Quantum well infrared photodetectors(QWIPs) based on intersubband transitions hold significant potential for high bandwidth operation. In this work, we establish a carrier transport optimization model incorporating el...Quantum well infrared photodetectors(QWIPs) based on intersubband transitions hold significant potential for high bandwidth operation. In this work, we establish a carrier transport optimization model incorporating electron injection at the emitter to investigate the carrier dynamics time and impedance spectroscopy in GaAs/AlGaAs QWIPs. Our findings provide novel evidence that the escape time of electrons is the key limiting factor for the 3-dB bandwidth of QWIPs. Moreover, to characterize the impact of carrier dynamics time and non-equilibrium space charge region on impedance, we developed an equivalent circuit model where depletion region resistance and capacitance are employed to describe non-equilibrium space charge region. Using this model, we discovered that under illumination, both net charge accumulation caused by variations in carrier dynamics times within quantum wells and changes in width of non-equilibrium space charge region exert different dominant influences on depletion region capacitance at various doping concentrations.展开更多
Chalcogenide superlattices Sb_(2)Te_(3)-GeTe is a candidate for interfacial phase-change memory(iPCM) data storage devices.By employing terahertz emission spectroscopy and the transient reflectance spectroscopy togeth...Chalcogenide superlattices Sb_(2)Te_(3)-GeTe is a candidate for interfacial phase-change memory(iPCM) data storage devices.By employing terahertz emission spectroscopy and the transient reflectance spectroscopy together,we investigate the ultrafast photoexcited carrier dynamics and current transients in Sb_(2)Te_(3)-GeTe superlattices.Sample orientation and excitation polarization dependences of the THz emission confirm that ultrafast thermo-electric,shift and injection currents contribute to the THz generation in Sb_(2)Te_(3)-GeTe superlattices.By decreasing the thickness and increasing the number of GeTe and Sb_(2)Te_(3) layer,the interlayer coupling can be enhanced,which significantly reduces the contribution from circular photo-galvanic effect(CPGE).A photo-induced bleaching in the transient reflectance spectroscopy probed in the range of~1100 nm to~1400 nm further demonstrates a gapped state resulting from the interlayer coupling.These demonstrates play an important role in the development of iPCM-based high-speed optoelectronic devices.展开更多
The fast developing semiconductor industry is pushing to shrink and speed up transistors. This trend requires us to understand carrier dynamics in semiconductor heterojunctions with both high spatial and temporal reso...The fast developing semiconductor industry is pushing to shrink and speed up transistors. This trend requires us to understand carrier dynamics in semiconductor heterojunctions with both high spatial and temporal resolutions. Recently, we have successfully set up a timeresolved photoemission electron microscopy (TR-PEEM), which integrates the spectroscopic technique to measure electron densities at specific energy levels in space. This instrument provides us an unprecedented access to the evolution of electrons in terms of spatial location, time resolution, and energy, representing a new type of 4D spectro-microscopy. Here in this work, we present measurements of semiconductor performance with a time resolution of 184 fs, electron kinetic energy resolution of 150 meV, and spatial resolution of about 150 nm or better. We obtained time-resolved micro-area photoelectron spectra and energy-resolved TR-PEEM images on the Pb island on Si(111). These experimental results suggest that this instrument has the potential to be a powerful tool for investigating the carrier dynamics in various heterojunctions, which will deepen our understanding of semiconductor properties in the submicron/nanometer spatial scales and ultrafast time scales.展开更多
Understanding the effect of additive on the interfacial charge-carrier transfer dynamics is very crucial to obtaining highly efficient perovskite solar cells(PSCs).Herein,we designed a simple additive,dimethyl oxalate...Understanding the effect of additive on the interfacial charge-carrier transfer dynamics is very crucial to obtaining highly efficient perovskite solar cells(PSCs).Herein,we designed a simple additive,dimethyl oxalate(DO),functioning as an effective defect passivator of perovskite grain boundaries via the coordination interaction between the carbonyl(C=O)and the exposed Pb^(2+).The modification with DO produces pinhole-free and compact perovskite films,enhancing the transportation capability of carriers.As a consequence,the DO-treated PSCs exhibited a power conversion efficiency(PCE)of 22.19%,which is significantly higher than that of the control device without additive(19.58%).More importantly,detailed transient absorption characterization reveals that the use of additive can decrease the hot-carrier cooling dynamics,improve the carrier transfer,and eliminate nonradiative recombination in PSCs.This present work provides a profound understanding the additives effect on the carrier dynamics in PSCs toward the Shockley-Queisser limit.展开更多
Despite that organic-inorganic lead halide perovskites have attracted enormous scientific attention for energy conversion applications over the recent years,the influence of temperature and the type of the employed ho...Despite that organic-inorganic lead halide perovskites have attracted enormous scientific attention for energy conversion applications over the recent years,the influence of temperature and the type of the employed hole transport layer(HTL)on the charge carrier dynamics and recombination processes in perovskite photovoltaic devices is still largely unexplored.In particular,significant knowledge is missing on how these crucial parameters for radiative and non-radiative recombinations,as well as for efficient charge extraction vary among different perovskite crystalline phases that are induced by temperature variation.Herein,we perform micro photoluminescence(pPL)and ultrafast time resolved transient absorption spectroscopy(TAS)in Glass/Perovskite and two dierent Glass/ITO/HTL/Perovskite configurations at temperatures below room temperature,in order to probe the charge carrier dynamics of different perovskite crystalline phases,while considering also the effect of the employed HTL polymer.Namely,CH_(3)NH_(3)Pbb films were deposited on Glass,PEDOT:PSS and PTAA polymers,and the developed Glass/CH_(3)NH_(3)PbI_(3)and Glass/ITO/HTL/CH_(3)NH_(3)PbI_(3)architectures were studied from 85 K up to 215 K in order to explore the charge extraction dynamics of the CH_(3)NH_(3)PbI_(3)orthorhombic and tetragonal crystalline phases.It is observed an unusual blueshift of the bandgap with temperature and the dual emission at temperature below of 100 K and also,that the charge carrier dynamics,as expressed by hole injection times and free carrier recombination rates,are strongly depended on the actual pervoskite crystal phase,as well as,from the selected hole transport material.展开更多
OaAs has been widely used to fabricate a variety of optoelectronic devices by virtue of its superior performance, and it is very important to accurately measure its electrical and optical properties. In this study, a ...OaAs has been widely used to fabricate a variety of optoelectronic devices by virtue of its superior performance, and it is very important to accurately measure its electrical and optical properties. In this study, a semi- insulation （SI） GaAs wafer is investigated by the terahertz （THz） non-destructive testing technology. Using an air biased coherent generation and detection THz time domain spectroscopy system, the THz time domain waveform and spectrum of SI-GaAs are obtained by the time domain spectroscopy module, and its optical- electrical characteristics including complex refractive index, permittivity and dielectric loss angle are calculated. Its carrier lifetime is measured by the optical-pump THz-probe module, and the THz pulse induced intervalley scattering in photo-excited SI-GaAs is discussed.展开更多
In recent years,one-dimensional(1D)nanomaterials have raised researcher's interest because of their unique structur-al characteristic to generate and confine the optical signal and their promising prospects in pho...In recent years,one-dimensional(1D)nanomaterials have raised researcher's interest because of their unique structur-al characteristic to generate and confine the optical signal and their promising prospects in photonic applications.In this re-view,we summarized the recent research advances on the spectroscopy and carrier dynamics of 1D nanostructures.First,the condensation and propagation of exciton-polaritons in nanowires(NWs)are introduced.Second,we discussed the properties of 1D photonic crystal(PC)and applications in photonic-plasmonic structures.Third,the observation of topological edge states in 1D topological structures is introduced.Finally,the perspective on the potential opportunities and remaining chal-lenges of 1D nanomaterials is proposed.展开更多
Ultrafast time-resolved optical transmissions in purified and as-grown single-walled carbon nanotube films are measured at a temperature of 200K. The signal of the purified sample shows a crossover from photobleaching...Ultrafast time-resolved optical transmissions in purified and as-grown single-walled carbon nanotube films are measured at a temperature of 200K. The signal of the purified sample shows a crossover from photobleaching to photoabsorption. The former and the latter are interpreted as the state filling and the red shift of the π-plasmon, respectively. The signal of the as-grown sample can be perfectly fitted by a single-exponential with a time constant of 232fs. The disappearance of the negative component in the as-grown sample is attributed to the charge transfer between the semiconducting nanotubes and the impurities.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
Cuprous oxide(Cu_(2)O)has attracted plenty of attention for potential nonlinear photonic applications due to its superior third-order nonlinear optical property such as two-photon absorption.In this paper,we investiga...Cuprous oxide(Cu_(2)O)has attracted plenty of attention for potential nonlinear photonic applications due to its superior third-order nonlinear optical property such as two-photon absorption.In this paper,we investigated the two-photon excitation induced carrier dynamics of a Cu_(2)O thin film prepared by radio-frequency magnetron sputtering,using the femtosecond transient absorption experiments.Biexponential dynamics including an ultrafast carrier scattering(<1 ps)followed by a carrier recombination(>50 ps)were observed.The time constant of carrier scattering under two-photon excitation is larger than that under one-photon excitation,due to the different transition selection rules and smaller absorption coefficient of the two-photon excitation.展开更多
Two-dimensional transition metal dichalcogenides(TMDs)have intriguing physic properties and offer an exciting platform to explore many features that are important for future devices.In this work,we synthesized monolay...Two-dimensional transition metal dichalcogenides(TMDs)have intriguing physic properties and offer an exciting platform to explore many features that are important for future devices.In this work,we synthesized monolayer WS_(2)as an example to study the optical response with hydrostatic pressure.The Raman results show a continuous tuning of the lattice vibrations that is induced by hydrostatic pressure.We further demonstrate an efficient pressure-induced change of the band structure and carrier dynamics via transient absorption measurements.We found that two time constants can be attributed to the capture process of two kinds of defect states,with the pressure increasing from 0.55 GPa to 2.91 GPa,both of capture processes were accelerated,and there is an inflection point within the pressure range of 1.56 GPa to 1.89 GPa.Our findings provide valuable information for the design of future optoelectronic devices.展开更多
Defect-mediated processes in two-dimensional transition metal dichalcogenides have a significant influence on their carrier dynamics and transport properties,however,the detailed mechanisms remain poorly understood.He...Defect-mediated processes in two-dimensional transition metal dichalcogenides have a significant influence on their carrier dynamics and transport properties,however,the detailed mechanisms remain poorly understood.Here,we present a comprehensive ultrafast study on defect-mediated carrier dynamics in ion exchange prepared few-layer MoS2 by femtosecond time-resolved Vis-NIR-MIR spectroscopy.The broadband photobleaching feature observed in the near-infrared transient spectrum discloses that the mid-gap defect states are widely distributed in few-layer MoS2 nanosheets.The processes of fast trapping of carriers by defect states and the following nonradiative recombination of trapped carriers are clearly revealed,demonstrating the mid-gap defect states play a significant role in the photoinduced carrier dynamics.The positive to negative crossover of the signal observed in the mid-infrared transient spectrum further uncovers some occupied shallow defect states distributed at less than0.24 e V below the conduction band minimum.These defect states can act as effective carrier trap centers to assist the nonradiative recombination of photo-induced carriers in few-layer MoS2 on the picosecond time scale.展开更多
Efficient and stable photocathodes with versatility are of significance in photoassisted lithium-ion batteries(PLIBs),while there is always a request on fast carrier transport in electrochemical active photocathodes.P...Efficient and stable photocathodes with versatility are of significance in photoassisted lithium-ion batteries(PLIBs),while there is always a request on fast carrier transport in electrochemical active photocathodes.Present work proposes a general approach of creating bulk heterojunction to boost the carrier mobility of photocathodes by simply laser assisted embedding of plasmonic nanocrystals.When employed in PLIBs,it was found effective for synchronously enhanced photocharge separation and transport in light charging process.Additionally,experimental photon spectroscopy,finite difference time domain method simulation and theoretical analyses demonstrate that the improved carrier dynamics are driven by the plasmonic-induced hot electron injection from metal to TiO_(2),as well as the enhanced conductivity in TiO2 matrix due to the formation of oxygen vacancies after Schottky contact.Benefiting from these merits,several benchmark values in performance of TiO2-based photocathode applied in PLIBs are set,including the capacity of 276 mAh g^(−1) at 0.2 A g^(−1) under illumination,photoconversion efficiency of 1.276%at 3 A g^(−1),less capacity and Columbic efficiency loss even through 200 cycles.These results exemplify the potential of the bulk heterojunction strategy in developing highly efficient and stable photoassisted energy storage systems.展开更多
In this work, we demonstrated the successful construction of metal-free zero- dimensional/two-dimensional carbon nanodot （CND）-hybridized protonatedg=C3N4 （pCN） （CND/pCN） heterojunction photocatalysts b; means o...In this work, we demonstrated the successful construction of metal-free zero- dimensional/two-dimensional carbon nanodot （CND）-hybridized protonatedg=C3N4 （pCN） （CND/pCN） heterojunction photocatalysts b; means of electrostatic attraction. We experimentally found that CNDs with an average diameter of 4.4 nm were uniformly distributed on the surface of pCN using electron microscopy analysis. The CND/pCN-3 sample with a CND content of 3 wt.% showed thehighest catalytic activity in the CO2 photoreduction process under visible and simulated solar light. This process results in the evolution of CH4 and CO. Thetotal amounts of CH4 and CO generated by the CND/pCN-3 photocatalyst after 10 h of visible-light activity were found to be 29.23 and 58.82 molgcatalyst-1, respectively. These values were 3.6 and 2.28 times higher, respectively, than thearn＊ounts generated when using pCN alone. The corresponding apparent quantum efficiency （AQE） was calculated to be 0.076%. Furthermore, the CND/pCN-3 sample demonstrated high stability and durability after four consecutive photoreaction cycles, with no significant decrease in the catalytic activity.展开更多
Carrier dynamics and surface reaction are two critical processes for determining the performance of photocatalytic reaction.Highly designable polymer-based photocatalysts have shown promising protectives in energetic ...Carrier dynamics and surface reaction are two critical processes for determining the performance of photocatalytic reaction.Highly designable polymer-based photocatalysts have shown promising protectives in energetic and environmental applications.In this prospective,we first distinguished the differences of physiochemical properties between polymer-based semiconductors and traditional inorganic semiconductors.Then,the effects of single-atom sites on the charge dynamics and reaction kinetics of polymer-based photocatalysts are further elaborated.Time(excitation)-space(wavefunction)population analysis,which can provide relevant information to clarify the structure-excitation relationships after introducing the single atom sites was also reviewed.In the future,with the further development of artificial intelligence,the establishment of an energy function with a regression accuracy close to or reaching the level of density functional theory is highly desired to infer the energetic diagram of the photocatalytic systems at the excited states.Furthermore,coordination structures,interaction with inorganic semiconductors,photocatalytic stability and solvent effects should also be carefully considered in the future studies of polymer-based photocatalyst.展开更多
Novel physical properties emerge when the thickness of charge density wave(CDW)materials is reduced to the atomic level,owing to the significant modification of the electronic band structure and correlation effects.He...Novel physical properties emerge when the thickness of charge density wave(CDW)materials is reduced to the atomic level,owing to the significant modification of the electronic band structure and correlation effects.Here,we investigate the layer-dependent CDW phase transition and evolution of the nonequilibrium state of 1T-TaS_(2)nanoflakes using pump-probe spectroscopy.Both the low-energy single-particle and collective excitation relaxations exhibit sharp changes at〜210 K,indicating a phase transition from commensurate CDW to nearly commensurate CDW state.The single particle process reveals that the phase transition stiffness(PTS)is thickness-dependent.Moreover,a small PTS is observed in thin nanoflakes,which is attributed to the reduced thickness that increases the fluctuation and inhibits the nucleation and growth of discommensurations.In addition,the phase mode vanishes when the discommensuration network appears.Our results suggest that the carrier dynamics could be an efficient operational approach to measuring the quantum phase transition in correlated materials.展开更多
All-inorganic cesium lead halide perovskites （CsPbX3, X=CF, Br-, I-） could provide comparableoptoelectronic properties as a promising class of materials for photovoltaic cell （PV）, photodetector andlight-emitting ...All-inorganic cesium lead halide perovskites （CsPbX3, X=CF, Br-, I-） could provide comparableoptoelectronic properties as a promising class of materials for photovoltaic cell （PV）, photodetector andlight-emitting diode （LED） with enhanced thermal and moisture stabilities compared to organic-inorganic lead halide species. However, fabrication of CsPbI3 perovskite via facile solution process hasbeen difficult due to instability of CsPbl3 in the perovskite cubic phase in ambient air. Herein, we reportthe synthesis of CsPbl3 perovskite microcrystals by low-temperature, catalyst-free, solution-phasemethod. By applying the time-resolve spectroscopic technique, we determine the carrier diffusioncoefficient of 0.6-1.2 cm2/s, the intrinsic carrier lifetimes of 200-1300 ns and diffusion length of4-10 μm in different individual CsPbl3 perovskite microcrystals. Our results suggest the CsPbl3 perovskitemicrocrystals synthesized by solution process exhibit high quality feature and are suitable forapplications in optoelectronic devices.展开更多
Broadband(1.6–18 THz) terahertz time-domain spectroscopy(THz-TDS) and time-resolved terahertz spectroscopy(TRTS) were performed on a 54 μm thick chalcogenide glass(As_(30)Se_(30)Te_(40)) sample with a two-color lase...Broadband(1.6–18 THz) terahertz time-domain spectroscopy(THz-TDS) and time-resolved terahertz spectroscopy(TRTS) were performed on a 54 μm thick chalcogenide glass(As_(30)Se_(30)Te_(40)) sample with a two-color laser-induced air plasma THz system in transmission and reflection modes, respectively. Two absorption bands at 2–3 and 5–8 THz were observed. TRTS reveals an ultrafast relaxation process of the photoinduced carrier response, well described by a rate equation model with a finite concentration of mid-bandgap trap states for self-trapped excitons.The photoinduced conductivity can be well described by the Drude–Smith conductivity model with a carrier scattering time of 12–17 fs, and we observe significant carrier localization effects. A fast refractive index change was observed 100 fs before the conductivity reached its maximum, with 2 orders of magnitude larger amplitude than expected for the optically induced THz Kerr effect, indicating that free carriers are responsible for the transient index change.展开更多
Defects at the grain boundaries(GBs)of perovskite film highly restrict both the efficiency and stability of perovskite solar cells(PSCs).Herein,organic small molecules of butanedioic acid(BA)and acetylenedicarboxylic ...Defects at the grain boundaries(GBs)of perovskite film highly restrict both the efficiency and stability of perovskite solar cells(PSCs).Herein,organic small molecules of butanedioic acid(BA)and acetylenedicarboxylic acid(AA),containing two carbonyl(C=O)groups and different core-units,were incorporated into perovskite as additives for PSCs application.Thanks to the strong coordination interaction between C=O group and under-coordinated Pb^(2+),the additives can effectively passivate film defects and regulate the perovskite crystallization,yielding high-quality perovskite films with lower defect densities.More importantly,the additives can efficiently regulate the charge transport behaviors in PSCs.Benefiting from the defects passivation and the regulation of charge carrier dynamics,the BA and AA-treaded PSCs show the power conversion efficiencies of 21.52%and 20.50%,which are higher than that of the control device(19.41%).Besides,the optimal devices exhibit a remarkable enhanced long-term stability and moisture tolerance compared to the pristine devices.Furthermore,the transient absorption spectrum reveals the mechanism of enhanced photovoltaic performances,attributing to the improvement of charge transport capability at the perovskite/Spiro-OMeTAD interfaces.This work affords a promising strategy to improve the efficiency and stability of PSCs through regulating the charge-carrier dynamic process in perovskite film.展开更多
Carrier lifetime is one of the most fundamental physical parameters that characterizes the average time of carrier recombination in any material.The control of carrier lifetime is the key to optimizing the device func...Carrier lifetime is one of the most fundamental physical parameters that characterizes the average time of carrier recombination in any material.The control of carrier lifetime is the key to optimizing the device function by tuning the electro-optical conversion quantum yield,carrier diffusion length,carrier collection process,etc.Till now,the prevailing modulation methods are mainly by defect engineering and temperature control,which have limitations in the modulation direction and amplitude of the carrier lifetime.Here,we report an effective modulation on the ultrafast dynamics of photoexcited carriers in two-dimensional(2D)MoS2 monolayer by uniaxial tensile strain.The combination of optical ultrafast pump-probe technique and time-resolved photoluminescence(PL)spectroscopy reveals that the carrier dynamics through Auger scattering,carrier-phonon scattering,and radiative recombination keep immune to the strain.But strikingly,the uniaxial tensile strain weakens the trapping of photoexcited carriers by defects and therefore prolongs the corresponding carrier lifetime up to 440%per percent applied strain.Our results open a new avenue to enlarge the carrier lifetime of 2D MoS2,which will facilitate its applications in high-efficient optoelectronic and photovoltaic devices.展开更多
基金financially supported by the National Natural Science Foundation of China (Grant No. 61991442)。
文摘Quantum well infrared photodetectors(QWIPs) based on intersubband transitions hold significant potential for high bandwidth operation. In this work, we establish a carrier transport optimization model incorporating electron injection at the emitter to investigate the carrier dynamics time and impedance spectroscopy in GaAs/AlGaAs QWIPs. Our findings provide novel evidence that the escape time of electrons is the key limiting factor for the 3-dB bandwidth of QWIPs. Moreover, to characterize the impact of carrier dynamics time and non-equilibrium space charge region on impedance, we developed an equivalent circuit model where depletion region resistance and capacitance are employed to describe non-equilibrium space charge region. Using this model, we discovered that under illumination, both net charge accumulation caused by variations in carrier dynamics times within quantum wells and changes in width of non-equilibrium space charge region exert different dominant influences on depletion region capacitance at various doping concentrations.
基金Project supported by the National Key Research and Development Program of China(Grant Nos.2023YFF0719200 and 2022YFA1404004)the National Natural Science Foundation of China(Grant Nos.62322115,61988102,61975110,62335012,and 12074248)+3 种基金111 Project(Grant No.D18014)the Key Project supported by Science and Technology Commission Shanghai Municipality(Grant No.YDZX20193100004960)Science and Technology Commission of Shanghai Municipality(Grant Nos.22JC1400200 and 21S31907400)General Administration of Customs People’s Republic of China(Grant No.2019HK006)。
文摘Chalcogenide superlattices Sb_(2)Te_(3)-GeTe is a candidate for interfacial phase-change memory(iPCM) data storage devices.By employing terahertz emission spectroscopy and the transient reflectance spectroscopy together,we investigate the ultrafast photoexcited carrier dynamics and current transients in Sb_(2)Te_(3)-GeTe superlattices.Sample orientation and excitation polarization dependences of the THz emission confirm that ultrafast thermo-electric,shift and injection currents contribute to the THz generation in Sb_(2)Te_(3)-GeTe superlattices.By decreasing the thickness and increasing the number of GeTe and Sb_(2)Te_(3) layer,the interlayer coupling can be enhanced,which significantly reduces the contribution from circular photo-galvanic effect(CPGE).A photo-induced bleaching in the transient reflectance spectroscopy probed in the range of~1100 nm to~1400 nm further demonstrates a gapped state resulting from the interlayer coupling.These demonstrates play an important role in the development of iPCM-based high-speed optoelectronic devices.
基金supported by the National Key R&D Program (No.2018YFA0208700 and No.2016YFA0200602)the National Natural Science Foundation of China (No.21688102 and No.21403222)+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDB17000000)the Youth Innovation Promotion Association of Chinese Academy of Sciences (No.2017224)
文摘The fast developing semiconductor industry is pushing to shrink and speed up transistors. This trend requires us to understand carrier dynamics in semiconductor heterojunctions with both high spatial and temporal resolutions. Recently, we have successfully set up a timeresolved photoemission electron microscopy (TR-PEEM), which integrates the spectroscopic technique to measure electron densities at specific energy levels in space. This instrument provides us an unprecedented access to the evolution of electrons in terms of spatial location, time resolution, and energy, representing a new type of 4D spectro-microscopy. Here in this work, we present measurements of semiconductor performance with a time resolution of 184 fs, electron kinetic energy resolution of 150 meV, and spatial resolution of about 150 nm or better. We obtained time-resolved micro-area photoelectron spectra and energy-resolved TR-PEEM images on the Pb island on Si(111). These experimental results suggest that this instrument has the potential to be a powerful tool for investigating the carrier dynamics in various heterojunctions, which will deepen our understanding of semiconductor properties in the submicron/nanometer spatial scales and ultrafast time scales.
基金the National Natural Science Foundation of China(22065038)the Key Project of Natural Science Foundation of Yunnan(KC10110419)+4 种基金High-Level Talents Introduction in Yunnan Province(C619300A010)the Fund for Excellent Young Scholars of Yunnan(K264202006820)International Joint Research Center for Advanced Energy Materials of Yunnan Province(202003AE140001)the Program for Excellent Young Talents of Yunnan UniversityMajor Science and Technology Project of Precious Metal Materials Genetic Engineering in Yunnan Province(No.2019ZE001-1,202002AB080001-6)for financial support.
文摘Understanding the effect of additive on the interfacial charge-carrier transfer dynamics is very crucial to obtaining highly efficient perovskite solar cells(PSCs).Herein,we designed a simple additive,dimethyl oxalate(DO),functioning as an effective defect passivator of perovskite grain boundaries via the coordination interaction between the carbonyl(C=O)and the exposed Pb^(2+).The modification with DO produces pinhole-free and compact perovskite films,enhancing the transportation capability of carriers.As a consequence,the DO-treated PSCs exhibited a power conversion efficiency(PCE)of 22.19%,which is significantly higher than that of the control device without additive(19.58%).More importantly,detailed transient absorption characterization reveals that the use of additive can decrease the hot-carrier cooling dynamics,improve the carrier transfer,and eliminate nonradiative recombination in PSCs.This present work provides a profound understanding the additives effect on the carrier dynamics in PSCs toward the Shockley-Queisser limit.
文摘Despite that organic-inorganic lead halide perovskites have attracted enormous scientific attention for energy conversion applications over the recent years,the influence of temperature and the type of the employed hole transport layer(HTL)on the charge carrier dynamics and recombination processes in perovskite photovoltaic devices is still largely unexplored.In particular,significant knowledge is missing on how these crucial parameters for radiative and non-radiative recombinations,as well as for efficient charge extraction vary among different perovskite crystalline phases that are induced by temperature variation.Herein,we perform micro photoluminescence(pPL)and ultrafast time resolved transient absorption spectroscopy(TAS)in Glass/Perovskite and two dierent Glass/ITO/HTL/Perovskite configurations at temperatures below room temperature,in order to probe the charge carrier dynamics of different perovskite crystalline phases,while considering also the effect of the employed HTL polymer.Namely,CH_(3)NH_(3)Pbb films were deposited on Glass,PEDOT:PSS and PTAA polymers,and the developed Glass/CH_(3)NH_(3)PbI_(3)and Glass/ITO/HTL/CH_(3)NH_(3)PbI_(3)architectures were studied from 85 K up to 215 K in order to explore the charge extraction dynamics of the CH_(3)NH_(3)PbI_(3)orthorhombic and tetragonal crystalline phases.It is observed an unusual blueshift of the bandgap with temperature and the dual emission at temperature below of 100 K and also,that the charge carrier dynamics,as expressed by hole injection times and free carrier recombination rates,are strongly depended on the actual pervoskite crystal phase,as well as,from the selected hole transport material.
基金Supported by the National Natural Science Foundation of China under Grant Nos 61575161 and 61427814the National Basic Research Program of China under Grant No 2014CB339800+1 种基金the Foundation of Shaanxi Key Science and Technology Innovation Team under Grant No 2014KTC-13the Special Financial Grant from the China Postdoctoral Science Foundation under Grant No 2013T60883
文摘OaAs has been widely used to fabricate a variety of optoelectronic devices by virtue of its superior performance, and it is very important to accurately measure its electrical and optical properties. In this study, a semi- insulation （SI） GaAs wafer is investigated by the terahertz （THz） non-destructive testing technology. Using an air biased coherent generation and detection THz time domain spectroscopy system, the THz time domain waveform and spectrum of SI-GaAs are obtained by the time domain spectroscopy module, and its optical- electrical characteristics including complex refractive index, permittivity and dielectric loss angle are calculated. Its carrier lifetime is measured by the optical-pump THz-probe module, and the THz pulse induced intervalley scattering in photo-excited SI-GaAs is discussed.
基金supported by the Strategic Priority Research Program of Chinese Academy of Sciences(XDB36000000)National Natural Science Foundation of China(22073022,11874130,12074086,22173025)+3 种基金the Support by the DNL Cooperation Fund,CAS(DNL202016)China Postdoctoral Science Foundation(2022M710925)Beijing Municipal Natural Science Foundation(1222030)the CAS Instrument Development Project(No.Y950291).
文摘In recent years,one-dimensional(1D)nanomaterials have raised researcher's interest because of their unique structur-al characteristic to generate and confine the optical signal and their promising prospects in photonic applications.In this re-view,we summarized the recent research advances on the spectroscopy and carrier dynamics of 1D nanostructures.First,the condensation and propagation of exciton-polaritons in nanowires(NWs)are introduced.Second,we discussed the properties of 1D photonic crystal(PC)and applications in photonic-plasmonic structures.Third,the observation of topological edge states in 1D topological structures is introduced.Finally,the perspective on the potential opportunities and remaining chal-lenges of 1D nanomaterials is proposed.
文摘Ultrafast time-resolved optical transmissions in purified and as-grown single-walled carbon nanotube films are measured at a temperature of 200K. The signal of the purified sample shows a crossover from photobleaching to photoabsorption. The former and the latter are interpreted as the state filling and the red shift of the π-plasmon, respectively. The signal of the as-grown sample can be perfectly fitted by a single-exponential with a time constant of 232fs. The disappearance of the negative component in the as-grown sample is attributed to the charge transfer between the semiconducting nanotubes and the impurities.
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.
基金Project supported by the National Natural Science Foundation of China(Grant No.61505178).
文摘Cuprous oxide(Cu_(2)O)has attracted plenty of attention for potential nonlinear photonic applications due to its superior third-order nonlinear optical property such as two-photon absorption.In this paper,we investigated the two-photon excitation induced carrier dynamics of a Cu_(2)O thin film prepared by radio-frequency magnetron sputtering,using the femtosecond transient absorption experiments.Biexponential dynamics including an ultrafast carrier scattering(<1 ps)followed by a carrier recombination(>50 ps)were observed.The time constant of carrier scattering under two-photon excitation is larger than that under one-photon excitation,due to the different transition selection rules and smaller absorption coefficient of the two-photon excitation.
基金This work was supported by Shenzhen Science and Technology Innovation Commission(JCYJ20220530153004010).
文摘Two-dimensional transition metal dichalcogenides(TMDs)have intriguing physic properties and offer an exciting platform to explore many features that are important for future devices.In this work,we synthesized monolayer WS_(2)as an example to study the optical response with hydrostatic pressure.The Raman results show a continuous tuning of the lattice vibrations that is induced by hydrostatic pressure.We further demonstrate an efficient pressure-induced change of the band structure and carrier dynamics via transient absorption measurements.We found that two time constants can be attributed to the capture process of two kinds of defect states,with the pressure increasing from 0.55 GPa to 2.91 GPa,both of capture processes were accelerated,and there is an inflection point within the pressure range of 1.56 GPa to 1.89 GPa.Our findings provide valuable information for the design of future optoelectronic devices.
基金supported by the National Key Research and Development Program of China(No.2018YFA0208700)the National Natural Science Foundation of China(No.21603270 and No.21773302)the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB30000000)。
文摘Defect-mediated processes in two-dimensional transition metal dichalcogenides have a significant influence on their carrier dynamics and transport properties,however,the detailed mechanisms remain poorly understood.Here,we present a comprehensive ultrafast study on defect-mediated carrier dynamics in ion exchange prepared few-layer MoS2 by femtosecond time-resolved Vis-NIR-MIR spectroscopy.The broadband photobleaching feature observed in the near-infrared transient spectrum discloses that the mid-gap defect states are widely distributed in few-layer MoS2 nanosheets.The processes of fast trapping of carriers by defect states and the following nonradiative recombination of trapped carriers are clearly revealed,demonstrating the mid-gap defect states play a significant role in the photoinduced carrier dynamics.The positive to negative crossover of the signal observed in the mid-infrared transient spectrum further uncovers some occupied shallow defect states distributed at less than0.24 e V below the conduction band minimum.These defect states can act as effective carrier trap centers to assist the nonradiative recombination of photo-induced carriers in few-layer MoS2 on the picosecond time scale.
基金supported by the project of the National Natural Science Foundation of China(52202115 and 52172101)Guangdong Basic and Applied Basic Research Foundation(2024A1515012325)+2 种基金the Natural Science Foundation of Chongqing,China(CSTB2022NSCQ-MSX1085)the Shaanxi Science and Technology Innovation Team(2023-CXTD-44)the Fundamental Research Funds for the Central Universities(G2022KY0604).
文摘Efficient and stable photocathodes with versatility are of significance in photoassisted lithium-ion batteries(PLIBs),while there is always a request on fast carrier transport in electrochemical active photocathodes.Present work proposes a general approach of creating bulk heterojunction to boost the carrier mobility of photocathodes by simply laser assisted embedding of plasmonic nanocrystals.When employed in PLIBs,it was found effective for synchronously enhanced photocharge separation and transport in light charging process.Additionally,experimental photon spectroscopy,finite difference time domain method simulation and theoretical analyses demonstrate that the improved carrier dynamics are driven by the plasmonic-induced hot electron injection from metal to TiO_(2),as well as the enhanced conductivity in TiO2 matrix due to the formation of oxygen vacancies after Schottky contact.Benefiting from these merits,several benchmark values in performance of TiO2-based photocathode applied in PLIBs are set,including the capacity of 276 mAh g^(−1) at 0.2 A g^(−1) under illumination,photoconversion efficiency of 1.276%at 3 A g^(−1),less capacity and Columbic efficiency loss even through 200 cycles.These results exemplify the potential of the bulk heterojunction strategy in developing highly efficient and stable photoassisted energy storage systems.
文摘In this work, we demonstrated the successful construction of metal-free zero- dimensional/two-dimensional carbon nanodot （CND）-hybridized protonatedg=C3N4 （pCN） （CND/pCN） heterojunction photocatalysts b; means of electrostatic attraction. We experimentally found that CNDs with an average diameter of 4.4 nm were uniformly distributed on the surface of pCN using electron microscopy analysis. The CND/pCN-3 sample with a CND content of 3 wt.% showed thehighest catalytic activity in the CO2 photoreduction process under visible and simulated solar light. This process results in the evolution of CH4 and CO. Thetotal amounts of CH4 and CO generated by the CND/pCN-3 photocatalyst after 10 h of visible-light activity were found to be 29.23 and 58.82 molgcatalyst-1, respectively. These values were 3.6 and 2.28 times higher, respectively, than thearn＊ounts generated when using pCN alone. The corresponding apparent quantum efficiency （AQE） was calculated to be 0.076%. Furthermore, the CND/pCN-3 sample demonstrated high stability and durability after four consecutive photoreaction cycles, with no significant decrease in the catalytic activity.
基金Mitsubishi Chemical Corporation,JSPS Grant-in-Aid for Scientific Research(B,No.20H02847)Grant-in-Aid for JSPS Fellows(DC2,No.20J13064)+2 种基金National Natural Science Foundation of China(No.21805191)Guangdong Basic and Applied Basic Research Foundation,China(No.2020A1515010982)Shenzhen Stable Support Project,China(No.20200812122947002).
文摘Carrier dynamics and surface reaction are two critical processes for determining the performance of photocatalytic reaction.Highly designable polymer-based photocatalysts have shown promising protectives in energetic and environmental applications.In this prospective,we first distinguished the differences of physiochemical properties between polymer-based semiconductors and traditional inorganic semiconductors.Then,the effects of single-atom sites on the charge dynamics and reaction kinetics of polymer-based photocatalysts are further elaborated.Time(excitation)-space(wavefunction)population analysis,which can provide relevant information to clarify the structure-excitation relationships after introducing the single atom sites was also reviewed.In the future,with the further development of artificial intelligence,the establishment of an energy function with a regression accuracy close to or reaching the level of density functional theory is highly desired to infer the energetic diagram of the photocatalytic systems at the excited states.Furthermore,coordination structures,interaction with inorganic semiconductors,photocatalytic stability and solvent effects should also be carefully considered in the future studies of polymer-based photocatalyst.
基金We thank Prof.Yong Wang(Nankai University)for the valued discussions.We acknowledge financial support from the National Key Research and Development Program of China(Nos.2017YFA0205000,2017YFA0303600,2016YFA0200701)the National Natural Science Foundation of China(Nos.21425310,21790353,21721002,21822502,21673058)+1 种基金Strategic Priority Research Program of Chinese Academy of Sciences(Nos.XDB36000000,XDB30000000)the Key Research Program of Frontier Sciences of CAS(No.QYZDB-SSW-SYS031).
文摘Novel physical properties emerge when the thickness of charge density wave(CDW)materials is reduced to the atomic level,owing to the significant modification of the electronic band structure and correlation effects.Here,we investigate the layer-dependent CDW phase transition and evolution of the nonequilibrium state of 1T-TaS_(2)nanoflakes using pump-probe spectroscopy.Both the low-energy single-particle and collective excitation relaxations exhibit sharp changes at〜210 K,indicating a phase transition from commensurate CDW to nearly commensurate CDW state.The single particle process reveals that the phase transition stiffness(PTS)is thickness-dependent.Moreover,a small PTS is observed in thin nanoflakes,which is attributed to the reduced thickness that increases the fluctuation and inhibits the nucleation and growth of discommensurations.In addition,the phase mode vanishes when the discommensuration network appears.Our results suggest that the carrier dynamics could be an efficient operational approach to measuring the quantum phase transition in correlated materials.
基金the financial support from the National Natural Science Foundation of China(No.21473192)the financial support from the National Natural Science Foundation of China(Nos.21373042 and 21677029)
文摘All-inorganic cesium lead halide perovskites （CsPbX3, X=CF, Br-, I-） could provide comparableoptoelectronic properties as a promising class of materials for photovoltaic cell （PV）, photodetector andlight-emitting diode （LED） with enhanced thermal and moisture stabilities compared to organic-inorganic lead halide species. However, fabrication of CsPbI3 perovskite via facile solution process hasbeen difficult due to instability of CsPbl3 in the perovskite cubic phase in ambient air. Herein, we reportthe synthesis of CsPbl3 perovskite microcrystals by low-temperature, catalyst-free, solution-phasemethod. By applying the time-resolve spectroscopic technique, we determine the carrier diffusioncoefficient of 0.6-1.2 cm2/s, the intrinsic carrier lifetimes of 200-1300 ns and diffusion length of4-10 μm in different individual CsPbl3 perovskite microcrystals. Our results suggest the CsPbl3 perovskitemicrocrystals synthesized by solution process exhibit high quality feature and are suitable forapplications in optoelectronic devices.
基金financial support from the Danish Research Council for Independent Research (FNU Project THz-BREW)
文摘Broadband(1.6–18 THz) terahertz time-domain spectroscopy(THz-TDS) and time-resolved terahertz spectroscopy(TRTS) were performed on a 54 μm thick chalcogenide glass(As_(30)Se_(30)Te_(40)) sample with a two-color laser-induced air plasma THz system in transmission and reflection modes, respectively. Two absorption bands at 2–3 and 5–8 THz were observed. TRTS reveals an ultrafast relaxation process of the photoinduced carrier response, well described by a rate equation model with a finite concentration of mid-bandgap trap states for self-trapped excitons.The photoinduced conductivity can be well described by the Drude–Smith conductivity model with a carrier scattering time of 12–17 fs, and we observe significant carrier localization effects. A fast refractive index change was observed 100 fs before the conductivity reached its maximum, with 2 orders of magnitude larger amplitude than expected for the optically induced THz Kerr effect, indicating that free carriers are responsible for the transient index change.
基金National Natural Science Foundation of China(No.22065038)High-Level Talents Introduction in Yunnan Province(No.C619300A010)+3 种基金the Fund for Excellent Young Scholars of Yunnan(No.202001AW070008)Spring City Plan:the Highlevel Talent Promotion and Training Project of Kunming(No.2022SCP005)for financial supportthe support from the Postdoctoral Research Foundation of Yunnan University(No.W8223004)the Postdoctoral Foundation of Department of Human Resources and Social Security of Yunnan Province(No.C615300504046)。
文摘Defects at the grain boundaries(GBs)of perovskite film highly restrict both the efficiency and stability of perovskite solar cells(PSCs).Herein,organic small molecules of butanedioic acid(BA)and acetylenedicarboxylic acid(AA),containing two carbonyl(C=O)groups and different core-units,were incorporated into perovskite as additives for PSCs application.Thanks to the strong coordination interaction between C=O group and under-coordinated Pb^(2+),the additives can effectively passivate film defects and regulate the perovskite crystallization,yielding high-quality perovskite films with lower defect densities.More importantly,the additives can efficiently regulate the charge transport behaviors in PSCs.Benefiting from the defects passivation and the regulation of charge carrier dynamics,the BA and AA-treaded PSCs show the power conversion efficiencies of 21.52%and 20.50%,which are higher than that of the control device(19.41%).Besides,the optimal devices exhibit a remarkable enhanced long-term stability and moisture tolerance compared to the pristine devices.Furthermore,the transient absorption spectrum reveals the mechanism of enhanced photovoltaic performances,attributing to the improvement of charge transport capability at the perovskite/Spiro-OMeTAD interfaces.This work affords a promising strategy to improve the efficiency and stability of PSCs through regulating the charge-carrier dynamic process in perovskite film.
基金Project supported by the Natural Science Foundation of Beijing,China(Grant No.JQ19004)the Excellent Talents Training Support Fund of Beijing,China(Grant No.2017000026833ZK11)+7 种基金the National Natural Science Foundation of China(Grant Nos.51991340 and 51991342)the National Key Research and Development Program of China(Grant Nos.2016YFA0300903 and 2016YFA0300804)the Key Research and Development Program of Guangdong Province,China(Grant Nos.2019B010931001,2020B010189001,2018B010109009,and 2018B030327001)the Science Fund from the Municipal Science&Technology Commission of Beijing,China(Grant No.Z191100007219005)the Graphene Innovation Program of Beijing,China(Grant No.Z181100004818003)the Fund from the Bureau of Industry and Information Technology of Shenzhen City,China(Graphene platform 201901161512)the Innovative and Entrepreneurial Research Team Program of Guangdong Province,China(Grant No.2016ZT06D348)the Fund from the Science,Technology,and Innovation Commission of Shenzhen Municipality,China(Grant No.KYTDPT20181011104202253).
文摘Carrier lifetime is one of the most fundamental physical parameters that characterizes the average time of carrier recombination in any material.The control of carrier lifetime is the key to optimizing the device function by tuning the electro-optical conversion quantum yield,carrier diffusion length,carrier collection process,etc.Till now,the prevailing modulation methods are mainly by defect engineering and temperature control,which have limitations in the modulation direction and amplitude of the carrier lifetime.Here,we report an effective modulation on the ultrafast dynamics of photoexcited carriers in two-dimensional(2D)MoS2 monolayer by uniaxial tensile strain.The combination of optical ultrafast pump-probe technique and time-resolved photoluminescence(PL)spectroscopy reveals that the carrier dynamics through Auger scattering,carrier-phonon scattering,and radiative recombination keep immune to the strain.But strikingly,the uniaxial tensile strain weakens the trapping of photoexcited carriers by defects and therefore prolongs the corresponding carrier lifetime up to 440%per percent applied strain.Our results open a new avenue to enlarge the carrier lifetime of 2D MoS2,which will facilitate its applications in high-efficient optoelectronic and photovoltaic devices.
