Non-radiative annihilation of singlet excitons on triplet excitons in organic molecular crystals

The per sec propability is calculated of the non-radiative annihilation of singlet excitons on triplet excitons in organic molecular cyrstals. The influence of the non-radiative annihilation of singlet excitons on triplet excitons on the quenching of crystal fluorescence caused by the radiative annihilation of singlet excitons is studied theoretically on the basis of formulae derived.Na Slovance 2, Praha 8, Czechoslovakia.     

Superliquid state of small-radius excitons in molecular crystals

The energy spectrum of non-ideal bosean gas of small-radius excitons in superliquid state in molecular crystals is theoretically investigated within the scope of Bogoljubov's theory. The conditions for the possibility of existence of the superliquid state are discussed. The critical temperature of the transition of the ideal bosean gas of the excitons to the condensed state are estimated.     

Non-conservation of excitons in finite molecular chain

We have analyzed a linear molecular chain with exciton excitations when the number of excitons is not conserved. The dispersion law depends on two independent variables and it is surfaced in a 3D plot. The same conclusion is valid for the concentrations of excitons and exciton pairs. As it was expected, physical characteristics of the finite chain depend on spatial coordinates. All results are compared to the corresponding results of an infinite chain.     

Optical absorption of triplet molecular excitons in alkali cyanides

The optical absorption spectra of alkali cyanides in the UV region present a set of weak absorption bands which are identified as triplet a'³Σ⁺ molecular excitons. The nature of the molecular exciton transitions in the ionic-molecular crystals is discussed and the existence of an admixture between molecular exciton and charge transfer exciton states is suggested.     

The role of Frenkel excitons in low-energy-electron diffraction theory for molecular crystals

In this paper a low-energy-electron diffraction theory for molecular crystals is established. The possibility of creating Frenkel excitons by the incident low-energy electrons is taken into account. The whole formalism is based on a set of diagram rules, which facilitates the evaluation of the differential scattering cross section. The influence of the bulk and surface excitons on the LEED intensities will be discussed in a series of subsequent papers.     

Diffusion equation for the quasi-incoherent motion of Frenkel excitons in molecular crystals

In a recent paper a master equation describing the quasi-incoherent motion of Frenkel excitons in molecular crystals has been derived within the Haken-Strobl model for the coupled coherent and incoherent motion of Frenkel excitons. Starting from this master equation and using only the translational symmetry of the crystal lattice, for crystals with one molecule in the unit cell a diffusion equation is derived. For crystals with several molecules in the unit cell instead of a diffusion equation one obtains a set of diffusion-like equations. These equations are solved explicitly for the case of two molecules in the unit cell and asymptotic expressions are discussed. It is shown that this asymptotic behaviour is again described by a diffusion equation.     

Effect of an electric field on the dissociation of electron-hole pairs interacting with triplet excitons in amorphous molecular semiconductors

The photoconductivity of amorphous molecular semiconductor films increases with the simultaneous photogeneration of singlet electron-hole pairs (EHPs) and triplet excitons but decreases when singlet EHPs are replaced by triplet EHPs. As the electric field increases, the influence of the triplet excitons on the photoconductivity of the films due to the dissociation of EHPs becomes less. It is concluded that as the electric field increases, the current-carrier mobility increases and the dissociation rate of EHPs becomes comparable to the spinconversion rate of EHPs interacting with triplet excitons. Fiz. Tverd. Tela (St. Petersburg) 39, 1020–1023 (June 1997)     

Molecular excitons in alkali cyanides

The emission bands of X irradiated Alkali Cyanides were measured at 4.2 K. This emission is associated to the radiative recombination of molecular (Frenkel type) excitons, for the first time observed in these ionic molecular crystals. The nature of the emitting state is discussed and identified as a long lived triplet state.     

Lowest optical excitations in molecular crystals: bound excitons versus free electron-hole pairs in anthracene

By solving the Bethe-Salpeter equation for the electron-hole Green function for crystalline anthracene we find the lowest absorption peak generated by strongly bound excitons or by a free electron-hole pair, depending on the polarization direction being parallel to the short or the long molecular axis, respectively. Both excitations are shifted to lower energies by pressure. The physical difference of these excitations is apparent from the electron-hole wave functions. Our findings are a major contribution to solve the long-standing puzzle about the nature of the lowest optical excitations in organic materials.     

The interaction of excitons in the superliquid state with phonons in molecular crystals

The energy spectrum of excitons in the superliquid state has been investigated in interaction with phonons in molecular crystals. The corresponding branches of the energy spectrum of elementary excitations have been determined and the effect of the interaction with phonons on their stability has been investigated and discussed. The possibility of the resonance excitation of hydrons by means of phonons is discussed.     

Contributions to the theory of singlet exciton decay into pairs of triplet excitons in organic molecular crystals

Probability of singlet exciton decay into pairs of triplet excitons in organic molecular crystals is calculated. The dependence of the calculated probability on the separation of created pairs of triplet excitons, on temperature as well as on variations of equilibrium positions of molecules caused by changes of the state of electron excitations in the crystal is discussed. In conclusion there is given the estimation of the order of the probability value.Na Slovance 2, Praha 8, Czechoslovakia.     

Scattering of excitons by excitons in semiconducting quantum well structures

We have theoretically investigated the scattering of excitons by excitons in a two-dimensional semiconducting quantum well system. The scattering cross sections have been calculated using the Born approximation for both the elastic and inelastic scattering of the excitons by excitons. The threshold for inelastic scattering is increased over the value in a bulk semiconductor because of the enhancement of the exciton binding energy by its confinement. The behavior of the scattering cross section as a function of the energy of relative motion of the excitons is different than in the bulk and the cross section is a more sensitive function of the ratio of the electron and hole masses than in the bulk.     

Self-trapping dynamics of excitons on a one-dimensional lattice

Lattice relaxation dynamics of one-dimensional excitons coupled with an optical lattice vibration mode is studied using molecular dynamics techniques. By investigating the time-evolution of the wave-function and other physical properties, it is found that not only the wavefunction of the relaxed state, a self-trapped exciton (STE), but also the relaxation dynamics changes by varying the strength of the electron-phonon interaction. Hence we can classify STEs into “large” STEs and “small” STEs by means of the difference in physical properties. Such difference is more enhanced for excitons than for polarons, since both the translational motion and the relative motion of the electron and hole is affected in excitons. Dispersion in the phonon frequency also plays an important role in this classification. Optical properties, the Stokes shift and the peak shift of photoinduced absorption, are also calculated.     

Resonant electronic energy transfer from excitons confined in silicon nanocrystals to oxygen molecules

We demonstrate efficient resonant energy transfer from excitons confined in silicon nanocrystals to molecular oxygen (MO). Quenching of photoluminescence (PL) of silicon nanocrystals by MO physisorbed on their surface is found to be most efficient when the energy of excitons coincides with triplet-singlet splitting energy of oxygen molecules. The dependence of PL quenching efficiency on nanocrystal surface termination is consistent with short-range resonant electron exchange mechanism of energy transfer. A highly developed surface of silicon nanocrystal assemblies and a long radiative lifetime of excitons are favorable for achieving a high efficiency of this process.     

Composite boson many-body theory for Frenkel excitons

We present a many-body theory for Frenkel excitons which takes into account their composite nature exactly. Our approach is based on four commutators similar to the ones we previously proposed for Wannier excitons. They allow us to calculate any physical quantity dealing with N excitons in terms of “Pauli scatterings” for carrier exchange in the absence of carrier interaction and “interaction scatterings” for carrier interactions in the absence of carrier exchange. We show that Frenkel excitons have a novel “transfer assisted exchange scattering”, specific to these excitons. It comes from indirect Coulomb processes between localized atomic states. These indirect processes, commonly called “electron-hole exchange” in the case of Wannier excitons and most often neglected, are crucial for Frenkel excitons, as they are the only ones responsible for the excitation transfer. We also show that in spite of the fact that Frenkel excitons are made of electrons and holes on the same atomic site, so that we could naively see them as elementary particles, they definitely are composite objects, their composite nature appearing through various properties, not always easy to guess. The present many-body theory for Frenkel excitons is thus going to appear as highly valuable to securely tackle their many-body physics, as in the case of nonlinear optical effects in organic semiconductors.     

Collective excitations in a system of excitons

A high density system of Frenkel excitons is investigated under the condition that no type of condensation occurs in the system. The dynamic interaction between excitons and the excitonphonon interaction are considered. It is shown that sound-like collective excitations can exist in systems of excitons and excitons and phonons. The damping of excitations caused by finite life time of excitons is also taken into account.The author wishes to express his thanks to Prof. M.Trlifaj for suggesting the present theme and for useful discussions.     

Ground state energy of N Frenkel excitons

By using the composite many-body theory for Frenkel excitons we have recently developed, we here derive the ground state energy of N Frenkel excitons in the Born approximation through the Hamiltonian mean value in a state made of N identical Q = 0 excitons. While this quantity reads as a density expansion in the case of Wannier excitons, due to many-body effects induced by fermion exchanges between N composite particles, we show that the Hamiltonian mean value for N Frenkel excitons only contains a first order term in density, just as for elementary bosons. Such a simple result comes from a subtle balance, difficult to guess a priori, between fermion exchanges for two or more Frenkel excitons appearing in Coulomb term and the ones appearing in the N exciton normalization factor – the cancellation being exact within terms in 1/N_s where N_s is the number of atomic sites in the sample. This result could make us naively believe that, due to the tight binding approximation on which Frenkel excitons are based, these excitons are just bare elementary bosons while their composite nature definitely appears at various stages in the precise calculation of the Hamiltonian mean value.     

Trapping excitons in a two-dimensional in-plane harmonic potential: experimental evidence for equilibration of indirect excitons

We have trapped a gas of long-lifetime, high-mobility excitons in an in-plane harmonic potential. Trapping is an important step toward the goal of a controlled Bose-Einstein condensate of excitons. We show that the repulsive interaction between the excitons plays a dominant role in the behavior of the excitons, in contrast with the weak interactions in atomic gases. We show that under proper conditions the excitons thermalize in the trap to a well-defined equilibrium spatial distribution.     

Optical traps for dark excitons

We propose a mechanism for optical trapping of dark excitons by linearly polarized unabsorbed standing waves, with a potential depth of the order of a few meV. Since this trapping, based on carrier exchanges with virtual excitons coupled to unabsorbed photons, equally acts on bright and dark states, Bose-Einstein condensation of excitons--which occurs in dark states--must appear as dark spots in a cloud of bright excitons, at the trap potential minima, when the temperature decreases.     

Surface excitons on ionic crystals

We have recorded electronic EEL spectra of (001) faces of a number of simple ionic solids, with higher resolution and much lower beam currents than in previous work. We are able to confirm reports that some, but not all, solids show surface excitons at lower energy than the bulk values. We propose a new model for surface excitons, involving the excitation of an electron to a Rydberg-like state outside the crystal surface.