Probe Laser Wavelength Research Articles

Sensitivity Improvements for Picosecond Ultrasonic Thickness Measurements in Gold and Tungsten Nanoscale Films

Picosecond ultrasonics, as a nondestructive and noncontact method, can be employed for nanoscale metallic film thickness measurements. The sensitivity of the system, which determines the measurement precision and practicability of this technique, is often limited by the weak intensity of the ultrasonic signal. To solve this problem, we investigate the distinct mechanisms involved in picosecond ultrasonic thickness measurement for two types of metals, namely tungsten (W) and gold (Au). For thickness measurement in W films, theory and simulation show that optimizing the pump and probe laser wavelengths, which determine the intensity and shape of the ultrasonic signal, is critical to improving measurement sensitivity, while for Au film measurements, where acoustic-induced beam distortion is dominant, the signal intensity can be optimized by selecting an appropriate aperture size and sample position. The above approaches are validated in experiments. A dual-wavelength pump–probe system is constructed based on a passively mode-locked ytterbium-doped fiber laser. The smoothing method and multipeak Gaussian fitting are employed for the extraction of ultrasonic time-of-flight. Subnanometer measurement precision is achieved in a series of W and Au films with thicknesses of 43–750 nm. This work can be applied to various high-precision, noncontact measurements of metal film thickness in the semiconductor industry.

Photothermal Gas Detection With a Dithered Low-Finesse Fiber-Optic Fabry-Pérot Interferometer

Pump-probe photothermal spectroscopy has been recently proposed for sensitive gas detection. The probe laser wavelength was usually locked at the quadrature point of an interferometer to provide a linear output of the phase signal. However, this detection scheme brings unwanted fluctuations to the interferometer. Here we report a novel phase demodulation method of the probe laser for photothermal spectroscopy to enhance the stability. We demonstrate a proof-of-concept experiment by performing photothermal detection of methane (CH <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">4</sub> ) inside a hollow-core fiber, which is sandwiched by two pieces of solid-core fibers to form a low-finesse fiber-optic Fabry-Pérot interferometer (FPI). Besides the wavelength modulation of the 1.65- <italic xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">μ</i> m pump laser, we employed a dither to modulate the injection current of the probe diode laser, which was frequency-locked to the FP cavity resonance. The photothermal signal was sensitively measured from the error signal of the feedback loop by demodulating the FPI output at the dither frequency. A normalized noise equivalent absorption (NNEA) coefficient of 7.5 × 10 <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">−9</sup> cm <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">−1</sup> WHz <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">−1/2</sup> was achieved in this work. A comparison to the conventional quadrature point locking technique was performed to reveal the remarkable sensor stability with immunity to optical disturbance.

Acoustic Vibration Modes of Gold–Silver Core–Shell Nanoparticles

Bimetallic Au/Ag core–shell cuboid nanoparticles (NPs) exhibit a complex plasmonic response dominated by a dipolar longitudinal mode and higher-order transverse modes in the near-UV, which may be exploited for a range of applications. In this paper, we take advantage of the strong signature of these modes in the NP ultrafast transient optical response, measured by pump-probe transient absorption (TA) spectroscopy, to explore the NP vibrational landscape. The fast Fourier transform analysis of the TA dynamics reveals specific vibration modes in the frequency range 15–150 GHz, further studied by numerical simulations based on the finite element method. While bare Au nanorods exhibit extensional and breathing modes, the bimetallic NPs undergo more complex motions, involving the displacement of facets, edges and corners. The amplitude and frequency of these modes are shown to depend on the Ag shell thickness, as the silver load modifies the NP aspect ratio and mass. Moreover, the contributions of the vibrational modes to the experimental TA spectra are shown to vary with the probe laser wavelength at which the signal is monitored. Using the combined simulations of the NP elastic and optical properties, we elucidate this influence by analyzing the effect of the mechanisms involved in the acousto-plasmonic coupling.

Rovibrational investigation of a new high-lying 0u + state of Cu2 by using two-color resonant four-wave-mixing spectroscopy.

A highly excited electronic state of dicopper is observed and characterized for the first time. The [39.6]0u +-X1Σg +(0g +) system is measured at rotational resolution by using degenerate and two-color resonant four-wave-mixing, as well as laser induced fluorescence spectroscopy. Double-resonance experiments are performed by labeling selected rotational levels of the ground state by tuning the probe laser wavelength to transitions in the well-known (1-0) band of the B0u +-X1Σg +(0g +) electronic system. Spectra obtained by scans of the pump laser in the UV wavelength range were then assigned unambiguously by the stringent double-resonance selection rules. The absence of a Q-band suggests a parallel transition (ΔΩ = 0) and determines the term symbol of the state as 0u + in Hund's case (c) notation. The equilibrium constants for 63Cu2 are Te = 39 559.921(92)cm-1, ωe = 277.70(14)cm-1, Be = 0.104 942(66)cm-1, and re = 2.2595(11) Å. These findings are supported by high-level ab initio calculations at the MRCI+Q level, which clearly identifies this state as resulting from a 4p ← 3d transition. In addition, three dark perturber states are found in the v = 1 and v = 2 vibrational levels of the new state. A deperturbation analysis characterizes the interaction and rationalizes the anomalous dips in the excitation spectrum of the [39.6]0u +-X1Σg +(0g +) system.

Absorption imaging of trapped atoms in presence of AC-Stark shift

In this work, the effect of AC-Stark shift of atomic energy levels in an optical dipole trap (ODT) on in situ absorption imaging of the trapped atoms has been investigated. The Stark shift of various energy levels of 87Rb atoms relevant for trapping in the optical dipole trap (ODT) has been calculated. The spatially varying AC-Stark shift of energy levels due to ODT beam results in position dependent absorption cross-section of the atom at the absorption probe laser wavelength, which significantly modifies the measured optical density (OD) of the trapped atom cloud during the in situ absorption imaging. We have estimated the number of atoms trapped in the ODT taking AC-Stark shift into account. The estimated numbers are found to be higher at higher ODT beam power, making a qualitative agreement with larger trap depth at higher ODT beam power. This work can be particularly useful in estimating the in situ loss rate of atoms from the trap during the evaporative cooling of the trapped atom cloud.

Imaging of triboelectric charge distribution induced in polyimide film by using optical second-harmonic generation: Electronic charge distribution and dipole alignment

By using an optical second-harmonic generation (SHG) microscope, we visualized spatial distribution of triboelectric charge in polyimide films, which are negatively charged by rubbing with a cotton belt. The origins of this triboelectric charging were excessive electronic charges and aligned dipoles. The excessive electronic charges were imaged using the probe laser wavelength of 1140 nm (SHG wavelength 570 nm), whereas the aligned dipoles were visualized by choosing the laser wavelength of 570 nm (SHG wavelength 285 nm). Combining the two visualized images showed that the dipolar alignment region with a width of 10 μm was induced on the rubbed polyimide surface, and at the same time, excess electronic charges were generated in that region. We conclude that dipolar alignment and electronic charging are main contributors, and the interaction between the two contributors plays an essential role in triboelectrification.

Linear and Nonlinear Thermal Lens Signal of the (Δν = 6) C-H Vibrational Overtone of Naphthalene in Liquid Solutions of n-Hexane.

The thermal lens technique is applied to vibrational overtone spectroscopy of solutions of naphthalene (C10H8) in liquid hexane. The C-H fifth vibrational (Δν = 6) overtone spectrum of C10H8 is detected at room temperature for mole fractions from 0.08 to 19 × 10-6 using n-C6H14 as solvent. By detecting the absorption band in a 19 ppm (parts per million) solution, the peak absorption of the signal is approximately (2.2 ± 0.3) × 10-7 cm-1. A plot of normalized integrated intensity as a function of the mole fraction of naphthalene in solution reveals a dependence of the magnitude of the signal with the probe laser wavelength. If the wavelength of the probe laser is 568 nm, the thermal lens signal (TLS) is linear as a function of the mole fraction of the solution. When the wavelength of the probe laser is 488 nm, the TLS is nonlinear as a function of the concentration. Three different models of nonlinear absorption are discussed. A two-color absorption model that includes the simultaneous absorption of the pump and probe lasers could explain the enhanced magnitude and the nonlinear behavior of the TLS for solutions of mole fraction < 0.1%.

Size Characterisation Method and Detection Enhancement of Plasmonic Nanoparticles in a Pump–Probe System

The optical resonance of metal nanoparticles can be used to enhance the generation and detection of their main vibrational mode. In this work, we show that this method allows the accurate characterisation of the particle’s size because the vibrational frequency of plasmonic nanoparticles only depends on their mechanical properties. Moreover, by a careful selection of the particle size and/or probe laser wavelength, the detected signal can be increased by a large factor (∼9 for the particles used in this work) under the same illumination conditions. Finally, we show experimentally that particles of different sizes inside the point spread function can be observed due to the differences in their vibrational states, which could provide a feasible route to super-resolution.

Ultrafast photodissociation dynamics of butanone in 3s Rydberg state

The initiation and subsequent control or exploration study of chemical transformation in real time by using ultrashort laser pulses aim at femtochemistry. The real-time investigations of ultrafast dynamics of excited molecules in gas and condensed phases have attracted a great deal of attention over the last two decades. As a kind of important organic compound, aliphatic ketone is an area of much interest for many research fields, especially for atmospheric photochemistry. Via photodissociation reaction, it can release carbonyl radical whose chemical character is active and can react with hydroxyl easily. As a typical aliphatic ketone, butanone has been a research focus over the past decades. The ultrafast dissociation dynamics of butanone after excitation to the second electronically excited state (S2) with a 195.8 nm pump pulse is studied by the femtosecond pump-probe technique combined with the time-of-flight mass spectrometry (TOF-MS). Time-resolved mass spectrometry (TRMS) has proven to be a powerful technique to study the ultrafast dynamics of excited states in molecules. In this technique, the MCP detector is capable of recording time-resolved ion yield measurements of different cations by monitoring the current output directly from the anode by using an oscilloscope. This enables a time-of-flight mass spectrum to be recorded at each delay time, which is controlled by a delay stage, and the measured total signal is then integrated, yielding a time-resolved ion yield transient, which is conducted by LABVIEW software. The pump wavelength in this work is set to be 195.8 nm and the probe laser wavelength is centered at 800 nm. The complex ultrafast dynamics in butanone with 3s Rydberg state excitation and its possible decay paths and following dissociation mechanism are given. Experimental results show that the Norrish I type dissociation kinetics of butanone exhibit rich features, for it has a methyl group and an ethyl group at position. The decay time constant of the parent transient is approximately 2.23 ps0.02 ps. There is only one time constant of 2.15 ps0.02 ps for the fitting of the propionyl transient. The best fit of acetyltransient is obtained with four time constants:1=(2.400.15) ps, 2=(1.100.25) ps, 3=(0.080.02) ps, and 4=(17.720.80) ps, corresponding to S2S1 internal conversion, the primary dissociation of the S1 state generating CH3CO(), internal conversion and secondary dissociation of CH3CO() respectively. Two competitive -CC bond dissociation processes are observed and discussed. They are dissociation channels through intramolecular vibrational energy redistribution (IVR) and/or by getting over the dissociation barrier in -cleavage of butanone. But hereunder the condition of this experiment, the dissociation is the result of IVR.

The design of the optical Thomson scattering diagnostic for the National Ignition Facility.

The National Ignition Facility (NIF) is a 192 laser beam facility designed to support the Stockpile Stewardship, High Energy Density and Inertial Confinement Fusion (ICF) programs. We report on the design of an Optical Thomson Scattering (OTS) diagnostic that has the potential to transform the community's understanding of NIF hohlraum physics by providing first principle, local, time-resolved measurements of under-dense plasma conditions. The system design allows operation with different probe laser wavelengths by manual selection of the appropriate beam splitter and gratings before the shot. A deep-UV probe beam (λ0-210 nm) will be used to optimize the scattered signal for plasma densities of 5 × 1020 electrons/cm3 while a 3ω probe will be used for experiments investigating lower density plasmas of 1 × 1019 electrons/cm3. We report the phase I design of a two phase design strategy. Phase I includes the OTS telescope, spectrometer, and streak camera; these will be used to assess the background levels at NIF. Phase II will include the design and installation of a probe laser.

Simulated performance of the optical Thomson scattering diagnostic designed for the National Ignition Facility.

An optical Thomson scattering diagnostic has been designed for the National Ignition Facility to characterize under-dense plasmas. We report on the design of the system and the expected performance for different target configurations. The diagnostic is designed to spatially and temporally resolve the Thomson scattered light from laser driven targets. The diagnostic will collect scattered light from a 50 × 50 × 200 μm volume. The optical design allows operation with different probe laser wavelengths. A deep-UV probe beam (λ0 = 210 nm) will be used to Thomson scatter from electron plasma densities of ∼5 × 1020 cm-3 while a 3ω probe will be used for plasma densities of ∼1 × 1019 cm-3. The diagnostic package contains two spectrometers: the first to resolve Thomson scattering from ion acoustic wave fluctuations and the second to resolve scattering from electron plasma wave fluctuations. Expected signal levels relative to background will be presented for typical target configurations (hohlraums and a planar foil).

Interruption of electronically excited Xe dimer formation by the photoassociation of Xe(6s[3/2]2)-Xe(5p(6) (1)S0) thermal collision pairs.

The diatomic collisional intermediate responsible for the formation of an electronically excited molecule by teratomic recombination has been observed in both the spectral and temporal domains by laser spectroscopy. We report experiments demonstrating thermal Xe(6s[3/2]2)-Xe(5p(6) (1)S0) atomic collision pairs to be the immediate precursor to the formation of Xe2 (∗)(a(3)Σu (+),A(1)Σu (+)) by the three body process: Xe(∗)(6s) + 2Xe ⟶ Xe2 (∗) + Xe, where the asterisk denotes an excited electronic state. Photoassociating Xe(6s)-Xe atomic pairs by free ⟵ free transitions of the collision complex interrupts the production of the electronically excited Xe dimer, thereby suppressing Xe2 spontaneous emission in the vacuum ultraviolet (VUV, λ ∼ 172 nm, A(1)Σu (+)→X(1)Σg (+)). Intercepting Xe(6s)-Xe pairs before the complex is stabilized by the arrival of the third atom in the teratomic collision process selectively depletes the pair population in a specific Franck-Condon region determined by the probe laser wavelength (λ). Measurements of the variation of VUV emission suppression with λ provide a spectral signature of the [Xe(6s[3/2]2) - Xe((1)S0)](∗) complex and map the probe laser wavelength onto the thermal energy (ϵ″) of the incoming collision pairs.

The preliminary design of the optical Thomson scattering diagnostic for the National Ignition Facility

The National Ignition Facility (NIF) is a 192 laser beam facility designed to support the Stockpile Stewardship, High Energy Density and Inertial Confinement Fusion programs. We report on the preliminary design of an Optical Thomson Scattering (OTS) diagnostic that has the potential to transform the community's understanding of NIF hohlraum physics by providing first principle, local, time-resolved measurements of under-dense plasma conditions. The system design allows operation with different probe laser wavelengths by manual selection of the appropriate beamsplitter and gratings before the shot. A deep-UV probe beam (λ0 between 185-215 nm) will optimally collect Thomson scattered light from plasma densities of 5 x 1020 electrons/cm3 while a 3ω probe will optimally collect Thomson scattered light from plasma densities of 1 x 1019 electrons/cm3. We report the phase I design of a two phase design strategy. Phase I includes the OTS recording system to measure background levels at NIF and phase II will include the integration of a probe laser.

Ultrafast Spectroscopy of Electron-Phonon Coupling in Gold

Transient reflectance of gold was measured using ultrafast spectroscopy by varying the wavelength of the probe laser beam in the visible range. Based on the band structure of gold, the influence of the probe beam wavelength on the signal trend is analyzed in terms of sensitivity, effect of nonthermalized electrons, and relaxation rate. It is found that probing around 490 nm renders the best sensitivity and a simple linear relation between the transient reflectance and the electron temperature. The two-temperature model (TTM) is applied to calculate the electron-phonon coupling factor by fitting the transient reflectance signal. This work clarifies the ultrafast energy transfer dynamics in gold and the importance of using proper probe laser wavelength for modeling the transient heat transfer process in metal.

Ultrafast Thermal Analysis of Surface Functionalized Gold Nanorods in Aqueous Solution

The thermal conductivity and heat capacity of surfactant and polyelectrolyte coatings of gold nanorods (GNRs) in aqueous solution are investigated by transient absorption, following femtosecond pumping of the longitudinal localized surface plasmons. Surfactant and polyelectrolyte layer thicknesses are measured by dynamic light scattering (DLS). The GNRs are initially coated with a bilayer of the quaternary ammonium surfactant cetyltrimethylammonium bromide (CTAB). The rate of change of the absorption of gold nanorods in aqueous solution varies with the probe laser wavelength due to the shift in the plasmon resonance created by heating of media around the particles. The cooling dynamics of gold nanorods are best measured by tuning the pump-probe laser wavelength to the absorption peak of the sample. The heat capacity of the surfactant layer is 2.0 ± 0.3 J cm(-3) K(-1); the thermal conductivity of the surfactant layer drops from 0.24 to 0.18 W m(-1) K(-1) at solution concentrations above the CTAB critical micelle concentration (cmc). Layer-by-layer polyelectrolyte coatings using poly(acrylic acid) (PAA) and polyallyamine hydrochloride (PAH) increase the thermal conductivity and heat capacity of the surface layer. PAH-terminated layers have increased thickness, thermal conductivity, and heat capacity relative to PAA-terminated layers; this effect is attributed to greater water penetration into PAH-terminated surface layers.

O(1D) + N2O Reaction: NO Vibrational and Rotational Distributions

The O((1)D) + N(2)O → 2NO(X (2)Π) reaction has been studied in a molecular beam experiment in which O(3) and N(2)O were coexpanded. The precursor O((1)D) was prepared by O(3) photodissociation at 266 nm, and the NO(X (2)Π) molecules born from the reaction as the O((1)D) recoiled out of the beam were detected by 1+1 REMPI over the 220-246 nm probe laser wavelength range. The resulting spectrum was simulated to extract rotational and vibrational distributions of the NO(X (2)Π) molecules. The product rotational distribution is found to be characterized by a constant rotational temperature of ≈4500 K for all observed bands, v = 0-9. An inverted vibrational distribution is observed. A consistent explanation of this and previous experimental results is possible if there are two channels for the reaction, one producing a nearly statistical vibrational distribution for low O((1)D)-N(2)O relative velocity collisions and a second producing the inverted distribution observed here for high relative velocity collisions. The former might correspond to an insertion/complex-formation reaction, while the latter might correspond to a stripping reaction. Velocity relaxation of the O((1)D) is argued to compete strongly with reaction in most bulb studies, so that these studies see predominantly the nearly statistical distribution. In contrast, the beam experiments do not detect the part of the vibrational distribution produced in low relative velocity reactions because the O((1)D) is not relaxed from its initial velocity before it either reacts or leaves the beam.

ChemInform Abstract: Photodissociation Dynamics of Mn2(CO)10 in Solution on Ultrafast Time Scales

A study of the photodissociation dynamics of Mn2(CO)10 and the vibrational relaxation of its subsequent photoproducts in solutions has been carried out using picosecond time‐resolved laser techniques. The molecule predissociates in less than 2–3 ps after excitation with a 295 nm photon. Two dissociation channels are open for this excitation wavelength, namely, the Mn–Mn bond breaking and the Mn–CO bond breaking, generating internally hot ⋅Mn(CO)5 and Mn2(CO)9, respectively. These two species have a different absorption spectrum in the visible region and are probed independently by varying the probe laser wavelength. The vibrational relaxation of these nascent photoproducts is observed for the first time. In cyclohexane the vibrationally hot Mn2(CO)9 reaches thermal equilibrium with the solvent through two distinct decay channels with time constants of 15 and 170 ps, respectively. The vibrationally cold Mn2(CO)9 then persists for many nanoseconds. The vibrational relaxation is found to be faster in the 2‐p...

Purely-long-range krypton molecules in singly and doubly excited binding potentials

Diatomic potentials for krypton are computed and also probed experimentally. For a probe-laser wavelength near 811 nm, several strong dipole-dipole interactions produce purely-long-range potential wells in the singly excited manifold of (s+p) potentials and in the doubly excited manifold of (p+p) and (s+d) potentials. Evidence of resonant photoassociation into bound states of these potential wells is observed in the emission of ions and ultraviolet photons from a magneto-optically trapped krypton cloud.

Non-adiabatic transition in C2H5OH+ on a light-dressed potential energy surface by ultrashort pump-and-probe laser pulses

We experimentally investigate how parameters of ultrashort laser pulses such as the pulse width and wavelength could induce changes in the dynamics of vibrational wave packets on the light-dressed-potential energy surface (LD-PES) of C2H5OH+ using a pump-and-probe pulse excitation scheme. The probability of non-adiabatic transition at 800 nm from the singly ionized ground state to the repulsive excited state leading to C–O bond breaking is enhanced when a probe laser pulse is delayed by ∼180 fs. At this pulse delay, on the other hand, C–C bond breaking is significantly suppressed. Therefore, the deformation of LD-PES is considered to change the direction of the wave packet traveling originally along the C–C stretching into the direction along the C–O stretching. This non-adiabatic transition leading to the redirection of the dissociating wave packet is found to occur more efficiently at the probe laser wavelengths at 400 nm than at 800 nm. The critical pulse delay is still ∼180 fs even at 400 nm.

Spin noise of conduction electrons inn-type bulk GaAs

We report a comprehensive study of stochastic electron spin fluctuations -- spin noise -- in lightly doped ($n$-type) bulk GaAs, which are measured using sensitive optical magnetometry based on off-resonant Faraday rotation. Frequency spectra of electron spin noise are studied as a function of electron density, magnetic field, temperature, probe laser wavelength and intensity, and interaction volume. Electron spin lifetimes $\tau_s$ are inferred from the width of the spin noise spectra, and are compared with direct measurements of $\tau_s$ using conventional Hanle effect methods. Both methods reveal a strong and similar dependence of $\tau_s$ on the wavelength and intensity of the probe laser, highlighting the undesired influence of sub-bandgap absorption effects on the nominally `non-perturbative' spin noise measurements. As a function of temperature, the spin noise power increases approximately linearly from 1.5 K to 30 K, as expected for degenerate electrons obeying Fermi-Dirac statistics, but with an additional zero-temperature offset. Finally, as the cross-sectional area of the probe laser shrinks and fewer electrons are probed, the measured Faraday rotation fluctuations due to electron spin noise are shown to increase, as expected.