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
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
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
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
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
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
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
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
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
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
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
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
The two-photon absorption(TPA)and TPA-induced frequency upconversion emission properties of the dyes 4-[P-(dicyanoethylamino)crystal]-N-methypyrdinium iodide and the complex of 4-[P-(dicyanoethylamino)crystal]-N...The two-photon absorption(TPA)and TPA-induced frequency upconversion emission properties of the dyes 4-[P-(dicyanoethylamino)crystal]-N-methypyrdinium iodide and the complex of 4-[P-(dicyanoethylamino)crystal]-N-methypyrdinium iodide and Ce(NO3)3 were experimentally studied.It was found that the TPA cross section for the dye sensitized by Ce3+ is two factors larger than that of the dye without being sensitized.A three-level system model of the dye molecules was used to analyze the enhancement of TPA by the sensitizer Ce3+,which indicated that the sensitizer results in the increase of the transition dipole moment from the one-photon allowed excited state(1Bu)to the two-photon allowed excited state(2Ag).展开更多
The influence of rotational isomerism on the two-photon absorption (TPA) of FTC chromophores has been investi- gated using the quadratic response theory with the B3LYP functional. Eight rotamers induced by three rot...The influence of rotational isomerism on the two-photon absorption (TPA) of FTC chromophores has been investi- gated using the quadratic response theory with the B3LYP functional. Eight rotamers induced by three rotatable single bonds in the molecule are fully optimized, and it is found that their conformational energies are nearly degenerate. Our calculations demonstrate that rotational isomerism has an important effect on the TPA cross sections. For a certain rotamer, the maximum TPA cross section is enhanced significantly. In addition, in the longer wavelength region, the rotational isomerism could lead to a large shift of the TPA position.展开更多
The linear and nonlinear optical properties of two metalloporphyrin complexes formed by the complementary coordination of central zinc or magnesium ions to the ligand 5, 10, 15-tri-(p-tolyl)-20-phenylethynylporphyri...The linear and nonlinear optical properties of two metalloporphyrin complexes formed by the complementary coordination of central zinc or magnesium ions to the ligand 5, 10, 15-tri-(p-tolyl)-20-phenylethynylporphyrin are theo- retically investigated by using the analytic response theory at the density functional theory level. The results indicate that the studied complexes present more symmetric geometry structures than the ligand. The charge-transfer states of the two complexes in the lower energy region are all almost degenerate but those of the ligand are well separated. The ratio of the two-photon absorption cross sections of the ligand, zinc-porphyrin and magnesium-porphyrin com- plexes is 1.0:1.5:1.8, demonstrating that the two-photon absorption capability can be greatly increased when the ligand is coordinated with a metal ion. Moreover, several physical micro-mechanisms including electron transitions and in- tramolecular charge-transfer processes are discussed to explore the differences in optical property between the ligand and two complexes.展开更多
This paper has theoretically designed a series of aggregate polymers on the basis of several para-nitroaniline monomers by hydrogen-bond interactions. At the level of time-dependent hybrid density functional theory, i...This paper has theoretically designed a series of aggregate polymers on the basis of several para-nitroaniline monomers by hydrogen-bond interactions. At the level of time-dependent hybrid density functional theory, it has optimized their geometrical structures and studied their two-photon absorption (TPA) properties by using analytical response theory. The calculated results exhibit that the aggregation effects not only bring out the conaiderable red shift of the excited energies but also greatly enhance the TPA intensities of the aggregate polymers in comparison with the para-nitroaniline monomer. The aggregate configurations also have an important influence on the TPA abilities of the polymers; the trimer has the largest TPA cross section. The electron transitions between the molecular orbits involving the strong TPA excitations of the trimer are depicted to illuminate the relationship between the intermolecular charge transfer and the TPA property.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
A nonresonant two-photon absorption process can be manipulated by tailoring the ultra-short laser pulse. In this paper, we theoretically demonstrate a highly selective population of two excited states in the nonresona...A nonresonant two-photon absorption process can be manipulated by tailoring the ultra-short laser pulse. In this paper, we theoretically demonstrate a highly selective population of two excited states in the nonresonant two- photon absorption process by rationally designing a spectral phase distribution. Our results show that one excited state is maximally populated while the other state population is widely tunable from zero to the maximum value. We believe that the theoretical results may play an important role in the selective population of a more complex nonlinear process comprising nonresonant two-photon absorption, such as resonance-mediated (2-~l)-three-photon absorption and (2q-1)-resonant multiphoton ionization.展开更多
We theoretically and experimentally study the polarization and phase control of two-photon absorption in an isotropic molecular system. We theoretically show that the two-photon transition probability decreases when t...We theoretically and experimentally study the polarization and phase control of two-photon absorption in an isotropic molecular system. We theoretically show that the two-photon transition probability decreases when the laser polarization changes from linear through elliptical to circular, and the laser polarization does not affect the control efficiency of two-photon transition probability by shaping the spectral phase. These theoretical results are experimentally confirmed in coumarin 480. Furthermore, we propose that the combination of the laser polarization with the spectral phase modulation can further increase the control efficiency of the two-photon absorption.展开更多
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.
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 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.
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 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.
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.
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.
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.
基金Supported by the National Natural Science Foundation of China(No.10074020).
文摘The two-photon absorption(TPA)and TPA-induced frequency upconversion emission properties of the dyes 4-[P-(dicyanoethylamino)crystal]-N-methypyrdinium iodide and the complex of 4-[P-(dicyanoethylamino)crystal]-N-methypyrdinium iodide and Ce(NO3)3 were experimentally studied.It was found that the TPA cross section for the dye sensitized by Ce3+ is two factors larger than that of the dye without being sensitized.A three-level system model of the dye molecules was used to analyze the enhancement of TPA by the sensitizer Ce3+,which indicated that the sensitizer results in the increase of the transition dipole moment from the one-photon allowed excited state(1Bu)to the two-photon allowed excited state(2Ag).
基金Project supported by the Young Scientists Fund of the National Natural Science Foundation of China (Grant No. 10904085)
文摘The influence of rotational isomerism on the two-photon absorption (TPA) of FTC chromophores has been investi- gated using the quadratic response theory with the B3LYP functional. Eight rotamers induced by three rotatable single bonds in the molecule are fully optimized, and it is found that their conformational energies are nearly degenerate. Our calculations demonstrate that rotational isomerism has an important effect on the TPA cross sections. For a certain rotamer, the maximum TPA cross section is enhanced significantly. In addition, in the longer wavelength region, the rotational isomerism could lead to a large shift of the TPA position.
基金supported by the National Natural Science Foundation of China (Grant No. 10974121)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, China (Grant No. J09LA13)
文摘The linear and nonlinear optical properties of two metalloporphyrin complexes formed by the complementary coordination of central zinc or magnesium ions to the ligand 5, 10, 15-tri-(p-tolyl)-20-phenylethynylporphyrin are theo- retically investigated by using the analytic response theory at the density functional theory level. The results indicate that the studied complexes present more symmetric geometry structures than the ligand. The charge-transfer states of the two complexes in the lower energy region are all almost degenerate but those of the ligand are well separated. The ratio of the two-photon absorption cross sections of the ligand, zinc-porphyrin and magnesium-porphyrin com- plexes is 1.0:1.5:1.8, demonstrating that the two-photon absorption capability can be greatly increased when the ligand is coordinated with a metal ion. Moreover, several physical micro-mechanisms including electron transitions and in- tramolecular charge-transfer processes are discussed to explore the differences in optical property between the ligand and two complexes.
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)Natural Science Foundation of Shandong Province of China(Grant No.Z2007A02)
文摘This paper has theoretically designed a series of aggregate polymers on the basis of several para-nitroaniline monomers by hydrogen-bond interactions. At the level of time-dependent hybrid density functional theory, it has optimized their geometrical structures and studied their two-photon absorption (TPA) properties by using analytical response theory. The calculated results exhibit that the aggregation effects not only bring out the conaiderable red shift of the excited energies but also greatly enhance the TPA intensities of the aggregate polymers in comparison with the para-nitroaniline monomer. The aggregate configurations also have an important influence on the TPA abilities of the polymers; the trimer has the largest TPA cross section. The electron transitions between the molecular orbits involving the strong TPA excitations of the trimer are depicted to illuminate the relationship between the intermolecular charge transfer and the TPA property.
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Project partly supported by the Shanghai Leading Academic Discipline Project (Grant No.B408)the Science Foundation of the Ministry of Education of China (Grant No.30800)+1 种基金the National Natural Science Fundation of China (Grant No.11004060)the Shanghai Municipal Science and Technology Commission (Grant Nos.10XD1401800,09142200501,09ZR1409300,09JC1404700,and 10JC1404500)
文摘A nonresonant two-photon absorption process can be manipulated by tailoring the ultra-short laser pulse. In this paper, we theoretically demonstrate a highly selective population of two excited states in the nonresonant two- photon absorption process by rationally designing a spectral phase distribution. Our results show that one excited state is maximally populated while the other state population is widely tunable from zero to the maximum value. We believe that the theoretical results may play an important role in the selective population of a more complex nonlinear process comprising nonresonant two-photon absorption, such as resonance-mediated (2-~l)-three-photon absorption and (2q-1)-resonant multiphoton ionization.
基金Project partly supported by the Science Foundation of the Ministry of Education of China(Grant No.30800)the National Natural Science Foundation of China(Grant Nos.11004060 and 11027403)the Shanghai Municipal Science and Technology Commission,China(Grant Nos.10XD1401800,09142200501,09ZR1409300,09JC1404700,and 10JC1404500)
文摘We theoretically and experimentally study the polarization and phase control of two-photon absorption in an isotropic molecular system. We theoretically show that the two-photon transition probability decreases when the laser polarization changes from linear through elliptical to circular, and the laser polarization does not affect the control efficiency of two-photon transition probability by shaping the spectral phase. These theoretical results are experimentally confirmed in coumarin 480. Furthermore, we propose that the combination of the laser polarization with the spectral phase modulation can further increase the control efficiency of the two-photon absorption.