Carbazole-core multi-branched chromophores 9-ethyl- 3, 6-bis （ 2- { 4- [ 5- （4-tert-butyl-phenyl） - [ 1, 3, 4 ] oxadiazol-2-yl ] - phenyl }-vinyl） -carbazole（3） and 9-ethyl-3-（ 2- {4-[ 5-（4-tert-butyl- phenyl...Carbazole-core multi-branched chromophores 9-ethyl- 3, 6-bis （ 2- { 4- [ 5- （4-tert-butyl-phenyl） - [ 1, 3, 4 ] oxadiazol-2-yl ] - phenyl }-vinyl） -carbazole（3） and 9-ethyl-3-（ 2- {4-[ 5-（4-tert-butyl- phenyl） -[ 1, 3, 4 ] oxadiazol-2-yl ] -phenyl }-vinyl ） -carbazole （ 2 ） are synthesized through Wittig reaction and characterized by nuclear magnetic resonance（NMR）and infrared（IR）. The two- photon absorption properties of chromophores are investigated. These chromophores exhibit large two-photon absorption crosssections and strong blue two-photon excited fluorescence. The cooperative enhancement of two-photon absorption（TPA） in the multi-branched structures is observed. This enhancement is partly attributed to the electronic coupling between the branches. The electronic push-pull structures in the arm and their cooperative effects help the extended charge transfer for TPA.展开更多
The analytic response theory at density functional theory level is applied to investigate onephoton and two-photon absorption properties of a series of recently synthesized pyrene-core derivatives. The theoretical res...The analytic response theory at density functional theory level is applied to investigate onephoton and two-photon absorption properties of a series of recently synthesized pyrene-core derivatives. The theoretical results show that there are a few charge-transfer states for each compound in the lower energy region. The one-photon absorption properties of the five investigated compounds are highly consistent with those given by experimental measurements. The two-photon absorption intensities of the compounds are greatly enhanced with the increments of the molecular sizes, in which the two-photon absorption cross section of the four-branched compound is about 5.6 times of that of the mono-branched molecule. Fhrthermore, it is shown that the two-photon absorption properties are sensitive to the geometrical arrangements.展开更多
Efficient Ti-catalyzed reductive coupling methodology was first employed to synthesize the symmetrical bis-donor stilbene, trans-4, 4'-bis[diphenyl amino] stilbene (BDPAS). X-ray diffraction analyses reveal that t...Efficient Ti-catalyzed reductive coupling methodology was first employed to synthesize the symmetrical bis-donor stilbene, trans-4, 4'-bis[diphenyl amino] stilbene (BDPAS). X-ray diffraction analyses reveal that this new crystal belongs to the triclinic crystal system of centro-symmetric P-1 space group. The DBPAS solution, with the linear transmission at wavelength of greater than or equal to 450 nm, possesses large two-photon absorption cross section as high as 39.4x10(-48) cm(4).s/photon resulting in strong two-photon induced blue fluorescence of 460 nm, pumped by 740 nm laser irradiation.展开更多
Perovskite nanocrystals(NCs) with high two-photon absorption(TPA) cross-section are of great interest due to their potential applications in three-dimensional optical data storage and multiphoton fluorescence microsco...Perovskite nanocrystals(NCs) with high two-photon absorption(TPA) cross-section are of great interest due to their potential applications in three-dimensional optical data storage and multiphoton fluorescence microscopy. Among various perovskite materials, FAPbBr_(3) NCs show a better development prospect due to their excellent stability. However, there are few reports on their nonlinear optical properties. In this work, the nonlinear optical behavior of FAPbBr_(3) NCs is studied.The methods of multiphoton absorption photoluminescence saturation and open aperture Z-scan technique were applied to determine the TPA cross-section of FAPbBr_(3)NCs, which was around 2.76 × 10^(-45)cm^(4)·s·photon^(-1) at 800 nm. In addition,temperature-dependent photoluminescence induced by TPA was investigated, and the small longitudinal optical phonon energy and electron–phonon coupling strength was obtained, which confirm the weak Pb–Br interaction. Meanwhile, it is found that the exciton binding energy in FAPbBr_(3) NCs was 69.668 me V, which may be ascribed to the strong hydrogen bond interaction. It is expected that our findings will promote the application of FAPbBr_(3) NCs in optoelectronic devices.展开更多
Two novel V-shaped symmetric chromophores： E-2,8-bis（4-vinyl-4-carbazol-9-yl）diben- zothiophene （abbreviated as SK-G1） and E-2,8-bis（4-vinyl-4-triphenylamino） dibenzothiophene （abbreviated as ST-G1） have been...Two novel V-shaped symmetric chromophores： E-2,8-bis（4-vinyl-4-carbazol-9-yl）diben- zothiophene （abbreviated as SK-G1） and E-2,8-bis（4-vinyl-4-triphenylamino） dibenzothiophene （abbreviated as ST-G1） have been synthesized and characterized. Their two photon absorption properties were measured by the open-aperture femtosecond Z-scan technique and the nanosecond nonlinear optical transmission （NLT）, respectively, when pumped by Ti： sapphire laser at 750 nm and 800 nm.展开更多
Two-photon absorption （TPA） and nonlinear refraction in AlN single crystals are revealed with the single beam Z-scan technique. A large TPA coefficient of 134-3 cm/CW at 355 nm and third-order nonlinear refractive i...Two-photon absorption （TPA） and nonlinear refraction in AlN single crystals are revealed with the single beam Z-scan technique. A large TPA coefficient of 134-3 cm/CW at 355 nm and third-order nonlinear refractive indices of-1.91±0.38×10-13 cm2/W at 355nm, 1.79±0.36 × 10-13 cm2/W at 532nm and 1.61±0.32 ×10-12 cm2/W at 1064nm are derived. It is inferred that the TPA-generated free carriers are responsible for the large negative nonlinear refractive index at 355 nm, while the oxygen impurity induced bandgap narrowing may account for the large third-order nonlinear refractive indices at 532nm and 1064nm. The large nonlinear optical responses of AIN promise wide applications in the deep ultraviolet nonlinear optical devices.展开更多
This paper theoretically studies the effects of the vacuum-induced coherence on one- and two-photon absorption in a four-level atomic medium. It finds that the one- and two-photon absorption and amplification properti...This paper theoretically studies the effects of the vacuum-induced coherence on one- and two-photon absorption in a four-level atomic medium. It finds that the one- and two-photon absorption and amplification properties are quite sensitive to the vacuum-induced coherence. It is also shown that the one- and two-photon absorption spectra can be dramatically affected by modulating the relative phase of the applied fields, With the proper choice of the relative phase, the amplification without inversion for the probe field can be realized.展开更多
Soliton dynamics are numerically investigated in a two-mode fiber with the two-photon absorption,and the effects of the two-photon absorption on the soliton propagation and interaction are demonstrated in different di...Soliton dynamics are numerically investigated in a two-mode fiber with the two-photon absorption,and the effects of the two-photon absorption on the soliton propagation and interaction are demonstrated in different dispersion regimes.Soliton dynamics depend strictly on the sign and magnitude of the group velocity dispersion(GVD)coefficient of each mode and the strength(coefficient)of the two-photon absorption.The two-photon absorption leads to the soliton collapse,enhances the neighboring soliton interaction in both modes,and increases the energy exchange between the two modes.Finally,an available control is proposed to suppress the effects by the use of the nonlinear gain with filter.展开更多
We investigate the influence of the vacuum-induced coherence on one- and two-photon absorption of the transient process in a four-level Y-type atomic system. We find that the one- and two-photon t, ransient absorption...We investigate the influence of the vacuum-induced coherence on one- and two-photon absorption of the transient process in a four-level Y-type atomic system. We find that the one- and two-photon t, ransient absorption and amplification properties are quite sensitive to the vacuum-induced coherence. It is also shown that the one- and two-photon absorption spectra of the transient process can be dramatically affected by modulating the relative phase of the applied fields. By apprdpriately choosing the relative phase, the amplification of the probe field can be achieved.展开更多
New two-photon absorption dyes including benzophenone parts, p-N,N-diphenylamino-p＇-phenacylstilbene （C1）, 4,4-di-（4- benzoylstyrene）yltriphenylamine （C2） and 4,4＇,4＇-tri（4-benzoylstyrene）yltriphenylamine ...New two-photon absorption dyes including benzophenone parts, p-N,N-diphenylamino-p＇-phenacylstilbene （C1）, 4,4-di-（4- benzoylstyrene）yltriphenylamine （C2） and 4,4＇,4＇-tri（4-benzoylstyrene）yltriphenylamine （C3）, were synthesized and characterized by ^1H NMR and elemental analysis. The ratio of the molar extinction coefficients of compounds was approximately equal to the ratio of the branch amount of the compounds, namely, C1：C2：C3 was 1：2：3. Extremely high fluorescence quantum yields were detected for these compounds. These molecules exhibited obvious two-photon upconcerted fluorescence as excited by 800 nm Ti：sapphire femtosecond laser.展开更多
Aggregation effect caused by the intermolecular hydrogen-bonding interactions on two-photon absorption prop- erties of （E）-4-（2-nitrovinyl） benzenamine molecules is studied at a hybrid density functional level. Th...Aggregation effect caused by the intermolecular hydrogen-bonding interactions on two-photon absorption prop- erties of （E）-4-（2-nitrovinyl） benzenamine molecules is studied at a hybrid density functional level. The geometry optimization studies indicate that there exist two probable conformations for the dimers and three for the trimers. A strong red-shift of the charge-transfer states is shown. The two-photon absorption cross sections of the molecule for certain conformations are greatly enhanced by the aggregation effect, from which a ratio of 1.0：2.6：3.6 is found for the molecule and its dimer and trimer with nearly planar structures. Namely, a 30 or 20 percent increase of the two-photon absorption cross section is observed.展开更多
Considering two beams propagate in semiconductor crystal, this paper discusses the polarization dependence of pump beam-induced intensity attenuation of probe beam due to two-photon absorption （TPA）. Numerical calcu...Considering two beams propagate in semiconductor crystal, this paper discusses the polarization dependence of pump beam-induced intensity attenuation of probe beam due to two-photon absorption （TPA）. Numerical calculation and experimental measurement demonstrate that TPA coefficient is polarization dependent. For homogeneous materials, probe beam attenuation arises from the imaginary part of diagonal and off-diagonal components of third-order nonlinear susceptibilities.展开更多
The protonation effects on one- and two-photon absorption properties of an octupolar molecule TA with 1,3,5-triazine core and pyrrole electron-donating end-groups have been studied at hybrid density functional theory ...The protonation effects on one- and two-photon absorption properties of an octupolar molecule TA with 1,3,5-triazine core and pyrrole electron-donating end-groups have been studied at hybrid density functional theory level. A computational scheme is developed to simulate a proton attached to an atom. The numerical results show that large changes in both one- and two-photon absorption properties are observed when the compound is transformed from neutral to threefold protonated states. When the compound is protonated, more charge transfer states appear and the absorption band has a red-shift. Furthermore, the two-photon absorption cross-section is largely enhanced. The theoretical calculations demonstrate the protonation effect on promoting the intramolecular charge transfer strength. The results present qualitative agreement with the experimental observations. A two-photon absorption switch with the compound TA based on the protonation effect is proposed.展开更多
Improving the up-conversion luminescence efficiency crucial in several related application areas. In this work, of rare-earth ions via the multi-photon absorption process is we theoretically propose a feasible scheme ...Improving the up-conversion luminescence efficiency crucial in several related application areas. In this work, of rare-earth ions via the multi-photon absorption process is we theoretically propose a feasible scheme to enhance the resonance-mediated two-photon absorption in Er3＋ ions by shaping the femtosecond laser field with a rectangle phase modulation. Our theoretical results show that the resonance-mediated two-photon absorption can be decomposed into the on-resonant and near-resonant parts, and the on-resonant part mainly comes from the contribution of laser central frequency components, while the near-resonant part mainly results from the excitation of low and high laser frequency components. So, the rectangle phase modulation can induce a constructive interference between the two parts by properly designing the modulation depth and width, and finally realizes the resonance-mediated two-photon absorption enhancement. More- over, our results also show that the enhancement efficiency of resonance-mediated two-photon absorption depends on the laser pulse width （or laser spectral bandwidth）, final state transition frequency, and intermediate and final state absorption bandwidths. The enhancement efficiency modulation can be attributed to the relative weight manipulation of on-resonant and near-resonant two-photon absorption in the whole excitation process. This study presents a clear physical insight for the quantum control of resonance-mediated two-photon absorption in the rare-earth ions, and there will be an important significance for improving the up-conversion luminescence efficiency of rare-earth ions.展开更多
Two new s-triazine derivatives, which belong to linear dipolar type and triangle octupolar type respectively, have been synthesized. The structure of the dipolar compound has been determined by X-ray diffraction. The ...Two new s-triazine derivatives, which belong to linear dipolar type and triangle octupolar type respectively, have been synthesized. The structure of the dipolar compound has been determined by X-ray diffraction. The two-photon absorption cross-section σ, and the two-photon excited fluorescence (TPEF) intensities are increased significantly from dipolar compound to octupolar compound.展开更多
One-photon absorption and two-photon absorption（TPA） properties of three tris（picolyl）amine-based zinc ion sensors are investigated by employing the density functional response theory in combination with the polar...One-photon absorption and two-photon absorption（TPA） properties of three tris（picolyl）amine-based zinc ion sensors are investigated by employing the density functional response theory in combination with the polarizable continuum model.The different isomer and coordination geometry of each probe are taken into account. Special emphasis is placed on the effects of isomerism and the coordination mode on the optical properties. The intra-molecular charge transfer（ICT）properties are specified by natural bond orbital charge analysis. It is shown that the isomerism has non-negligible effects on TPA properties of free ligands. It is found that both the TPA wavelength and the cross section are highly dependent on the coordination mode. When the zinc ion connects with the picolyl unit in the middle of a ligand, the zinc complex has a large TPA intensity in a long wavelength range due to the increased ICT mechanism.展开更多
By numerically solving the Maxwell-Bloch equations using an iterative predictor-corrector finite-difference time-domain technique, we investigate propagating properties of a few-cycle laser pulse in a 4,4＇-bis（di-n-...By numerically solving the Maxwell-Bloch equations using an iterative predictor-corrector finite-difference time-domain technique, we investigate propagating properties of a few-cycle laser pulse in a 4,4＇-bis（di-n-butylamino） stilbene （BDBAS） molecular medium when a static electric field exists. Dynamical two-photon absorption （TPA） cross sections are obtained and optical limiting （OL） behavior is displayed. The results show that when the static electric field intensity increases, the dynamical TPA cross section is enhanced and the OL behavior is improved. Moreover, both even- and odd-order harmonic spectral components are generated with existence of the static electric field because it breaks the inversion symmetry of the BDBAS molecule. This work provides a method to modulate the nonlinear optical properties of the BDBAS compounds.展开更多
Two-photon fluorescence dyes have shown promising applications in biomedical imaging.However,the substitution site effect on geometric structures and photophysical properties of fluorescence dyes is rarely illustrated...Two-photon fluorescence dyes have shown promising applications in biomedical imaging.However,the substitution site effect on geometric structures and photophysical properties of fluorescence dyes is rarely illustrated in detail.In this work,a series of new lipid droplets detection dyes are designed and studied,molecular optical properties and non-radiative transitions are analyzed.The intramolecular weak interaction and electron-hole analysis reveal its inner mechanisms.All dyes are proven to possess excellent photophysical properties with high fluorescence quantum efficiency and large stokes shift as well as remarkable two-photon absorption cross section.Our work reasonably elucidates the experimental measurements and the effects of substitution site on two-photon absorption and excited states properties of lipid droplets detection NAPBr dyes are highlighted,which could provide a theoretical perspective for designing efficient organic dyes for lipid droplets detection in biology and medicine fields.展开更多
The electronic structures, one-photon absorption （OPA） and two-photon absorption （TPA） properties of the azulenylporphyrins and azulene-fused porphyrins have been comparatively studied by using DFT/B3LYP/6-31G（d...The electronic structures, one-photon absorption （OPA） and two-photon absorption （TPA） properties of the azulenylporphyrins and azulene-fused porphyrins have been comparatively studied by using DFT/B3LYP/6-31G（d） and the ZINDO/SDCI method. With the number of azulenyl groups increasing, the OPA wavelengths of all molecules are red-shifted in 400-600 nm and the two-photon absorption cross section is gradually enlarged. The azulene-fused structures facilitate an expanding conjugated area and increasing TPA cross section. The origin of TPA properties of studied compounds is studied with a two-level model. In summary, the azulene-fused porphyrins exhibit strong two-photon absorption.展开更多
On the level of the time-dependent hybrid density functional theory, the one- and two-photon absorption properties of a series of symmetric 4-bis{2-[4-（2-aryl） phenyl]vinyl）-2,5-bisdialkoxybenzenes are studied resp...On the level of the time-dependent hybrid density functional theory, the one- and two-photon absorption properties of a series of symmetric 4-bis{2-[4-（2-aryl） phenyl]vinyl）-2,5-bisdialkoxybenzenes are studied respectively utilizing the analytic response theory and the few-state model methods. The calculated results show that the planarity of the geometrical structure plays a great role in enhancing the linear and nonlinear optical abilities of the molecule. However the effect of the length of the chain linked to the π-centre on the optical property is very little. For the investigated compounds, the A-π-A type charge-transfer molecules display more superior one- and two-photon absorption characteristics than the D-π-D type ones. Furthermore, the two-photon absorption results by use of few-state model are generally consistent with those by analytic response theory, demonstrating the reliability of the few-state model for evaluating the two-photon absorption cross section. The numerical simulations are in good agreement in tendency with the available experimental measurements.展开更多
基金The National Natural Science Foundation of China(No.60678042)the Natural Science Foundation of Jiangsu Province(No.BK2006553)the Pre-Research Project of the National Natural Science Foundation supported by Southeast University(No.9207041399)
文摘Carbazole-core multi-branched chromophores 9-ethyl- 3, 6-bis （ 2- { 4- [ 5- （4-tert-butyl-phenyl） - [ 1, 3, 4 ] oxadiazol-2-yl ] - phenyl }-vinyl） -carbazole（3） and 9-ethyl-3-（ 2- {4-[ 5-（4-tert-butyl- phenyl） -[ 1, 3, 4 ] oxadiazol-2-yl ] -phenyl }-vinyl ） -carbazole （ 2 ） are synthesized through Wittig reaction and characterized by nuclear magnetic resonance（NMR）and infrared（IR）. The two- photon absorption properties of chromophores are investigated. These chromophores exhibit large two-photon absorption crosssections and strong blue two-photon excited fluorescence. The cooperative enhancement of two-photon absorption（TPA） in the multi-branched structures is observed. This enhancement is partly attributed to the electronic coupling between the branches. The electronic push-pull structures in the arm and their cooperative effects help the extended charge transfer for TPA.
文摘The analytic response theory at density functional theory level is applied to investigate onephoton and two-photon absorption properties of a series of recently synthesized pyrene-core derivatives. The theoretical results show that there are a few charge-transfer states for each compound in the lower energy region. The one-photon absorption properties of the five investigated compounds are highly consistent with those given by experimental measurements. The two-photon absorption intensities of the compounds are greatly enhanced with the increments of the molecular sizes, in which the two-photon absorption cross section of the four-branched compound is about 5.6 times of that of the mono-branched molecule. Fhrthermore, it is shown that the two-photon absorption properties are sensitive to the geometrical arrangements.
文摘Efficient Ti-catalyzed reductive coupling methodology was first employed to synthesize the symmetrical bis-donor stilbene, trans-4, 4'-bis[diphenyl amino] stilbene (BDPAS). X-ray diffraction analyses reveal that this new crystal belongs to the triclinic crystal system of centro-symmetric P-1 space group. The DBPAS solution, with the linear transmission at wavelength of greater than or equal to 450 nm, possesses large two-photon absorption cross section as high as 39.4x10(-48) cm(4).s/photon resulting in strong two-photon induced blue fluorescence of 460 nm, pumped by 740 nm laser irradiation.
基金Project supported by the National Natural Science Foundation of China (Grant No. 62174079)the Fund from the Science, Technology, and Innovation Commission of Shenzhen Municipality (Grant Nos. JCYJ20220530113015035, JCYJ20210324120204011, JCYJ20190808121211510, and KQTD2015071710313656)。
文摘Perovskite nanocrystals(NCs) with high two-photon absorption(TPA) cross-section are of great interest due to their potential applications in three-dimensional optical data storage and multiphoton fluorescence microscopy. Among various perovskite materials, FAPbBr_(3) NCs show a better development prospect due to their excellent stability. However, there are few reports on their nonlinear optical properties. In this work, the nonlinear optical behavior of FAPbBr_(3) NCs is studied.The methods of multiphoton absorption photoluminescence saturation and open aperture Z-scan technique were applied to determine the TPA cross-section of FAPbBr_(3)NCs, which was around 2.76 × 10^(-45)cm^(4)·s·photon^(-1) at 800 nm. In addition,temperature-dependent photoluminescence induced by TPA was investigated, and the small longitudinal optical phonon energy and electron–phonon coupling strength was obtained, which confirm the weak Pb–Br interaction. Meanwhile, it is found that the exciton binding energy in FAPbBr_(3) NCs was 69.668 me V, which may be ascribed to the strong hydrogen bond interaction. It is expected that our findings will promote the application of FAPbBr_(3) NCs in optoelectronic devices.
基金the National Natural Science Foundation of China(No.50273024)the Foundation for the Author of National Excellent Doctoral Dissertation of PR China(FANEDD,No 200333)+1 种基金Natural Foundation of Jiangsu Province(No.BK2003031)the Foundation of Jiangsu Province Education Committee(No.03KJB 150115)for financial support.
文摘Two novel V-shaped symmetric chromophores： E-2,8-bis（4-vinyl-4-carbazol-9-yl）diben- zothiophene （abbreviated as SK-G1） and E-2,8-bis（4-vinyl-4-triphenylamino） dibenzothiophene （abbreviated as ST-G1） have been synthesized and characterized. Their two photon absorption properties were measured by the open-aperture femtosecond Z-scan technique and the nanosecond nonlinear optical transmission （NLT）, respectively, when pumped by Ti： sapphire laser at 750 nm and 800 nm.
基金Supported by the National Natural Science Foundation of China under Grant Nos 51372267,51210105026 and 51172270the National Basic Research Program of China under Grant No 2013CB932901
文摘Two-photon absorption （TPA） and nonlinear refraction in AlN single crystals are revealed with the single beam Z-scan technique. A large TPA coefficient of 134-3 cm/CW at 355 nm and third-order nonlinear refractive indices of-1.91±0.38×10-13 cm2/W at 355nm, 1.79±0.36 × 10-13 cm2/W at 532nm and 1.61±0.32 ×10-12 cm2/W at 1064nm are derived. It is inferred that the TPA-generated free carriers are responsible for the large negative nonlinear refractive index at 355 nm, while the oxygen impurity induced bandgap narrowing may account for the large third-order nonlinear refractive indices at 532nm and 1064nm. The large nonlinear optical responses of AIN promise wide applications in the deep ultraviolet nonlinear optical devices.
基金Project supported by the National Natural Science Foundation of China （Grant Nos 10575040 and 90503010）.Acknowledgments The authors would like to thank Dr Wu Ying for helpful discussions.
文摘This paper theoretically studies the effects of the vacuum-induced coherence on one- and two-photon absorption in a four-level atomic medium. It finds that the one- and two-photon absorption and amplification properties are quite sensitive to the vacuum-induced coherence. It is also shown that the one- and two-photon absorption spectra can be dramatically affected by modulating the relative phase of the applied fields, With the proper choice of the relative phase, the amplification without inversion for the probe field can be realized.
文摘Soliton dynamics are numerically investigated in a two-mode fiber with the two-photon absorption,and the effects of the two-photon absorption on the soliton propagation and interaction are demonstrated in different dispersion regimes.Soliton dynamics depend strictly on the sign and magnitude of the group velocity dispersion(GVD)coefficient of each mode and the strength(coefficient)of the two-photon absorption.The two-photon absorption leads to the soliton collapse,enhances the neighboring soliton interaction in both modes,and increases the energy exchange between the two modes.Finally,an available control is proposed to suppress the effects by the use of the nonlinear gain with filter.
基金The project supported in part by National Natural Science Foundation of China under Grant Nos. 60478029 and 10575040 The authors would like to thank Prof.Ying Wu for stimulating discussion.
文摘We investigate the influence of the vacuum-induced coherence on one- and two-photon absorption of the transient process in a four-level Y-type atomic system. We find that the one- and two-photon t, ransient absorption and amplification properties are quite sensitive to the vacuum-induced coherence. It is also shown that the one- and two-photon absorption spectra of the transient process can be dramatically affected by modulating the relative phase of the applied fields. By apprdpriately choosing the relative phase, the amplification of the probe field can be achieved.
基金support from National Natural Science Foundation of China(Nos. 20776165,20702065,20872184)"Key Foundation of Chongqing Science and Technology Commission"(No.CSTC 2008BA4020)+1 种基金"A Foundation for the Author of National Excellent Doctoral Dissertation of PR China(No.200735)"for financial supportsponsored by the Scientific Research Foundation for the Returned Overseas Chinese Scholars,State Education Ministry as well(Nos.20071108- 1,20071108-5)
文摘New two-photon absorption dyes including benzophenone parts, p-N,N-diphenylamino-p＇-phenacylstilbene （C1）, 4,4-di-（4- benzoylstyrene）yltriphenylamine （C2） and 4,4＇,4＇-tri（4-benzoylstyrene）yltriphenylamine （C3）, were synthesized and characterized by ^1H NMR and elemental analysis. The ratio of the molar extinction coefficients of compounds was approximately equal to the ratio of the branch amount of the compounds, namely, C1：C2：C3 was 1：2：3. Extremely high fluorescence quantum yields were detected for these compounds. These molecules exhibited obvious two-photon upconcerted fluorescence as excited by 800 nm Ti：sapphire femtosecond laser.
基金Project supported by the National Basic Research Program of China (Grant No. 2006CB806000)the Open Fund of the State Key Laboratory of High Field Laser Physics (Shanghai Institute of Optics and Fine Mechanics)the National Natural Science Foundation of China (Grant No. 10974121)
文摘Aggregation effect caused by the intermolecular hydrogen-bonding interactions on two-photon absorption prop- erties of （E）-4-（2-nitrovinyl） benzenamine molecules is studied at a hybrid density functional level. The geometry optimization studies indicate that there exist two probable conformations for the dimers and three for the trimers. A strong red-shift of the charge-transfer states is shown. The two-photon absorption cross sections of the molecule for certain conformations are greatly enhanced by the aggregation effect, from which a ratio of 1.0：2.6：3.6 is found for the molecule and its dimer and trimer with nearly planar structures. Namely, a 30 or 20 percent increase of the two-photon absorption cross section is observed.
文摘Considering two beams propagate in semiconductor crystal, this paper discusses the polarization dependence of pump beam-induced intensity attenuation of probe beam due to two-photon absorption （TPA）. Numerical calculation and experimental measurement demonstrate that TPA coefficient is polarization dependent. For homogeneous materials, probe beam attenuation arises from the imaginary part of diagonal and off-diagonal components of third-order nonlinear susceptibilities.
文摘The protonation effects on one- and two-photon absorption properties of an octupolar molecule TA with 1,3,5-triazine core and pyrrole electron-donating end-groups have been studied at hybrid density functional theory level. A computational scheme is developed to simulate a proton attached to an atom. The numerical results show that large changes in both one- and two-photon absorption properties are observed when the compound is transformed from neutral to threefold protonated states. When the compound is protonated, more charge transfer states appear and the absorption band has a red-shift. Furthermore, the two-photon absorption cross-section is largely enhanced. The theoretical calculations demonstrate the protonation effect on promoting the intramolecular charge transfer strength. The results present qualitative agreement with the experimental observations. A two-photon absorption switch with the compound TA based on the protonation effect is proposed.
基金Project supported by the National Natural Science Foundation of China(Grant No.11474096)the Science and Technology Commission of Shanghai Municipality,China(Grant Nos.14JC1401500,17ZR146900,and 16520721200)the Higher Education Key Program of He'nan Province of China(Grant No.17A140025)
文摘Improving the up-conversion luminescence efficiency crucial in several related application areas. In this work, of rare-earth ions via the multi-photon absorption process is we theoretically propose a feasible scheme to enhance the resonance-mediated two-photon absorption in Er3＋ ions by shaping the femtosecond laser field with a rectangle phase modulation. Our theoretical results show that the resonance-mediated two-photon absorption can be decomposed into the on-resonant and near-resonant parts, and the on-resonant part mainly comes from the contribution of laser central frequency components, while the near-resonant part mainly results from the excitation of low and high laser frequency components. So, the rectangle phase modulation can induce a constructive interference between the two parts by properly designing the modulation depth and width, and finally realizes the resonance-mediated two-photon absorption enhancement. More- over, our results also show that the enhancement efficiency of resonance-mediated two-photon absorption depends on the laser pulse width （or laser spectral bandwidth）, final state transition frequency, and intermediate and final state absorption bandwidths. The enhancement efficiency modulation can be attributed to the relative weight manipulation of on-resonant and near-resonant two-photon absorption in the whole excitation process. This study presents a clear physical insight for the quantum control of resonance-mediated two-photon absorption in the rare-earth ions, and there will be an important significance for improving the up-conversion luminescence efficiency of rare-earth ions.
基金supported by the National Natural Science Foundation of China(No.20172034,20472044)the Ph.D.Programs Foundation of Ministry of Education of China
文摘Two new s-triazine derivatives, which belong to linear dipolar type and triangle octupolar type respectively, have been synthesized. The structure of the dipolar compound has been determined by X-ray diffraction. The two-photon absorption cross-section σ, and the two-photon excited fluorescence (TPEF) intensities are increased significantly from dipolar compound to octupolar compound.
基金Project supported by the Natural Science Foundation of Shandong Province,China(Grant No.ZR2014AM026)the Taishan Scholar Project of Shandong Province,China
文摘One-photon absorption and two-photon absorption（TPA） properties of three tris（picolyl）amine-based zinc ion sensors are investigated by employing the density functional response theory in combination with the polarizable continuum model.The different isomer and coordination geometry of each probe are taken into account. Special emphasis is placed on the effects of isomerism and the coordination mode on the optical properties. The intra-molecular charge transfer（ICT）properties are specified by natural bond orbital charge analysis. It is shown that the isomerism has non-negligible effects on TPA properties of free ligands. It is found that both the TPA wavelength and the cross section are highly dependent on the coordination mode. When the zinc ion connects with the picolyl unit in the middle of a ligand, the zinc complex has a large TPA intensity in a long wavelength range due to the increased ICT mechanism.
文摘By numerically solving the Maxwell-Bloch equations using an iterative predictor-corrector finite-difference time-domain technique, we investigate propagating properties of a few-cycle laser pulse in a 4,4＇-bis（di-n-butylamino） stilbene （BDBAS） molecular medium when a static electric field exists. Dynamical two-photon absorption （TPA） cross sections are obtained and optical limiting （OL） behavior is displayed. The results show that when the static electric field intensity increases, the dynamical TPA cross section is enhanced and the OL behavior is improved. Moreover, both even- and odd-order harmonic spectral components are generated with existence of the static electric field because it breaks the inversion symmetry of the BDBAS molecule. This work provides a method to modulate the nonlinear optical properties of the BDBAS compounds.
基金This work was supported by the National Natural Science Foundation of China(No.11804196 and No.11904210)the Project funded by China Postdoctoral Science Foundation(No.2018M642689)the Open Fund of Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates,(South China University of Technology)(No.2019B030301003).
文摘Two-photon fluorescence dyes have shown promising applications in biomedical imaging.However,the substitution site effect on geometric structures and photophysical properties of fluorescence dyes is rarely illustrated in detail.In this work,a series of new lipid droplets detection dyes are designed and studied,molecular optical properties and non-radiative transitions are analyzed.The intramolecular weak interaction and electron-hole analysis reveal its inner mechanisms.All dyes are proven to possess excellent photophysical properties with high fluorescence quantum efficiency and large stokes shift as well as remarkable two-photon absorption cross section.Our work reasonably elucidates the experimental measurements and the effects of substitution site on two-photon absorption and excited states properties of lipid droplets detection NAPBr dyes are highlighted,which could provide a theoretical perspective for designing efficient organic dyes for lipid droplets detection in biology and medicine fields.
基金Project supported by the National Natural Science Foundation of China the Open Project of State Key Laboratory of Supramolecular Structure and Materials of Jilin University (Grant No SKLSSM200716)
文摘The electronic structures, one-photon absorption （OPA） and two-photon absorption （TPA） properties of the azulenylporphyrins and azulene-fused porphyrins have been comparatively studied by using DFT/B3LYP/6-31G（d） and the ZINDO/SDCI method. With the number of azulenyl groups increasing, the OPA wavelengths of all molecules are red-shifted in 400-600 nm and the two-photon absorption cross section is gradually enlarged. The azulene-fused structures facilitate an expanding conjugated area and increasing TPA cross section. The origin of TPA properties of studied compounds is studied with a two-level model. In summary, the azulene-fused porphyrins exhibit strong two-photon absorption.
基金Project supported by the State Key Development Program for Basic Research of China(Grant No.2006CB806000)the Open Fund of the State Key Laboratory of High Field Laser Physics(Shanghai Institute of Optics and Fine Mechanics),Higher Educational Science and Technology Program of Shandong Province(Grant No.J09LA13)
文摘On the level of the time-dependent hybrid density functional theory, the one- and two-photon absorption properties of a series of symmetric 4-bis{2-[4-（2-aryl） phenyl]vinyl）-2,5-bisdialkoxybenzenes are studied respectively utilizing the analytic response theory and the few-state model methods. The calculated results show that the planarity of the geometrical structure plays a great role in enhancing the linear and nonlinear optical abilities of the molecule. However the effect of the length of the chain linked to the π-centre on the optical property is very little. For the investigated compounds, the A-π-A type charge-transfer molecules display more superior one- and two-photon absorption characteristics than the D-π-D type ones. Furthermore, the two-photon absorption results by use of few-state model are generally consistent with those by analytic response theory, demonstrating the reliability of the few-state model for evaluating the two-photon absorption cross section. The numerical simulations are in good agreement in tendency with the available experimental measurements.
