Exciton

About: Exciton is a research topic. Over the lifetime, 31603 publications have been published within this topic receiving 810642 citations.

A transferable model for singlet-fission kinetics

Abstract: Exciton fission is a process that occurs in certain organic materials whereby one singlet exciton splits into two independent triplets. In photovoltaic devices these two triplet excitons can each generate an electron, producing quantum yields per photon of >100% and potentially enabling single-junction power efficiencies above 40%. Here, we measure fission dynamics using ultrafast photoinduced absorption and present a first-principles expression that successfully reproduces the fission rate in materials with vastly different structures. Fission is non-adiabatic and Marcus-like in weakly interacting systems, becoming adiabatic and coupling-independent at larger interaction strengths. In neat films, we demonstrate fission yields near unity even when monomers are separated by >5 A. For efficient solar cells, however, we show that fission must outcompete charge generation from the singlet exciton. This work lays the foundation for tailoring molecular properties like solubility and energy level alignment while maintaining the high fission yield required for photovoltaic applications.

Exciton radiative lifetime in transition metal dichalcogenide monolayers

Abstract: We have investigated the exciton dynamics in transition metal dichalcogenide monolayers using time-resolved photoluminescence experiments performed with optimized time resolution. For MoS e2 monolayer, we measureτ 0 rad = 1.8 ± 0.2 ps at T = 7 K that we interpret as the intrinsic radiative recombination time. Similar values are found for WSe2 monolayers. Our detailed analysis suggests the following scenario: at low temperature( T ≲ 50 K ), the exciton oscillator strength is so large that the entire light can be emitted before the time required for the establishment of a thermalized exciton distribution. For higher lattice temperatures, the photoluminescence dynamics is characterized by two regimes with very different characteristic times. First the photoluminescence intensity drops drastically with a decay time in the range of the picosecond driven by the escape of excitons from the radiative window due to exciton-phonon interactions. Following this first nonthermal regime, a thermalized exciton population is established gradually yielding longer photoluminescence decay times in the nanosecond range. Both the exciton effective radiative recombination and nonradiative recombination channels including exciton-exciton annihilation control the latter. Finally the temperature dependence of the measured exciton and trion dynamics indicates that the two populations are not in thermodynamical equilibrium.

Exciton regeneration at polymeric semiconductor heterojunctions.

Abstract: Control of the band-edge offsets at heterojunctions between organic semiconductors allows efficient operation of either photovoltaic or light-emitting diodes. We investigate systems where the exciton is marginally stable against charge separation and show via E-field-dependent time-resolved photoluminescence spectroscopy that excitons that have undergone charge separation at a heterojunction can be efficiently regenerated. This is because the charge transfer produces a geminate electron-hole pair (separation 2.2 –3.1 nm) which may collapse into an exciplex and then endothermically (EA � 100–200 meV) back transfer towards the exciton. DOI: 10.1103/PhysRevLett.92.247402

Ultrafast Dynamics of Exciton Fission in Polycrystalline Pentacene

Abstract: We use ultrafast transient absorption spectroscopy with sub-20 fs time resolution and broad spectral coverage to directly probe the process of exciton fission in polycrystalline thin films of pentacene. We observe that the overwhelming majority of initially photogenerated singlet excitons evolve into triplet excitons on an ∼80 fs time scale independent of the excitation wavelength. This implies that exciton fission occurs at a rate comparable to phonon-mediated exciton localization processes and may proceed directly from the initial, delocalized, state. The singlet population is identified due to the brief presence of stimulated emission, which is emitted at wavelengths which vary with the photon energy of the excitation pulse, a violation of Kasha’s Rule that confirms that the lowest-lying singlet state is extremely short-lived. This direct demonstration that triplet generation is both rapid and efficient establishes multiple exciton generation by exciton fission as an attractive route to increased effic...

Exciton binding energies in organic semiconductors

Abstract: The exciton binding energy is one of the key parameters that govern the physics of many opto-electronic organic devices. It is shown that the previously reported values for the exciton binding energies in many organic semiconductors, which differ by more than an order of magnitude, can be consistently rationalized within the framework of the charging energy of the molecular units, with a simple dependence of the exciton binding energy on the length of these units. The implications of this result are discussed.