Light-hole Excitons Research Articles

Chirality in Atomically Thin CdSe Nanoplatelets Capped with Thiol-Free Amino Acid Ligands: Circular Dichroism vs. Carboxylate Group Coordination.

Chiral semiconductor nanostructures and nanoparticles are promising materials for applications in biological sensing, enantioselective separation, photonics, and spin-polarized devices. Here, we studied the induction of chirality in atomically thin only two-monolayer-thick CdSe nanoplatelets (NPLs) grown using a colloidal method and exchanged with L-alanine and L-phenylalanine as model thiol-free chiral ligands. We have developed a novel two-step approach to completely exchange the native oleic acid ligands for chiral amino acids at the basal planes of NPLs. We performed an analysis of the optical and chiroptical properties of the chiral CdSe nanoplatelets with amino acids, which was supplemented by an analysis of the composition and coordination of ligands. After the exchange, the nanoplatelets retained heavy-hole, light-hole, and spin-orbit split-off exciton absorbance and bright heavy-hole exciton luminescence. Capping with thiol-free enantiomer amino acid ligands induced the pronounced chirality of excitons in the nanoplatelets, as proven by circular dichroism spectroscopy, with a high dissymmetry g-factor of up to 3.4 × 10-3 achieved for heavy-hole excitons in the case of L-phenylalanine.

Double resonant Raman scattering and photoluminescence mediated by heavy and light hole excitons in a (Cd, Mn)Te quantum well in external magnetic field

Double resonant Raman scattering and photoluminescence mediated by heavy and light hole excitons in a (Cd, Mn)Te quantum well in external magnetic field

Cation Exchange and Spontaneous Crystal Repair Resulting in Ultrathin, Planar CdS Nanosheets.

Cation exchange has become a major postsynthetic tool to obtain nanocrystals with a combination of stoichiometry, size, and shape that is challenging to achieve by direct wet-chemical synthesis. Here, we report on the transformation of highly anisotropic, ultrathin, and planar PbS nanosheets into CdS nanosheets of the same dimensions. We monitor the evolution of the Cd-for-Pb exchange by ex-situ TEM, HAADF-STEM, and EDX. We observe that in the early stages of the exchange the sheets show large in-sheet voids that repair spontaneously upon further exchange and annealing, resulting in ultrathin, planar, and crystalline CdS nanosheets. After cation exchange, the nanosheets show broad sub-band gap luminescence, as often observed in CdS nanocrystals. The photoluminescence excitation spectrum reveals the heavy- and light-hole exciton features, with very strong quantum confinement and large electron-hole Coulomb energy, typical for 2D ultrathin Cd-chalcogenide nanosheets.

Erratum: Heavy-hole–light-hole exciton system in GaAs/AlGaAs quantum wells [Phys. Rev. B 106 , 085407 (2022)

Received 10 March 2023DOI:https://doi.org/10.1103/PhysRevB.107.119902©2023 American Physical SocietyPhysics Subject Headings (PhySH)Research AreasExciton polaritonExcitonsPhysical SystemsQuantum wellsTechniquesLiquid helium coolingLuttinger–Kohn modelMolecular beam epitaxyReflectivityCondensed Matter, Materials & Applied Physics

Quantum beat of heavy-hole and light-hole excitons originating from interband Stark-ladder transitions in a biased GaAs/AlAs superlattice

The letter reports the quantum beat of heavy-hole (HH) and light-hole (LH) excitons originating from interband Stark-ladder transitions in a GaAs/AlAs superlattice. Under the condition that the pump photon energy was well below the LH-related transition energy, only Bloch oscillation was observed. As the pump photon energy was increased, another oscillatory signal with a frequency of ∼6 THz was superimposed. The calculation considering related transitions indicates that the oscillation is due to the quantum beat of HH and LH excitons originating from the interband Stark-ladder transitions between the hole states and the electron state in the first-nearest-neighbor quantum wells.

Measuring the Ultrafast Spectral Diffusion and Vibronic Coupling Dynamics in CdSe Colloidal Quantum Wells using Two-Dimensional Electronic Spectroscopy.

We measure the ultrafast spectral diffusion, vibronic dynamics, and energy relaxation of a CdSe colloidal quantum wells (CQWs) system at room temperature using two-dimensional electronic spectroscopy (2DES). The energy relaxation of light-hole (LH) excitons and hot carriers to heavy-hole (HH) excitons is resolved with a time scale of ∼210 fs. We observe the equilibration dynamics between the spectroscopically accessible HH excitonic state and a dark state with a time scale of ∼160 fs. We use the center line slope analysis to quantify the spectral diffusion dynamics in HH excitons, which contains an apparent sub-200 fs decay together with oscillatory features resolved at 4 and 25 meV. These observations can be explained by the coupling to various lattice phonon modes. We further perform quantum calculations that can replicate and explain the observed dynamics. The 4 meV mode is observed to be in the near-critically damped regime and may be mediating the transition between the bright and dark HH excitons. These findings show that 2DES can provide a comprehensive and detailed characterization of the ultrafast spectral properties in CQWs and similar nanomaterials.

Effects of Pump Photon Energy on Generation and Ultrafast Relaxation of Excitons and Charge Carriers in CdSe Nanoplatelets.

We studied the initial nature and relaxation of photoexcited electronic states in CdSe nanoplatelets (NPLs). Ultrafast transient optical absorption (TA) measurements were combined with the theoretical analysis of the formation and decay of excitons, biexcitons, free charge carriers, and trions. In the latter, photons and excitons were treated as bosons and free charge carriers as fermions. The initial quantum yields of heavy-hole (HH) excitons, light-hole (LH) excitons, and charge carriers vary strongly with photon energy, while thermal relaxation occurs always within 1 ps. After that, the population of LH excitons is negligible due to relaxation to HH excitons or decay into free electrons and holes. Up to the highest average number of about four absorbed photons per NPL in our experiments, we found no signatures of the presence of biexcitons or larger complexes. Biexcitons were only observed due to the interaction of a probe-generated exciton with an exciton produced previously by the pump pulse. For higher pump photon energies, the initial presence of more free charge carriers leads to formation of trions by probe photons. On increasing the number of absorbed pump photons in an NPL, the yield of excitons becomes higher as compared to free charge carriers, since electron-hole recombination becomes more likely. In addition to a TA absorption feature at energy below the HH exciton peak, we also observed a TA signal at the high-energy side of this peak, which we attribute to formation of LH-HH biexcitons or trions consisting of a charge and LH exciton.

Ultrafast quantum-path interferometry of photo-absorption involving excitons in a GaAs multiple-quantum-well structure

Using a pump–probe protocol with pairs of relative-phase-locked femtosecond pulses, we gathered transient reflectivity measurements from a multiple quantum well structure of GaAs/Al0.3Ga0.7As at 10 K. Quantum beating between heavy-hole and light-hole excitons was observed as an oscillation in the transient reflectivity. Its intensity was coherently controlled by controlling the delay between two successive pump pulses. We found characteristic interference fringes arising from the interference of the photo-induced excitons traversing entangled quantum paths. As established in theory, these fringes are peculiar to this dual-pulse excitation via photo-absorption.

Effects of strain and hydrostatic pressure on exciton properties in asymmetric zinc-blende (In,Ga)N/GaN coupled double quantum wells

Within the effective mass approximation, we studied the light-hole and heavy-hole exciton states and their optical properties, such as oscillator strength and radiative decay time, in asymmetric zinc-blende GaN/InxGa1−xN/GaN/InyGa1−yN/GaN coupled double quantum wells. The variational method was performed under strain and hydrostatic pressure. The light-hole and heavy-hole exciton binding energies as a function of the left-well width and/or right-well width, middle-barrier thickness, and indium concentration x(y) of (In,Ga)N material are analyzed in detail. The light-hole and heavy-hole exciton binding energies show an increasing trend with increase of hydrostatic pressure. The hydrostatic pressure not only results in an increase in exciton binding energy, interband transition energy, and oscillator strength but also a decrease in the emission wavelength and radiative decay time. In addition, the biaxial strain dependence of the emission wavelength, radiative decay time, and interband transition energy of the exciton is very remarkable.

Effects of external perturbations on light absorption by light/heavy hole excitons in a semi-parabolic quantum well

The effects of electric, magnetic, and intense terahertz laser fields on optoelectronic properties are investigated in a GaAs/AlxGa1-xAs semi-parabolic quantum well. The binding energy, exciton light absorption coefficients, interband transition energies, and dipole elements in the matrix are studied within the structure of the parabolic band and effective-mass approximations. The transition energy difference between the ground-state electron energy level and the ground-state heavy hole (light hole) energy level and matrix elements are carried out as functions of external perturbations with a constant well size. The results exhibit that the exciton binding energies of heavy and light holes reduce as long as the laser dressing parameter is larger. The optical absorption of light hole exciton in the system is stronger than the heavy hole exciton. And the excitonic energies, transition energies, and absorption coefficients are much more sensitive and controlled by changing the external perturbations.

Light Hole Excitons in Strain-Coupled Bilayer Quantum Dots with Small Fine-Structure Splitting

In this work, we measure polarization-resolved photoluminescence spectra from excitonic complexes in tens of single InAs/GaAs quantum dots (QDs) at the telecom O-band with strain-coupled bilayer structure. QDs often show fine-structure splitting (FSS) ~100 μeV in uniform anisotropy and valence-band mixing of heavy holes (HH) and light holes (LH); the biaxial strain also induces LH excitons with small FSS (especially XX, <5 μeV, 70% of QDs); delocalized LH reduces the Coulomb interaction between holes Vhh and enhances population on LH excitons XX, XX11, X11+ and XX21+.

Heavy-hole–light-hole exciton system in GaAs/AlGaAs quantum wells

Light-hole (lh) excitons (Xlhs) in quantum wells (QWs) are hardly studied compared with heavy-hole (hh) excitons (Xhhs), mainly due to the difficulties of their experimental observation. In this paper, a comprehensive study of both types of excitons in high-quality GaAs/AlGaAs QWs of different widths is performed. We focus on the energy positions of exciton resonances and the exciton-light interaction. The effect of mixing lhs and hhs in GaAs-based structures on these exciton characteristics is investigated. The corrections to the exciton energy due to mixing are only a fraction of millielectronvolts for wide QWs, in which the energy levels of Xhhs and Xlhs are close to each other. It is also experimentally found that the oscillator strength of Xlhs is $\ensuremath{\sim}2.5$ times less than that of Xhhs. This value noticeably deviates from the 3:1 oscillator strength ratio known for optical transitions between free electron and hole states. This deviation originates from the different squeezing of the Xlh and Xhh wave functions due to distinct values of the effective masses of the Xlh and Xhh in the heterostructure. Mixing of hh and lh valence bands is not so important.

Quantum beats of light-hole and heavy-hole excitons in reflection spectra of GaAs/AlGaAs quantum well

In this work we experimentally study dynamics of the heavy-hole and light-hole exciton states in a quantum well under coherent excitation of both excitonic resonances using co- and cross-linear and circular polarizations of pump and probe beams. Oscillations of basic parameters of excitonic resonances are observed. Their dependence on the polarization of the pump and probe beams is used to determine the structure of states of the heavy-hole and light-hole excitons by means of theoretical modelling of experimental data. Keywords: quantum well, excitons, quantum beats, light-hole exciton, heavy-hole exciton.

Non-trivial dependence of spectral characteristics of excitons in quantum wells on the resonant optical excitation power

Basic exciton parameters, such as the energy of exciton transition and the radiative and nonradiative broadenings, are experimentally studied by means of reflectance spectroscopy for a heterostructure with a 14-nm GaAs/AlGaAs quantum well. Particular attention is paid to the nonradiative broadening which is sensitive to densities of free carriers and long-lived nonradiative excitons. A sublinear increase of the broadening of the heavy-hole and light-hole exciton resonances is observed when the light-hole exciton resonance is excited with increasing power. A simple model is developed, which allows one to well reproduce the observed dependence. Keywords: exciton, quantum well, nonradiative broadening.

Identifying a Generic and Detrimental Role of Fano Resonance in Spin Generation in Semiconductor Nanostructures.

Fano resonance is a fundamental physical process that strongly affects the electronic transport, optical, and vibronic properties of matter. Here, we provide the first experimental demonstration of its profound effect on spin properties in semiconductor nanostructures. We show that electron spin generation in InAs/GaAs quantum-dot structures is completely quenched upon spin injection from adjacent InGaAs wetting layers at the Fano resonance due to coupling of light-hole excitons and the heavy-hole continuum of the interband optical transitions, mediated by an anisotropic exchange interaction. Using a master equation approach, we show that such quenching of spin generation is robust and independent of Fano parameters. This work therefore identifies spin-dependent Fano resonance as a universal spin loss channel in quantum-dot systems with an inherent symmetry-breaking effect.

Modulation of exciton states through resonant excitation by continuous wave lasers in a GaAs/AlAs multiple quantum well

Interactions between excitons with different energies are significant in device application, particularly in the emission of intense terahertz (THz) waves caused by difference frequency mixing. In this paper, the interactions of excitons generated by two resonant continuous-wave laser beams are assessed via the change in reflectivity. While calculations suggest that the reflectivity change depends on the exciton number, experimental results measured for various excitation powers, probe powers, and excitation energies (heavy-hole (HH) and light-hole (LH) excitons) show different profiles. Furthermore, the signals probed at a HH exciton differ from those at a LH exciton. These results indicate the importance of careful control of excitation levels for THz wave generation.

Light hole states in a strained quantum dot: Numerical calculation and phenomenological models

Starting from the numerical solution of the 6-band \textbf{k.p} description of a lattice-mismatched ellipsoidal quantum dot situated inside a nanowire, including a spin Zeeman effect with values appropriate to a dilute magnetic semiconductor, we propose and test phenomenological models of the effect of the built-in strain on the heavy hole, light hole and exciton states. We test the validity and the limits of a description restricted to a ($\Gamma_8$) quadruplet of ground states and we demonstrate the role of the interactions of the light-hole state with light-hole excited states. We show that the built-in axial strain not only defines the character, heavy-hole or light-hole, of the ground state, but also mixes significantly the light-hole state with the split-off band's states: Even for a spin-orbit energy as large as 1 eV, that mixing induces first-order modifications of properties such as the spin value and anisotropy, the oscillator strength, and the electron-hole exchange, for which we extend the description to the light-hole exciton. CdTe/ZnTe quantum dots are mainly used as a test case but the concepts we discuss apply to many heterostructures, from mismatched II-VI and III-V quantum dots and nanowires, to III-V nanostructures submitted to an applied stress and to silicon nanodevices with even smaller residual strains.

Emission characteristics variation of GaAs0.92Sb0.08/Al0.3Ga0.7As strained multiple quantum wells caused by rapid thermal annealing

Rapid thermal annealing is an effective way to improve the optical properties of semiconductor materials and devices. In this paper, the emission characteristics of GaAs0.92Sb0.08/Al0.3Ga0.7As multiple quantum wells, which investigated by temperature-dependent photoluminescence, are adjusted through strain and interfacial diffusion via rapid thermal annealing. The light-hole (LH) exciton emission and the heavy-hole (HH) exciton emission are observed at room temperature. After annealing, the LH and HH emission peaks have blue shift. It can be ascribed to the variation of interfacial strain at low annealing temperature and the interfacial diffusion between barrier layer and well layer at high annealing temperature. This work is of great significance for emission adjustment of strained multiple quantum wells.

Dark exciton preparation in a quantum dot by a longitudinal light field tuned to higher exciton states

Several important proposals to use semiconductor quantum dots in quantum information technology rely on the control of the dark exciton ground states, such as dark exciton based qubits with a $\mu$s life time. In this paper, we present an efficient way to occupy the dark exciton ground state by a single short laser pulse. The scheme is based on an optical excitation with a longitudinal field component featured by, e.g., radially polarized beams or certain Laguerre-Gauss or Bessel beams. Utilizing this component, we show within a configuration interaction approach that high-energy exciton states composed of light-hole excitons and higher dark heavy-hole excitons can be addressed. When the higher exciton relaxes, a dark exciton in its ground state is created.

Нетривиальная зависимость спектральных характеристик экситонов в квантовых ямах от мощности резонансного оптического возбуждения

Basic exciton parameters, the energy of exciton transition and the radiative and nonradiative broadenings, are experimentally studied by means of reflectance spectroscopy for a heterostructure with the 14-nm GaAs/AlGaAs quantum well. Particular attention is paid to the nonradiative broadening which is sensitive to optical creation of free carriers and long-lived nonradiative excitons. A sublinear increase of the broadening of the heavy-hole and light-hole exciton resonances is observed when the light-hole exciton resonance is excited with increasing power. A simple model is developed, which allows one to well reproduce the observed dependence.