High-resolution 133Cs 6S-6D, 6S-8S two-photon spectroscopy using an intracavity scheme

This Letter presents an intracavity scheme for diode laser based two-photon spectroscopy. To demonstrate generality, three (133)Cs hyperfine transition groups of different wavelengths are shown. For the 6S-6D transitions, we achieved a 10(2) times better signal-to-noise ratio than in previous work [J. Phys. Soc. Jpn. 74, 2487 (2005)] with 10(-3) times less laser power, revealing some previously vague and unobserved spectra. Possible mutual influences between the two-photon absorber and laser cavity were investigated for the first time to our knowledge, which leads to the application of a reliable hand-sized optical frequency reference. Our approach is applicable for most of the two-photon spectroscopy of alkali atoms.     

Development of two-color laser system for high-resolution polarization spectroscopy measurements of atomic hydrogen

We have developed a high-spectral-resolution laser system for two-photon pump, polarization spectroscopy probe (TPP-PSP) measurements of atomic hydrogen in flames. In the TPP-PSP technique, a 243-nm laser beam excites the two-photon 1S-2S transition, and excited n=2 atoms are then detected by polarization spectroscopy of the n=2 to n=3 transition using 656-nm laser radiation. The single-frequency-mode 243 and 656-nm beams are produced using injection-seeded optical parametric generators coupled with pulsed dye amplifiers. The use of single-mode lasers allows accurate measurement of signal line shapes and intensities even with significant pulse-to-pulse fluctuations in pulse energies. Use of single-mode lasers and introduction of a scheme to select nearly constant laser energies enable repeatable extraction of important spectral features in atomic hydrogen transitions.     

Theoretical analysis on two-photon absorption spectroscopy in a confined four-level atomic system

We investigate theoretically two-photon absorption spectroscopy modified by a control field in a confined Y-type four-level system. Dicke-narrowing effect occurs both in two-photon absorption lines and the dips of transparency against two-photon absorption due to enhanced contribution of slow atoms. We also find that the suppression and the enhancement of two-photon absorption can be modified by changing the strength of the control field and the detuning of three laser fields. This control of two-photon absorption may have some applications in information processing and optical devices.     

Quantum coherent control of two-photon transitions by square phase-modulation

A femtosecond laser pulse can be tailored to control the two-photon transitions using the ultra-fast pulse-shaping technique. This paper theoretically and experimentally demonstrates that two-photon transitions in molecular system with broad absorption line can be effectively controlled by square phase-modulation in frequency domain, and the influence of all parameters characterizing the square phase-modulation on two-photon transitions is systemically investigated and discussed. The obtained results have potential application in nonlinear spectroscopy and molecular physics.     

Absorption and subsequent emission saturation of two-photon excited materials: theory and experiment

The saturation of two-photon absorption and the subsequent photoluminescence of matter under ultrafast laser pulse excitation are studied. For this purpose the experimental results of using two organic conjugated polymers as model substances are discussed theoretically. One model is based on the commonly used hyperbolic approach, whereas the new theory introduced correctly describes the saturation in two-photon spectroscopy and fits the experiment closely. The new model permits microscopic analysis of the absorption saturation process and makes possible an estimate of the two-photon absorption coefficient from the saturation intensity.     

Robust tunable single-frequency operation of a diode laser by a self-pumped phase-conjugate reflector and a high-finesse filter

A novel form of extended-cavity diode laser attains robust tunable single-frequency operation with narrow linewidth. The laser cavity includes a self-pumped photorefractive phase-conjugate reflector for wavelength-adaptive narrowband feedback and a compact high-finesse tunable intracavity ring filter for single-longitudinal-mode selectivity and control. Its performance around 830 nm is verified with a simple Fabry-Perot laser diode and by Doppler-free two-photon spectroscopy in atomic cesium.     

Two-photon spectroscopy in a fast atomic beam

We suggest the use of a fast atomic beam to obtain resonance enhancement in Doppler-free two-photon spectroscopy. The method requires only one laser frequency thus avoiding the complications due to a residual Doppler shift.     

Direct frequency comb measurements of absolute optical frequencies and population transfer dynamics

A phase-stabilized femtosecond laser comb is directly used for high-resolution spectroscopy and absolute optical frequency measurements of one- and two-photon transitions in laser-cooled 87Rb atoms. Absolute atomic transition frequencies, such as the 5S1/2 F=2-->7S1/2 F"=2 two-photon resonance measured at 788,794 768,921 (44) kHz, are determined without a priori knowledge about their values. Detailed dynamics of population transfer driven by a sequence of pulses are uncovered and taken into account for the measurement of the 5P states via resonantly enhanced two-photon transitions.     

CdTe量子点-铜酞菁复合体系荧光共振能量转移的研究

以波长为780 nm、重复频率为76 MHz、脉宽为130 fs的飞秒激光作为激发光源, 采用超快时间分辨光谱技术研究了CdTe量子点-铜酞菁复合体系的荧光共振能量转移. 实验结果表明, 在780 nm的双光子激发条件下, 复合体系中CdTe量子点的荧光寿命随着铜酞菁溶液浓度的增加而减少, 荧光共振能量转移效率增加. 同时也研究了激发功率对荧光共振能量转移效率的影响. 结果表明, 随着激发光功率的增加, 复合体系溶液中CdTe量子点的荧光寿命增加, 荧光共振能量转移效率减小, 其物理机理是因为高激发功率下的热效应和由双光子诱导的高阶激发态的跃迁. 当激发光功率为200 mW时, 双光子荧光共振能量转移效率为43.8%. 研究表明CdTe量子点-铜酞菁复合体系是非常有潜力的第三代光敏剂.     

Nonlinear optical techniques for plasma diagnostics

The application of various nonlinear optical laser spectroscopic techniques to plasma diagnostics are reported. The techniques discussed in this paper are two-photon laser induced fluorescence spectroscopy, double-resonant four-wave mixing, coherent anti-Stokes Raman-scattering (CARS), and a combination of emission spectroscopy and CARS. They are applied to measurements of atomic hydrogen densities, molecular temperature, chemical composition, electric field distributions, and vibrational population distribution. The basic principles are described and important aspects of the methods are discussed in context with application to various kinds of discharges at low and elevated pressures     

Inverse Raman effect: A quantitative spectroscopic technique

The inverse Raman effect extends the general applicability of Raman spectroscopy to unstable species, fluorescing compounds and low pressure gases. A critical examination of the theory leads to optimization of the experimental variables. Interference effects from two-photon absorption processes are discussed. An experimental apparatus based on a giant-pulse ruby laser and a broad-band laser-pumped dye laser is described. Experimental correlations with ordinary Raman scattering cross sections are presented. The effects of inhomogeneous laser beams on the measurements are examined.     

A direct frequency comb for two-photon transition spectroscopy in a cesium vapor

A phase-stabilized femtosecond frequency comb is used to measure high-resolution spectra of two-photon transition 62S1/2-62P1/2,3/2-82S1/2 in a cesium vapor.The broadband laser output from a femtosecond frequency comb is split into counter-propagating parts,shaped in an original way,and focused into a room-temperature cesium vapor.We obtain high-resolution two-photon spectroscopy by scanning the repetition rate of femtosecond frequency comb,and through absolute frequency measurements.     

Sub-Doppler Rydberg spectroscopy by laser-induced two-step recombination at the ESR

For the first time, laser induced radiative electron capture (LIREC) has been combined with sub-Doppler two-photon spectroscopy between Rydberg states of hydrogen-like argon. This revised version was published online in July 2006 with corrections to the Cover Date.     

Power Broadening of Two-Photon Coherent Resonances on Rydberg Atomic Transitions in a Magneto-Optical Trap

We study power broadening of coherent two-photon resonances on Rydberg transitions in lithium-7 atoms in a magneto-optical trap (MOT). We apply the spectroscopic technique based on the reduction of resonance fluorescence in the MOT. One of the main contributions to the spectral broadening is associated with heating of the trapped atoms by laser cooling beams. We suggest a new nondestructive method to measure the atomic temperature in a working MOT using two-photon spectroscopy with variable directions of probe beams.     

A novel femtosecond-laser formation of CdS nanocrystallites in zirconia matrices

A novel method for direct laser writing of two-dimensional cadmium sulfide (CdS) semiconductor nanoparticle microstructures is reported. A two photon or a higher-order multiphoton absorption process, originating from femtosecond laser pulses, was used to decompose CdS precursors dispersed in a zirconia thin film previously dip-coated on a glass substrate. The kinetics of nanoparticle formation as a function of laser power were monitored in situ by photoluminescence spectroscopy. Raman spectroscopy was also performed to characterize the structural changes of the zirconia matrix under irradiation and to verify the formation of CdS nanoparticles. Results show that CdS nanoparticles were formed by two-photon absorption (TPA) with or without the help of an additional carbazole photoinitiator.     

双光子吸收材料二苯乙烯衍生物的合成及光谱性质

设计、合成并用红外光谱、1H NMR、元素分析表征了三种用于双光子吸收材料的二苯乙烯衍生物,4,4′-双(二苯氨基-反式-苯乙烯基)联苯(BPSBP),4,4′-双(二乙氨基-反式-苯乙烯基)联苯(BESBP)和4,4′-双(9-咔唑基-反式-苯乙烯基)联苯(BCSBP)。实验结果表明三者最强的单光子吸收出现在350～400 nm之间,且单光子吸收和荧光光谱中表现出明显的溶剂化显色效应,揭示了分子内对称电荷转移的本质,双光子荧光光谱则揭示了单光子和双光子吸收具有相同的发射机理。利用双光子上转换荧光法测试发现,三种双光子吸收材料在800 nm飞秒激光的激发下具有较大的吸收截面,分别为892,617和483 GM,这表明在双光子领域有潜在的应用价值。     

Two-photon spectroscopy of 15NH3 with isotopic CO2 lasers and double resonance studies with a new coincidence

Eleven transitions of the ν₂ band of ¹⁵NH₃ were measured by the technique of infrared-microwave two-photon spectroscopy using an isotopic CO₂ laser and 20-mW microwave power. By combining these results with those of previous two-photon measurements and with Stark laser spectroscopy results, the spectroscopic constants of this band were calculated. Using the previously unknown coincidence between the R(18) ¹³CO₂ laser line and the _asQ(5,4) infrared transition, velocity tuned multiple-photon Lamb-dip signals were observed. Very intense double resonance signals were observed on the (5,4), (6,4), and (4,4) microwave transitions and the magnitude of these effects was compared to those observed previously in ¹⁴NH₃.     

Measurement of the 1s-2s energy interval in muonium

The 1s-2s interval has been measured in the muonium (&mgr;(+)e(-)) atom by Doppler-free two-photon pulsed laser spectroscopy. The frequency separation of the states was determined to be 2 455 528 941.0(9.8) MHz, in good agreement with quantum electrodynamics. The result may be interpreted as a measurement of the muon-electron charge ratio as -1-1.1(2.1)x10(-9). We expect significantly higher accuracy at future high flux muon sources and from cw laser technology.     

飞秒激光双光子微细加工技术及研究现状

飞秒激光双光子微细加工技术以其特有的高精度三维微加工优势,成为微型机械加工领域新的发展方向之一。介绍了飞秒激光双光子微细加工技术的原理和应用的现状。结合目前已有的微细加工技术,对双光子微细加工技术的特点加以评述。简要报道了利用飞秒激光双光子微细加工技术的一些研究进展。探讨了飞秒激光双光子微细加工技术今后的发展方向及其存在的基本问题。     

Doppler-free two-photon modulation transfer spectroscopy in sodium dimers

We performed an experiment to investigate modulation transfer spectroscopy in two-photon transition of Na₂ using a CW dye laser. Comparing with UV fluorescence detection, the signals obtained by modulation transfer spectroscopy have a very high S/N without the Doppler background problem and its line shape is in agreement with theoretical calculations.Project supported by National Natural Science Fund of ChinaPermanent address: Shanghai University of Technology, Shanghai 200072, People's Republic of China