The ultrafast carrier relaxation processes in CdTe quantum dots are investigated by femtosecond fluorescence upconversion spectroscopy.Photo-excited hole relaxing to the edge of the forbidden gap takes a maximal time ...The ultrafast carrier relaxation processes in CdTe quantum dots are investigated by femtosecond fluorescence upconversion spectroscopy.Photo-excited hole relaxing to the edge of the forbidden gap takes a maximal time of ~ 1.6 ps with exciting at 400 nm,depending on the state of the photo-excited hole.The shallow trapped states and deep trap states in the forbidden gap are confirmed for CdTe quantum dots.In addition,Auger relaxation of trapped carriers is observed to occur with a time constant of ~ 5 ps.A schematic model of photodynamics is established based on the results of the spectroscopy studies.Our work demonstrates that femtosecond fluorescence up-conversion spectroscopy is a suitable and effective tool in studying the transportation and conversion dynamics of photon energy in a nanosystem.展开更多
The rapid internal conversion dynamics at room temperature is determined by using the femtosecond time-resolved fluorescence depletion measurements of a complex solvated molecule of LD 700 (rhodamine 700) combined w...The rapid internal conversion dynamics at room temperature is determined by using the femtosecond time-resolved fluorescence depletion measurements of a complex solvated molecule of LD 700 (rhodamine 700) combined with steadystate absorption and fluorescence spectroscopy, as well as quantum chemical calculation. The molecule is excited by a 50 fs laser pulse at 400 nm which directly populated the highly excited singlet state, the rapid internal conversions (ICs) are observed, which leads to the directional changes of the emission transition moment following photoexcitation to the highly excited singlet state S5 of LD 700.展开更多
Oxy-fluoride glasses with composition of 25SiO2-65PbF2-9.4AlF3-0.1HoF3-0.5YbF3 were prepared. Their up-conversion fluorescence characteristics were investigated by 980 nm laser. Two emission peaks were observed at 540...Oxy-fluoride glasses with composition of 25SiO2-65PbF2-9.4AlF3-0.1HoF3-0.5YbF3 were prepared. Their up-conversion fluorescence characteristics were investigated by 980 nm laser. Two emission peaks were observed at 540 and 650 nm. The up-conversion mechanism and processes were analyzed. The relationship between pumping power and relative intensity of emissions was discussed. From the dependence, it is known that the emissions centered at 540 and 650 nm are both attributed to two-photon process.展开更多
The green and red up-conversion emissions centred at about 534, 549 and 663 nm of wavelength, corresponding respectively to the ^2H11/2 → ^4I15/2, ^4S3/2 → ^4I15/2 and ^4F9/2 → ^4I15/2 transitions of Er^3+ ions, h...The green and red up-conversion emissions centred at about 534, 549 and 663 nm of wavelength, corresponding respectively to the ^2H11/2 → ^4I15/2, ^4S3/2 → ^4I15/2 and ^4F9/2 → ^4I15/2 transitions of Er^3+ ions, have been observed for the Er^3+-doped silicate glass excited by a 978 nm semiconductor laser beam. Excitation power dependent behaviour of the up-conversion emission intensity indicates that a two-photon absorption up-conversion process is responsible for the green and red up-conversion emissions. The temperature dependence of the green up-conversion emissions is also studied in a temperature range of 296-673 K, which shows that Er^3+-doped silicate glass can be used as a sensor in high-temperature measurement.展开更多
The miniaturized femtosecond laser in near infrared-Ⅱregion is the core equipment of threephoton microscopy.In this paper,we design a compact and robust illumination source that emits dual-color linearly polarized li...The miniaturized femtosecond laser in near infrared-Ⅱregion is the core equipment of threephoton microscopy.In this paper,we design a compact and robust illumination source that emits dual-color linearly polarized light for three-photon microscopy.Based on an all-polarizationmaintaining passive mode-locked fiber laser,we shift the center wavelength of the pulses to the 1.7m band utilizing cascade Raman effect,thereby generate dual-wavelength pulses.To enhance clarity,the two wavelengths are separated through the graded-index multimode fiber.Then we obtain the dual-pulse sequences with 1639.4 nm and 1683.7 nm wavelengths,920 fs pulse duration,and 23.75 MHz pulse repetition rate.The average power of the signal is 53.64mW,corresponding to a single pulse energy of 2.25 nJ.This illumination source can be further amplified and compressed for three-photon fluorescence imaging,especially dual-color three-photon fluorescence imaging,making it an ideal option for biomedical applications.展开更多
This study investigated direct fluorescence generation from a nematic liquid crystal(NLC)NJU-LDn-4 under femtosecond laser excitation.The absorption,transmittance,excitation,and emission spectra of the NLC were assess...This study investigated direct fluorescence generation from a nematic liquid crystal(NLC)NJU-LDn-4 under femtosecond laser excitation.The absorption,transmittance,excitation,and emission spectra of the NLC were assessed.The relationship between the femtosecond pump power and fluorescence intensity was analyzed,revealing a quadratic increase and indicating that two-photon absorption(2PA)is the primary fluorescence mechanism.The LC microstructure was designed using photoalignment technology,allowing the generated fluorescence to reflect the corresponding structure.This research can establish a foundation for tunable LC microstructured fluorescence,with potential applications in fluorescence microscopy and optoelectronics.展开更多
Multiphoton absorption of femtosecond laser pulses focused through an objective with high numerical aperture(NA)can be used to image and manipulate cellular and intracellular objects.This review highlights recent adva...Multiphoton absorption of femtosecond laser pulses focused through an objective with high numerical aperture(NA)can be used to image and manipulate cellular and intracellular objects.This review highlights recent advances in intracellular manipulation,including nanosurgery and labeling in living cells with femtosecond lasers.展开更多
The optical nonlinearity in polycrystalline zinc selenide(ZnSe),excited with 775 nm,1 kHz femtosecond laser pulses was investigated via the nonlinear transmission with material thickness and the Z scan technique.The m...The optical nonlinearity in polycrystalline zinc selenide(ZnSe),excited with 775 nm,1 kHz femtosecond laser pulses was investigated via the nonlinear transmission with material thickness and the Z scan technique.The measured two photon absorption coefficientβwas intensity dependent,inferring that reverse saturated absorption(RSA)is also relevant dur-ing high intensity excitation in ZnSe.At low peak intensity I<5 GW cm^(-2),we findβ=3.5 cm GW^(-1) at 775 nm.The spec-tral properties of the broad blueish two-photon induced fluorescence(460 nm-500 nm)was studied,displaying self-ab-sorption near the band edge while the upper state lifetime was measured to be τ_(e)~3.3 ns.Stimulated emission was ob-served when pumping a 0.5 mm thick polycrystalline ZnSe sample within an optical cavity,confirmed by significant line narrowing fromΔλ=11 nm(cavity blocked)toΔλ=2.8 nm at peak wavelength λ_(p)=475 nm while the upper state life-time also decreased.These results suggest that with more optimum pumping conditions and crystal cooling,polycrystal-line ZnSe might reach lasing threshold via two-photon pumping atλ=775 nm.展开更多
Rosmarinic acid(RA)is promising as a natural and nontoxic food additive.However,many analysis methods for RA generally depend on large instruments and single signals for quantitative detection.A new upconversion fluor...Rosmarinic acid(RA)is promising as a natural and nontoxic food additive.However,many analysis methods for RA generally depend on large instruments and single signals for quantitative detection.A new upconversion fluorescence,colorimetric and photothermal multi-modal sensing strategy is developed for the quantification of RA.β-cyclodextrin(CD)modified citric acid(Cit)wrapped NaYF_(4):Yb/Er-Cit-CD(Y:Yb/Er-Cit-CD)up-conversion nanocomposite has been synthesized,which emits green fluorescence at 550nm under 980nm near-infrared(NIR)excitation.In the presence of oxidized 3,3',5,5'-tetramethylbenzidine(oxTMB),the green fluorescence is significantly quenched attributed to the fluorescence inner filter effect(IFE)between oxTMB and Y:Yb/Er-Cit-CD.When RA is intervened,blue oxTMB is reduced to colorless 3,3',5,5'-tetramethylbenzidine(TMB)inducing the recovery of up-conversion fluorescence.At the same time,colorimetric and photothermal signals readout can be easily achieved thanks to the color indication and photothermal effect of the oxTMB.The constructed Y:Yb/Er-Cit-CD/oxTMB sensor displays high sensitivity,visibility and simplicity for RA,and the limits of detection(LOD)for fluorescence,colorimetric and photothermal were 0.004μmol/L,0.036μmol/L and 0.043μmol/L,respectively.This sensing system is successfully performed for the detection of RA in food samples.展开更多
Our experiments show that external focusing and initial laser energy strongly influences filament generated by the femtosecond Ti–sapphire laser in air. The experimental measurements show the filament length can be e...Our experiments show that external focusing and initial laser energy strongly influences filament generated by the femtosecond Ti–sapphire laser in air. The experimental measurements show the filament length can be extended both by increasing the laser energy and focal length of focusing lens. On the other hand, the plasma fluorescence emission can be enhanced by increasing the laser energy with fixed focal length or decreasing the focal length. In addition, the collapse distance measured experimentally are larger than the calculated ones owing to the group-velocity-dispersion effect. In addition, we find that the line widths of the spectral lines from N2 is independent of filament positions, laser energies and external focusing.展开更多
The spectral phase of the femtosecond laser field is an important parameter that affects the up-conversion(UC)luminescence efficiency of dopant lanthanide ions.In this work,we report an experi-mental study on controll...The spectral phase of the femtosecond laser field is an important parameter that affects the up-conversion(UC)luminescence efficiency of dopant lanthanide ions.In this work,we report an experi-mental study on controlling the UC lmiiinescence efficiency in Sm^3+:NaYF4 glass by 800-nm femtosec-ond laser pulse shaping using spectral phase modulation.The optimal phase control strategy efficiently enhances or suppresses the UC luminescence intensity.Based on the laser-power dependence of the UC luminescence intensity and its comparison with the luminescence spectrum under direct 266-nm fem-tosecond lciser irradiation,we propose herein an excitation model combining non-resonant two-photon absorption with resonance-media ted three-photon absorption to explain the experimental observations.展开更多
Femtosecond time-resolved fluorescence depletion spectroscopy was used in the study of the orientation relaxation of Rhodamine 700(LD700) and Oxazine 750(OX750) in DMSO. The anisotropy functions of the dye molecules w...Femtosecond time-resolved fluorescence depletion spectroscopy was used in the study of the orientation relaxation of Rhodamine 700(LD700) and Oxazine 750(OX750) in DMSO. The anisotropy functions of the dye molecules were obtained from the fluorescence depletion spectra, as the polarization of probe pulse is parallel and perpendicular respectively. The results show that the transition dipole moment of the pump and the probe of LD700 and OX750 are parallel. The time constants of the orientation relaxation of these dye molecules in DMSO are 1.8 and 1.9 ps for LD700 and OX750, respectively.展开更多
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 11074003 and 20973001)the Key Program of Educational Commission of Anhui Province of China (Grant No. KJ2010A132)
文摘The ultrafast carrier relaxation processes in CdTe quantum dots are investigated by femtosecond fluorescence upconversion spectroscopy.Photo-excited hole relaxing to the edge of the forbidden gap takes a maximal time of ~ 1.6 ps with exciting at 400 nm,depending on the state of the photo-excited hole.The shallow trapped states and deep trap states in the forbidden gap are confirmed for CdTe quantum dots.In addition,Auger relaxation of trapped carriers is observed to occur with a time constant of ~ 5 ps.A schematic model of photodynamics is established based on the results of the spectroscopy studies.Our work demonstrates that femtosecond fluorescence up-conversion spectroscopy is a suitable and effective tool in studying the transportation and conversion dynamics of photon energy in a nanosystem.
基金Project supported by the National Natural Science Foundation of China (Grant Nos 20773139,20825314 and 20833008)the State Key Program for Basic Research of China (Grant Nos 2006CB806000 and 2007CB815200)the Knowledge Innovation Program of the Chinese Academy of Sciences (Grant No KJCX2.Y.W.H06)
文摘The rapid internal conversion dynamics at room temperature is determined by using the femtosecond time-resolved fluorescence depletion measurements of a complex solvated molecule of LD 700 (rhodamine 700) combined with steadystate absorption and fluorescence spectroscopy, as well as quantum chemical calculation. The molecule is excited by a 50 fs laser pulse at 400 nm which directly populated the highly excited singlet state, the rapid internal conversions (ICs) are observed, which leads to the directional changes of the emission transition moment following photoexcitation to the highly excited singlet state S5 of LD 700.
文摘Oxy-fluoride glasses with composition of 25SiO2-65PbF2-9.4AlF3-0.1HoF3-0.5YbF3 were prepared. Their up-conversion fluorescence characteristics were investigated by 980 nm laser. Two emission peaks were observed at 540 and 650 nm. The up-conversion mechanism and processes were analyzed. The relationship between pumping power and relative intensity of emissions was discussed. From the dependence, it is known that the emissions centered at 540 and 650 nm are both attributed to two-photon process.
基金Project supported by the National Natural Science Foundation of China (Grant No 60477023)the Natural Science Foundation of Science and Technology Commission of Liaoning Province, China (Grant No 20062137)
文摘The green and red up-conversion emissions centred at about 534, 549 and 663 nm of wavelength, corresponding respectively to the ^2H11/2 → ^4I15/2, ^4S3/2 → ^4I15/2 and ^4F9/2 → ^4I15/2 transitions of Er^3+ ions, have been observed for the Er^3+-doped silicate glass excited by a 978 nm semiconductor laser beam. Excitation power dependent behaviour of the up-conversion emission intensity indicates that a two-photon absorption up-conversion process is responsible for the green and red up-conversion emissions. The temperature dependence of the green up-conversion emissions is also studied in a temperature range of 296-673 K, which shows that Er^3+-doped silicate glass can be used as a sensor in high-temperature measurement.
基金supported by the Fundamental Re-search Funds for the Central Universities(HYGJXM202309).
文摘The miniaturized femtosecond laser in near infrared-Ⅱregion is the core equipment of threephoton microscopy.In this paper,we design a compact and robust illumination source that emits dual-color linearly polarized light for three-photon microscopy.Based on an all-polarizationmaintaining passive mode-locked fiber laser,we shift the center wavelength of the pulses to the 1.7m band utilizing cascade Raman effect,thereby generate dual-wavelength pulses.To enhance clarity,the two wavelengths are separated through the graded-index multimode fiber.Then we obtain the dual-pulse sequences with 1639.4 nm and 1683.7 nm wavelengths,920 fs pulse duration,and 23.75 MHz pulse repetition rate.The average power of the signal is 53.64mW,corresponding to a single pulse energy of 2.25 nJ.This illumination source can be further amplified and compressed for three-photon fluorescence imaging,especially dual-color three-photon fluorescence imaging,making it an ideal option for biomedical applications.
基金supported by the National Key Research and Development Program of China(No.2022YFA1405000)the Natural Science Foundation of Jiangsu Province(Nos.BK20211277 and BK20210179)+2 种基金the National Natural Science Foundation of China(NSFC)(No.62105143)the Frontier Leading Technology Basic Research Project of Jiangsu Province(No.BK20212004)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX23_0971)。
文摘This study investigated direct fluorescence generation from a nematic liquid crystal(NLC)NJU-LDn-4 under femtosecond laser excitation.The absorption,transmittance,excitation,and emission spectra of the NLC were assessed.The relationship between the femtosecond pump power and fluorescence intensity was analyzed,revealing a quadratic increase and indicating that two-photon absorption(2PA)is the primary fluorescence mechanism.The LC microstructure was designed using photoalignment technology,allowing the generated fluorescence to reflect the corresponding structure.This research can establish a foundation for tunable LC microstructured fluorescence,with potential applications in fluorescence microscopy and optoelectronics.
文摘Multiphoton absorption of femtosecond laser pulses focused through an objective with high numerical aperture(NA)can be used to image and manipulate cellular and intracellular objects.This review highlights recent advances in intracellular manipulation,including nanosurgery and labeling in living cells with femtosecond lasers.
文摘The optical nonlinearity in polycrystalline zinc selenide(ZnSe),excited with 775 nm,1 kHz femtosecond laser pulses was investigated via the nonlinear transmission with material thickness and the Z scan technique.The measured two photon absorption coefficientβwas intensity dependent,inferring that reverse saturated absorption(RSA)is also relevant dur-ing high intensity excitation in ZnSe.At low peak intensity I<5 GW cm^(-2),we findβ=3.5 cm GW^(-1) at 775 nm.The spec-tral properties of the broad blueish two-photon induced fluorescence(460 nm-500 nm)was studied,displaying self-ab-sorption near the band edge while the upper state lifetime was measured to be τ_(e)~3.3 ns.Stimulated emission was ob-served when pumping a 0.5 mm thick polycrystalline ZnSe sample within an optical cavity,confirmed by significant line narrowing fromΔλ=11 nm(cavity blocked)toΔλ=2.8 nm at peak wavelength λ_(p)=475 nm while the upper state life-time also decreased.These results suggest that with more optimum pumping conditions and crystal cooling,polycrystal-line ZnSe might reach lasing threshold via two-photon pumping atλ=775 nm.
基金supported by the National Natural Science Foundation of China(No.21305097)General Project of Education Department in Sichuan(No.035Z2270)+1 种基金Sichuan Key Discipline Construction Project of Traditional Chinese Medicine(No.2021-16-4)Double-Support Plan of Disciplinary Construction in Sichuan Agricultural University-Innovation Team Projects(No.P202108).
文摘Rosmarinic acid(RA)is promising as a natural and nontoxic food additive.However,many analysis methods for RA generally depend on large instruments and single signals for quantitative detection.A new upconversion fluorescence,colorimetric and photothermal multi-modal sensing strategy is developed for the quantification of RA.β-cyclodextrin(CD)modified citric acid(Cit)wrapped NaYF_(4):Yb/Er-Cit-CD(Y:Yb/Er-Cit-CD)up-conversion nanocomposite has been synthesized,which emits green fluorescence at 550nm under 980nm near-infrared(NIR)excitation.In the presence of oxidized 3,3',5,5'-tetramethylbenzidine(oxTMB),the green fluorescence is significantly quenched attributed to the fluorescence inner filter effect(IFE)between oxTMB and Y:Yb/Er-Cit-CD.When RA is intervened,blue oxTMB is reduced to colorless 3,3',5,5'-tetramethylbenzidine(TMB)inducing the recovery of up-conversion fluorescence.At the same time,colorimetric and photothermal signals readout can be easily achieved thanks to the color indication and photothermal effect of the oxTMB.The constructed Y:Yb/Er-Cit-CD/oxTMB sensor displays high sensitivity,visibility and simplicity for RA,and the limits of detection(LOD)for fluorescence,colorimetric and photothermal were 0.004μmol/L,0.036μmol/L and 0.043μmol/L,respectively.This sensing system is successfully performed for the detection of RA in food samples.
基金supported by the National Basic Research Program of China (No.2013CB922200)the National Natural Science Foundation of China (Nos.11474129,and 11504129)+1 种基金the Research Fund for the Doctoral Program of Higher Education (No.20130061110021)the Graduate Innovation Fund of Jilin University (No.2015091)
文摘Our experiments show that external focusing and initial laser energy strongly influences filament generated by the femtosecond Ti–sapphire laser in air. The experimental measurements show the filament length can be extended both by increasing the laser energy and focal length of focusing lens. On the other hand, the plasma fluorescence emission can be enhanced by increasing the laser energy with fixed focal length or decreasing the focal length. In addition, the collapse distance measured experimentally are larger than the calculated ones owing to the group-velocity-dispersion effect. In addition, we find that the line widths of the spectral lines from N2 is independent of filament positions, laser energies and external focusing.
基金the Na-tional Natural Science Foundation of China(Grant Nos.91850202,11774094,11727810,11804097,and 61720106009)the Science and Technology Commission of Shanghai Municipality(Grant No.17ZR146900)+1 种基金the China Postdoctoral Science Foundation(Grant No.2018M641958)ECNU Academic Innovation Promotion Program for Excellent Doctoral Students(Grant No.YBNLTS2019-011).
文摘The spectral phase of the femtosecond laser field is an important parameter that affects the up-conversion(UC)luminescence efficiency of dopant lanthanide ions.In this work,we report an experi-mental study on controlling the UC lmiiinescence efficiency in Sm^3+:NaYF4 glass by 800-nm femtosec-ond laser pulse shaping using spectral phase modulation.The optimal phase control strategy efficiently enhances or suppresses the UC luminescence intensity.Based on the laser-power dependence of the UC luminescence intensity and its comparison with the luminescence spectrum under direct 266-nm fem-tosecond lciser irradiation,we propose herein an excitation model combining non-resonant two-photon absorption with resonance-media ted three-photon absorption to explain the experimental observations.
文摘Femtosecond time-resolved fluorescence depletion spectroscopy was used in the study of the orientation relaxation of Rhodamine 700(LD700) and Oxazine 750(OX750) in DMSO. The anisotropy functions of the dye molecules were obtained from the fluorescence depletion spectra, as the polarization of probe pulse is parallel and perpendicular respectively. The results show that the transition dipole moment of the pump and the probe of LD700 and OX750 are parallel. The time constants of the orientation relaxation of these dye molecules in DMSO are 1.8 and 1.9 ps for LD700 and OX750, respectively.