Highly selective population of two excited states in nonresonant two-photon absorption

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+1)-three-photon absorption and (2+1)-resonant multiphoton ionization.     

Multichannel selective femtosecond coherent control based on symmetry properties

We present and implement a new scheme for extended multichannel selective femtosecond coherent control based on symmetry properties of the excitation channels. Here, an atomic nonresonant two-photon absorption channel is coherently incorporated in a resonance-mediated (2+1) three-photon absorption channel. By proper pulse shaping, utilizing the invariance of the two-photon absorption to specific phase transformations of the pulse, the three-photon absorption is tuned independently over an order-of-magnitude yield range for any possible two-photon absorption yield. Noticeable is a set of "two-photon dark pulses" inducing widely tunable three-photon absorption.     

Ultrafast dynamics of all-trans--carotene explored by resonant and nonresonant photoexcitations

Excitation energy dependence of transmittance change has been investigated in -carotene. The signal induced by nonresonant excitation is ascribed to the ac Stark effect and the two-photon absorption of the excitation and probe pulses in three-level systems. The ultrafast response following resonant excitation is assigned to the two-photon absorption and the transient absorption of the photogenerated S(2) state with a lifetime of 150 fs. The long-debated S(2)-S(1) relaxation in beta-carotene can be explained by a two-state model (S(2), S(1)) without involving any intermediate states.     

反-4,4''-双(N,N-二丁胺基)二苯乙烯分子双光子吸收性质研究

对于实验室合成的反-4,4'-双(N,N-二丁胺基)二苯乙烯分子,实验测量了该分子的单光子和双光子荧光谱,然后从理论上研究了其单光子和双光子吸收特性.研究结果表明,在低能量范围内,分子的单光子吸收主要发生在分子的第一激发态,而分子的双光子吸收主要发生在分子的第二和第四激发态上.该分子在相应系列衍生物中具有最大的双光子吸收截面.分子的相关能对分子的激发态能量影响较大.我们给出了分子基态与电荷转移态的电荷转移过程,并从理论上定性解释了双光子聚合反应的聚合机理.     

Upconversion fluorescence spectroscopy of Er~(3+)-doped lead oxyfluorosilicate glass

Upconversion fluorescence emission of Er3+-doped oxyfluorosilicate glass excited at 975 nm is experimentally investigated. The results reveal that the intense green and red emission, and weak blue emission centered at 525, 543, 655, and 410 nm, respectively. A two-photon upconversion process is assigned to the green and red emission while a three-photon process is responsible for blue upconversion. The possible upconversion mechanisms are discussed based on excited state absorption and energy transfer between excited Er3+ ions. The intense upconversion fluorescence of Er3+-doped lead oxyfluorosilicate glass may be a potentially useful material for developing upconversion optical devices.     

二苯乙烯衍生物分子双光子吸收截面：官能团对称性的影响

选取了具有不同对称性的二苯乙烯系列衍生物分子，在HF水平上，利用响应函数方法，研究了该系列分子的单光子和双光子特性. 研究结果表明，该系列分子具有较强的双光子特性. 在可见光范围内，反对称分子的最大双光子吸收态是第一激发态，而对称分子的最大双光子吸收出现在第四激发态. 相对于对称分子而言，反对称分子具有更大的双光子吸收截面. 因此，分子的对称性是否比不对称性更有利于增大分子的双光子吸收截面，还与分子的π中心部分的特性有关. 还给出了电荷转移态的电荷迁移过程. 关键词： 双光子吸收 响应函数方法 非线性光学     

Application of optimal control theory to ultrafast nonresonant multiphoton transitions in polyatomic molecules

Optimal control theory (OCT) including nonresonant multiphoton transitions (NMT) in the femtosecond time regime has been implemented. The NMT process is modelled using an effective time-dependent Schrödinger equation, which considers a reduced space of the two levels which are involved in the transition, coupled to a density of high-lying off-resonant states. The specification of OCT to two-photon transitions is done within the rotating wave approximation. As an application, the transfer and displacement of a wavepacket in the organometallic system CpMn(CO)₃, from the ground to an electronically excited state using two nonresonant photons, is simulated.     

Experimental demonstration of selective coherent population transfer via a continuum

We report the first experimental demonstration of coherent population transfer, induced by stimulated Raman adiabatic passage, via continuum states. Population is transferred from the metastable state 2s(1)S(0) to the excited state 4s(1)S(0) in helium atoms in a two-photon process mediated by coherent interaction with the ionization continuum. While incoherent techniques usually do not permit any population transfer in such a process, we show that stimulated Raman adiabatic passage allows significant population transfer to take place also via ultrafast decay channels.     

Nonlinear electronic line shape determination in Yb3+-doped phosphate glass

Nonlinear refraction spectroscopy has been performed in Yb3+-doped phosphate glass to determinate the line shape of real and imaginary parts of n2 (n2' and n2"). The n2' spectrum presented an asymmetric feature due to the interference of resonant and nonresonant contributions, where the nonresonant term arises from the polarizability difference between excited and ground states (delta alpha). The measurements were performed in the transient regime to determine population dynamics and the pump saturation intensity at 975 nm (peak of the absorption spectrum). Because of the small quantum defect of Yb3+, we estimated that the magnitude of the thermal lens effect is approximately 20 times smaller than the population lens effect, caused by n2.     

Ultrafast S1 and ICT state dynamics of a marine carotenoid probed by femtosecond one- and two-photon pump-probe spectroscopy

Ultrafast relaxation kinetics of fucoxanthin in polar and non-polar solvents have been studied by femtosecond pump-probe spectroscopy. Transient absorption associated with S₁ or intramolecular charge transfer (ICT) excited state has been observed following either one-photon excitation to the optically allowed S₂ state or two-photon excitation to the symmetry-forbidden S₁ state. The results suggest that the ICT state formed after excitation of fucoxanthin in a polar solvent is a distinct excited state from S₁.     

Theoretical investigation on nonlinear absorption of multilevel organic molecular system in ns, ps and fs regime

The nonlinear absorption properties of organic materials in nanosecond (ns), picoseond (ps) and femtosecond (fs) regime were theoretically investigated by rate equations based on multilevel organic molecular system, respectively. The simulation results show that the RSA is mainly due to the absorption contribution of the triplet first excited state in the ns regime and that of the singlet first excited state in the ps regime, both of which are a third-order nonlinear phenomena. The RSA in fs regime is mainly due to the excited state absorption (ESA) induced by two-photon absorption (TPA), which is a fifth-order nonlinear phenomenon.     

The Dynamic Behaviour Analysis of Up－Conversion Luminescence in ErP_5O_（14） Glass

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Nonresonant two-photon generation of excitonic matter in a CuCl pellet

A pressed CuCl pellet is optically excited at 2 K using an excitation energy in the range from 1892 to 2843 meV, which is far below the bandgap. The steady-state population dynamics unambiguously indicates an unusual two-photon generation of ground-state excitons. At high-excitation levels, the observed spectra exhibit rich spectral features arising from electron-hole plasma and electron-hole droplets formation. This nonresonant two-photon excitation is presumably assisted by impurity bands due to grain boundaries and surfaces in this random semiconductor.     

Nonlinear atomic response to intense ultrashort x rays

The nonlinear absorption mechanisms of neon atoms to intense, femtosecond kilovolt x rays are investigated. The production of Ne(9+) is observed at x-ray frequencies below the Ne(8+), 1s(2) absorption edge and demonstrates a clear quadratic dependence on fluence. Theoretical analysis shows that the production is a combination of the two-photon ionization of Ne(8+) ground state and a high-order sequential process involving single-photon production and ionization of transient excited states on a time scale faster than the Auger decay. We find that the nonlinear direct two-photon ionization cross section is orders of magnitude higher than expected from previous calculations.     

Two- and three-photon excitation of Gd in CaAl12O19

We have employed two-photon excitation to study the higher energy levels of Gd³⁺ ions in CaAl₁₂O₁₉ and we compare the results with those obtained using conventional UV excitation techniques. Under two-photon excitation, the luminescence intensity exhibits an unusual temporal behavior, a very long build-up followed by a decrease by orders of magnitude, ascribed to a recombination-assisted luminescence excitation mechanism assuming photo-ionization of Gd³⁺ ions and trapping of free electrons on deep traps.

We also find that the two-photon excitation spectra contain an additional broadening contribution which can be attributed to homogeneous broadening of excitation levels caused by excited state absorption into the conduction band. We believe that this may be a general phenomenon whenever participating photons produce ionization of impurity ions from metastable excited states. The phenomenon can manifest itself also in two-photon ionization spectral hole burning and in up-conversion processes (in the latter case, the homogeneous broadening can be caused by an intra-ion excited-state absorption).     

Fluorescence Studies of Melanin by Stepwise Two-Photon Femtosecond Laser Excitation

Fluorescence of synthetic melanin in the solvents H₂O, KOH, ethylene glycol monomethyl ether, and dimethyl sulfoxide has been excited by two-photon absorption at 800 nm, using 120-fs pulses with photon flux densities of 10²⁷ cm^–2.S^–1. Compared to the one-photon (400-nm)-induced fluorescence of melanin, the overall spectral shape is red-shifted and shows a strong environment sensitivity. The decay of the two-photon-induced fluorescence (TPF) of melanin is three-exponential, with a shortest main component of about 200 ps. The results of the TPF studies in line with the unique light absorption property of melanin of a monotonously decreasing absorption spectrum between the near UV-region and the near infrared region indicate that the TPF is realized via stepwise absorption of two 800-nm photons. In comparison to the simultaneous absorption of two photons, the stepwise process needs lower photon flux densities to get a sufficient population of the fluorescent level. This stepwise process offers new possibilities of selective excitation of melanin in skin tissue in a spectral region where there is no overlap with any absorption of another fluorescent tissue component. The first results with different samples of excised human skin tissue (healthy, nevus cell nevi, malignant melanoma) suggest that fluorescence excited in this way yields information on malignant transformation.     

Theory of energy- and time-resolved two-photon photoemission from metal surfaces – influence of pulse duration and excitation condition

The theory of energy- and time-resolved two-photon photoemission (2PPE) spectra of metal surfaces is presented using density matrix formulation for a three-level system consisting of an initial occupied, intermediate unoccupied and final photoelectron states. A perturbation expansion method is employed to calculate the energy-resolved 2PPE spectrum for continuous light beams. We have obtained analytical expressions of the 2PPE spectrum corresponding to a step-by-step one-photon process through the intermediate state and a direct two-photon-ionization process via virtual transition. It is demonstrated that the intermediate state can also be populated via the nonresonant virtual process. This indicates an absolute importance of “pure dephasing” associated with the transition between the initial and intermediate states. Evolution of the 2PPE spectrum as a function of the pump photon energy is calculated to demonstrate the conditions under which the intrinsic linewidth (total dephasing time) can be deduced from the lineshape analysis. It is also found that the intensity ratio of the two peaks due to the initial and the intermediate states in 2PPE spectrum can be used to estimate the pure dephasing time. Transient behavior of the excited-state population following pulse excitation is calculated with a focus on how the ultrafast relaxation times of the excited states such as image-potential states of metal surfaces are deduced from the transient 2PPE response observed with a pulse laser with much longer duration. The time-resolved 2PPE spectra are calculated for varying detuning from the resonant excitation from the initial state to the intermediate state. Transient responses of the 2PPE signal due to direct ionization and step-by-step processes are also calculated to demonstrate that the nonresonant former process has an influence on the analysis of the cross-correlation trace of the intermediate state, by which the population relaxation time is estimated. Attempts are also made to apply the present theory to a recent time-resolved 2PPE study of the relaxation dynamics of the image-potential states as well as hot electrons in Cu(100) and Ag(100) surfaces. Received: 23 May 2000 / Accepted: 2 September 2000 / Published online: 12 October 2000     

Optical bistability in four-level nonradiative dyes

We describe conditions under which optical bistability may be observed in a Fabry-Perot filled with saturably absorbing dye. Bistability occurs due to an intensity-dependent phase shift arising from nonresonant dispersion caused by an excited metastable state which is excited to the process of saturable absorption. Preliminary experiments confirm the theoretical predictions using BDN.     

Nonlinear absorption of CS2 at the wavelength of 400 nm with femtosecond pulses

Nonlinear absorption of carbon disulfide (CS₂) was investigated by Z-scan technique and time-resolved pump-probe technique with femtosecond pulses at 400 nm wavelength. By the two techniques, we confirmed that the nonlinear absorption of CS₂ arise from a combination of two-photon absorption (TPA) and the excited state absorption induced by TPA under the incident laser pulses with 400 nm wavelength. The coefficient of TPA, the absorption cross-section of low excited state and lifetime of low excited state were obtained by theoretical fitting the experimental results. The results indicated that the CS₂ has good optical limiting capability at 400 nm wavelength.     

TmP5O14晶体的上转换发光的研究

报道室温下TmP₅O₁₄晶体在脉冲DCM染料激光激发下产生的紫外和深紫色上转换发光现象.测量发现在300—500nm波长范围内主要有两组上转换荧光,一是较强的¹D₂→³H₆,³F₄的360和450nm的双光子荧光,另一是¹I6→³F₄的347nm的三光于荧光,发现了由 关键词：