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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Using genetic algorithms to discover novel ground-state triplet conjugated polymers

Stable ground-state triplet π-conjugated copolymers have many interesting electronic and optoelectronic properties. However, the large number of potential monomer combinations makes it impractical to synthesize or even just use density functional theory (DFT) to calculate their triplet ground-state stability. Furthermore, we present a genetic algorithm implementation that uses the semi-empirical GFN2-xTB to find ground-state triplet polymer candidates. We find more than 1400 polymer candidates with a triplet ground-state stability of up to 4 eV versus the singlet. Additionally, we explore the properties of the monomers of those candidates in order to understand the design rules which promote the formation of a stable ground-state triplet in π-conjugated polymers.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Diphotons from electroweak triplet-singlet mixing

The neutral component of a real pseudoscalar electroweak (EW) triplet can produce a diphoton excess at 750 GeV, if it is somewhat mixed with an EW singlet pseudoscalar. This triplet-singlet mixing allows for greater freedom in the diboson branching ratios than the singlet-only case, but it is still possible to probe the parameter space extensively with 300 fb -1 . The charged component of the triplet is pair produced at the LHC, which results in a striking signal in the form of a pair of Wγ resonances with an irreducible rate of 0.27 fb. Other signatures include multiboson final states from cascade decays of the triplet-singlet neutral states. In conclusion, a large class of composite models feature both EW singlet and triplet pseudo-Nambu-Goldstone bosons in their spectrum, with the diboson couplings generated by axial anomalies.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2016

Long-lived two-dimensional triplet magnetoexcitons in a Hall insulator

An experimental technique is developed to perform photoexcitation of an ensemble of translationinvariant triplet excitons, to manipulate this ensemble, and to detect the properties of its components. In particular, the influence of temperature on the radiationless decay during the relaxation of an exciton spin into the ground state of a Hall insulator at a filling factor ν = 2 is studied. The generation of photoexcited electrons and holes is controlled using photoinduced resonance reflection spectra, which makes it possible to estimate the density of light-generated electron–hole pairs and to independently control the self-consistent generation of electrons at the first Landau level and holes (vacancies) at the ground (zero) cyclotron electronic level. The existence of triplet excitons is established from inelastic light scattering spectra, which are used to determine the singlet–triplet exciton splitting. The lifetimes of triplet excitons, which are closely related to the relaxation time of an electron spin, are extremely long: they reach 100 μs in perfect GaAs/AlGaAs heterostructures with a high mobility of two-dimensional electrons at low temperatures. These long spin relaxation times are qualitatively explained, and the expected collective behavior of high-density triplet magnetoexcitons at sufficiently low temperatures, which is related to their Bose nature, is discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Primary donor triplet states of Photosystem I and II studied by Q-band pulse ENDOR spectroscopy

The photoexcited triplet state of the “primary donors” in the two photosystems of oxygenic photosynthesis has been investigated by means of electron-nuclear double resonance (ENDOR) at Q-band (34 GHz). The data obtained represent the first set of 1 H hyperfine coupling tensors of the 3 P700 triplet state in PSI and expand the existing data set for 3 P680. We achieved an extensive assignment of the observed electron-nuclear hyperfine coupling constants (hfcs) corresponding to the methine α-protons and the methyl group β-protons of the chlorophyll (Chl) macrocycle. The data clearly confirm that in both photosystems the primary donor triplet is located on one specific monomeric Chl at cryogenic temperature. In comparison to previous transient ENDOR and pulse ENDOR experiments at standard X-band (9–10 GHz), the pulse Q-band ENDOR spectra demonstrate both improved signal-to-noise ratio and increased resolution. The observed ENDOR spectra for 3 P700 and 3 P680 differ in terms of the intensity loss of lines from specific methyl group protons, which is explained by hindered methyl group rotation produced by binding site effects. Contact analysis of the methyl groups in the PSI crystal structure in combination with the ENDOR analysis of 3 P700 suggests that the triplet is located on the Chl a' (P A ) in PSI. The results also provide additional evidence for the localization of 3 P680 on the accessory Chl D1 in PSII.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2024

Triplet Exciton Sensitization of Silicon Mediated by Defect States in Hafnium Oxynitride

Singlet exciton fission has the potential to increase the efficiency of crystalline silicon solar cells beyond the conventional single junction limit. Perhaps the largest obstacle to achieving this enhancement is uncertainty about energy coupling mechanisms at the interfaces between silicon and exciton fission materials such as tetracene. Here, the previously reported silicon‐hafnium oxynitride‐tetracene structure is studied and a combination of magnetic‐field‐dependent silicon photoluminescence measurements and density functional theory calculations is used to probe the influence of the interlayer composition on the triplet transfer process across the hafnium oxynitride interlayer. It is found that hafnium oxide interlayers do not show triplet exciton sensitization of silicon, and that nitrogen content in hafnium oxynitride layers is correlated with enhanced sensitization. Calculation results reveal that defects in hafnium oxynitride interlayers with higher nitrogen content introduce states close to the band‐edge of silicon, which can mediate the triplet exciton transfer process. Some defects introduce additional deleterious mid‐gap states, which may explain observed silicon photoluminescence quenching. These results show that band‐edge states can mediate the triplet exciton transfer process, potentially through a sequential charge transfer mechanism.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Lattice Symmetry-Guided Charge Transport in 2D Supramolecular Polymers Promotes Triplet Formation

Singlet-to-triplet intersystem crossing (ISC) in organic molecules is intimately connected with their geometries: by modifying the molecular shape, symmetry selection rules pertaining to spin-orbit coupling can be partially relieved, leading to extra matrix elements for increased ISC. As an analog to this molecular design concept, the study finds that the lattice symmetry of supramolecular polymers also defines their triplet formation efficiencies. A supramolecular polymer self-assembled from weakly interacting molecules is considered. Its 2D oblique unit cell effectively renders it as a coplanar array of 1D molecular columns weakly bound to each other. Using momentum-resolved photoluminescence imaging in combination with Monte Carlo simulations, the study found that photogenerated charge carriers in the supramolecular polymer predominantly recombine as spin-uncorrelated carrier pairs through inter-column charge transfer states. This lattice-defined recombination pathway leads to a substantial triplet formation efficiency (≈60%) in the supramolecular polymer. These findings suggest that lattice symmetry of micro-/macroscopic structures relying on intermolecular interactions can be strategized for controlled triplet formation.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Back in bismuth: controlling triplet energy transfer, phosphorescence, and radioluminescence via supramolecular interactions

Five bismuth(III)-organic phases that consist of supramolecular assemblies of Bi-2,6-pyridinedicarboxylate structural units and substituted 1,10-phenanthroline molecules (R-Phen; R = H, 5-methyl, 5-chloro, 2,9-dimethyl, and 2,9-dicholoro) were synthesized. All five compounds exhibited solid-state photoluminescence. Whereas the phases containing 2,9-dimethylphenanthroline (Me 2 Phen) and 2,9-dichlorophenanthroline (Cl 2 Phen) displayed solely phosphorescence, the structures built from 5-methylphenanthroline and 5-chlorophenanthroline showed exclusively fluorescence. The remaining phase, consisting of phenanthrolinium, exhibited both fluorescence and phosphoresence. It was determined that phosphorescence arises from triplet state emission (T 1 → S 0 ) of substituted R-Phen units while fluorescence originates from Bi(III) coordinated pyrdinedicarboxylate ligands. Bismuth induces spin–orbit coupling for triplet state population and additionally acts as a heavy metal attenuator for X-ray luminescence (radioluminescence). The electronic structure was mapped and excitation pathway investigated via density functional theory calculations. Computational findings indicate favorable conditions for triplet energy transfer from donor Bi(III)-organic units to acceptor R-Phen derivatives. It is proposed that for the phosphorescent compounds, strong π–π interactions promote electron transfer, whereas the compounds that exhibit purely fluorescence lack any such π–π interactions and undergo triplet energy transfer. In conclusion, these results provide a useful platform for probing structure–property relationships of luminescent bismuth-organic compounds, and specifically highlights the role of noncovalent interactions in achieving room temperature phosphorescence and radioluminescence.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

An ab initio investigation of the ground and low-lying singlet and triplet electronic states of XNO{sub 2} and XONO (X = Cl, Br, and I)

A systematic ab initio treatment of the nitryl halides (XNO{sub 2}) and the cis- and trans- conformers of the halide nitrites (XONO), where X = Cl, Br, and I, have been carried out using highly correlated methods with sequences of correlation consistent basis sets. Equilibrium geometries and harmonic frequencies have been accurately calculated in all cases at the explicitly correlated CCSD(T)-F12b level of theory, including the effects of core-valence correlation for the former. Where experimental values are available for the equilibrium structures (ClNO{sub 2} and BrNO{sub 2}), the present calculations are in excellent agreement; however, the X-O distances are slightly too long by about 0.01 Å due to missing multireference effects. Accurate predictions for the iodine species are made for the first time. The vertical electronic excitation spectra have been calculated using equation-of-motion coupled cluster methods for the low-lying singlet states and multireference configuration interaction for both singlet and triplet states. The latter also included the effects of spin-orbit coupling to provide oscillator strengths for the ground state singlet to excited triplet transitions. While for ClNO{sub 2} the transitions to excited singlet states all occur at wavelengths shorter than 310 nm, there is one longer wavelength singlet transition in BrNO{sub 2} and two in the case of INO{sub 2}. The long wavelength tail in the XNO{sub 2} species is predicted to be dominated by transitions to triplet states. In addition to red-shifting from X = Cl to I, the triplet transitions also increase in oscillator strength, becoming comparable to many of the singlet transitions in the case of INO{sub 2}. Hence in particular, the latter species should be very photolabile. Similar trends are observed and reported for the halogen nitrites, many of which for the first time.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2014

Ground state of naphthyl cation: Singlet or triplet?

We present a benchmark theoretical investigation on the electronic structure and singlet-triplet(S-T) gap of 1- and 2-naphthyl cations using the CCSD(T) method. Our calculations reveal that the ground states of both the naphthyl cations are singlet, contrary to the results obtained by DFT/B3LYP calculations reported in previous theoretical studies. However, the triplet states obtained in the two structural isomers of naphthyl cation are completely different. The triplet state in 1-naphthyl cation is (π,σ) type, whereas in 2-naphthyl cation it is (σ,σ{sup ′}) type. The S-T gaps in naphthyl cations and the relative stability ordering of the singlet and the triplet states are highly sensitive to the basis-set quality as well as level of correlation, and demand for inclusion of perturbative triples in the coupled-cluster ansatz.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Exchange interaction between the triplet exciton and the localized spin in copper-phthalocyanine

Triplet excitonic state in the organic molecule may arise from a singlet excitation and the following inter-system crossing. Especially for a spin-bearing molecule, an exchange interaction between the triplet exciton and the original spin on the molecule can be expected. In this paper, such exchange interaction in copper-phthalocyanine (CuPc, spin-1/2 ) was investigated from first-principles by using density-functional theory within a variety of approximations to the exchange correlation, ranging from local-density approximation to long-range corrected hybrid-exchange functional. The magnitude of the computed exchange interaction is in the order of meV with the minimum value (1.5 meV, ferromagnetic) given by the long-range corrected hybrid-exchange functional CAM-B3LYP. This exchange interaction can therefore give rise to a spin coherence with an oscillation period in the order of picoseconds, which is much shorter than the triplet lifetime in CuPc (typically tens of nanoseconds). This implies that it might be possible to manipulate the localized spin on Cu experimentally using optical excitation and inter-system crossing well before the triplet state disappears.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Simultaneous monitoring of singlet and triplet exciton variations in solid organic semiconductors driven by an external static magnetic field

The research field of organic spintronics has remarkably and rapidly become a promising research area for delivering a range of high-performance devices, such as magnetic-field sensors, spin valves, and magnetically modulated organic light emitting devices (OLEDs). Plenty of microscopic physical and chemical models based on exciton or charge interactions have been proposed to explain organic magneto-optoelectronic phenomena. However, the simultaneous observation of singlet- and triplet-exciton variations in an external magnetic field is still unfeasible, preventing a thorough theoretical description of the spin dynamics in organic semiconductors. Here, we show that we can simultaneously observe variations of singlet excitons and triplet excitons in an external magnetic field, by designing an OLED structure employing a singlet-exciton filtering and detection layer in conjunction with a separate triplet-exciton detection layer. This OLED structure enables the observation of a Lorentzian and a non-Lorentzian line-shape magnetoresponse for singlet excitons and triplet excitons, respectively.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Theory of triplet optical absorption in oligoacenes: From naphthalene to heptacene

In this paper, we present a detailed theory of the triplet states of oligoacenes containing up to seven rings, i.e., starting from naphthalene all the way up to heptacene. In particular, we present results on the optical absorption from the first triplet excited state 1{sup 3}B{sub 2u}{sup +} of these oligomers, computed using the Pariser-Parr-Pople model Hamiltonian, and a correlated electron approach employing the configuration-interaction methodology at various levels. Excitation energies of various triplets states obtained by our calculations are in good agreement with the experimental results, where available. The computed triplet spectra of oligoacenes exhibits rich structure dominated by two absorption peaks of high intensities, which are well separated in energy, and are caused by photons polarized along the conjugation direction. This prediction of ours can be tested in future experiments performed on oriented samples of oligoacenes.

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

Signatures of superconducting triplet pairing in Ni–Ga-bilayer junctions

Ni–Ga bilayers are a versatile platform for exploring the competition between strongly antagonistic ferromagnetic and superconducting phases. We characterize the impact of this competition on the transport properties of highly-ballistic Al/Al 2 O 3 (/EuS)/Ni–Ga tunnel junctions from both experimental and theoretical points of view. While the conductance spectra of junctions comprising Ni (3 nm)–Ga (60 nm) bilayers can be well understood within the framework of earlier results, which associate the emerging main conductance maxima with the junction films’ superconducting gaps, thinner Ni (1.6 nm)–Ga (30 nm) bilayers entail completely different physics, and give rise to novel large-bias (when compared to the superconducting gap of the thin Al film as a reference) conductance-peak subseries that we term conductance shoulders. These conductance shoulders might attract considerable attention also in similar magnetic superconducting bilayer junctions, as we predict them to offer an experimentally well-accessible transport signature of superconducting triplet pairings that are induced around the interface of the Ni–Ga bilayer. We further substantiate this claim performing complementary polarized neutron reflectometry measurements on the bilayers, from which we deduce (1) a nonuniform magnetization structure in Ga in a several nanometer-thick area around the Ni–Ga boundary and can simultaneously (2) satisfactorily fit the obtained data only considering the paramagnetic Meissner response scenario. While the latter provides independent experimental evidence of induced triplet superconductivity inside the Ni–Ga bilayer, the former might serve as the first experimental hint of its potential microscopic physical origin. Finally, we introduce a simple phenomenological toy model to confirm also from the theoretical standpoint that superconducting triplet pairings around the Ni–Ga interface can indeed lead to the experimentally observed conductance shoulders, which convinces that our claims are robust and physically justified. Arranging our work in a broader context, we expect that Ni–Ga-bilayer junctions could have a strong potential for future superconducting-spintronics applications whenever an efficient engineering of triplet-pairing superconductivity is required.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Theory of the Little-Parks effect in spin-triplet superconductors

The celebrated Little-Parks effect in mesoscopic superconducting rings has recently gained great attention due to its potential to probe half-quantum vortices in spin-triplet superconductors. However, despite the large number of works reporting anomalous Little-Parks measurements attributed to unconventional superconductivity, the general signatures of spin-triplet pairing in the Little-Parks effect have been less systematically investigated. Here we use Ginzburg-Landau theory to study the Little-Parks effect in a spin-triplet superconducting ring that supports half-quantum vortices; we calculate the field-induced Little-Parks oscillations of both the critical temperature itself and the residual resistance resulting from thermal vortex tunneling below the critical temperature. Here we observe two separate critical temperatures with a single-spin superconducting state in between and find that due to the existence of half-quantum vortices, each minimum in the upper critical temperature splits into two minima for the lower critical temperature. From a rigorous calculation of the residual resistance, we confirm that these two minima in the lower critical temperature translate into two maxima in the residual resistance below and establish the general conditions under which the two maxima can be practically resolved. In particular, we identify a fundamental trade-off between sharpening each maximum and keeping the overall magnitude of the resistance large. Our results will guide experimental efforts in designing mesoscopic ring geometries for probing half-quantum vortices in spin-triplet candidate materials on the device scale.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2011

Left-right symmetric model with SU(2)-triplet fermions

We consider an SU(3){sub c} x SU(2){sub L} x SU(2){sub R} x U(1){sub B-L} left-right symmetric model with three Higgs scalars including an SU(2){sub L} doublet, an SU(2){sub R} doublet and an SU(2){sub L} x SU(2){sub R} bidoublet. In addition to usual SU(2)-doublet fermions, our model contains SU(2)-triplet fermions with Majorana masses. The neutral components of the left-handed triplets can contribute a canonical seesaw while the neutral components of the right-handed triplets associated with the right-handed neutrinos can contribute a double/inverse-type seesaw. Our model can be embedded into an SO(10) grand unification theory where the triplets belong to the 45=(1,3,1,0)+(1,1,3,0)+... representations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2012

Field Tolerances for the Triplet Quadrupoles of the LHC High Luminosity Lattice

It has been proposed to implement the so-called Achromatic Telescopic Squeezing (ATS) scheme in the LHC high luminosity (HL) lattice to reduce beta functions at the Interaction Points (IP) up to a factor of 8. As a result, the nominal 4.5 km peak beta functions reached in the Inner Triplets (IT) at collision will be increased by the same factor. This, therefore, justifies the installation of new, larger aperture, superconducting IT quadrupoles. The higher beta functions will enhance the effects of the triplet quadrupole field errors leading to smaller beam dynamic aperture (DA). To maintain the acceptable DA, the effects of the triplet field errors must be re-evaluated, thus specifying new tolerances. Such a study has been performed for the so-called '4444' collision option of the HL-LHC layout version SLHCV3.01, where the IP beta functions are reduced by a factor of 4 in both planes with respect to a pre-squeezed value of 60 cm at two collision points. The dynamic aperture calculations were performed using SixTrack. The impact on the triplet field quality is presented.

43 PARTICLE ACCELERATORS↗
DOE OSTI2017

Triplet Harvesting from Intramolecular Singlet Fission in Polytetracene

Abstract Singlet fission (SF), a promising mechanism of multiple exciton generation, has only recently been engineered as a fast, efficient, intramolecular process (iSF). The challenge now lies in designing and optimizing iSF materials that can be practically applied in high‐performance optoelectronic devices. However, most of the reported iSF systems, such as those based on donor–acceptor polymers or pentacene, have low triplet energies, which limits their applications. Tetracene‐based materials can overcome significant challenges, as the tetracene triplet state is practically useful, ≈1.2 eV. Here, the synthesis and excited state dynamics of a conjugated tetracene homopolymer are studied. This polymer undergoes ultrafast iSF in solution, generating high‐energy triplets on a sub‐picosecond time scale. Magnetic‐field‐dependent photocurrent measurements of polytetracene‐based devices demonstrate the first example of iSF‐generated triplet extraction in devices, exhibiting the potential of iSF materials for use in next‐generation devices.

Pun, Andrew B.↗
DOE OSTI2017

Gas‐Phase Synthesis of the Elusive Cyclooctatetraenyl Radical (C 8 H 7 ) via Triplet Aromatic Cyclooctatetraene (C 8 H 8 ) and Non‐Aromatic Cyclooctatriene (C 8 H 8 ) Intermediates

Abstract The 1,2,4,7‐cyclooctatetraenyl radical (C 8 H 7 ) has been synthesized for the very first time via the bimolecular gas‐phase reaction of ground‐state carbon atoms with 1,3,5‐cycloheptatriene (C 7 H 8 ) on the triplet surface under single‐collision conditions. The barrier‐less route to the cyclic 1,2,4,7‐cyclooctatetraenyl radical accesses exotic reaction intermediates on the triplet surface, which cannot be synthesized via classical organic chemistry methods: the triplet non‐aromatic 2,4,6‐cyclooctatriene (C 8 H 8 ) and the triplet aromatic 1,3,5,7‐cyclooctatetraene (C 8 H 8 ). Our approach provides a clean gas‐phase synthesis of this hitherto elusive cyclic radical species 1,2,4,7‐cyclooctatetraenyl via a single‐collision event and opens up a versatile, unconventional path to access this previously largely obscure class of cyclooctatetraenyl radicals, which have been impossible to access through classical synthetic methods.

Lucas, Michael↗