Femtosecond near-field scanning optical microscopy

We have developed an instrument for optically measuring carrier dynamics in thin-film materials with ≈150 nm lateral resolution, ≈250 fs temporal resolution and high sensitivity. This is accomplished by combining an ultrafast pump–probe laser spectroscopic technique with a near-field scanning optical microscope. A diffraction-limited pump and near-field probe configuration is used, with a novel detection system that allows for either two-colour or degenerate pump and probe photon energies, permitting greater measurement flexibility than that reported in earlier published work. The capabilities of this instrument are proven through near-field degenerate pump–probe studies of carrier dynamics in GaAs/AlGaAs single quantum well samples locally patterned by focused ion beam (FIB) implantation. We find that lateral carrier diffusion across the nanometre-scale FIB pattern plays a significant role in the decay of the excited carriers within ≈1 μm of the implanted stripes, an effect which could not have been resolved with a far-field system.     

Femtosecond near-field scanning optical microscopy

We have developed an instrument for optically measuring carrier dynamics in thin-film materials with approximately 150 nm lateral resolution, approximately 250 fs temporal resolution and high sensitivity. This is accomplished by combining an ultrafast pump-probe laser spectroscopic technique with a near-field scanning optical microscope. A diffraction-limited pump and near-field probe configuration is used, with a novel detection system that allows for either two-colour or degenerate pump and probe photon energies, permitting greater measurement flexibility than that reported in earlier published work. The capabilities of this instrument are proven through near-field degenerate pump-probe studies of carrier dynamics in GaAs/AIGaAs single quantum well samples locally patterned by focused ion beam (FIB) implantation. We find that lateral carrier diffusion across the nanometre-scale FIB pattern plays a significant role in the decay of the excited carriers within approximately 1 microm of the implanted stripes, an effect which could not have been resolved with a far-field system.     

Development of high-repetition-rate laser pump/x-ray probe methodologies for synchrotron facilities

We describe our implementation of a high repetition rate (54 kHz-6.5 MHz), high power (>10 W), laser system at the 7ID beamline at the Advanced Photon Source for laser pump/x-ray probe studies of optically driven molecular processes. Laser pulses at 1.06 μm wavelength and variable duration (10 or 130 ps) are synchronized to the storage ring rf signal to a precision of ~250 fs rms. Frequency doubling and tripling of the laser radiation using nonlinear optical techniques have been applied to generate 532 and 355 nm light. We demonstrate that by combining a microfocused x-ray probe with focused optical laser radiation the requisite fluence (with <10 μJ/pulse) for efficient optical excitation can be readily achieved with a compact and commercial laser system at megahertz repetition rates. We present results showing the time-evolution of near-edge x-ray spectra of a well-studied, laser-excited metalloporphyrin, Ni(II)-tetramesitylporphyrin. The use of high repetition rate, short pulse lasers as pump sources will dramatically enhance the duty cycle and efficiency in data acquisition and hence capabilities for laser-pump/x-ray probe studies of ultrafast structural dynamics at synchrotron sources.     

Ultrasensitive ultraviolet-visible 20 fs absorption spectroscopy of low vapor pressure molecules in the gas phase

We describe an ultrasensitive pump-probe spectrometer for transient absorption measurements in the gas phase and in solution. The tunable UV pump and the visible (450-740 nm) probe pulses are generated by two independently tunable noncollinear optical parametric amplifiers, providing a temporal resolution of 20 fs. A homebuilt low gain photodetector is used to accommodate strong probe pulses with a shot noise significantly lower than the overall measurement noise. A matched digitizing scheme for single shot analysis of the light pulses at kilohertz repetition rates that minimizes the electronic noise contributions to the transient absorption signal is developed. The data processing scheme is optimized to yield best suppression of the laser excess noise and thereby transient absorbance changes down to 1.1 x 10(-6) can be resolved. A collinear focusing geometry optimized for a 50 mm interaction length combined with a heatable gas cell allows us to perform measurements on substances with low vapor pressures, e.g., on medium sized molecules which are crystalline at room temperature. As an application example highlighting the capability of this instrument, we present the direct time-domain observation of the ultrafast excited state intramolecular proton transfer of 2-(2(')-hydroxyphenyl)benzothiazole in the gas phase. We are able to compare the resulting dynamics in the gas phase and in solution with a temporal precision of better than 5 fs.     

Note: Optical trigger device with sub-picosecond timing jitter and stability

We are presenting the design, construction, and overall performance of the optical trigger device. This device generates an electrical signal synchronously to the detected ultra-short optical pulse. The device was designed for application in satellite laser ranging and laser time transfer experiments, time correlated photon counting and similar experiments, where picosecond timing resolution and detection delay stability are required. It consists of the ultrafast optical detector, signal discriminator, output pulse forming circuit, and output driver circuits. It was constructed as a single compact device to optimize their matching and maintain stability. The detector consists of an avalanche photodiode--both silicon and germanium types may be used to cover the wavelength range of 350-1550 nm. The analogue signal of this photodiode is sensed by the ultrafast comparator with 8 GHz bandwidth. The ps clock distribution circuit is used to generate the fast rise/fall time output pulses of pre-set length. The trigger device timing performance is excellent: the random component of the timing jitter is typically 880 fs, the temperature dependence of the detection delay was measured to be 370 fs/K. The systematic error contribution depends on the laser used and its stability. The sub-ps values have been obtained for various laser sources.     

Ultrafast time-domain spectroscopy based on high-speed asynchronous optical sampling

High-speed asynchronous optical sampling (ASOPS) is a novel technique for ultrafast time-domain spectroscopy (TDS). It employs two mode-locked femtosecond oscillators operating at a fixed repetition frequency difference as sources of pump and probe pulses. We present a system where the 1 GHz pulse repetition frequencies of two Ti:sapphire oscillators are linked at an offset of Deltaf(R)=10 kHz. As a result, their relative time delay is repetitively ramped from zero to 1 ns within a scan time of 100 micros. Mechanical delay scanners common to conventional TDS systems are eliminated, thus systematic errors due to beam pointing instabilities and spot size variations are avoided when long time delays are scanned. Owing to the multikilohertz scan-rate, high-speed ASOPS permits data acquisition speeds impossible with conventional schemes. Within only 1 s of data acquisition time, a signal resolution of 6 x 10(-7) is achieved for optical pump-probe spectroscopy over a time-delay window of 1 ns. When applied to terahertz TDS, the same acquisition time yields high-resolution terahertz spectra with 37 dB signal-to-noise ratio under nitrogen purging of the spectrometer. Spectra with 57 dB are obtained within 2 min. A new approach to perform the offset lock between the two femtosecond oscillators in a master-slave configuration using a frequency shifter at the third harmonic of the pulse repetition frequency is employed. This approach permits an unprecedented time-delay resolution of better than 160 fs. High-speed ASOPS provides the functionality of an all-optical oscilloscope with a bandwidth in excess of 3000 GHz and with 1 GHz frequency resolution.     

Generation, transport, and detection of linear accelerator based femtosecond-terahertz pulses

The generation and detection of intense terahertz (THz) radiation has drawn a great attention recently. The dramatically enhanced energy and peak electric field of the coherent THz radiation can be generated by coherent superposition of radiated fields emitted by ultrafast electron bunches. The femtosecond (fs)-THz beamline construction at the Pohang Accelerator Laboratory (PAL) was completed in the end of 2009. The fs-THz beamline at PAL can supply ultrafast and intense fs-THz radiation from a 75 MeV linear accelerator. The radiation is expected to have frequency up to 3 THz (～100 cm(-1)) and the pulse width of <200 fs with pulse energy up to 10 μJ. This intense THz source has great potential for applications in nonlinear optical phenomena and fields such as material science, biomedical science, chemistry, and physics, etc.     

Inducing superconductivity at a nanoscale: photodoping with a near-field scanning optical microscope

The local modification of an insulating GdBa2Cu3O6.5 thin film, made superconducting by illumination with a near-field scanning optical microscope (NSOM), is reported. A 100-nm aperture NSOM probe acts as a sub-wavelength light source of wavelength lambda(exc) = 480-650 nm, locally generating photocarriers in an otherwise insulating GdBa2-Cu3O6.5 thin film. Of the photogenerated electron-hole pairs, electrons are trapped in the crystallographic lattice, defining an electrostatic confining potential to enable the holes to move. Reflectance measurements at lambda = 1.55 microm at room temperature show that photocarriers can be induced and constrained to move on a approximately 200 nm scale for all investigated lambda(exc). Photogenerated wires present a superconducting critical temperature Tc= 12 K with a critical current density Jc = 10(4) A cm(-2). Exploiting the flexibility provided by photodoping through a NSOM probe, a junction was written by photodoping a wire with a narrow (approximately 50 nm) under-illuminated gap. The strong magnetic field modulation of the critical current provides a clear signature of the existence of a Josephson effect in the junction.     

Synchrotron-based ultrafast x-ray diffraction at high repetition rates

We present a setup for ultrafast x-ray diffraction (UXRD) based at the storage ring BESSY II, in particular, a pump laser that excites the sample using 250 fs laser-pulses at repetition rates ranging from 208 kHz to 1.25 MHz. We discuss issues connected to the high heat-load and spatio-temporal alignment strategies in the context of a UXRD experiment at high repetition rates. The spatial overlap between laser pump and x-ray probe pulse is obtained with 10 μm precision and transient lattice changes can be recorded with an accuracy of δa/a(0) = 10(-6). We also compare time-resolved x-ray diffraction signals from a laser excited LSMO/STO superlattice with phonon dynamics simulations. From the analysis we determine the x-ray pulse duration to 120 ps in standard operation mode and below 10 ps in low-α mode.     

Combining optical tweezers and scanning probe microscopy to study DNA-protein interactions

We present the first results obtained with a new instrument designed and built to study DNA-protein interactions at the single molecule level. This microscope combines optical tweezers with scanning probe microscopy and allows us to locate DNA-binding proteins on a single suspended DNA molecule. A single DNA molecule is stretched taut using the optical tweezers, while a probe is scanned along the molecule. Interaction forces between the probe and the sample are measured with the optical tweezers. The instrument thus enables us to correlate mechanical and functional properties of bound proteins with the tension within the DNA molecule. The typical friction force between a micropipette used as probe and a naked DNA molecule was found to be <1 pN. A 16 micro m DNA molecule with approximately 10-15 digoxygenin (DIG) molecules located over a 90 nm range in the middle of the DNA was used as a model system. By scanning with an antidigoxygenin (alpha-DIG) antibody-coated pipette we were able to localize these sites by exploiting the high binding affinity between this antibody-antigen pair. The estimated experimental resolution assuming an infinitesimally thin and rigid probe and a single alpha-DIG/DIG bond was 15 nm.     

Dual-trap optical tweezers with real-time force clamp control

Single molecule force clamp experiments are widely used to investigate how enzymes, molecular motors, and other molecular mechanisms work. We developed a dual-trap optical tweezers instrument with real-time (200 kHz update rate) force clamp control that can exert 0-100 pN forces on trapped beads. A model for force clamp experiments in the dumbbell-geometry is presented. We observe good agreement between predicted and observed power spectra of bead position and force fluctuations. The model can be used to predict and optimize the dynamics of real-time force clamp optical tweezers instruments. The results from a proof-of-principle experiment in which lambda exonuclease converts a double-stranded DNA tether, held at constant tension, into its single-stranded form, show that the developed instrument is suitable for experiments in single molecule biology.     

Remote transfer of ultrastable frequency references via fiber networks

Three distinct techniques exist for distributing an ultrastable frequency reference over optical fibers. For the distribution of a microwave frequency reference, an amplitude-modulated continuous wave (cw) laser can be used. Over kilometer-scale lengths this approach provides an instability at 1 s of approximately 3 x 10(-14) without stabilization of the fiber-induced noise and approximately 1 x 10(-14) with active noise cancellation. An optical frequency reference can be transferred by directly transmitting a stabilized cw laser over fiber and then disseminated to other optical and microwave regions using an optical frequency comb. This provides an instability at 1 s of 2 x 10(-14) without active noise cancellation and 3 x 10(-15) with active noise cancellation [Recent results reduce the instability at 1 s to 6 x 10(-18).] Finally, microwave and optical frequency references can be simultaneously transmitted using an optical frequency comb, and we expect the optical transfer to be similar in performance to the cw optical frequency transfer. The instability at 1 s for transfer of a microwave frequency reference with the comb is approximately 3 x 10(-14) without active noise cancellation and <7 x 10(-15) with active stabilization. The comb can also distribute a microwave frequency reference with root-mean-square timing jitter below 16 fs integrated over the Nyquist bandwidth of the pulse train (approximately 50 MHz) when high-bandwidth active noise cancellation is employed, which is important for remote synchronization applications.     

Optical extinction monitor using cw cavity enhanced detection

We present details of an apparatus capable of measuring optical extinction (i.e., scattering and/or absorption) with high precision and sensitivity. The apparatus employs one variant of cavity enhanced detection, specifically cavity attenuated phase shift spectroscopy, using a near-confocal arrangement of two high reflectivity (R approximately 0.9999) mirrors in tandem with an enclosed cell 26 cm in length, a light emitting diode (LED), and a vacuum photodiode detector. The square wave modulated light from the LED passes through the absorption cell and is detected as a distorted wave form which is characterized by a phase shift with respect to the initial modulation. The amount of that phase shift is a function of fixed instrument properties-cell length, mirror reflectivity, and modulation frequency-and of the presence of a scatterer or absorber (air, particles, trace gases, etc.) within the cell. The specific implementation reported here employs a blue LED; the wavelength and spectral bandpass of the measurement are defined by the use of an interference filter centered at 440 nm with a 20 nm wide bandpass. The monitor is enclosed within a standard 19 in. rack-mounted instrumentation box, weighs 10 kg, and uses 70 W of electrical power including a vacuum pump. Measurements of the phase shift induced by Rayleigh scattering from several gases (which range in extinction coefficient from 0.4-32 Mm(-1)) exhibit a highly linear dependence (r(2)=0.999 97) when plotted as the co-tangent of the phase shift versus the expected extinction. Using heterodyne demodulation techniques, we demonstrate a detection limit of 0.04 Mm(-1) (4 x 10(-10) cm(-1)) (2sigma) in 10 s integration time and a base line drift of less than +/-0.1 Mm(-1) over a 24 h period. Detection limits decrease as the square root of integration time out to approximately 150 s.     

Femtosecond broadband stimulated Raman spectroscopy: Apparatus and methods

The laser, detection system, and methods that enable femtosecond broadband stimulated Raman spectroscopy (FSRS) are presented in detail. FSRS is a unique tool for obtaining high time resolution (<100 fs) vibrational spectra with an instrument response limited frequency resolution of <10 cm(-1). A titanium:Sapphire-based laser system produces the three different pulses needed for FSRS: (1) A femtosecond visible actinic pump that initiates the photochemistry, (2) a narrow bandwidth picosecond Raman pump that provides the energy reservoir for amplification of the probe, and (3) a femtosecond continuum probe that is amplified at Raman resonances shifted from the Raman pump. The dependence of the stimulated Raman signal on experimental parameters is explored, demonstrating the expected exponential increase in Raman intensity with concentration, pathlength, and Raman pump power. Raman spectra collected under different electronic resonance conditions using highly fluorescent samples highlight the fluorescence rejection capabilities of FSRS. Data are also presented illustrating our ability: (i) To obtain spectra when there is a large transient absorption change by using a shifted excitation difference technique and (ii) to obtain high time resolution vibrational spectra of transient electronic states.     

A Fluorimeter on the Basis of a Femtosecond Cr<Superscript>+4</Superscript>: Forsterite Laser

An apparatus for measuring luminescence lifetimes using the femtosecond up-conversion method is presented. A laser system based on a chromium–forsterite crystal with a lasing wavelength of 1250 nm is used to generate ultrashort pulses. Luminescence is excited in a sample by optical harmonics that are generated in nonlinear optical crystals. The width of the instrument function of the system is 200 fs. Methods for optimizing the signal-to-noise ratio in measurements are discussed. The results of measurements of the fluorescence- decay dynamics and the anisotropy of aqueous solutions of an inclusion complex of the 4-DASPI styrene dye in cucurbit[6]uril on short (5 ps) and long (500 ps) time scales are presented.     

Experimental diagnostic module for ultrafast combined interferometry of the processes of interaction of ultrashort laser pulses with condensed media in vacuum

An experimental diagnostic module based on a femtosecond laser system (τ_0.5 ∼ 45-70 fs, 7n = 266, 400, and 800 nm) and the experimental technique for ultrafast combined interferometric investigation of the interaction of ultrashort laser pulses with condensed media in vacuum are described. A combined interferometric microscope built according to the Michelson and Mach-Zehnder schemes allows studies of the dynamics of optico-thermophysical and gas-dynamic proc esses at the surface of a target (the crater depth and diameter, optical properties) and in a plasma plume (velocity of expanding particles, electron density, optical characteristics) at a time resolution of 5 - 10^-14 s in the range of delays 10^-13-10^-7 susing two probing wavelengths (7n = 400, 800 nm) in vacuum (to 5 - 10^-5 mbar). Setting a mechanical shutter in the reference arm of the interferometer also allows obtaining of shadow photographs without changing the optical scheme.     

Time-resolved near-edge x-ray absorption fine structure spectroscopy on photo-induced phase transitions using a tabletop soft-x-ray spectrometer

We present a table-top soft-x-ray spectrometer for the wavelength range λ = 1-5 nm based on a stable laser-driven x-ray source, making use of a gas-puff target. With this setup, optical light-pump/soft-x-ray probe near-edge x-ray absorption fine structure (NEXAFS) experiments with a temporal resolution of about 230 ps are feasible. Pump-probe NEXAFS measurements were carried out in the "water-window" region (2.28 nm-4.36 nm) on the manganite Pr(0.7)Ca(0.3)MnO(3), investigating diminutive changes of the oxygen K edge that derive from an optically induced phase transition. The results show the practicability of the table-top soft-x-ray spectrometer on demanding investigations so far exclusively conducted at synchrotron radiation sources.     

A compact streak camera for 150 fs time resolved measurement of bright pulses in ultrafast electron diffraction

We have developed a compact streak camera suitable for measuring the duration of highly charged subrelativistic femtosecond electron bunches with an energy bandwidth in the order of 0.1%, as frequently used in ultrafast electron diffraction (UED) experiments for the investigation of ultrafast structural dynamics. The device operates in accumulation mode with 50 fs shot-to-shot timing jitter, and at a 30 keV electron energy, the full width at half maximum temporal resolution is 150 fs. Measured durations of pulses from our UED gun agree well with the predictions from the detailed charged particle trajectory simulations.     

Acousto-optic modulator system for femtosecond laser pulses

Femtosecond laser pulses have made a revolution in multiphoton excitation microscopy, micromachining, and optical storage for their unprecedented high peak power. However, modulation of their intensity with acousto-optic modulator (AOM) is frustrated by dispersion which results in a significant stretch in pulse width. Here we report a scheme composed of two acousto-optic deflectors (AODs) to modulate the intensity of the femtosecond laser pulses with simultaneous compensation for the temporal dispersion. With commercial AODs, we demonstrated such an AOM system for the femtosecond laser pulses with overall transmission efficiency of around 80%. The pulse width of the exit beam is 115-177 fs for an input pulse of 110 fs, across the wavelength range of 720-920 nm when the temporal dispersion compensation is optimally tuned at 800 nm. The fluorescence intensity in a two-photon microscopy experiment performed using this system increased 5.5-fold over that of the uncompensated AOM.