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At least 19 records

Student Travel Support for the Inaugural Gordon Research Seminar on Multiphoton Processes (Final Technical Report)

This project provided financial support for early-career participants of the 2022 Gordon Research Seminar (GRS) on Multiphoton Processes, which was held on June 11 & 12, 2022 in Smithfield, Rhode Island, in conjunction with the Gordon Research Conference (GRC) on the same topic, held on June 12-17, 2022 in the same location. The GRC on Multiphoton Processes is an established conference series in the field of Atomic, Molecular and Optical (AMO) Physics with intense lasers. It regularly attracts around one hundred fifty researchers from around the world to present and discuss their forefront research featuring light-matter interaction in a variety of systems, ranging from atoms and molecules to nanosystems. In order to increase the attendance of early-career researchers at the GRC, in particular graduate students, post-docs, and other scientists with comparable levels of experience and education, the general assembly of the GRC on Multiphoton Processes decided during their last session in 2018 to organize a Gordon Research Seminar in conjunction with the next conference and organized and attended by early-career researchers. The GRS's primary intent is to provide a forum to graduate students and post-docs working in the field of intense and ultrafast AMO physics to present and exchange new data and cutting-edge ideas and to network with their peers at other research institutions around the U.S. and the world.

74 ATOMIC AND MOLECULAR PHYSICS↗

Multiphoton Process and Anomalous Potential of Cell Membrane by Laser Radiation

In this paper, by the use of quantum biology and quantum optics, the laser induced potential variation of cell membrane has been studied. Theoretically, we have found a method of calculating the monophoton and multiphoton processes in the formation of the anomalous potential of cell membrane. In contrast with the experimental results, our numerical result is in the same order. Therefore, we have found the possibility of cancer caused by the laser induced anomalous cell potential.

Zhang, Kaixi↗

Line broadening in multiphoton processes with a resonant intermediate transition

It is found that the line width of the excitation spectrum for multiphoton ionization is broadened much more severely than the cascade fluorescence originating from the resonant intermediate level. These results derive from the mutual effects of the ionizing and resonating transitions, which are not properly accounted for in perturbative treatments. In general, the ionization line shape can be expressed as the sum of two Lorentzian components, each with different degrees of broadening. This line shape reduces to that of the resonating transition in the limit of vanishing intensities. Moreover, the fluorescence line shape may also exhibit a second component whose amplitude may become important under certain conditions.

Wang, C. C.↗

Calculation of multiphoton ionization processes

We propose an accurate and efficient procedure in the calculation of multiphoton ionization processes. In addition to the calculational advantage, this procedure also enables us to study the relative contributions of the resonant and nonresonant intermediate states.

Chang, T. N.↗

Formation of integrated optics components by multiphoton photorefractive processes

Phase holograms have been formed in pure outdiffused LiNbO3 waveguides using the photorefractive effect initiated by two-photon absorption. Efficient holograms were recorded with two guided waves, of less than 100 W peak power, and less than 10 microJ optical energy. This technique automatically compensates for wave front perturbations in the guide and allows the formation of various integrated components such as wavelength multiplexers and optical switches.

Verber, C. M.↗

Pathways to excitation of atoms with bicircular laser pulses

We study the excitation of the hydrogen atom by bichromatic circularly polarized laser pulses using numerical solutions of the time-dependent Schrödinger equation. The results are in agreement with the selection rules for multiphoton processes in such fields, namely, excited states are populated in which orbital angular momentum and magnetic quantum numbers are either both odd or both even, independent of the relative helicity, peak intensity, and pulse duration of the pulses. For co-rotating pulses the results show that excitation predominantly proceeds to states with magnetic quantum number of the same helicity as the laser pulses. Besides pathways via direct photon absorption from the ground state our results indicate that a transfer of population among the Rydberg states occurs via Λ-type transitions. In the case of counter-rotating pulses the largest excitation probability is found for Rydberg states that differ in magnetic quantum number by Δm=±3. This pattern allows us to estimate how many photons from each of the two bichromatic fields have been absorbed. Finally, we confirm that a population in Rydberg states beyond a maximum orbital angular quantum number is unlikely.

74 ATOMIC AND MOLECULAR PHYSICS↗

Upconversion of Infrared Light by Graphitic Microparticles Due to Photoinduced Structural Modification

Recent reports of upconversion and white light emission from graphitic particles warrant an explanation of the physics behind the process. A model is offered, wherein the upconversion is facilitated by photoinduced electronic structure modification allowing for multiphoton processes. As per the prediction of the model, it is experimentally shown that graphite upconverts infrared light centered around 1.31 μm (0.95 eV) to broadband white light centered around 0.85 μm (1.46 eV). The results suggest that upconversion from shortwave infrared (≈3 μm, 0.45 eV) to visible region may be possible. The experiments show that the population dynamics of the electronic states involved in this upconversion process occur in the timescale of milliseconds.

Sharma, Rohin↗

In-Situ Laser Diagnostics to Understand Plasma-Surface Interactions in Titanium Thin Film Deposition

During the current project period the following tasks were completed: (1) We demonstrated the feasibility of a new way of measuring CH3 radicals in a plasma environment using a single, femtosecond (fs) pulsed laser for the first time, in a CH4 + Ar flow. A single fs pulsed Ti:Sa laser was split into two beams and with beam conversion using crystals we generatedtwo beams of 275 nm and 205 nm. The 275 nm was used to predissociate the CH3 radicals to CH2+H, followed by 205 nm Two Photon Laser Induced Fluorescence (TALIF) detection of H atoms, with a 11 ns delay from 275 nm predissociation pulse. (2) We demonstrated preliminary CH3 concentration measurements with spatial (< 100 µm) and time resolution (< 10 ns) by image processing of H and Kr TALIF signal images. (3) The methodology to quantify CH3 concentrations was developed. (4) Preliminary measurements of laser dissociation cross sections for CH4 and CH3 to (CH3+H), and (CH2+H), respectively, were conducted. (5) 275 nm laser dissociation of CH4 is a multiphoton process, and the CH4 dissociation cross section is a more sensitive function of the laser pulse energy than CH4 concentration. In the coming months, we will make more precise measurements of the dissociation cross sections, 𝑘275, 𝐶𝐻4 and 𝑘275, 𝐶𝐻3, by varying the laser energy while keeping the flow composition and conditions constant. This will enable more precise quantification of CH3 radical concentrations. More detailed measurements of CH3 radicals will be conducted in the following months of 2025 (Sept-Dec) in a Titanium Isopropoxide (TIP) + H2 + Ar flow meant for pure phase Ti thin film deposition by Chemical Vapor Deposition (CVD). More precise measurements of 275 nm laser dissociation cross sections for CH4 (to CH3 + H) and CH3 (to CH2 + H) will be conducted in the future. Detailed 275 nm laser predissociation cross sections for CH4 and CH3 dissociation to (CH3+H), and (CH2+H), respectively, as a function of gas heating, plasma power, and laser pulse energy will be evaluated. This will enable quantification of CH3 concentrations in the precursor flow over a substrate with time and spatial resolution. Comparison of the concentrations with 2D numerical simulations can lead to understanding of plasma surface interactions during pure metallic Ti thin film deposition using environmentally safer non-halogen TIP precursor. Flow conditions for pure Ti thin film deposition using non-halogen precursor (TIP) will be identified in the following months.

Uddi, Mruthunjaya [Advanced Cooling Technologies, ↗

A new concept in laser-assisted chemistry - The electronic-field representation

Electronic-field representation is proposed as a technique for laser-assisted chemistry. Specifically, it is shown that several field-assisted chemical processes can be described in terms of mixed matter-field quantum states and their associated energies. The technique may be used to analyze the effects exerted by an intense laser on both bound and unbound molecular systems, and to investigate other field-induced effects including multiphoton processes, emission, and photodissociation.

George, T. F.↗

Dual Emission Bands of a 2D Perovskite Single Crystal with Charge Transfer State Characteristics

Several hybrid halide 2D-perovskite species emit light with an emergent and controversial broadband emission Stokes-shifted down from the narrow band emission. This work uncovers the sub- and above-bandgap emission and absorption characteristics of PEA 2 PbI 4 prepared with gap states introduced during single crystal growth. Here, gap states led to coexistent intrinsic and heterostructured electronic frameworks that are selectively accessible with ultraviolet (UV) and infrared (IR) light, respectively, resulting in the phenomenon of photoluminescence (PL) switching from narrowband green to broadband red. Electron-energy dependent cathodoluminescence shows a relative increase in the broadband red PL intensity as the electron penetration depth increases from 30 nm to 2 μm, confirming the heterostructured framework is formed in the bulk of the crystal. Excitation–emission power slope of 2.5 and up-conversion pump transient absorption (TA) spectra suggest that the IR up-conversion excitation with red photoluminescence, peaked at 655 nm, is a multiphoton process occurring in the heterostructured framework through a nonlinear optical response. The energetic pathways toward the dual emission bands are revealed by pump–probe transient absorption spectroscopy, showing energetically broad gap states with high sensitivity to an IR pump are upconverted and subsequently quickly relax from high to low energy levels within 4 ps. Furthermore, the up-conversion red PL demonstrates a linear polarization with magnetic field effects, thus affirming that the band-like heterostructured framework is crystallographically aligned with characteristics of spatially extended charge-transfer states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Anticorrelation of compressibility and resistivity in a microwave-irradiated two-dimensional electron system

Here, we report our direct study of the compressibility on an ultrahigh mobility two-dimensional electron system ( μ e ~ 1 × 10 7 cm 2 /V s) in GaAs/AlGaAs quantum wells under microwave irradiation. The field penetration current results show that the quantum capacitance oscillates with microwave-induced resistance oscillations, yet, the trend is opposite with respect to the compressibility of equilibrium states in previous theoretical explanations. The anomalous phenomena provide a platform for study on the nonequilibrium system under microwaves. Moreover, the quantum capacitance indication for a multiphoton process around j = 1 / 2 is detected under an intensive microwave below 30 GHz.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Ruby laser induced emission from NO2

Two different types of emission from excited NO2 were observed using pulsed ruby laser light at 6943 A. The first type of fluorescence was seen in the near IR and results from the single photon excitation of NO2 from the ground 2-A1 state. By observing the emission as a function of time an unexpected behavior was observed in the near IR and could be explained by a consecutive deactivation mechanism, wherein a secondary species is preferentially detected. A second type of emission recently observed in the blue spectral region is weaker and is due to a multiphoton process. The intensity of the blue emission is a function of the cube of the laser intensity at low pressures and approaches the square at high pressures. This variation is attributed to simultaneous deactivation of the excited NO2 intermediate by collision (square) and by anti-Stokes Raman scattering off of the excited NO2 (cube).

Hakala, D. F.↗

Overview of laser applications to chemistry

The discussion is in three parts. First, laser spectroscopy is discussed with consideration given to single-photon and multiphoton processes. Second, attention is given to the use of lasers in studying molecular interactions and reaction dynamics. Finally, the paper discusses the relationship between chemistry and laser development.

George, T. F.↗

International Conference on Vacuum Ultraviolet Radiation Physics, 8th, Lunds Universitet, Sweden, Aug. 4-8, 1986, Proceedings

The interactions of VUV radiation with solids are explored in reviews and reports of recent theoretical and experimental investigations from the fields of atomic and molecular physics, solid-state physics, and VUV instrumentation. Topics examined include photoabsorption and photoionization, multiphoton processes, plasma physics, VUV lasers, time-resolved spectroscopy, synchrotron radiation centers, solid-state spectroscopy, and dynamical processes involving localized levels. Consideration is given to the fundamental principles of photoemission, spin-polarized photoemission, inverse photoemission, semiconductors, organic materials, and adsorbates.

Nilsson, Per-Olof↗

Transmission spectroscopy of CF 4 molecules in intense x-ray fields

The nonlinear interaction of x rays with matter is at the heart of understanding and controlling ultrafast molecular dynamics from an atom-specific viewpoint, providing new scientific and analytical opportunities to explore the structure and dynamics of small quantum systems. At increasingly high x-ray intensity, the sensitivity of ultrashort x-ray pulses to specific electronic states and emerging short-lived transient intermediates is of particular relevance for our understanding of fundamental multiphoton absorption processes. In this work, intense x-ray free-electron laser (XFEL) pulses at the European XFEL are combined with a gas cell and grating spectrometer for a high-intensity transmission spectroscopy study of multiphoton-induced ultrafast molecular fragmentation dynamics in CF 4 . This approach unlocks the direct intrapulse observation of transient fragments, including neutral atoms, by their characteristic absorption lines in the transmitted broadband x-ray spectrum. The dynamics with and without initially producing fluorine 𝐾-shell holes are studied by tuning the central photon energy. The absorption spectra are measured at different FEL intensities to observe nonlinear effects. Transient isolated fluorine atoms and ions are spectroscopically recorded within the ultrashort pulse duration of a few tens of femtoseconds. An isosbestic point that signifies the correlated transition between intact neutral CF 4 molecules and charged atomic fragments is observed near the fluorine 𝐾 edge. The dissociation dynamics and the multiphoton absorption-induced dynamics encoded in the spectra are theoretically interpreted. Overall, this study demonstrates the potential of high-intensity x-ray transmission spectroscopy to study ultrafast molecular dynamics with sensitivity to specific intermediate species and their electronic structure.

74 ATOMIC AND MOLECULAR PHYSICS↗

Multichannel photoelectron phase lag across atomic barium autoionizing resonances

Phase lag associated with coherent control where an excited system decays into more than one product channel has been subjected to numerous investigations. Although previous theoretical studies have treated the phase lag across resonances in model calculations, quantitative agreement has never been achieved between the theoretical model and an experimental measurement of the phase lag from the ω-2ω ionization of atomic barium. Yamazaki and Elliot, Phys. Rev. Lett. 98, 053001 (2007); Phys. Rev. A 76, 053401 (2007), suggesting that a toy model with phenomenological parameters is inadequate to describe the observed phase lag behavior. Here the phase lag is treated quantitatively in a multichannel coupling formulation, and our calculation based on a multichannel quantum defect and R-matrix treatment achieves good agreement with the experimental observations. Our treatment also develops formulas to describe the effects of hyperfine depolarization on multiphoton ionization processes. Moreover, we identify resonances between Ba + 5d 3/2 and 5d 5/2 thresholds that have apparently never been experimentally observed and classified.

74 ATOMIC AND MOLECULAR PHYSICS↗