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At least 19 records

Efficient up-conversion in CsPbBr 3 nanocrystals via phonon-driven exciton-polaron formation

Lead halide perovskite nanocrystals demonstrate efficient up-conversion, although the precise mechanism remains a subject of active research. This study utilizes steady-state and time-resolved spectroscopy methods to unravel the mechanism driving the up-conversion process in CsPbBr 3 nanocrystals. Employing above- and below-gap photoluminescence measurements, we extract a distinct phonon mode with an energy of ~7 meV and identify the Pb-Br-Pb bending mode as the phonon involved in the up-conversion process. This result was corroborated by Raman spectroscopy. We confirm an up-conversion efficiency reaching up to 75%. Transient absorption measurements under conditions of sub-gap excitation also unexpectedly reveal coherent phonons for the subset of nanocrystals undergoing up-conversion. This coherence implies that the up-conversion and subsequent relaxation is accompanied by a synchronized and phased lattice motion. This study reveals that efficient up-conversion in CsPbBr 3 nanocrystals is powered by a unique interplay between the soft lattice structure, phonons, and excited states dynamics.

Anti-Stokes Photoluminescence↗

High-quantum-efficiency infrared up-conversion.

Experimental study in which 100% conversion of infrared photons into visible photons was achieved through three wave interactions in a nonlinear medium. The first experimental evidence of overconversion is presented, and the classical theory of up-conversion in the high-conversion-efficiency region is confirmed. A laser pump light feedback technique is described that promises to make the process practical with modestly powerful pump lasers and less than perfect nonlinear crystals. The nonlinear medium used was a LiIO3 crystal that cannot be 90-deg phase-matched. The 'walk off' that resulted helped make possible the attainment of 100% conversion efficiency.

Gurski, T. R.↗

Infrared up-conversion with resonantly two-photon pumped metal vapors

Observation of efficient up-conversion of low-level IR radiation near 10 microns to the near ultraviolet. Radiation at 9.26 micron is converted to 3305 A with a photon conversion efficiency of 58% and a corresponding power gain of 16.2. The process employs resonant two-photon pumping of the nonallowed 3s-3d transition in Na.

Bloom, D. M.↗

Stimulated Raman up-conversion of electromagnetic waves by a gyrating electron beam

A gyrating electron beam supports negative energy modes near the harmonics of electron-cyclotron frequency. An electromagnetic wave passing through such a beam parametrically up-converts into high-frequency electromagnetic modes separated from the pump frequency by the electron-cyclotron harmonics. The growth rate for this process varies directly as the oscillatory velocity of beam electrons caused by the pump and as square root of the beam density. It has a maximum at values of scattering angle close to 180 deg and is also implicitly dependent on the beam veocity and the cyclotron frequency of electrons. The effect of a cold electron component is to reduce the growth rate.

Sharma, O. P.↗

Multiple Raman up-conversion of radiation from pre-existing Langmuir turbulence

Little is known regarding the mechanisms involved in the production of radiation at frequencies which are much higher than the maximum plasma frequency in nonmagnetic plasmas. It is pointed out that radiation at high multiples of the plasma frequency has been observed in laser-pellet experiments, in relativistic beam-plasma interactions, and in low-energy beam-plasma interactions. Radiation at twice the plasma frequency can be produced by coalescence of two Langmuir waves. Another approach is based on radiation near the plasma frequency or its second harmonic, produced by instability or by external sources. Raman scatter from preexisting Langmuir turbulence is permitted repeatedly. At each step such scattering will produce frequency upshifts (anti-Stokes process) and downshifts (Stokes process). The present paper is concerned with this process. Attention is given to equilibrium spectra, analytic approximations, laser-plasma interaction and coherent radiation from relativistic electron beams.

Russell, D.↗

Frequency up-conversion of a high-power microwave pulse propagating in a self-generated plasma

In the study of the propagation of a high-power microwave pulse, one of the main concerns is how to minimize the energy loss of the pulse before reaching the destination. A frequency autoconversion process that can lead to reflectionless propagation of powerful electromagnetic pulses in self-generated plasmas is studied. The theory shows that, under the proper condition, the carrier frequency omega of the pulse shifts upward during the growth of local plasma frequency omega(pe). Thus, the self-generated plasma remains underdense to the pulse. A chamber experiment to demonstrate the frequency autoconversion during the pulse propagation through the self-generated plasma is conducted. The detected frequency shift is compared with the theoretical result calculated by using the measured electron density distribution along the propagation path of the pulse. Good agreement is obtained.

Kuo, S. P.↗

Observation of frequency up-conversion in the propagation of a high-power microwave pulse in a self-generated plasma

A chamber experiment is conducted to study the propagation of a high-power microwave pulse. The results show that the pulse is experiencing frequency up-shift while ionizing the background air if the initial carrier frequency of the pulse is higher than the electron plasma frequency at the incident boundary. Such a frequency autoconversion process may lead to reflectionless propagation of a high-power microwave pulse through the atmosphere.

Kuo, S. P.↗

Investigation of loss processes of Tm and Tm,Ho in YAG

The loss of excitation from various manifolds of Tm and Tm,Ho in YAG as a function of temperature and concentration is studied. Two probable loss mechanisms - a Tm up-conversion and a Ho up-conversion - are identified. A 785-nm CW diode laser with 400-nW peak power was focused to a small spot on the sample. The emission from the sample observed at 90 deg was monitored through a monochromator with slits open to 3 mm. Intensity of emission was measured by varying the power of the excitation source using a set of neutral density filters. Power is reported as the percentage of the peak power, and the intensity curves were normalized below 20 percent of transmission. The fact that there is emission above the pump energy indicates an up-conversion from excited manifolds. Nonlinear changes in the intensity of the emission from the Tm 3F4 manifold with the pump power reveals a loss of excitation from this manifold. The linear dependence of the 5I7 manifold emission with pump power at low Tm and high Ho concentrations and the gain of energy in the 5I6 manifold of Ho indicate that the 5I7 manifold loss is due to the coupling of Tm and Ho ions.

Armagan, G.↗

Ku-band miniature modulators

Ku-band microminiature modulators were designed to convert a 10 mW signal at 400 MHz to a 10 mW signal at 15 GHz. The designs incorporate gallium arsenide Schottky barrier varactors used in upper-sideband up-converters. The use of Ku-band microstrip circulators and hairpin resonator bandpass filters at 2.1 GHz and 2.5 GHz is included. The design and fabrication of a single up-conversion unit with a double up-conversion unit are compared. Various filter configurations are studies, and the use of both alumina and quartz substrates are considered. The various impedance matching networks are evaluated using computer aided design techniques.

Ernst, R. L.↗

Resonantly two-photon pumped frequency converter

This letter describes a resonantly two-photon pumped frequency converter with application to the generation of tunable ultraviolet and vacuum ultraviolet radiation and also to infrared-to-visible up-conversion and imaging. Calculations show that up-conversion power efficiencies in excess of 100% should be obtained with tunable dye lasers having peak powers in the hundred watt to kilowatt range.

Harris, S. E.↗

Infrared fiber optic focal plane dispersers

Far infrared transmissive fiber optics as a component in the design of integrated far infrared focal plane array utilization is discussed. A tightly packed bundle of fibers is placed at the focal plane, where an array of infrared detectors would normally reside, and then fanned out in two or three dimensions to individual detectors. Subsequently, the detectors are multiplexed by cryogenic electronics for relay of the data. A second possible application is frequency up-conversion (v sub 1 + v sub 2 = v sub 3), which takes advantage of the nonlinear optical index of refraction of certain infrared transmissive materials in fiber form. Again, a fiber bundle is utilized as above, but now a laser of frequency v sub 1 is mixed with the incoming radiation of frequency v sub 1 within the nonlinear fiber material. The sum, v sub 2 is then detected by near infrared or visible detectors which are more sensitive than those available at v sub 2. Due to the geometrical size limitations of detectors such as photomultipliers, the focal plane dispersal technique is advantageous for imaging up-conversion.

Goebel, J. H.↗

Direct Observation of Ultrafast Defect-Bound and Free Exciton Dynamics in Defect-Engineered WS 2 Monolayers

Defects in two-dimensional transition metal dichalcogenides (TMDCs) broadly affect their optical and electronic properties. Directly capturing the ultrafast processes of exciton trapping and defect-bound exciton formation is crucial for understanding and advancing defect-mediated optoelectronics and quantum technologies. However, the weak transient optical absorption of defect-bound excitons has limited their experimental observation to date. Here, we report the direct observation of the ultrafast dynamics of defect-bound excitons in monolayer WS 2 crystals with a high density of monosulfur vacancies (V S ) and W-site defect complexes (S W V S ) resulting from synthesis by alkali metal halide-assisted chemical vapor deposition. The dynamics of excitons bound to these defects, along with their coherent interactions with free excitons, are elucidated using ultrafast optical spectroscopy. Using above band-edge photoexcitation, we find that both free and defect-bound excitons simultaneously form within 300 fs from hot carrier relaxation. The defect-bound excitons exhibit shorter lifetimes than free excitons, leading to a population difference of the corresponding excitonic states and free exciton trapping within a 1–100 ps window. Band-edge photoexcitation of free and defect-bound exciton states reveals ultrafast interconversion within ∼150 fs (comparable to our temporal resolution), indicating possible coherent coupling between these states. We further demonstrate efficient up-conversion of defect-bound excitons to free excitons with photon energies up to ∼300 meV below the free exciton resonance. In conclusion, these findings provide insights into the ultrafast dynamics of defect-bound excitons in TMDCs and their coupling with free excitons, which are relevant to defect-engineered optoelectronic, quantum photonic, and valleytronic applications.

36 MATERIALS SCIENCE↗

Stacked-mosaic amplifier and diode delivery concept for kJ-class inertial fusion energy laser driver

We report on a laser amplifier architecture designed as a modular element for scaling to multi-megajoule laser facilities intended for inertial fusion energy (IFE) power plants. This kilojoule-class module features a stacked mosaic of gain media integrated with a diode delivery system for efficient optical pumping of the mosaic-structured gain medium, enabling high-repetition-rate operation at high wall plug efficiencies, necessary for an IFE driver. Details of a diode delivery system capable of pumping the mosaic architecture are presented. Comprehensive numerical modeling demonstrates that the stacked-mosaic approach reduces transverse gain by five orders of magnitude compared to a conventional full-aperture Yb:YAG based amplifier, substantially suppressing transverse amplified spontaneous emission (TASE) and enabling enhanced longitudinal energy extraction. Detailed analysis of thermal management and wavefront distortion in a 4 × 4 mosaic array indicates that temperature gradients and thermally induced aberrations are effectively controlled using gas cooling and commercially available phase-plate and deformable mirror technologies. We further discuss the applicability of a stacked-mosaic architecture to direct-drive IFE schemes, where broad spectral bandwidth is critical, and its compatibility with frequency conversion modules for up-conversion to blue wavelengths. Finally, an example point design for a 10 kJ, 10 Hz Yb:YAG module operating at 175 K with wall-plug efficiency exceeding 10 % is presented, underscoring the feasibility of this approach for next-generation high-energy lasers for IFE drivers. The results establish the stacked-mosaic amplifier as a scalable, robust platform not only for IFE but also for a broad range of advanced scientific and industrial laser applications.

Lasers↗

Investigation of laser dynamics, modulation and control by means of intra-cavity time varying perturbation

Projects aimed at the generation of tunable visible, infrared, and ultraviolet light, and on the control of this light by means of novel mode-locking and modulation techniques are discussed. During this period the following projects have been active: (1) studies of transient mode-locking of the Nd:YAG laser and the application of short optical pulses; (2) experimental investigations of the Na-Xe excimer laser system; (3) further development of techniques for vacuum ultraviolet holography; and (4) theoretical and initial experimental studies of a new device which should prove very useful for both infrared up-conversion and generation of tunable UV radiation - a two-photon resonantly pumped frequency converter.

Harris, S. E.↗

Effects of focusing on third-order nonlinear processes in isotropic media

Third-order nonlinear processes in isotropic media have been successfully used for tripling the efficiency of high-power laser radiation for the production of tunable and fixed-frequency coherent vacuum UV radiation and for up-conversion of IR radiation. The effects of focusing on two processes of this type are studied theoretically and experimentally.

Bjorklund, G. C.↗

IR pumped third-harmonic generation and sum-frequency generation in diatomic molecules

The potential efficiency of using nonlinear up-conversion techniques for the high efficiency type lasers (CO,CO2, and chemical) is assessed. Results indicate that: the small pump photon energy necessitates the use of molecular media for conversion if resonance enhancement is to be used and that molecular systems present several problems. These difficulties include: their levels are complex; their transition probabilities are often unknown; and the oscillator strengths among vibrational levels in the ground electronic state of a molecule are much smaller than those among electronic states of an atom, thus limiting the magnitude of nonlinear interactions. It is shown that this problem can be eliminated by making use of vibronic transitions which, being primarily electronic transitions have much larger matrix elements and efficient conversion can be achieved with molecular systems.

She, C. Y.↗

The NATO III 5 MHz Distribution System

A high performance 5 MHz distribution system is described which has extremely low phase noise and jitter characteristics and provides multiple buffered outputs. The system is completely redundant with automatic switchover and is self-testing. Since the 5 MHz reference signals distributed by the NATO III distribution system are used for up-conversion and multiplicative functions, a high degree of phase stability and isolation between outputs is necessary. Unique circuit design and packaging concepts insure that the isolation between outputs is sufficient to quarantee a phase perturbation of less than 0.0016 deg when other outputs are open circuited, short circuited or terminated in 50 ohms. Circuit design techniques include high isolation cascode amplifiers. Negative feedback stabilizes system gain and minimizes circuit phase noise contributions. Balanced lines, in lieu of single ended coaxial transmission media, minimize pickup.

Vulcan, A.↗

Nonlinear optical processes for the mid-IR region

The 2 - 5 micron (mid-IR) region is of interest for a number of applications. Efficient up-conversion and down-conversion techniques are being developed to obtain optical sources at mid-IR wavelengths. These techniques are reviewed and recent results using AgGaSe2 are reported. Gain in AgGaSe2 as high as 13 has been observed with a pump wavelength of 1.73 microns and a signal wavelength of 3.39 microns. Optical parametric oscillation in the 2.9 - 6.8 micron region has also been demonstrated.

Schepler, K. L.↗