Exciton Dephasing Time Research Articles

Manipulation of optical coherence of quantum-well excitons by transverse magnetic field

We have studied experimentally spin-dependent photon echoes from excitons in an InGaAs/GaAs quantum well subject to a transverse magnetic field (Voigt geometry). Larmor precession of the spins of the electron and heavy hole in an exciton leads to a periodic transfer of coherence between bright and dark exciton states. The increase in dephasing time due to the transition to the dark states could be useful for coherent control development. A comprehensive analysis shows a good agreement between a four-wave mixing experiment and the predictions of a theoretical treatment based on a five-level exciton model comprising a ground state and two pairs of bright and dark states. The extracted optical dephasing time of bright and dark excitons is equal to 30 and 130 ps, respectively. Exploiting the photon echo reveals evidence of electron Larmor precession with in-plane $g$ factor $|{g}_{e,\ensuremath{\perp}}|=0.44\ifmmode\pm\else\textpm\fi{}0.05$ and heavy hole precession as well. The precession frequency of the latter depends nonlinearly on the applied magnetic field, and the corresponding $g$ factor reaches a value of $|{g}_{h,\ensuremath{\perp}}|\ensuremath{\approx}0.3$ at $B=6$ T. Estimates for the heavy hole $g$-factor spreading as well as the isotropic exchange interaction constant are provided.

Exciton-acoustic phonon coupling revealed by resonant excitation of single perovskite nanocrystals

Single perovskite nanocrystals have attracted great research attention very recently due to their potential quantum-information applications, which critically depend on the development of powerful optical techniques to resolve delicate exciton photophysics. Here we have realized resonant and near-resonant excitations of single perovskite CsPbI3 nanocrystals, with the scattered laser light contributing to only ~10% of the total collected signals. This allows us to estimate an ultranarrow photoluminescence excitation linewidth of ~11.32 µeV for the emission state of a single CsPbI3 nanocrystal, corresponding to an exciton dephasing time of ~116.29 ps. Meanwhile, size-quantized acoustic phonons can be resolved from a single CsPbI3 nanocrystal, whose coupling with the exciton is proposed to arise from the piezoelectric potential. The ability to collect resonance fluorescence from single CsPbI3 nanocrystals, with the subsequent revelation of exciton-acoustic phonon coupling, has marked a critical step towards their steady advancement into superior quantum-light sources.

Exciton Dephasing in Tungsten Diselenide Atomic Layer.

An intrinsic exciton dephasing is the coherence loss of exciton dipole oscillation, while the total exciton dephasing originates from coherence loss due to exciton-exciton interaction and excitonphonon coupling. In this article, the total exciton dephasing time of tungsten diselenide (WSe₂) atomic layers was analyzed as functions of excitation intensity with exciton-exciton coupling strength and temperature with exciton-phonon coupling strength. It was hypothesized that the total exciton dephasing time is shortened as the exciton-exciton interaction and the exciton-phonon coupling are increased. The coherence loss analysis revealed that the exciton dephasing time of WSe₂ atomic layers is due to mainly the temperature rather than the excitation intensity.

Coherent dynamics of exciton orbital angular momentum transferred by optical vortex pulses

The coherent dynamics of the exciton center-of-mass motion in bulk GaN are studied using degenerate four-wave-mixing (FWM) spectroscopy with Laguerre-Gaussian (LG) mode pulses. We evaluate the exciton orbital angular momentum (OAM) dynamics from the degree of OAM, which is derived from the distributions of OAM (topological charge) of the FWM signals. When excitons are excited with two single-mode LG pulses, the exciton OAM decay time significantly exceeds the exciton dephasing time, which can be attributed to high uniformity of the exciton dephasing in our bulk sample because the decoherence of the exciton OAM is governed by the angular variation in the exciton dephasing. We also analyze the topological charge $(\ensuremath{\ell})$ dependence of the OAM decay using a multiple-mode LG pump pulse, which allows us to simultaneously observe the dynamics of the exciton OAM for different $\ensuremath{\ell}$ values under the same excitation conditions. The OAM decay times of the $\ensuremath{\ell}=1$ component are usually longer than those of the $\ensuremath{\ell}=0$ component. The $\ensuremath{\ell}\text{-dependent}$ OAM decay is supported by a phenomenological model which takes into account the local nonuniformity of the exciton dephasing.

Time-resolved observation of coherent excitonic nonlinear response with a table-top narrowband THz pulse wave

By combining a tilted-pulse-intensity-front scheme using a LiNbO3 crystal and a chirped-pulse-beating method, we generated a narrowband intense terahertz (THz) pulse, which had a maximum electric field of more than 10 kV/cm at around 2 THz, a bandwidth of ∼50 GHz, and frequency tunability from 0.5 to 2 THz. By performing THz-pump and near-infrared-probe experiments on GaAs quantum wells, we observed that the resonant excitation of the intraexcitonic 1s-2p transition induces a clear and large Autler-Townes splitting. Our time-resolved measurements show that the splitting energy observed in the rising edge region of electric field is larger than in the constant region. This result implies that the splitting energy depends on the time-averaged THz field over the excitonic dephasing time rather than that at the instant of the exciton creation by a probe pulse.

Coherent Control of the Optical Emission in a Single Organic Quantum Wire

We report on the first coherent control experiments on a purely electronic exciton state in an extended quasi-perfect organic quantum wire, a polydiacetylene chain isolated in the crystalline matrix of its own monomer. The time-integrated luminescence of a single wire is measured as the relative phase between two exciting sub-picosecond laser pulses is varied. From visibility functions the exciton dephasing time is extracted and its temperature dependence studied. Our work points the predominant role of thermalization upon the phase relaxation dynamics. By means of microscopic imaging spectroscopy we also show that despite local excitation coherent control is achieved on states delocalized over the chain at the micrometric scale.

Pure optical dephasing dynamics in semiconducting single-walled carbon nanotubes

We report a detailed study of ultrafast exciton dephasing processes in semiconducting single-walled carbon nanotubes employing a sample highly enriched in a single tube species, the (6,5) tube. Systematic measurements of femtosecond pump-probe, two-pulse photon echo, and three-pulse photon echo peak shift over a broad range of excitation intensities and lattice temperature (from 4.4 to 292 K) enable us to quantify the timescales of pure optical dephasing (T(2)(*)), along with exciton-exciton and exciton-phonon scattering, environmental effects as well as spectral diffusion. While the exciton dephasing time (T(2)) increases from 205 fs at room temperature to 320 fs at 70 K, we found that further decrease of the lattice temperature leads to a shortening of the T(2) times. This complex temperature dependence was found to arise from an enhanced relaxation of exciton population at lattice temperatures below 80 K. By quantitatively accounting the contribution from the population relaxation, the corresponding pure optical dephasing times increase monotonically from 225 fs at room temperature to 508 fs at 4.4 K. We further found that below 180 K, the pure dephasing rate (1/T(2)(*)) scales linearly with temperature with a slope of 6.7 ± 0.6 μeV/K, which suggests dephasing arising from one-phonon scattering (i.e., acoustic phonons). In view of the large dynamic disorder of the surrounding environment, the origin of the long room temperature pure dephasing time is proposed to result from reduced strength of exciton-phonon coupling by motional narrowing over nuclear fluctuations. This consideration further suggests the occurrence of remarkable initial exciton delocalization and makes nanotubes ideal to study many-body effects in spatially confined systems.

Coherent transfer of orbital angular momentum to excitons by optical four-wave mixing

We demonstrate the coherent transfer of optical orbital angular momentum (OAM) to the center of mass momentum of excitons in semiconductor GaN using a four-wave mixing (FWM) process. When we apply the optical vortex (OV) as an excitation pulse, the diffracted FWM signal exhibits phase singularities that satisfy the OAM conservation law, which remain clear within the exciton dephasing time (approximately 1ps). We also demonstrate the arbitrary control of the topological charge in the output signal by changing the OAM of the input pulse. The results provide a way of controlling the optical OAM through carriers in solids. Moreover, the time evolution of the FWM with OAM leads to the study of the closed-loop carrier coherence in materials.

Numerical analysis of the effects of carrier dynamics on the switch-on and gain-switching of quantum dot lasers

A systematic analysis of the influence of the capture, inter-level relaxation and exciton dephasing time constants on the dynamic behavior of quantum dot Fabry-Perot semiconductor lasers is done taking into account the lasing from the ground and excited states. The simulation results show that the carrier time constants studied influence significantly the static characteristic of the laser, its switch-on response and the pulses generated by gain-switching.

Ultrafast Response Induced by Interference Effects between Weakly Confined Exciton States

We report an ultrafast response of weakly confined excitons in GaAs thin films observed by a degenerate four-wave-mixing (DFWM) technique. The time-domain signals excited by broadband pulses show an oscillatory structure with a period that varies according to the pulse spectral width and an ultrafast response comparable to the pulse width; on the other hand, the exciton dephasing time is hardly changed by the excitation spectral width. This ultrafast response is much faster than the radiative lifetime expected on the basis of the nonlocal response theory. The DFWM spectra measured at various time delays clearly indicate the contribution of weakly confined excitons to the ultrafast response. Moreover, in the measurement of excitation-energy dependence, the time-domain signals excited by a controlled spectral width exhibit the variation of the oscillation period and response time. These characteristics are similar to those of the excitation spectral width dependence. From the analysis of oscillatory structu...

Experimental investigation of excitonic spin relaxation dynamics in GaN

By performing nondegenerate pump-probe experiments, we study the relaxation dynamics of spin-polarized A and B excitons in wurtzite epitaxial GaN. By analyzing the differential reflectivity spectra $(\ensuremath{\Delta}R∕R)$ of the two circularly polarized probe components, we are able to identify each spin relaxation channel (electron, light- and heavy-hole spin flips) separately and to extract characteristic times of the different spin relaxation processes. In addition, spectral oscillatory features are observed for negative delays. They show a rapid rise determined by the fast dephasing time ${T}_{2}$ of the excitonic transitions. We show that the high density of dislocations increases the spin relaxation of electrons and holes through the Elliot--Yafet mechanism and makes the exciton dephasing time very short. The measured heavy-hole relaxation time, which is not extremely short compared to the electron relaxation time, can be related to the band structure, in which the degeneracy between different spin valence bands is partially lifted.

Negligible Pure Dephasing in InAs Self-Assembled Quantum Dots

We measured the dephasing time and radiative lifetime of excitons in InAs quantum dots fabricated using the strain compensation technique. The dephasing time at 3 K was as long as 2.86 ns using transient four-wave mixing measurements at an excitation wavelength of 1.468 µm. This ultralong dephasing time was due to the significant suppression of pure dephasing.

Ultrafast Exciton Dynamics in (AlAs)0.3/(GaAs)0.7 Ultrashort-Pperiod Superlattice

We investigated the optical properties of a direct-transition-type ultrashort-period (AlAs)0.3/(GaAs)0.7 superlattice. The exciton dephasing time of this superlattice measured by transient degenerate four-wave mixing spectroscopy was shorter than that of normal mixed crystal Al0.3Ga0.7As. This is attributed to the structural difference between both structures due to the growth procedure difference.

Coherent dynamics of excitons in a stack of self-assembled InAs quantum dots at 1.5-μm waveband

We investigate the excitonic dephasing in a stack of self-assembled quantum dots (SAQDs) by using a four-wave-mixing (FWM) technique performed in the optical telecomm-fiber wavelength region at 6 K. A sample used in our experiment is a 150-layer stack of InAs SAQDs embedded in InGaAlAs grown on InP(3 1 1)B substrate fabricated by molecular beam epitaxy. By using a novel strain-controlled technique, the resonant wavelength of the exciton ground state (GS) ranges from 1.25 to 1.5 μm which is much longer than that in typical In(Ga)As SAQDs. In the weak excitation region, the intrinsic dephasing time of excitons at the excitation wavelength of 1.43 μm reaches 770 ps which is much longer than that in most SAQDs with the resonant wavelength of <1 μm. We also find a strong anisotoropy of the signal intensity with respect to the crystal axis attributed to the orientation of InP(3 1 1)B substrate and the elongated shape of QDs.

On the origin of time-resolved pump–probe differential signal from excitons in quantum wells

We investigate the origin and nature of femtosecond time-resolved (TR) pump–probe differential (PPD) signal from the exciton resonance in semiconductor quantum wells (QWs) in the coherent regime. The excitonic PPD signal is expressed as a sum of interferences of the excitonic nonlinear polarization with the incident probe field and the linear polarization induced by the probe. A nonzero excitonic TR-PPD signal from QWs can occur for time t larger than the pulse width ( t p) when the exciton dephasing time is longer than t p, and this signal can originate only from the second interference term for both the negative and positive pump–probe delays, the contribution from the first interference term being zero for t> t p. This is in contrast with the case of PPD signal in the spectral domain where the first interference term plays a major role. We discuss the effects of many body interactions on the TR-PPD signal. It is shown that excitation-induced dephasing can cause a significant increase in the rise time of the TR-PPD signal.

Exciton dephasing in quantum dot molecules.

We have measured the exciton dephasing time in InAs/GaAs quantum dot molecules having different interdot barrier thicknesses in the temperature range from 5 to 60 K, using a highly sensitive four-wave mixing heterodyne technique. At 5 K dephasing times of several hundred picoseconds are found. Moreover, a systematic dependence of the dephasing dynamics on the barrier thickness is observed. These results show how the quantum-mechanical coupling of the electronic wave functions in the molecules affects both the exciton radiative lifetime and the exciton-acoustic phonon interaction.

All-optical quantum dot implementation for quantum computing

We present an all-optical scheme for a solid-state implementation of quantum information processing. The combined effect of static electric fields and ultrafast sequences of multi-color laser pulses on a semiconductor quantum dot array is investigated. We show how these ingredients can be used to perform single- as well as two-qubit gate operations, by exploiting the ground-state excitonic transitions as computational degrees of freedom. We demonstrate that by these means it is possible to implement basic quantum-computation operations on a time scale much shorter than the exciton dephasing time.

Observation of homogeneous optical spectrum in CdSe quantum dots using femtosecond accumulated photon echo

We performed heterodyne-detected accumulated photon echo experiments in CdSe quantum dots. The excitonic dephasing time T 2 was directly observed under very low excitation density of 10 −3 photons per dot. The echo signal consists of two exponential decays: the fast decay component is due to the confined acoustic phonon sideband, while the slow one to the zero–phonon line. The sharp zero–phonon line width increased linearly with the temperature rise, and its linear temperature coefficient was proportional to 1/ R 2. This feature agrees well with the theory based on the interaction between confined excitons and acoustic phonons through deformation potential. The 1/ R-dependent homogeneous broadening at the low temperature suggests the surface scattering.

Exciton spin relaxation in semiconductor quantum wells: the role of disorder

On high-quality (Zn,Cd)Se/ZnSe quantum wells we found that the decay of the exciton spin transients after resonant excitation with circularly polarized light is even faster than the exciton dephasing time. We demonstrate that this fact is a direct consequence of (alloy) disorder, giving rise to a kind of inhomogeneous broadening and associated interference effects for the spin dynamics across the band of localized exciton states.

Well-width dependence of exciton-phonon scattering inInxGa1−xAs/GaAssingle quantum wells

The temperature and density dependencies of the exciton dephasing time in In0.18Ga0.82As/GaAs single quantum wells with different thicknesses have been measured by degenerate four-wave mixing. The exciton-phonon scattering contribution to the dephasing is isolated by extrapolating the dephasing rate to zero-exciton density. From the temperature dependence of this rate we have deduced the linewidth broadening coefficients for acoustic and optical phonons. We find acoustic-phonon coefficients that increase from 1.6 to 3 μeV/K when increasing the well width from 1 to 4 nm. This is in quantitative agreement with theoretical predictions when the spatial extension of the exciton wave function, strongly penetrating into the GaAs barrier in thin InxGa1-xAs quantum wells, is taken into account. The optical-phonon coefficient does not show a systematic dependence on well thickness, and is comparable with the value for bulk GaAs.