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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Electron Transfer Going the Distance: Mn-Doped ZnSe as a Model Photocatalytic System

In this work, time-resolved photoluminescence and transient absorption spectroscopy are used to examine the influence that long excited state lifetimes of Mn-doped nanocrystals have on the mechanisms of photo-induced electron transfer (PET) in photocatalytic systems. Mn-doped ZnSe nanocrystals can undergo PET over their nearly millisecond excited state lifetime, which enables electron transfer to viologens in solution over large encounter distances in comparison to molecular length scales. The long excited state lifetimes also enable diffusion of the excited nanocrystals over hundreds of nanometers in solution, allowing them to react with molecular species at nanomolar concentrations. The ability to capture and sustain optical energy in spin-forbidden transitions among crystal field states of the Mn ions opens opportunities to explore the influence that long excited state lifetimes have on photocatalytic reaction mechanisms involving molecular species such as CO 2 that can be difficult to concentrate or attach to nanocrystal surfaces.

14 SOLAR ENERGY↗
DOE OSTI2022

Revisiting the K-edge X-ray absorption fine structure of Si, Ge–Si alloys, and the isoelectronic series: CuBr, ZnSe, GaAs, and Ge

Extended X-ray absorption fine structure (EXAFS) has evolved into an unprecedented local-structure technique that is routinely used to study materials’ problems in the biological, chemical, and physical sciences. Like many other experimental techniques, EXAFS also requires that several key atomic parameters must be known a priori before structural information can be quantitatively determined. Utilizing current analytical methods, we revisit the isoelectronic series CuBr, ZnSe, GaAs, and Ge originally studied by Stern et al. during the early development of EXAFS. We demonstrate that the ab initio EXAFS code FEFF accurately predicts the atomic phase shifts and backscattering amplitudes that are primarily functions of the sum of atomic numbers Z along an EXAFS scattering path. We also investigate quantitative fitting and first- and second-shell phase transferability together with problems that arise if a backscattering atom is identified incorrectly in an EXAFS fitting model. Features in the near-edge region, on the other hand, are shown to require a comprehensive treatment of the band structure and density-of-states, including effects of the screened Coulomb interaction between the photoelectron and core hole. Here, we demonstrate that the Bethe–Salpeter equation (BSE) accurately captures the NEXAFS (or XANES) portion of the spectrum for the isoelectronic series in addition to Si and Ge–Si alloys, including within a few eV of the absorption edge, where band structure and excitonic effects are most important.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

High-order ( N = 4–6) multiphoton absorption and mid-infrared Kerr nonlinearity in GaP, ZnSe, GaSe, and ZGP crystals

We report a study of high-order multiphoton absorption, nonlinear refraction, and their anisotropy in four notable mid-infrared χ (2) crystals: GaP, ZnSe, GaSe, and ZGP using femtosecond pulses at 2.35 μm with peak intensity in excess of 200 GW/cm 2 . We found that the nonlinear absorption obeys a perturbation model with multiphoton absorption (MPA) orders from N = 4–6, in agreement with the bandgaps of the crystals. A study of the role of free carrier absorption, performed by changing the pulse duration from 30 to 70 fs while maintaining a constant peak intensity, showed that, at our intensity levels, free carriers generated during the MPA process absorb much more strongly than would be expected from their known linear absorption cross section. Possible mechanisms for this anomalous behavior are high-field effects, such as intravalley scattering in the conduction band and absorption to higher lying bands. Nonlinear refractive indices were measured using (i) closed aperture Z-scan and (ii) spectral broadening due to self-phase modulation, both methods agreeing with each other.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Kinetics of the luminescence decay of Fe{sup 2+} impurity centres in polycrystalline ZnSe upon excitation by an electron beam

The kinetics of the decay of the luminescence of Fe{sup 2+} ions is measured at nitrogen temperature in polycrystalline ZnSe excited by a short pulse of accelerated electrons. The time dependence of the luminescence intensity differs from the exponential one, observed upon excitation of luminescence by a short light pulse. The obtained nonexponential dependence is theoretically described. The explanation is based on the quenching effect of the excited state of the Fe{sup 2+} ion by free electrons of the volume charge of the current of accelerated electrons in the sample (Auger effect). It was shown that the relaxation of the volume charge after the electron-accelerating voltage is removed makes a significant contribution to the decay kinetics of the impurity luminescence. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Single quantum emitters with spin ground states based on Cl bound excitons in ZnSe

Defects in wide-band-gap semiconductors are promising qubit candidates for quantum communication and computation. Epitaxially grown II-VI semiconductors are particularly promising host materials due to their direct band gap and potential for isotopic purification to a spin-zero nuclear background. Here, we show an alternative type of single photon emitter with potential electron spin qubits based on Cl impurities in ZnSe. We utilize a quantum well to increase the binding energies of donor emission and confirm single photon emission with short radiative lifetimes of 192 ps. Furthermore, we verify that the ground state of the Cl donor complex contains a single electron by observing two-electron-satellite emission, leaving the electron in higher orbital states. We also characterize the Zeeman splitting of the exciton transition by performing polarization-resolved magnetic spectroscopy on single emitters. Our results suggest single Cl impurities are suitable as a single photon source with a potential photonic interface.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Lattice vibrations and energy landscape of the isoelectronic semiconductor series CuBr, ZnSe, GaAs, and Ge: The special case of CuBr and its $\mathcal{d}$-level chemistry

Here we have examined the lattice vibrations and the energy landscape of the isoelectronic diamond and zincblende semiconductor series CuBr, ZnSe, GaAs, and Ge. Vibrations are found to be an increasing function of ionicity, with the cation sublattice always vibrating more strongly than the anion sublattice. These findings are consistent with density functional theory (DFT) calculations of the energy landscape and temperature-dependent molecular dynamics simulations of the atomic-position fluctuations. For CuBr, inclusion of the Cu 3d Hubbard U term is found necessary to stabilize the zincblende structure and to bring its vibrational amplitudes into agreement with experiment. In addition, vibrations are found to strongly affect the CuBr near-edge x-ray absorption fine structure that we have successfully modeled by including displacements in our theoretical Bethe-Salpeter equation calculations. Reverse Monte Carlo structural refinements using large atomic configurations to simultaneously fit x-ray absorption and x-ray total-scattering data support these conclusions, and they reveal strong Cu-Br first-neighbor correlations and asymmetric distributions of interatomic distances in the temperature ranges of both negative and positive thermal expansion. Delineation of the CuBr valence band photoelectron spectrum into its Cu 3d and Br 4p states uniquely reveals their covalent mixing and further supports the DFT results.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Sequential multidimensional heteroepitaxy of chalcogen-sharing 3D ZnSe and 2D MoSe 2 with quasi van der Waals interface engineering

Two-dimensional (2D) materials are emerging as a promising platform for epitaxial growth, largely free from the constraints of lattice constant and thermal expansion coefficient mismatches. Among them, transition metal dichalcogenides (TMDs), known for their superior electrical properties, are ideal for ultrathin semiconductor applications. Their unique epitaxial characteristics enable seamless integration with 3D materials, facilitating the development of gate stacks and heterojunction devices. In this regard, developing a process for growing high-quality 3D epitaxial materials before and after the growth of 2D TMDs and understanding the 2D/3D interface are crucial. This study demonstrates the sequential growth of fully epitaxial ZnSe/MoSe 2 /ZnSe heterostructures using metal-organic chemical vapor deposition. ZnSe and MoSe 2 , sharing chalcogen elements, enable large-area quasi van der Waals epitaxy with sharp interfaces without intermediate phase. Multiscale analysis involving transmission electron microscopy and density functional theory calculation reveals lattice commensurability, van der Waals gaps, termination, and interfacial reconstruction. Understanding these interactions is crucial for advancing multidimensional integration of 2D and 3D materials.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Room temperature, nanosecond, 60 mJ/pulse Fe:ZnSe master oscillator power amplifier system operating at 3.8-5.0 µm

We report on a RT gain-switched Fe:ZnSe master oscillator power amplifier (MOPA) system tunable over 3.8–5.0 µm pumped by radiation of Er:YAG laser operating at 2.94 µm. The mechanically Q-switched Er:YAG laser with output energy up to 220 mJ was used as a pump source for a master oscillator and three-stage power amplifier. The maximum output energies in 200 ns pulses exceeded 60, 56, and 48 mJ at 4.4, 4.3, and 4.1 µm, respectively, under 220 mJ of pump energy. The extraction energy efficiencies were measured to be 25, 30, and 40% at the first, second, and third stages, respectively.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Lasing in 15 atm CO 2 cell optically pumped by a Fe:ZnSe laser

10 µm lasing is studied in a compact CO 2 -He cell pressurized up to 15 atm when optically pumped by a ∼50 mJ Fe:ZnSe laser tunable around 4.3 µm. The optimal pump wavelength and partial pressure of CO 2 for generating 10 µm pulses are found to be ∼4.4 µm and 0.75 atm, respectively. Without cavity optimization, the optical-to-optical conversion efficiency reached ∼10% at a total pressure of 7 atm. The gain lifetime is measured to be ∼1 µs at pressures above 10 atm, indicating the feasibility of using high-pressure optically pumped CO 2 for the efficient amplification of picosecond 10 µm pulses.

Tovey, Dana↗
DOE OSTI2020

Cross-section of electrical impact excitation in bulk n-type monocrystalline Al:Cr:ZnSe

Middle-infrared luminescence of bulk Al:Cr:ZnSe crystal under direct electrical excitation of Cr 2+ , 5 E− 5 T 2 transition, is reported. Effective cross-section of electrical excitation was estimated based on comparative luminescence measurements under electrical and optical (1560 nm) excitations. Calculation of the threshold current density for lasing under electrical excitation of this material was also performed.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Hot-pressed ceramic Fe:ZnSe gain-switched laser

We report the first room temperature gain-switched Fe:ZnSe hot-pressed ceramic laser pumped by 2.94 µm radiation of mechanically Q-switched Er:YAG laser. The maximum output energy at 4.2 µm was 41 mJ at 3 Hz repetition rate and 120 ns pulse duration. The measured slope efficiency was 25% with respect to the absorbed energy. This technique could be attractive for the future development of high-energy short-pulse solid-state mid-IR systems.

36 MATERIALS SCIENCE↗
NASA NTRS1974

Ion implanted epitaxially grown ZnSe

The epitaxial growth of ZnSe on (100) Ge using the close-spaced transport process is described. Substrate temperature of 575 C and source temperatures of 675 C yield 10 micron, single crystal layers in 10 hours. The Ge substrates provides a nonreplenishable chemical transport agent and the epitaxial layer thickness is limited to approximately 10 microns. Grown epitaxial layers show excellent photoluminescence structure at 77 K. Grown layers exhibit high resistivity, and annealing in Zn vapor at 575 C reduces the resistivity to 10-100 ohms-cm. Zinc vapor annealing quenches the visible photoluminescence.

Source record↗
NASA NTRS1971

Laser modulation of optical absorption in ZnSe

The possibility of producing and detecting laser induced modulation of absorption (LIMA) in ZnSe crystals using a moderate laser intensity of about 6 mw output was investigated. The modulation is smaller than that previously obtained with higher laser photon flux, but is not too difficult to detect. Modulation of the order of a few parts in 10 to the 5th power, up to one part in 10 to the 4th power appears typical at the present. LIMA pulse shapes were recorded with varying system resolutions at a half dozen wavelengths in the visible, from 4800 A to 6000 A. Detailed data were taken, particularly at 5000 A, for a range of time intervals following laser pulse turn-on. Quantitative study of the excitation and decay kinetics of these is underway, though analysis is not complete. Major features are discussed with attention centered upon the detailed measurements made most recently at 5000 A.

Major, R. W.↗
NASA NTRS1987

Preliminary results on CuInSe2/ZnSe solar cells using reactively sputter-deposited ZnSe

In this paper preliminary results on CuInSe2/ZnSe thin film heterojunction photovoltaic devices are presented. High-conductivity ZnSe films were reactively sutter-deposited onto CuInSe2 films and overcoated with ZnO to reduce the sheet resistance. The highest short-circuit current density, as determined from a spectral response weighted for air mass 1.5 global insolation, was 37.4 mA/sq cm. The highest pen-circuit voltage observed was 430 mV.

Nouhi, A.↗
NASA NTRS1989

The growth of ZnSe single crystals by physical vapor transport

ZnSe single crystals have been grown in sealed quartz ampoules by the physical vapor transport method. Complete transport of the starting material and single site growth have been achieved with no material adhering to the ampoule wall. Growth is initiated in a narrow channel in the cold finger attached to the growth end of the ampoule. The highest growth rate to date has been 280 mg/day which corresponds to an average transport rate of about 1.93 mmol/day. The largest single crystal, measuring 1 cm x 4 mm x 2 mm, had a total growing time of 11 days or an average growth rate of 171 mg/day.

Cheng, Hai-Yuin↗