Isotope-selective excitation of 41Ca isotope in Doppler-free two-photon continuous-wave excitation: a case study

Seven schemes are studied theoretically for Doppler-free two-photon excitation of rare (41)Ca isotope using single-mode continuous-wave lasers. The ionization efficiencies and optical selectivities for all the schemes are calculated for various powers of the excitation and ionization lasers and for various focusing conditions of the two lasers. To maximize the ionization efficiencies and the optical selectivities, wavelength-dependent Stark compensation is used. Certain laser wavelengths of the ionization step termed as magic wavelengths are identified for compensating the Stark shift induced by the excitation laser. The effects of the Stark-shift-induced asymmetry and its reversal by selecting the appropriate magic wavelength for the ionization step for various excitation and ionization laser intensities are investigated. The ionization efficiency and optical selectivity for the best scheme after Stark compensation are found to be 8.4 x 10(-4) and approximately 9 x 10(3), respectively.     

Line shapes in triple-resonance ionization spectroscopy

Line shapes in high-resolution triple-resonance ionization spectroscopy have been calculated and compared with experimental measurements on the 4s2 1S0 --> 4s4p 1P1 --> 4s4d 1D2 --> 4snf 1F3 --> Ca+ system of calcium. Calculations based on the density matrix formalism integrated the fundamental equations over experimental atomic angular and velocity distributions and laser intensity profiles. The measurements reveal and confirm all predicted structures arising from the complex coupling of four atomic states with three laser fields and the Doppler distribution of the atomic ensemble. Effects of different laser beam geometries on the line shapes have been investigated. The agreement between calculated and experimental spectra is generally good over a dynamic range of 10 orders of magnitude. Thus these calculations can accurately predict optical isotopic selectivity in multistep resonance ionization, with a value of S(opt) approximately 10(10) expected for detection of the ultratrace isotope 41Ca.     

A two-color three-photon ionization scheme for the efficient and selective ionization of a chlorinated aromatic hydrocarbon

A two-color three-photon ionization scheme, for the efficient and selective ionization of a chlorinated aromatic hydrocarbon that has an ionization potential higher than the two-photon energy of the laser used for excitation, is described. In this technique, an ultraviolet (UV) laser, i.e., the second harmonic emission of a fundamental (VIS) laser, is used for excitation and a UV and VIS laser for the subsequent two-photon ionization from the electronic excited state. A sample of o-chlorophenol was used as a model compound to demonstrate the advantage of this technique. The signal in supersonic jet/resonance-enhanced multiphoton ionization/mass spectrometry was increased approximately 4 times by the introduction of the VIS beam, when the polarization was adjusted to be parallel to the UV beam. Thus, the two-color three-photon (2UV+VIS) ionization scheme is more sensitive than one-color three-photon (3UV) ionization. The merits of this method over other ionization schemes such as two-color two-photon (UV(1)+UV(2)) ionization are discussed in terms of sensitivity and selectivity in spectrometric analysis.     

Synthesis and upconversion luminescence of uniform beta-NaYF4:Yb3+/Tm3+ hexagonal nanoplates

Yb3+ and Tm3+-codoped hexagonal-phase NaYF4 powders were prepared by a facile hydrothermal method. The results of X-ray powder diffraction (XRD) and scanning electron microscopy (SEM) showed that the as-prepared powders were well crystallized nanoplates with high size-uniformity. Under the excitation from a 980 nm laser diode, upconversion (UC) emissions centered at approximately 291 nm (1I6 --> 3H6), approximately 346 nm (1I6 --> 3F4), approximately 361 nm (1D2 --> 3H6), approximately 451 nm (1D2 --> 3F4), approximately 474 nm (1G4 --> 3H6), approximately 644 nm (1G4 --> 3F4), and approximately 799 nm (3H4 --> 3H6) were observed in the sample. Furthermore, the intensity dependence of UC emissions on excitation power was measured. The results indicated that populating the 1I6, 1D2, 1G4, and 3H4 states were five-photon, four-photon, three-photon, and two-photon UC processes, respectively.     

Concept for polychromatic laser guide stars: one-photon excitation of the 4P3/2 level of a sodium atom

One challenge for polychromatic laser guide stars is to create a sufficiently intense source in the UV. The flux required for the measurement of differential tip-tilt is the main issue that we address. We describe a model that has been validated using on-sky data. We present a method that excites the 4P3/2 sodium level using a one-photon excitation at 330 nm. It is more efficient than the two-photon excitation previously suggested since its power slope flux is 3 x 10(4) photons/s/m2/W instead of 1.3 x 10(3) photons/s/m2/W. This method is very promising both in terms of flux and system simplicity.     

Minimizing urine autofluorescence under multi-photon excitation conditions

We report on the effects of excitation wavelength, laser power, and phase resolution on the multi-photon-excited autofluorescence (background) from human urine. When compared to the autofluorescence under one-photon excitation conditions (lambda(ex) = 260-480 nm), the urine multi-photon-excited autofluorescence (lambda(ex) = 725-950 nm) can be less complicated. However, at higher laser powers, the multi-photon-excited autofluorescence spectra that are produced by excitation above ~775 nm are more complex in comparison to the corresponding one-photon-excited autofluorescence. The origin of these more complex spectra arises from simultaneous two- and three-photon-driven excitation of intrinsic luminescent species within the urine. At lower laser powers, three-photon-driven processes are minimized and the autofluorescence spectrum is simplified. Phase resolution is used to further minimize the urine autofluorescence, but it cannot fully eliminate autofluorescence even when excitation is performed under multi-photon conditions at 950 nm. For detecting 250 nM Rhodamine 6G (a mock analyte) dissolved in urine, we find that the two-photon excitation is superior in comparison to one-photon excitation by 5- to 70-fold, depending on the excitation wavelength. Phase resolution combined with two-photon excitation leads to an additional 5- to 7-fold improvement in signal-to-background ratios in comparison to steady-state two-photon excitation.     

Return flux budget of polychromatic laser guide stars

The polychromatic laser guide star (PLGS) is one of the solutions proposed to extend the sky coverage by large telescopes to 100% by enabling a complete knowledge of all perturbation orders of the wavefront. The knowledge of the tip-tilt is deduced from the monitoring of the chromatic components of the PLGS, from 330 nm to the visible or near infrared. Here we study the original scheme to create the PLGS by resonant excitation of the mesospheric sodium by two pulsed lasers (tens of kilohertz repetition rate, tens of watts average power, tens of nanoseconds pulse duration), at 589 and 569 nm, respectively. The efficiency of this process is investigated numerically by means of both Bloch equation and rate equation models. The influence of numerous laser parameters is studied. In the best case, having optimized all laser parameters, the return flux at 330 nm should not exceed 7x10(4) photons/s/m2 for 2x18 W laser average power at the mesosphere. This maximum is obtained for a modeless laser whose spot diameter corresponds to 4 times the diffraction limit. For a diffraction-limited spot, the return flux falls down to 4x10(4)photons/s/m2.     

Frequency-stabilized 1520-nm diode laser with rubidium 5S(1/2) --> 7S(1/2) two-photon absorption

A 760-nm light source of >10 mW is obtained from a frequency-doubled external-cavity diode laser by use of using an erbium-doped fiber amplifier and a periodically poled lithium niobate waveguide. The 5S(1/2) --> 7S(1/2) two-photon transitions of rubidium are observed with such a light source. This laser frequency is locked to the Rb two-photon transitions with an instability of 10 kHz (1 s). Our experimental scheme provides a compact, high-performance frequency, standard in the S band (1480-1530 nm) for fiber-optic communication and sensing applications.     

Efficient pumping scheme for neodymium-doped materials by direct excitation of the upper lasing level

An efficient pumping scheme that involves direct excitation of the upper lasing level of the Nd(3+) ion is demonstrated experimentally. The results obtained for direct upper laser level pumping of Nd:YAG R2 (869 nm) and Nd:YVO(4) (880 nm) were compared with traditional ~808-nm pump band excitation. A tunable cw Ti:sapphire laser was used as the pump source. In Nd:YAG, the oscillator slope efficiency increased by 10% and the threshold decreased by 11%. In Nd:YVO(4), the slope efficiency increased by 5% and the threshold decreased by 11%. These results agree with theory. The increase in optical efficiency indicates that laser material thermal loading can be substantially reduced.     

Precision stabilization of the optical frequency in a large ring laser gyroscope

Pressure-induced fractional changes of 10(-7) in the geometry of a large He-Ne ring laser gyroscope induce backscatter phase changes and thus a fractional pulling of the Sagnac frequency of ~5 x 10(-3). To counter this, the optical frequency was stabilized against an iodine-stabilized laser with a high-finesse Fabry-Perot interferometer and piezoelectric control of the ring perimeter. This scheme, although limited in principle by residual geometric asymmetry and in practice by low beam powers (10 pW), stabilized the perimeter to 2.4 nm (6 x 10(-10) or 300 kHz for the optical frequency) and the Sagnac frequency to 100 parts per million over several days.     

High-density optical data storage with one-photon and two-photon near-field fluorescence microscopy

A spatially localized photochemical reaction induced by near-field femtosecond laser pulses is demonstrated on a nanometer scale and used for high-density optical data storage. Recorded domains down to 120 and 70 nm are obtained with one-photon and two-photon excitation, respectively. It is shown that the local-field confinement that is due to the quadratic dependence of two-photon excitation on light intensity has the potential to increase the near-field optical storage density.     

Investigation of nonlinear dynamics in CdS by time-resolved nondegenerate pump–probe system with phase object

The time-resolved nondegenerate pump–probe system with phase object is employed for investigation of nonlinear absorption and refraction dynamics in CdS. The 532?nm laser beam with 21?ps duration is used as the excitation and the laser beams of 600 and 680?nm with 10?ps duration from optical parametric generation are used for probing. The experimental results at both probe wavelengths show free-carrier absorption and large free-carrier refraction along with two-photon absorption and bound electronic optical Kerr effect. By numerically fitting the experimental data based on the nondegenerate pump–probe theory, the nondegenerate two-photon absorption coefficient, the nondegenerate Kerr coefficient, the free-carrier decay time, the free-carrier absorptive cross-section and free-carrier refractive coefficient at different wavelengths are all determined.     

Two-photon Absorption and Nonlinear Optical Properties of A New Organic Dye DEASPI

A new organic dye trans-4- [p-(N,N-diethylamino) styryl]-N-methylpyridinium iodide (abbreviated' as DEASPI thereafter) with large two-photon absorption (TPA) cross section and excellent upconverted lasing properties was synthesized. The melting point and decompound point were measured to be 230 degreesC and 264.7 degreesC respectively. The molecular TPA cross section was measured to be sigma (2)=6.9x10(-48) cm(4).s/photon at 1064 nm by using an open aperture Z-scan system. The linear and nonlinear optical properties of this dye were systematically studied. The highest net upconversion efficiency from the absorbed pump energy to the output upconverted lasing energy is as high as 18.6% at the pump energy of 2.17 mJ from a mode-locked Nd:YAG ps laser. The nonlinear transmittance at the wavelengths from 720 to 1100 nm was measured. The dye solution also shows a clear optical power limiting effect.     

Three- and four-photon absorption of a multiphoton absorbing fluorescent probe

High-order multiphoton excitation processes are becoming a reality for fluorescence imaging and phototherapy treatment because they afford minimization of scattered light losses and a reduction of unwanted linear absorption in the living organism transparency window, making them less susceptible to photodamage, while improving the irradiation penetration depth and spatial resolution. We report the four-photon-excited fluorescence emission of (7-benzothiazol-2-yl-9,-didecylfluoren-2-yl)diphenylamine in hexane and its four-photon absorption cross section sigma4' = 8.1 x 10(-109) cm8 s3 photon(-3) for the transition S0 --> S1 when excited at 1600 nm with a tunable optical parametric generator (OPG) pumped by picosecond laser pulses. When pumped at 1200 nm, three-photon absorption was observed, corresponding to the same transition.     

Trace detection of krypton using laser-induced fluorescence

Highly sensitive detection of neutral Kr atoms was accomplished by the use of laser-induced fluorescence. In one experiment, Kr at 40 parts per 10(12) in He was detected at a signal-to-noise ratio of 500 by time-resolved fluorescence measurements. The Kr metastable 1s(5) level was populated by cascade after two-photon excitation to the 2p(6) level by the frequency-tripled output of a pulsed single-longitudinalmode dye laser. After a delay, when scattered laser light and cascade resonance fluorescence became negligible, trace quantities of Kr were detected by the use of a pulsed-laser pumping scheme. In a related experiment, (78)Kr/(86)Kr isotope ratios ranging from 1 to 0.1 were measured with a resonant isotopic depletion technique first proposed by Makarov [Sov. J. Quantum Electron. 13, 722 (1983)]. The (86)Kr metastable population was selectively depleted by optical pumping to a higher-lying state that relaxed to the ground state by means of radiative cascade. After the (78)Kr/(86)Kr ratio of metastables had been enriched by a factor of 10, the (78)Kr population was probed by pulsed excitation. Premixed (78)Kr/(86)Kr ratios were measured to within an accuracy of 10%, even for unresolved, Doppler-broadened transitions.     

Nanoshells for in vivo imaging using two-photon excitation microscopy

Gold nanoshells have been intensively investigated and applied to various biomedical fields because of their flexible optical tunability and biological compatibility. They hold great potential to serve as luminescent contrast agents excitable with near-infrared (NIR) lasers. In this paper, we describe the development of nanoshells with a peak of plasmon resonance at 800 nm and their subsequent use for in vivo blood vessel imaging using two-photon excitation microscopy at an excitation wavelength of 750 nm. We were able to image single nanoshell particles in blood vessels and generate optical contrast for blood vessel structure using luminescent signals. These results confirm the feasibility of engineering nanoshells with controlled optical properties for single-particle-based in vivo imaging.     

Microfluorometric detection of catecholamines with multiphoton-excited fluorescence

We demonstrate sensitive spatially resolved detection of physiological chromophores that emit in the ultraviolet (<330 nm). An atypical laser source (a visible wavelength femtosecond optical parametric oscillator), and an unconventional collection geometry (a lensless detector that detects the forward-emitted fluorescence) enable this detection. We report the excitation spectra of the catecholamines dopamine and norepinephrine, together with near-UV emitters serotonin and tryptophan, in the range of 550-595 nm. We estimate the molecular two-photon action cross section of dopamine, norepinephrine, and serotonin to be 1.2 mGM (1 GM, or Goppert Mayor, is equal to 10(-58) m4 s(-1) photon(-1)), 2 mGM, and 43 mGM, respectively, at 560 nm. The sensitivity achieved by this method holds promise for the microscopic imaging of vesicular catecholamines in live cells.     

Thermal lens micro optical systems

This paper describes two types of miniaturized thermal lens optical systems that use optical fibers, SELFOC microlenses and light sources. The first system consists of a compact diode pumped solid-state laser (532 nm) as an excitation light source, a laser diode (635 nm) as a probe light source, an acoustoptic modulator as an excitation light modulator, fiber-based and conventional optics, and a detection system that combines a pinhole, an interference filter, and a photodiode. The second system consists of two laser diodes as the excitation (658 nm) and probe (780 nm) light sources, fiber-based optics, and the same detection system as the first one. The performance of the two systems was evaluated by the limit of detection (LOD) using standard solutions of sunset yellow (SY) and nickel(II) phthalocyaninetetrasulfonic acid tetrasodium salt (NiP). The LODs of the first system for SY and second system for NiP were calculated to be 3.7 x 10(-8) (1.7 x 10(-6) AU) and 7.7 x 10(-9) M (3.4 x10(-6) AU), respectively. These results were consistent with the expected values obtained from photothermal parameters.     

A REMPI method for the ultrasensitive detection of NO and NO2 using atmospheric pressure laser ionization mass spectrometry

We report on the development of a quasi-simultaneous highly selective method for NO and NO2 detection at the ultratrace level. Atmospheric pressure laser ionization (APLI), recently introduced by our group, is used to detect both compounds at low parts per trillion by volume (pptv) mixing ratios. APLI is based on resonance-enhanced multiphoton ionization mass spectrometry. Two-color pump-probe experiments employing a single excimer pumped dye laser combination allow for the ultrasensitive measurement of NO and NO2 within a narrow range of maximum pumping efficiency of the laser dye Coumarin 120. NO is detected via excitation of the long-lived A 2sigma+ (nu' = 1) level at 215.36 nm and subsequently ionized with 308-nm radiation provided by the excimer pump laser. NO2 is ionized after double resonant excitation of the A2B1 and 3psigma manifolds in a (1 + 1' + 1(')) process using 431.65 + 308 nm. The selectivity of the NO measurement exceeds 2,000 with respect to NO2 and N2O5. For NO2, a selectivity of >3,000 with respect to N2O5 and organic nitrates is observed. The current APLI detection limit of NO and NO2 is 0.5 and 5 pptv, respectively, with a 20-s integration time.     

Fixed-wavelength operation of a copper-laser-pumped dye laser injection seeded by low-power He-Ne lasers

The design and operating characteristics of a dye laser pumped by a 3-W copper-vapor laser (CVL) and injection seeded by low-power (1-5 mW) He-Ne lasers at 633 nm are reported. An extremely simple optical arrangement is used wherein the output mirror of the He-Ne laser and a third mirror form the dye laser cavity. Laser efficiency in fixed-wavelength operation has been investigated for variable CVL pump power, He-Ne injection power and polarization, and cavity output coupling for a standard Rhodamine 590/Rhodamine 640 dye solution. Over 90% of free-running (unseeded) laser power is obtained in fixed-wavelength (seeded) operation at low CVL pump powers (≤1 W), dropping to approximately 60% at 3-W pump power. Maximum CVL pump to dye laser optical conversion efficiency in narrow-band, fixed-wavelength operation at 633 nm was 12%.