Excitonic Photoluminescence in Pentacene Single Crystal

Aoki-Matsumoto, Tamao; Furuta, Kenta; Yamada, Toshi; Moriya, H.; Mizuno, Ken-ichi; Matsui, Atsuo

doi:10.1142/9789812811387_0042

Cited by 4 publications

(10 citation statements)

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“…33). The features that we observe are consistent with previously reported emission spectra of pentacene single crystals 49,50 and high-quality 20 nm thin layers 52 , all of which report bands at around 1.85 eV, 1.65 eV, 1.5 eV and 1.35 eV. In Fig.…”

Section: Resultssupporting

confidence: 92%

“…5c), provided that its intensity is partially suppressed, as expected for emission enabled by Herzberg-Teller intensity borrowing. Within this context, intensity borrowing from S 1 , which is expected to become superradiant below ∼ 10 K 11,38,55,56 , may explain the observed temperature dependence of the 0-0 peak 49,52 . The 0-0 energy is slightly below that of two triplets in pentacene 57 (vertical line, Fig.…”

Section: Resultsmentioning

confidence: 96%

“…Having demonstrated that emissive triplet-pairs are populated through bimolecular TTA in a polycrystalline endothermic SF material, we now turn to our highly ordered, exothermic model system: single crystals of pentacene. Previous reports of pentacene photoluminescence are scarce, and the spectral assignments 49,50 were made before the recent boom in singlet fission research. We therefore start by revisiting this literature and find evidence that the observed emission is consistent with 1 (TT).…”

Section: Resultsmentioning

confidence: 99%

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Emissive spin-0 triplet-pairs are a direct product of triplet–triplet annihilation in pentacene single crystals and anthradithiophene films

et al. 2020

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Singlet fission and triplet-triplet annihilation represent two highly promising ways of increasing the efficiency of photovoltaic devices. Both processes are believed to be mediated by a biexcitonic triplet-pair state, 1 (TT). Recently however, controversy has arisen over the role of 1 (TT) in triplet-triplet annihilation.Here we use intensity-dependent, low-temperature photoluminescence measurements, combined with kinetic modelling, to show that distinct 1 (TT) emission arises directly from triplet-triplet annihilation in high-quality pentacene single crystals and anthradithiophene (diF-TES-ADT) thin films. This work demonstrates that a real, emissive triplet-pair state acts as an intermediate in both singlet fission and triplet-triplet annihilation and that this is true for both endo-and exo-thermic singlet fission materials.

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Section: Resultssupporting

confidence: 92%

Section: Resultsmentioning

confidence: 96%

Section: Resultsmentioning

confidence: 99%

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Emissive spin-0 triplet-pairs are a direct product of triplet–triplet annihilation in pentacene single crystals and anthradithiophene films

et al. 2020

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“…Rubrene ( Supplementary Fig. 10 ) likewise shows evidence of a temperature-dependent long-lived PL feature, somewhat obscured by the similarity of the S 1 and 1 (TT) energies; even pentacene has been shown to demonstrate similarly shaped emission in films 51 and crystals 52 . Under Herzberg–Teller coupling the 0–0 peak is suppressed 53 ; thus, we assign the most prominent feature in the 1 (TT) spectrum to the 0–1 peak, akin to emission from the ‘triplet-pair’-like 54 S 1 state in polyenes 55 .…”

Section: Resultsmentioning

confidence: 99%

The entangled triplet pair state in acene and heteroacene materials

et al. 2017

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Entanglement of states is one of the most surprising and counter-intuitive consequences of quantum mechanics, with potent applications in cryptography and computing. In organic materials, one particularly significant manifestation is the spin-entangled triplet-pair state, which mediates the spin-conserving fission of one spin-0 singlet exciton into two spin-1 triplet excitons. Despite long theoretical and experimental exploration, the nature of the triplet-pair state and inter-triplet interactions have proved elusive. Here we use a range of organic semiconductors that undergo singlet exciton fission to reveal the photophysical properties of entangled triplet-pair states. We find that the triplet pair is bound with respect to free triplets with an energy that is largely material independent (∼30 meV). During its lifetime, the component triplets behave cooperatively as a singlet and emit light through a Herzberg–Teller-type mechanism, resulting in vibronically structured photoluminescence. In photovoltaic blends, charge transfer can occur from the bound triplet pairs with >100% photon-to-charge conversion efficiency.

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“…In considering substitution effect in the multi-band system, the Dingle temperature is more informative rather than the dHvA frequencies, since each frequency may vary with keeping the total volume of the FS. Recent experiments have revealed a contrastive behavior depending on direction of the magnetic field: dHvA signals vanish by the substitution on both La and Ce sides for H ⊥ c, while the dHvA amplitude A osc shows a minimum at 0 < x < 1 for H c. 36) Because the magnetization in this system shows a strong Ising anisotropy, we can regard the results for H ⊥ c as low-field region, and the results for H c as high-field region. Then, the tendency is consistent with our results for the Dingle temperature T γ , considering A osc ∝ exp(−T γ ).…”

Section: Summary and Discussionmentioning

confidence: 99%

Effect of Disorder on Fermi Surface in Heavy Electron Systems

2010

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The Kondo lattice model with substitutional disorder is studied with attention to the size of the Fermi surface and the associated Dingle temperature. The model serves for understanding heavy-fermion Ce compounds alloyed with La according to substitution CexLa1−x. The Fermi surface is identified from the steepest change of the momentum distribution of conduction electrons, and is derived at low enough temperature by the dynamical mean-field theory (DMFT) combined with the coherent potential approximation (CPA). The Fermi surface without magnetic field increases in size with decreasing x from x = 1 (Ce end), and disappears at suchx that gives the same number of localized spins as that of conduction electrons. From the opposite limit of x = 0 (La end), the Fermi surface broadens quickly as x increases, but stays at the same position as that of the La end. With increasing magnetic field, a metamagnetic transition occurs, and the Fermi surface above the critical field changes continuously across the whole range of x. The Dingle temperature takes a maximum around x = 0.5. Implication of the results to experimental observation is discussed.

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Excitonic Photoluminescence in Pentacene Single Crystal

Cited by 4 publications

References 0 publications

Emissive spin-0 triplet-pairs are a direct product of triplet–triplet annihilation in pentacene single crystals and anthradithiophene films

Emissive spin-0 triplet-pairs are a direct product of triplet–triplet annihilation in pentacene single crystals and anthradithiophene films

The entangled triplet pair state in acene and heteroacene materials

Effect of Disorder on Fermi Surface in Heavy Electron Systems

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