenching occurred, and surface complexation was observed to occur, in which the activated functional groups were absorbed on the amorphous Al（OH）3. Two-dimensional FT-IR correlation spectroscopy indicated the sequence of HA structural change during coagulation with aluminum, with IR bands affected in the order of COOH〉 COO-〉NH deformation of amide Ⅱ〉 aliphatic hydroxyl C／OH at p H 5, and COO-〉aliphatic hydroxyl C／OH at p H 7. This study provides a promising pathway for analysis and insight into the priority of functional groups in the interaction between organic matters and metal coagulants.展开更多
Generalized two-dimensional correlation spectroscopy （2DCOS） and its derivate technique, perturbation correlation moving window （PCMW）, have found great potential in studying a series of physico-chemical phenomena...Generalized two-dimensional correlation spectroscopy （2DCOS） and its derivate technique, perturbation correlation moving window （PCMW）, have found great potential in studying a series of physico-chemical phenomena in stimuli-responsive polymeric systems. By spreading peaks along a second dimension, 2DCOS can significantly enhance spectral resolution and discern the sequence of group dynamics applicable to various external perturbation-induced spectroscopic changes, especially in infrared （IR）, near-infrared （NIR） and Raman spectroscopy. On the basis of 2DCOS synchronous power spectra changing, PCMW proves to be a powerful tool to monitor complicated spectral variations and to find transition points and ranges. This article reviews the recent work of our research group in the application of 2DCOS and PCMW in thermoresponsive polymers, mainly focused on liquid crystalline polymers and lower critical solution temperature （LCST）-type polymers. Details of group motions and chain conformational changes upon temperature perturbation can thus be elucidated at the molecular level, which contribute to the understanding of their phase transition nature.展开更多
Angle-resolved polarized Raman（ARPR） spectroscopy can be utilized to assign the Raman modes based on crystal symmetry and Raman selection rules and also to characterize the crystallographic orientation of anisotropi...Angle-resolved polarized Raman（ARPR） spectroscopy can be utilized to assign the Raman modes based on crystal symmetry and Raman selection rules and also to characterize the crystallographic orientation of anisotropic materials.However, polarized Raman measurements can be implemented by several different configurations and thus lead to different results. In this work, we systematically analyze three typical polarization configurations： 1） to change the polarization of the incident laser, 2） to rotate the sample, and 3） to set a half-wave plate in the common optical path of incident laser and scattered Raman signal to simultaneously vary their polarization directions. We provide a general approach of polarization analysis on the Raman intensity under the three polarization configurations and demonstrate that the latter two cases are equivalent to each other. Because the basal plane of highly ordered pyrolytic graphite（HOPG） exhibits isotropic feature and its edge plane is highly anisotropic, HOPG can be treated as a modelling system to study ARPR spectroscopy of twodimensional materials on their basal and edge planes. Therefore, we verify the ARPR behaviors of HOPG on its basal and edge planes at three different polarization configurations. The orientation direction of HOPG edge plane can be accurately determined by the angle-resolved polarization-dependent G mode intensity without rotating sample, which shows potential application for orientation determination of other anisotropic and vertically standing two-dimensional materials and other materials.展开更多
Recent noteworthy developments in the field of two-dimensional（2D） correlation spectroscopy are reviewed.2D correlation spectroscopy has become a very popular tool due to its versatility and relative ease of use.The...Recent noteworthy developments in the field of two-dimensional（2D） correlation spectroscopy are reviewed.2D correlation spectroscopy has become a very popular tool due to its versatility and relative ease of use.The technique utilizes a spectroscopic or other analytical probe from a number of selections for a broad range of sample systems by employing different types of external perturbations to induce systematic variations in intensities of spectra.Such spectral intensity variations are then converted into2 D spectra by a form of correlation analysis for subsequent interpretation.Many different types of 2D correlation approaches have been proposed.In particular,2D hetero-correlation and multiple perturbation correlation analyses,including orthogonal sample design scheme,are discussed in this review.Additional references to other important developments in the field of 2D correlation spectroscopy,such as projection correlation and codistribution analysis,were also provided.展开更多
Chinese liquor Moutai is the “National alcoholic drink” in China and plays a very important role of social activities in Chinese people’s life. In pursuit of high profits, some illegal counterfeit Moutai liquors ha...Chinese liquor Moutai is the “National alcoholic drink” in China and plays a very important role of social activities in Chinese people’s life. In pursuit of high profits, some illegal counterfeit Moutai liquors have begun to appear in the market. Therefore, it is an urgent need for new techniques to discriminate the genuine and counterfeit Moutai liquor. In this work, the conventional Ultraviolet-Visible (UV-Vis) spectroscopy and two-dimensional correlation UV-Vis spectroscopy are applied to obtain the UV-Vis characteristic of Moutai liquor and counterfeit one, respectively. The experimental results reveal that the conventional UV-Vis spectra of the genuine and counterfeit Moutai liquor are similar. However, the two-dimensional correlation UV-Vis spectra of them are different and this method would be applied to differentiate the counterfeit Moutai liquor from the genuine Moutai liquor. Compared with conventional methods, this novel method has the advantages of easy operation, simple instrumentation and direct recognition, which make it a potential tool in the fields of food safety.展开更多
A novel compound, （4,4＇-Hbpy）3[NaMo8O26]（4,4＇-bpy）2（H2O）4 1 （bpy=bipydine）, was synthesized by the hydrothermal method. Single-crystal X-ray diffraction shows that compound 1 belongs to the monoclinic system...A novel compound, （4,4＇-Hbpy）3[NaMo8O26]（4,4＇-bpy）2（H2O）4 1 （bpy=bipydine）, was synthesized by the hydrothermal method. Single-crystal X-ray diffraction shows that compound 1 belongs to the monoclinic system, space group C2/m with a=19.1921（5）, b=18.6931（6）, c=9.3821（3） A° β=104.8020（11）°, V=3254.22（17）A°^3 C50H51Mo8N10NaO30, Mr=2062.52, Z=2, F（000）=2016, μ=1.591 mm^-1 and Dc=2.105 g/cm^3. The final R=0.0283 and wR=0.0912 for 3118 observed reflections （I〉20（I））. Compound 1 contains the β-[Mo8O26]^4-anion, sodium ion, 4,4＇-bpy and lattice crystalline water molecules. The β-[MosO26] units link the sodium ion to form a chain structure. The infinitechains of [Na（Mo8O26）]^3- blocks are surrounded by protonized 4,4＇-bpy cations, 4,4＇-bpy and lattice crystalline water molecules. The 2D-IR correlation spectroscopy study indicates that the stretching vibrations of Mo=O occur more preferentially due to the thermal effect. The TGA analysis shows that compound 1 has high thermal stability.展开更多
Two-dimensional Fourier transform(2D FT) spectroscopy is an important technology that developed in recent decades and has many advantages over other ultrafast spectroscopy methods. Although 2D FT spectroscopy provides...Two-dimensional Fourier transform(2D FT) spectroscopy is an important technology that developed in recent decades and has many advantages over other ultrafast spectroscopy methods. Although 2D FT spectroscopy provides great opportunities for studying various complex systems, the experimental implementation and theoretical description of 2D FT spectroscopy measurement still face many challenges, which limits their wide application.Recently, the 2D FT spectroscopy reaches maturity due to many new developments which greatly reduces the technical barrier in the experimental implementation of the 2D FT spectrometer. There have been several different approaches developed for the optical design of the 2D FT spectrometer, each with its own advantages and limitations. Thus, a procedure to help an experimentalist to build a 2D FT spectroscopy experimental apparatus is needed.This tutorial review is intending to provide an accessible introduction for a beginner to build a 2D FT spectrometer.展开更多
Coherent exciton-phonon coupling in CdSe/ZnS nanocrystals have been investigated by temperature-dependent two-dimensional electronic spectroscopy （2DES） measurements. Benefiting from the ability of 2DES to dissect a...Coherent exciton-phonon coupling in CdSe/ZnS nanocrystals have been investigated by temperature-dependent two-dimensional electronic spectroscopy （2DES） measurements. Benefiting from the ability of 2DES to dissect assembles in nanocrystal films, we have dearly identified experimental evidences of coherent coupling between exciton and phonon in CdSe/ZnS nanocrystals. In time domain, 2DES signals of excitonic transitions beat at a frequency resonant to a longitudinal optical phonon mode; in energy domain, phonon side bands are distinct at both Stokes and anti-Stokes sides. When temperature increases, phonon-induced exciton dephasing is observed with dramatic broadening of homogeneous linewidth. The results suggest exciton-phonon coupling is essential in elucidating the quantum dynamics of excitonic transitions in semiconductor nanocrystals.展开更多
Ultrathin van der Waals(vdW)magnets provide a possibility to access magnetic ordering in the two-dimensional(2D)limit,which are expected to be applied in the spintronic devices.Raman spectroscopy is a powerful charact...Ultrathin van der Waals(vdW)magnets provide a possibility to access magnetic ordering in the two-dimensional(2D)limit,which are expected to be applied in the spintronic devices.Raman spectroscopy is a powerful characterization method to investigate the spin-related properties in 2D vdW magnets,including magnon and spin–lattice interaction,which are hardly accessible by other optical methods.In this paper,the recent progress of various magnetic properties in 2D vdW magnets studied by Raman spectroscopy is reviewed,including the magnetic transition,spin-wave,spin–lattice interaction,symmetry tuning induced by spin ordering,and nonreciprocal magneto-phonon Raman scattering.展开更多
The proliferation of wearable biodevices has boosted the development of soft,innovative,and multifunctional materials for human health monitoring.The integration of wearable sensors with intelligent systems is an over...The proliferation of wearable biodevices has boosted the development of soft,innovative,and multifunctional materials for human health monitoring.The integration of wearable sensors with intelligent systems is an overwhelming tendency,providing powerful tools for remote health monitoring and personal health management.Among many candidates,two-dimensional(2D)materials stand out due to several exotic mechanical,electrical,optical,and chemical properties that can be efficiently integrated into atomic-thin films.While previous reviews on 2D materials for biodevices primarily focus on conventional configurations and materials like graphene,the rapid development of new 2D materials with exotic properties has opened up novel applications,particularly in smart interaction and integrated functionalities.This review aims to consolidate recent progress,highlight the unique advantages of 2D materials,and guide future research by discussing existing challenges and opportunities in applying 2D materials for smart wearable biodevices.We begin with an in-depth analysis of the advantages,sensing mechanisms,and potential applications of 2D materials in wearable biodevice fabrication.Following this,we systematically discuss state-of-the-art biodevices based on 2D materials for monitoring various physiological signals within the human body.Special attention is given to showcasing the integration of multi-functionality in 2D smart devices,mainly including self-power supply,integrated diagnosis/treatment,and human–machine interaction.Finally,the review concludes with a concise summary of existing challenges and prospective solutions concerning the utilization of2D materials for advanced biodevices.展开更多
The two-dimensional layered transition metal dichalcogenides provide new opportunities in future valley-based in- formation processing and also provide an ideal platform to study excitonic effects. At the center of va...The two-dimensional layered transition metal dichalcogenides provide new opportunities in future valley-based in- formation processing and also provide an ideal platform to study excitonic effects. At the center of various device physics toward their possible electronic and optoelectronic applications is understanding the dynamical evolution of various many- particle electronic states, especially exciton which dominates the optoelectronic response of TMDs, under the novel con- text of valley degree of freedom. Here, we provide a brief review of experimental advances in using helicity-resolved ultrafast spectroscopy, especially ultrafast pump-probe spectroscopy, to study the dynamical evolution of valley-related many-particle electronic states in semiconducting monolayer transitional metal dichalcogenides.展开更多
A number of useful techniques associated with two-dimensional correlation spectroscopy(2DCOS)to improve its performance and utility have been developed in the last 30years.Evolution of these 2DCOS techniques,including...A number of useful techniques associated with two-dimensional correlation spectroscopy(2DCOS)to improve its performance and utility have been developed in the last 30years.Evolution of these 2DCOS techniques,including some of the very recent developments,is reviewed with examples.Topics include merged or modified asynchronous 2Dcorrelation spectrum,two-dimensional codistribution spectroscopy(2DCDS),Pareto scaling,and null-space projection treatment of spectral dataset.展开更多
A series of soy protein isolate(SPI)films plasticized by glycerol(Gly)were studied using attenuated total reflectance-Fourier transform infrared spectroscopy(ATR/FTIR).Perturbation-correlation movingwindow two-dimensi...A series of soy protein isolate(SPI)films plasticized by glycerol(Gly)were studied using attenuated total reflectance-Fourier transform infrared spectroscopy(ATR/FTIR).Perturbation-correlation movingwindow two-dimensional(PCMW2D)and two-dimensional correlation(2DCOS)analyses were applied to the amideⅠband and thus the hydrogen bond interaction between SPI and Gly was systematically investigated.When Gly concentrations were in the range 0~35%,the hydrogen bond amongβ-sheets was replaced by the one between SPI chain and Gly molecule,which caused these protein chains being changed toα-helix.However,the transformation ofβ-sheet toα-helix was saturated and both of them tend to change to random coil when Gly concentrations were in the range 35%~60%.展开更多
Two-dimensional elec tronic spec troscopy(2DES)is a powerful met hod to probe the coherent electron dynamics in complicated systems.Stabilizing the phase difference of the incident ultrashort pulses is the mos t chall...Two-dimensional elec tronic spec troscopy(2DES)is a powerful met hod to probe the coherent electron dynamics in complicated systems.Stabilizing the phase difference of the incident ultrashort pulses is the mos t challenging par t for experimen tal demonstration of 2DES.Here,we present a tuto rial review on the 2DES proto cols based on active phase managements which are originally developed for quantum optics experiments.We introduce the 2DES techniques in box and pump-probe geometries with phase stabilization realized by interferometry,and outline the fully collinear 2DES approach with the frequency tagging by acoustic optical modulators and frequency combs.The combination of active phase managements,ultrashort pulses and other spectroscopic methods may open new opportunities to tackle essential challenges related to excited states.展开更多
A functional interlayer based on two-dimensional(2D)porous modified vermiculite nanosheets(PVS)was obtained by acid-etching vermiculite nanosheets.The as-obtained 2D porous nanosheets exhibited a high specific surface...A functional interlayer based on two-dimensional(2D)porous modified vermiculite nanosheets(PVS)was obtained by acid-etching vermiculite nanosheets.The as-obtained 2D porous nanosheets exhibited a high specific surface area of 427 m^(2)·g^(-1)and rich surface active sites,which help restrain polysulfides(LiPSs)through good physi-cal and chemical adsorption,while simultaneously accelerating the nucleation and dissolution kinetics of Li_(2)S,effec-tively suppressing the shuttle effect.The assembled lithium-sulfur batteries(LSBs)employing the PVS-based inter-layer delivered a high initial discharge capacity of 1386 mAh·g^(-1)at 0.1C(167.5 mAh·g^(-1)),long-term cycling stabil-ity,and good rate property.展开更多
基金This work was supported by the National Natural Science Foundation of China （No.21033008 and No.21073169）the National Basic Research Program of China （No.2010CB923300 and No.2011CB921400）and the Hong Kong RGC （No.604709） and UGC （AoE/P04/08-2） is gratefully acknowledged.
文摘To advance hierarchical equations of motion as a standard theory for quantum dissipative dynamics, we put forward a mixed Heisenberg-SchrSdinger scheme with block-matrix implementation on efficient evaluation of nonlinear optical response function. The new approach is also integrated with optimized hierarchical theory and numerical filtering algorithm. Different configurations of coherent two-dimensional spectroscopy of model excitonic dimer systems are investigated, with focusing on the effects of intermolecular transfer coupling and bi-exciton interaction.
基金supported by the NSFC(12474071)Natural Science Foundation of Shandong Province(ZR2024YQ051,ZR2025QB50)+6 种基金Guangdong Basic and Applied Basic Research Foundation(2025A1515011191)the Shanghai Sailing Program(23YF1402200,23YF1402400)funded by Basic Research Program of Jiangsu(BK20240424)Open Research Fund of State Key Laboratory of Crystal Materials(KF2406)Taishan Scholar Foundation of Shandong Province(tsqn202408006,tsqn202507058)Young Talent of Lifting engineering for Science and Technology in Shandong,China(SDAST2024QTB002)the Qilu Young Scholar Program of Shandong University。
文摘As emerging two-dimensional(2D)materials,carbides and nitrides(MXenes)could be solid solutions or organized structures made up of multi-atomic layers.With remarkable and adjustable electrical,optical,mechanical,and electrochemical characteristics,MXenes have shown great potential in brain-inspired neuromorphic computing electronics,including neuromorphic gas sensors,pressure sensors and photodetectors.This paper provides a forward-looking review of the research progress regarding MXenes in the neuromorphic sensing domain and discussed the critical challenges that need to be resolved.Key bottlenecks such as insufficient long-term stability under environmental exposure,high costs,scalability limitations in large-scale production,and mechanical mismatch in wearable integration hinder their practical deployment.Furthermore,unresolved issues like interfacial compatibility in heterostructures and energy inefficiency in neu-romorphic signal conversion demand urgent attention.The review offers insights into future research directions enhance the fundamental understanding of MXene properties and promote further integration into neuromorphic computing applications through the convergence with various emerging technologies.
基金supported by the National Natural Science Foundation of China(Nos.22205196 and 52371240)the Natural Science Foundation of Jiangsu Province(No.BK20210790)the start-up fundings from Yangzhou University.
文摘Two-dimensional conjugated metal-organic framework(2D c-MOF)nanosheets have garnered significant research interest owing to their suite of distinctive properties.Consequently,diverse synthetic methodologies have been established for the fabrication of 2D c-MOFs exhibiting welldefined nanosheet morphology.In addition,the structural engineering of 2D c-MOF nanosheets for energy storage and conversion has emerged as a prominent research focus.This review comprehensively summarizes recent advancements in 2D c-MOF nanosheets.We commence with a concise overview of diverse synthesis strategies for these materials.Subsequently,progress in their utilization as electrode materials or catalysts for batteries,supercapacitors,and electrocatalysis/photocatalysis is systematically examined.Finally,prevailing challenges and prospective research directions are discussed.Collectively,this review aims to stimulate the development of sophisticated 2D c-MOF nanosheets for high-performance energy applications.
基金supported by the National Natural Science Foundation of China(Nos.52422505 and 12274124)the Innovative Research Group Project of the National Natural Science Foundation of China(No.52321002).
文摘Nanoscale confinement environments often affect the transport mechanisms of nanofluids.Understanding the dynamic behavior of molecules in two-dimensional(2D)confined channels is of great importance in the areas of sensing,catalysis and energy storage.As a popular candidate for a new type of gas sensing material,MXenes have the problem of nonselectivity towards polar gases with slow responses,which severely limits their applications.Here,we report a study on regulating the confinement effect of 2D channels between MXene layers through annealing treatment and ion(Na^(+))intercalation for high-performance ammonia(NH_(3))sensing.Firstly,the annealing treatment accurately modulates the size of the 2D channels to effectively block the entry of large-size gas molecules and improve the selectivity for NH_(3).Ab initio molecular dynamics(AIMD)also confirms that the modulated channel size has a special"nano-pumping effect",which can accelerate the dynamic behavior of NH_(3) molecules in the 2D confined space.Moreover,the intercalation of Na+ions increases the adsorption capacity of NH_(3).Therefore,the"nano-pumping effect"and theintercalation of Na+ions effectively enhance the response speed and sensitivity of MXene to NH_(3),respectively.The experimental results show that the modified Ti_(3)C_(2) exhibits high sensitivity(0.17),rapid response(181 s),excellent selectivity and stability towards NH_(3).
基金supported by the National Natural Science Foundation of China(No.20573022,No.20425415)the National Basic Research Pro-gram of China(2005CB623800),the PHD Program of M0E(20050246010)the"Qimingxing"Project(No.04QM1402)of Shanghai Municipal Science and Technology Commission,and the"Shuguang"Project(No.01SG05)of the Shanghai Municipal Education Commission and Shanghai Education Development Foundation.
文摘To consider the reliability and performance of electronic devices based on polyimide derivatives, dynamic water sorption and diffusion behavior in a polyimide derivative： poly（4＇4 oxydiphenylene pyromellitimide） （PMDA-ODA）/silica nanocomposite was investigated by two-dimensional ATR-FTIR spectroscopy, by which three states of water molecules owning different H-bonding strength were distinguished. The amounts and strength of H-bonding also played a significant role in determining the diffusion rate of the different states of water molecules. The type of aggregated water molecules which also formed H-bonding with silicic acid （residues） or polyimide system was the last one diffusing to the polymer side in contact with the ATR crystal element because the polymeric matrix blocked their diffusion to a great extent. The diffusion coefficient was also estimated to gain the information of the dynamic diffusion behavior.
基金supported by the National Key Technology Support Program(No.2014BAC13B06)the National Natural Science Foundation of China(Nos.51378414,51178376)+1 种基金the Program for Innovative Research Team in Shaanxi(No.2013KCT-13)the Program for New Century Excellent Talents in the University of Ministry of Education of China(No.NCET-12-1043)
文摘In this study, two-dimensional correlation spectroscopy integrated with synchronous fluorescence and infrared absorption spectroscopy was employed to investigate the interaction between humic acids and aluminum coagulant at slightly acidic and neutral p H. Higher fluorescence quenching was produced for fulvic-like and humic-like fractions at p H 5. At p H 5, the humic-like fractions originating from the carboxylic acid, carboxyl and polysaccharide compounds were bound to aluminum first, followed by the fulvic-like fractions originating from the carboxyl and polysaccharide compounds. This finding also demonstrated that the activated functional groups of HA were involved in forming the Al-HA complex, which was accompanied by the removal of other groups by co-precipitation.Meanwhile, at p H 7, almost no fluorescence quenching occurred, and surface complexation was observed to occur, in which the activated functional groups were absorbed on the amorphous Al（OH）3. Two-dimensional FT-IR correlation spectroscopy indicated the sequence of HA structural change during coagulation with aluminum, with IR bands affected in the order of COOH〉 COO-〉NH deformation of amide Ⅱ〉 aliphatic hydroxyl C／OH at p H 5, and COO-〉aliphatic hydroxyl C／OH at p H 7. This study provides a promising pathway for analysis and insight into the priority of functional groups in the interaction between organic matters and metal coagulants.
基金financially supported by the National Natural Science Foundation of China(Nos.21274030,51473038 and 21604024)the Natural Science Foundation of Shanghai(No.17ZR1440400)+1 种基金the Open Project of State Key Laboratory of Chemical Engineering(No.SKL-Ch E-16C02)“Chenguang Plan”
文摘Generalized two-dimensional correlation spectroscopy （2DCOS） and its derivate technique, perturbation correlation moving window （PCMW）, have found great potential in studying a series of physico-chemical phenomena in stimuli-responsive polymeric systems. By spreading peaks along a second dimension, 2DCOS can significantly enhance spectral resolution and discern the sequence of group dynamics applicable to various external perturbation-induced spectroscopic changes, especially in infrared （IR）, near-infrared （NIR） and Raman spectroscopy. On the basis of 2DCOS synchronous power spectra changing, PCMW proves to be a powerful tool to monitor complicated spectral variations and to find transition points and ranges. This article reviews the recent work of our research group in the application of 2DCOS and PCMW in thermoresponsive polymers, mainly focused on liquid crystalline polymers and lower critical solution temperature （LCST）-type polymers. Details of group motions and chain conformational changes upon temperature perturbation can thus be elucidated at the molecular level, which contribute to the understanding of their phase transition nature.
基金supported by the National Key Research and Development Program of China(Grant No.2016YFA0301204)the National Natural Science Foundation of China(Grant Nos.11604326,11434010,11474277,and 11225421)
文摘Angle-resolved polarized Raman（ARPR） spectroscopy can be utilized to assign the Raman modes based on crystal symmetry and Raman selection rules and also to characterize the crystallographic orientation of anisotropic materials.However, polarized Raman measurements can be implemented by several different configurations and thus lead to different results. In this work, we systematically analyze three typical polarization configurations： 1） to change the polarization of the incident laser, 2） to rotate the sample, and 3） to set a half-wave plate in the common optical path of incident laser and scattered Raman signal to simultaneously vary their polarization directions. We provide a general approach of polarization analysis on the Raman intensity under the three polarization configurations and demonstrate that the latter two cases are equivalent to each other. Because the basal plane of highly ordered pyrolytic graphite（HOPG） exhibits isotropic feature and its edge plane is highly anisotropic, HOPG can be treated as a modelling system to study ARPR spectroscopy of twodimensional materials on their basal and edge planes. Therefore, we verify the ARPR behaviors of HOPG on its basal and edge planes at three different polarization configurations. The orientation direction of HOPG edge plane can be accurately determined by the angle-resolved polarization-dependent G mode intensity without rotating sample, which shows potential application for orientation determination of other anisotropic and vertically standing two-dimensional materials and other materials.
文摘Recent noteworthy developments in the field of two-dimensional（2D） correlation spectroscopy are reviewed.2D correlation spectroscopy has become a very popular tool due to its versatility and relative ease of use.The technique utilizes a spectroscopic or other analytical probe from a number of selections for a broad range of sample systems by employing different types of external perturbations to induce systematic variations in intensities of spectra.Such spectral intensity variations are then converted into2 D spectra by a form of correlation analysis for subsequent interpretation.Many different types of 2D correlation approaches have been proposed.In particular,2D hetero-correlation and multiple perturbation correlation analyses,including orthogonal sample design scheme,are discussed in this review.Additional references to other important developments in the field of 2D correlation spectroscopy,such as projection correlation and codistribution analysis,were also provided.
文摘Chinese liquor Moutai is the “National alcoholic drink” in China and plays a very important role of social activities in Chinese people’s life. In pursuit of high profits, some illegal counterfeit Moutai liquors have begun to appear in the market. Therefore, it is an urgent need for new techniques to discriminate the genuine and counterfeit Moutai liquor. In this work, the conventional Ultraviolet-Visible (UV-Vis) spectroscopy and two-dimensional correlation UV-Vis spectroscopy are applied to obtain the UV-Vis characteristic of Moutai liquor and counterfeit one, respectively. The experimental results reveal that the conventional UV-Vis spectra of the genuine and counterfeit Moutai liquor are similar. However, the two-dimensional correlation UV-Vis spectra of them are different and this method would be applied to differentiate the counterfeit Moutai liquor from the genuine Moutai liquor. Compared with conventional methods, this novel method has the advantages of easy operation, simple instrumentation and direct recognition, which make it a potential tool in the fields of food safety.
基金This work was supported by the Foundation of Education Committee of Fujian Province (K02028, JB04049), the State Key Laboratory of Structural Chemistry, and Science and Technology Foundation of Fuzhou University
文摘A novel compound, （4,4＇-Hbpy）3[NaMo8O26]（4,4＇-bpy）2（H2O）4 1 （bpy=bipydine）, was synthesized by the hydrothermal method. Single-crystal X-ray diffraction shows that compound 1 belongs to the monoclinic system, space group C2/m with a=19.1921（5）, b=18.6931（6）, c=9.3821（3） A° β=104.8020（11）°, V=3254.22（17）A°^3 C50H51Mo8N10NaO30, Mr=2062.52, Z=2, F（000）=2016, μ=1.591 mm^-1 and Dc=2.105 g/cm^3. The final R=0.0283 and wR=0.0912 for 3118 observed reflections （I〉20（I））. Compound 1 contains the β-[Mo8O26]^4-anion, sodium ion, 4,4＇-bpy and lattice crystalline water molecules. The β-[MosO26] units link the sodium ion to form a chain structure. The infinitechains of [Na（Mo8O26）]^3- blocks are surrounded by protonized 4,4＇-bpy cations, 4,4＇-bpy and lattice crystalline water molecules. The 2D-IR correlation spectroscopy study indicates that the stretching vibrations of Mo=O occur more preferentially due to the thermal effect. The TGA analysis shows that compound 1 has high thermal stability.
基金the National Natural Science Foundation of China(No.91753118 and No.21773012)the Fundamental Research Funds for Central Universities。
文摘Two-dimensional Fourier transform(2D FT) spectroscopy is an important technology that developed in recent decades and has many advantages over other ultrafast spectroscopy methods. Although 2D FT spectroscopy provides great opportunities for studying various complex systems, the experimental implementation and theoretical description of 2D FT spectroscopy measurement still face many challenges, which limits their wide application.Recently, the 2D FT spectroscopy reaches maturity due to many new developments which greatly reduces the technical barrier in the experimental implementation of the 2D FT spectrometer. There have been several different approaches developed for the optical design of the 2D FT spectrometer, each with its own advantages and limitations. Thus, a procedure to help an experimentalist to build a 2D FT spectroscopy experimental apparatus is needed.This tutorial review is intending to provide an accessible introduction for a beginner to build a 2D FT spectrometer.
文摘Coherent exciton-phonon coupling in CdSe/ZnS nanocrystals have been investigated by temperature-dependent two-dimensional electronic spectroscopy （2DES） measurements. Benefiting from the ability of 2DES to dissect assembles in nanocrystal films, we have dearly identified experimental evidences of coherent coupling between exciton and phonon in CdSe/ZnS nanocrystals. In time domain, 2DES signals of excitonic transitions beat at a frequency resonant to a longitudinal optical phonon mode; in energy domain, phonon side bands are distinct at both Stokes and anti-Stokes sides. When temperature increases, phonon-induced exciton dephasing is observed with dramatic broadening of homogeneous linewidth. The results suggest exciton-phonon coupling is essential in elucidating the quantum dynamics of excitonic transitions in semiconductor nanocrystals.
基金Project supported by Beijing Natural Science Foundation,China(Grant No.JQ18014)the National Natural Science Foundation of China(Grant No.12074371)Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB28000000),and CAS Interdisciplinary Innovation Team.
文摘Ultrathin van der Waals(vdW)magnets provide a possibility to access magnetic ordering in the two-dimensional(2D)limit,which are expected to be applied in the spintronic devices.Raman spectroscopy is a powerful characterization method to investigate the spin-related properties in 2D vdW magnets,including magnon and spin–lattice interaction,which are hardly accessible by other optical methods.In this paper,the recent progress of various magnetic properties in 2D vdW magnets studied by Raman spectroscopy is reviewed,including the magnetic transition,spin-wave,spin–lattice interaction,symmetry tuning induced by spin ordering,and nonreciprocal magneto-phonon Raman scattering.
基金the support from the National Natural Science Foundation of China(22272004,62272041)the Fundamental Research Funds for the Central Universities(YWF-22-L-1256)+1 种基金the National Key R&D Program of China(2023YFC3402600)the Beijing Institute of Technology Research Fund Program for Young Scholars(No.1870011182126)。
文摘The proliferation of wearable biodevices has boosted the development of soft,innovative,and multifunctional materials for human health monitoring.The integration of wearable sensors with intelligent systems is an overwhelming tendency,providing powerful tools for remote health monitoring and personal health management.Among many candidates,two-dimensional(2D)materials stand out due to several exotic mechanical,electrical,optical,and chemical properties that can be efficiently integrated into atomic-thin films.While previous reviews on 2D materials for biodevices primarily focus on conventional configurations and materials like graphene,the rapid development of new 2D materials with exotic properties has opened up novel applications,particularly in smart interaction and integrated functionalities.This review aims to consolidate recent progress,highlight the unique advantages of 2D materials,and guide future research by discussing existing challenges and opportunities in applying 2D materials for smart wearable biodevices.We begin with an in-depth analysis of the advantages,sensing mechanisms,and potential applications of 2D materials in wearable biodevice fabrication.Following this,we systematically discuss state-of-the-art biodevices based on 2D materials for monitoring various physiological signals within the human body.Special attention is given to showcasing the integration of multi-functionality in 2D smart devices,mainly including self-power supply,integrated diagnosis/treatment,and human–machine interaction.Finally,the review concludes with a concise summary of existing challenges and prospective solutions concerning the utilization of2D materials for advanced biodevices.
基金Project supported by the National Basic Research Program of China(Grant Nos.2012CB921300 and 2014CB920900)the National Key Research and Development Program of China(Grant No.2016YFA0300802)+1 种基金the National Natural Science Foundation of China(Grant Nos.11274015,11674013,and 21405109)the Recruitment Program of Global Experts,China,and Beijing Natural Science Foundation,China(Grant No.4142024)
文摘The two-dimensional layered transition metal dichalcogenides provide new opportunities in future valley-based in- formation processing and also provide an ideal platform to study excitonic effects. At the center of various device physics toward their possible electronic and optoelectronic applications is understanding the dynamical evolution of various many- particle electronic states, especially exciton which dominates the optoelectronic response of TMDs, under the novel con- text of valley degree of freedom. Here, we provide a brief review of experimental advances in using helicity-resolved ultrafast spectroscopy, especially ultrafast pump-probe spectroscopy, to study the dynamical evolution of valley-related many-particle electronic states in semiconducting monolayer transitional metal dichalcogenides.
文摘A number of useful techniques associated with two-dimensional correlation spectroscopy(2DCOS)to improve its performance and utility have been developed in the last 30years.Evolution of these 2DCOS techniques,including some of the very recent developments,is reviewed with examples.Topics include merged or modified asynchronous 2Dcorrelation spectrum,two-dimensional codistribution spectroscopy(2DCDS),Pareto scaling,and null-space projection treatment of spectral dataset.
文摘A series of soy protein isolate(SPI)films plasticized by glycerol(Gly)were studied using attenuated total reflectance-Fourier transform infrared spectroscopy(ATR/FTIR).Perturbation-correlation movingwindow two-dimensional(PCMW2D)and two-dimensional correlation(2DCOS)analyses were applied to the amideⅠband and thus the hydrogen bond interaction between SPI and Gly was systematically investigated.When Gly concentrations were in the range 0~35%,the hydrogen bond amongβ-sheets was replaced by the one between SPI chain and Gly molecule,which caused these protein chains being changed toα-helix.However,the transformation ofβ-sheet toα-helix was saturated and both of them tend to change to random coil when Gly concentrations were in the range 35%~60%.
基金This work is supported by the National Key R&D Program of China(No.2017YFA0303700 and No.2018YFA0209101)the National Natural Science Foundation of China(No.21922302,No.21873047,No.11904168,No.91833305,and No.91850105)+1 种基金the Priority Academic Program Development of Jiangsu Higher Education Institutionsthe Fundamental Research Funds for the Central University.
文摘Two-dimensional elec tronic spec troscopy(2DES)is a powerful met hod to probe the coherent electron dynamics in complicated systems.Stabilizing the phase difference of the incident ultrashort pulses is the mos t challenging par t for experimen tal demonstration of 2DES.Here,we present a tuto rial review on the 2DES proto cols based on active phase managements which are originally developed for quantum optics experiments.We introduce the 2DES techniques in box and pump-probe geometries with phase stabilization realized by interferometry,and outline the fully collinear 2DES approach with the frequency tagging by acoustic optical modulators and frequency combs.The combination of active phase managements,ultrashort pulses and other spectroscopic methods may open new opportunities to tackle essential challenges related to excited states.
文摘A functional interlayer based on two-dimensional(2D)porous modified vermiculite nanosheets(PVS)was obtained by acid-etching vermiculite nanosheets.The as-obtained 2D porous nanosheets exhibited a high specific surface area of 427 m^(2)·g^(-1)and rich surface active sites,which help restrain polysulfides(LiPSs)through good physi-cal and chemical adsorption,while simultaneously accelerating the nucleation and dissolution kinetics of Li_(2)S,effec-tively suppressing the shuttle effect.The assembled lithium-sulfur batteries(LSBs)employing the PVS-based inter-layer delivered a high initial discharge capacity of 1386 mAh·g^(-1)at 0.1C(167.5 mAh·g^(-1)),long-term cycling stabil-ity,and good rate property.
