Two-exciton State Research Articles (Page 1)

One- and two-exciton states of pair centers of Kramers Nd3+ions in Nd-doped CaF2 and SrF2 crystals, and their possible use as qubits

An attractive Bose-Hubbard model is applied for describing quantum self-trapping in an extended star graph. In the strong coupling limit and when two excitons are created on the core of the star, the dynamics is dominated by pair states whose properties are governed by the branch number N. When N = 2, the star reduces to a linear chain so that the energy does not self-localize. Conversely, when N ≥ 3, restructuring of the eigenstates arises and a low-energy state occurs describing a pair localized on the core of the star. Preferentially excited, this localized state gives rise to quantum self-trapping of the energy, a process that intensifies as N increases.

The optical properties of atomically thin transition metal dichalcogenides are dominated by Coulomb bound quasi-particles, such as excitons, trions, and biexcitons. Due to the number and density of possible states, attributing different spectral peaks to the specific origin can be difficult. In particular, there has been much conjecture around the presence, binding energy and/or nature of biexcitons in these materials. In this work, we remove any ambiguity in identifying and separating the optically excited biexciton in monolayer WS2 using two-quantum multidimensional coherent spectroscopy (2Q-MDCS), a technique that directly and selectively probes doubly-excited states, such as biexcitons. The energy difference between the unbound two-exciton state and the biexciton is the fundamental definition of biexciton binding energy and is measured to be 26 ± 2 meV. Furthermore, resolving the biexciton peaks in 2Q-MDCS allows us to identify that the biexciton observed here is composed of two bright excitons in opposite valleys.

The engineering and manipulation of delocalized molecular exciton states is a key component for artificial biomimetic light harvesting complexes as well as alternative circuitry platforms based on exciton propagation. Here we examine the consequences of strong electronic coupling in cyanine homodimers on DNA duplex scaffolds. The most closely spaced dyes, attached to positions directly across the double-helix from one another, exhibit pronounced Davydov splitting due to strong electronic coupling. We demonstrate that the DNA scaffold is sufficiently robust to support observation of the transition from the lowest energy (J-like) one-exciton state to the nonlocal two-exciton state, where each cyanine dye is in the excited state. This transition proceeds via sequential photon absorption and persists for the lifetime of the exciton, establishing this as a controlled method for creating two-exciton states. Our observations suggest that DNA-organized dye networks have potential as platforms for molecular logic gates and entangled photon emission based on delocalized two-exciton states.

We propose a scheme to induce weak-light nonlinearity in a double quantum dot. The scheme positively utilizes locality and dissipation of an external auxiliary system. As a plausible setup, we consider a complex system in which a localized plasmon field from a metallic nanotip couples with only one of the coupled quantum dots. The perturbative calculation with respect to the light intensity shows that, even by a sufficiently weak light, a dipole-forbidden two-exciton NOON state is prepared as the steady state. This result can be explained by combining the two factors: decoherence-induced quantum state preparation and two-photon resonance. The present work implies that the positive usage of both the locality and the dissipation in the external auxiliary system is promising for inducing two-photon processes effectively, and provides one guideline to weak-light nonlinearities.

Quasi-two-dimensional lead halide perovskites, MAn-1PbnX3n+1, are quantum confined materials with an ever-developing range of optoelectronic device applications. Like other semiconductors, the correlated motion of electrons and holes dominates the material's response to optical excitation influencing its electrical and optical properties such as charge formation and mobility. However, the effects of many-particle correlation have been relatively unexplored in perovskite because of the difficultly of probing these states directly. Here, we use double quantum coherence spectroscopy to explore the formation and localization of multiexciton states in these materials. Between the most confined domains, we demonstrate the presence of an interwell, two-exciton excited state. This demonstrates that the four-body Coulomb interaction electronically couples neighboring wells despite weak electron/hole hybridization in these materials. Additionally, in contrast with inorganic semiconductor quantum wells, we demonstrate a rapid decrease in the dephasing time as wells become thicker, indicating that exciton delocalization is not limited by structural inhomogeneity in low-dimensional perovskite.

Here, we study the photoluminescence (PL) time trajectories of single CdSe/ZnS nanocrystals (NCs) as a function of the laser excitation power. At the low laser power, the PL intensity of a single NC switches between the “on” and “off” levels arising from the neutral and positively charged single excitons, respectively. With the increasing laser power, an intermediate “grey” level is formed due to the optical emission from a charged multiexciton state composed of two excitons and an extra electron. Both the inter-photon correlation and the PL decay measurements demonstrate that lifetime-indistinguishable photon pairs are emitted from this negatively charged two-exciton state.

Based on the generating function formalism, we investigate broadband photon statistics of emission for single dimers and trimers driven by a continuous monochromatic laser field. In particular, we study the first and second moments of the emission statistics, which are the fluorescence excitation line shape and Mandel's Q parameter. Numerical results for this line shape and the Q parameter versus laser frequency in the limit of long measurement times are obtained. We show that in the limit of small Rabi frequencies and laser frequencies close to resonance with one of the one-exciton states, the results for the line shape and Q parameter reduce to those of a two-level monomer. For laser frequencies halfway the transition frequency of a two-exciton state, the photon bunching effect associated with two-photon absorption processes is observed. This super-Poissonian peak is characterized in terms of the ratio between the two-photon absorption line shape and the underlying two-level monomer line shapes. Upon increasing the Rabi frequency, the Q parameter shows a transition from super- to sub- to super-Poissonian statistics. Results of broadband photon statistics are also discussed in the context of a transition (frequency) resolved photon detection scheme, photon tracking, which provides a greater insight in the different physical processes that occur in the multi-level systems.

Coherently coupled plasmons and excitons give rise to new optical excitations--plexcitons--due to the strong coupling of these two oscillator systems. Time-resolved studies of J-aggregate-Au nanoshell complexes when the nanoshell plasmon and J-aggregate exciton energies are degenerate probe the dynamical behavior of this coupled system. Transient absorption of the interacting plasmon-exciton system is observed, in dramatic contrast to the photoinduced transmission of the pristine J-aggregate. An additional, transient Fano-shaped modulation within the Fano dip is also observable. The behavior of the J-aggregate-Au nanoshell complex is described by a combined one-exciton and two-exciton state model coupled to the nanoshell plasmon.

We apply the fermion commutation technique for composite bosons to polariton-polariton scattering in semiconductor planar microcavities. Derivations are presented in a simple and physically transparent fashion. A procedure of orthogonolization of the initial and final two-exciton state wavefunctions is used to calculate the effective scattering matrix elements and the scattering rates. We show how the bosonic stimulation of the scattering appears in this full fermionic approach whose equivalence to the bosonization method is thus demonstrated in the regime of low exciton density. We find an additional contribution to polariton-polariton scattering due to the exciton oscillator strength saturation, which we analyze as well. We present a theory of the polariton-polariton scattering with opposite spin orientations and show that this scattering process takes place mainly via dark excitonic states. Analytical estimations of the effective scattering amplitudes are given.

Optical sectioning is performed by collecting the fluorescent emission of two-exciton states in colloidal quantum dots. The two-exciton state is created by two consecutive resonant absorption events, thus requiring unprecedented low excitation energy and peak powers as low as 10(5) W/cm(2). The depth resolution is shown to be equivalent to that of standard multiphoton microscopy, and it was found to deteriorate only slowly as saturation of the two-exciton state is approached, owing to signal contribution from higher excitonic states.

Excited-state dynamics in light-harvesting complex of Rhodobacter sphaeroides

The authors report on the photoluminescence spectroscopy of a single GaSb∕GaAs type II quantum dot (QD) at 8K. A sharp exciton emission with a linewidth of less than 250μeV was observed. Two-exciton emission at the higher energy side of the exciton emission indicates that the two excitons in a type II QD do not form a bound biexciton. The energies of the exciton and two-exciton states were calculated using an atomic pseudopotential model, which provides a quantitative description of the antibound nature of the two-exciton state in type II QDs.

We have theoretically shown that efficient generation of multi-electron-hole pairs by a single photon observed recently in semiconductor nanocrystals1-4 is caused by breaking the single electron approximation for carriers with kinetic energy above the effective energy gap. Due to strong Coulomb interaction, these states form a coherent superposition with charged excitons of the same energy. This concept allows us to define the conditions for dominant two-exciton generations by a single photon: the thermalization rate of a single exciton, initiated by light, should be lower than both the two-exciton state thermalization rate and the rate of Coulomb coupling between single and two exciton states. Possible experimental manifestations of our model are discussed.

In this article the third-order response of an excitonically coupled dimer is studied. The three-pulse photon echo signals were calculated by extracting polarization components from the total polarization in the corresponding phase-matched directions. The total nonlinear response was obtained by numeric propagation of the density matrix, with the exciton-vibrational coupling modeled via Redfield relaxation theory. The full two-dimensional three-pulse photon echo signals and the peak shift were analyzed in terms of the density-matrix dynamics of coherence dephasing and population relaxation. The location of the two-exciton state was found to be essential for proper modeling of the three-pulse photon echo. In particular, an oscillation in the three-pulse photon echo peak shift is found if the two-exciton state is displaced. The oscillations can be related to the dynamics of the one-exciton coherences.

We have performed femtosecond pump-probe spectroscopy measurements in 1,1’-diethyl- 3,3’-bis(4-sulfobutyl)-5,5’,6,6’-tetrachlorobenz imidazolocarbocyanine (also known as TDBC) J aggregates adsorbed onto silver colloidal surfaces. We show that the dependence on probe power and wavelength of the induced emission band dynamics, intensity, and position can only be explained by assuming stimulated emission from the one-exciton state. The stimulated emission originates from the amplification of the one-exciton state emission by an induced transition from the two-exciton state to the one-exciton state. One of the key causes of the stimulated emission is the formation of coherently coupled TDBC molecules on colloidal silver surfaces.

The effect of the excited two-exciton state on the transition from the ground state to the third molecular state is studied for a three-level molecular aggregate. Based on a Green function technique, the analytical expression is given for the line shape of pump–probe differential spectrum. A redshift peak of the transition from the ground state to the third state has been found because of introducing the coupling of the excited two-exciton states to the third state. Further, the dependence of the spectra on the aggregate length shows that the delocalization length of the exciton is decreased with an increase in the coupling strength. This result indicates that the coupling induces the exciton localization, leading to the reduction of the effective molecular number in the molecular aggregates.

Two-exciton migration dynamics of a molecular aggregate is performed using the density matrix approach. Exciton–exciton correlation is shown to cause an oscillatory behavior in the one-exciton population dynamics. Such a feature is found to be well explained by the bypass transition from the ground to a one-exciton forbidden state via a two-exciton state.

We theoretically analyze the optical response from an ultrathin film built up of oriented molecular aggregates, the operating states of which are represented by Frenkel exciton states. A four-level model, involving transitions between the ground, one-exciton and two-exciton states, exciton-exciton annihilation from the two-exciton state as well as relaxation from the annihilation level back to the one-exciton and ground states, is used for describing the film optical response. It is proved that the exciton-exciton annihilation may act not as a destructive but, on the contrary, as a constructive factor tending towards the occurrence of bistability. In particular, the effect of inhomogeneous broadening of the exciton optical transition, preventing the bistable behavior, may be suppressed considerably due to a fast exciton-exciton annihilation.

An analytical expression of the third order nonlinear susceptibility χ(3) has been derived rigorously for a system of interacting Frenkel excitons in a one-dimensional chain of size N with the periodic boundary conditions. It has been clarified that the magnitude of interacting potential between excitons strongly influences the size dependence of χ(3) in the long wavelength approximation, which is well explained in terms of the cancellation effect between the contributions from [ground state] - [one-exciton] transitions and those from [one-exciton] - [two-exciton state] transitions.