Exciton Spin Research Articles

Anomalous spin exciton with a magnetoroton minimum in a quantum Hall ferromagnet at a filling factor ν=2

In ZnO-based two-dimensional electron systems with strong Coulomb interaction, the anomalous spin-exciton branch is revealed. As probed by inelastic light scattering, in a ferromagnetic quantum-Hall state with the filling factor $\ensuremath{\nu}=2$, a spin exciton has a negative momentum dispersion with steepness dependent on the electron density. The negative dispersion of the spin exciton is associated with its interaction with higher-energy spin-flip modes that exist near $\ensuremath{\nu}=2$. Surprisingly, the anti-Stokes light scattering on spin excitons at ferromagnetic state $\ensuremath{\nu}=2$ is amplified by orders of magnitude, indicating the macroscopic accumulation of these excitations. The experimental findings are confirmed by the exact diagonalization method---these calculations show a magnetoroton minimum in the dispersion of spin excitons and also the attractive interaction between magnetoroton spin excitations.

Recent Progress on Metal‐Based Nanomaterials: Fabrications, Optical Properties, and Applications in Ultrafast Photonics

AbstractNanomaterials have demonstrated excellent mechanical, thermal, optical, and electrical properties in various fields, including 1D carbon nanotubes, as well as 2D materials starting from graphene. Metal‐based nanomaterials, mainly divided into metal and metal oxide nanoparticles, also gradually come into the sight of ultrafast photonics applications due to the outstanding optical properties. The optical properties of metal nanoparticles can be enhanced by the interaction between conduction electrons with electric fields that is called surface plasmon resonance. As for metal oxide nanoparticles, optical properties are closely related to bandgap structures. When it comes to transition metal oxides, other phenomena also play important roles in optical absorption such as spin inversion and excitons of iron. Moreover, preparation methods of materials are also crucial for their properties and further applications. Therefore, in this review, commonly used physical and chemical fabrication methods for metal‐based nanomaterials are first introduced. Then the optical properties of typical metal and metal oxide nanoparticles are discussed specifically. In addition, the applications of metal‐based nanomaterials in ultrafast lasers based on mode‐locked and Q‐switched techniques are also summarized. Finally, a summary and outlook toward the synthesis, optical properties, and applications in ultrafast photonics of metal‐based nanomaterials are presented.

Exciton recombination and spin relaxation in strong magnetic fields in ultrathin (In,Al)As/AlAs quantum wells with indirect band gap and type-I band alignment

The exciton recombination and spin dynamics are studied in monolayer-thick (In,Al)As/AlAs quantum wells characterized by an indirect band gap and a type-I band alignment. The exciton recombination time and the photoluminescence intensity are strongly dependent on strength and orientation of an applied magnetic field. In contrast to no effect of an in-plane field, at a temperature of 1.8 K a magnetic field applied parallel to the growth axis drastically slows down the recombination and reduces the intensity of photoluminescence. The magnetic-field-induced circular polarization of photoluminescence is studied as a function of the magnetic field strength and direction, as well as sample temperature. The observed nonmonotonic behavior of these functions is provided by the interplay of bright and dark exciton states contributing to the emission. Taking into account the magnetic-field-induced redistribution of the indirect excitons between their bright and dark states, we evaluate the heavy-hole longitudinal $g$ factor of 3.6, the radiative recombination time for the bright excitons of 0.13 ms, and the nonradiative recombination time of the bright and dark excitons of 0.43 ms, as well as the spin relaxation times of electron of $25\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{s}$ and heavy hole of $16\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{s}$, bound in the exciton.

Manganese doping for enhanced magnetic brightening and circular polarization control of dark excitons in paramagnetic layered hybrid metal-halide perovskites

Materials combining semiconductor functionalities with spin control are desired for the advancement of quantum technologies. Here, we study the magneto-optical properties of novel paramagnetic Ruddlesden-Popper hybrid perovskites Mn:(PEA)2PbI4 (PEA = phenethylammonium) and report magnetically brightened excitonic luminescence with strong circular polarization from the interaction with isolated Mn2+ ions. Using a combination of superconducting quantum interference device (SQUID) magnetometry, magneto-absorption and transient optical spectroscopy, we find that a dark exciton population is brightened by state mixing with the bright excitons in the presence of a magnetic field. Unexpectedly, the circular polarization of the dark exciton luminescence follows the Brillouin-shaped magnetization with a saturation polarization of 13% at 4 K and 6 T. From high-field transient magneto-luminescence we attribute our observations to spin-dependent exciton dynamics at early times after excitation, with first indications for a Mn-mediated spin-flip process. Our findings demonstrate manganese doping as a powerful approach to control excitonic spin physics in Ruddlesden-Popper perovskites, which will stimulate research on this highly tuneable material platform with promise for tailored interactions between magnetic moments and excitonic states.

Enhanced exciton binding energy, Zeeman splitting and spin polarization in hybrid layered nanosheets comprised of (Cd, Mn)Se and nitrogen-doped graphene oxide: implication for semiconductor devices

The exciton properties of (Cd,Mn)Se-NrGO (nitrogen doped reduced graphene oxide) hybrid layered nanosheets have been studied in a magnetic field up to 10 T and compared to those of (Cd,Mn)Se nanosheets. The temperature dependent photoluminescence reveals the hybridization of inter-band exciton and intra-center Mn transition with enhancement of the binding energy of exciton-Mn hybridized state (80 meV with respect to 60 meV in (Cd,Mn)Se nanosheets) and increase of exciton—phonon coupling strength to 90 meV (with respect to 55 meV in (Cd,Mn)Se nanosheets). The circularly polarized magneto—photoluminescence at 2 K provides evidence for magnetic field induced exciton spin polarization and the realization of excitonic giant Zeeman splitting with g eff as high as 165.4 ± 10.3, much larger than in the case of (Cd,Mn)Se nanosheets (63.9 ± 6.6), promising for implementation in spin active semiconductor devices.

Leveraging Molecular Properties to Tailor Mixed-Dimensional Heterostructures beyond Energy Level Alignment.

The surface sensitivity and lack of dielectric screening in two-dimensional (2D) materials provide numerous intriguing opportunities to tailor their properties using adsorbed π-electron organic molecules. These organic-2D mixed-dimensional heterojunctions are often considered solely in terms of their energy level alignment, i.e., the relative energies of the frontier molecular orbitals versus the 2D material conduction and valence band edges. While this simple model is frequently adequate to describe doping and photoinduced charge transfer, the tools of molecular chemistry enable additional manipulation of properties in organic-2D heterojunctions that are not accessible in other solid-state systems. Fully exploiting these possibilities requires consideration of the details of the organic adlayer beyond its energy level alignment, including hybridization and electrostatics, molecular orientation and thin-film morphology, nonfrontier orbitals and defects, excitonic states, spin, and chirality. This Perspective explores how these relatively overlooked molecular properties offer unique opportunities for tuning optical and electronic characteristics, thereby guiding the rational design of organic-2D mixed-dimensional heterojunctions with emergent properties.

Spinorial formulation of the GW -BSE equations and spin properties of excitons in two-dimensional transition metal dichalcogenides

In many paradigmatic materials, like Transition Metal Dichalcogenides, the role played by the spin degrees of freedom is as important as the one played by the electron-electron interaction. Thus an accurate treatment of the two effects and of their interaction is necessary for an accurate and predictive study of the optical and electronic properties of these materials. Despite the GW-BSE approach correctly accounts for electronic correlations the spin-orbit coupling effect is often neglected or treated perturbatively. Recently spinorial formulations of GW-BSE have become available in different flavours in material-science codes. Still an accurate validation and comparison of different approaches is missing. In this work we go through the derivation of non collinear GW-BSE approach. The scheme is applied to transition metal dichalcogenides comparing perturbative and full spinorial approach. Our calculations reveal that dark-bright exciton splittings are generally improved when the spin orbit coupling is included non perturbatively. The exchange-driven intravalley mixing between the A and B exciton is found to be extremely important in the case of MoSe$_2$. We finally define the excitonic spin and use it to sharply analyze the spinorial properties of Transition Metal Dichalcogenides excitonic states.

Topological nature of the Kondo insulator SmB6 and its sensitiveness to Sm vacancy

The true topological nature of the Kondo insulator SmB$_6$ remains to be unveiled. Our previous tunneling study not only found evidence for the existence of surface Dirac fermions, but it also uncovered that they inherently interact with the spin excitons, collective excitations in the bulk. We have extended such a spectroscopic investigation into crystals containing a Sm deficiency. The bulk hybridization gap is found to be insensitive to the deficiency up to 1% studied here, but the surface states in Sm-deficient crystals exhibit quite different temperature evolutions from those in stoichiometric ones. We attribute this to the topological surface states remaining incoherent down to the lowest measurement temperature due to their continued interaction with the spin excitons that remain uncondensed. This result shows that the detailed topological nature of SmB$_6$ could vary drastically in the presence of disorder in the lattice. This sensitiveness to disorder is seemingly contradictory to the celebrated topological protection, but it can be understood as being due to the intimate interplay between strong correlations and topological effects.

Self-oxidation-formed boron oxide as a tunnel barrier in SmB6 junctions

Samarium hexaboride (SmB6) belongs to a novel class of quantum matter known as topological Kondo insulators. By utilizing planar tunneling spectroscopy, signatures of spin excitons that interact with the topological surface states have been observed. To uncover additional details about this interaction, the effect on the characteristic features by plasma cleaning and ion beam etching processes, employed to clean the SmB6 crystal surface, are examined. Additionally, the effect of the plasma oxidation process used to form the tunnel barrier is analysed. Comparing the conductance spectra to simulations based on the Blonder-Tinkham-Klapwijk model revealed that the junctions with the highest resistances also had the weakest barrier strengths. Such seemingly contradictory observations may be explained by considering a barrier containing layers of B6O or B3O in addition to B2O3. This suboxide formation appears to be most dominant at higher ion beam energies as well as lower plasma oxidation powers.

Anomalous nonlinear optical effect and enhanced emission by magnetic excitons in CVD grown cobalt-doped ZnSe nanoribbon

The magnetic excitons in diluted magnetic semiconductor (DMS) have varied formats due to the inhomogeneous phases out of doping concentration and/or structural relaxations or defects. Here the high quality cobalt-doped zinc blende ZnSe nanoribbons (NRs) were synthesized, showing bright and color-variable emissions from blue, yellow to a little mixed white colors. Their power and temperature dependent micro-photoluminescence (PL) spectra have been obtained in which two emission bands, one magnetic exciton band near the band-edge and a Co2+ high-level d–d transition emission band at 550 nm out of their ferromagnetic (FM) coupled aggregates in ZnSe lattice, both bands could also be reflected by a nonlinear optical absorption enhancement. The easy formed stacking fault defects in a chemical vapor deposition (CVD) grown ZnSe zincblende NR took part in the above optical processes out of magnetic polaronic excitons (PXs). The femtosecond (fs) laser pulse pumping on single ZnSe:Co NR produces obvious lasing behavior but with profile of a complicated magnetic exciton interactions with indication of a crossover from collective exciton magnetic polarons (EMP) to bound magnetic polaron (BMP) scattering in Co doped ZnSe NR. These findings indicate the complication of the magnetic coupling natures in varied DMS structures, whose optical properties have been found to be highly nonlinear, due to the involvement of the spin–spin, spin–exciton and spin–phonon interactions, verified by the theoretic calculation in Yang X-T et al (2019 Interstitial Zn-modulated ferromagnetism in Co-doped ZnSe Mater. Res. Express 6 106121).

Plasmon-to-exciton spin conversion in semiconductor-metal hybrid nanostructures

Optical control of electronic spins is the basis for ultrafast spintronics: circularly polarized light in combination with spin-orbit coupling of the electronic states allows for spin manipulation in condensed matter. However, the conventional approach is limited to spin orientation along one particular orientation that is dictated by the direction of photon propagation. Plasmonics opens new capabilities, allowing one to tailor the light polarization at the nanoscale. Here, we demonstrate ultrafast optical excitation of electron spin on femtosecond time scales via plasmon to exciton spin conversion. By time-resolving the THz spin dynamics in a hybrid (Cd,Mn)Te quantum well structure covered with a metallic grating, we unambiguously determine the orientation of the photoexcited electron spins which is locked to the propagation direction of surface plasmon-polaritons. Using the spin of the incident photons as additional degree of freedom, one can orient the photoexcited electron spin at will in a two-dimensional plane.

Spin stiffness of a Fermi liquid in the ν=1 quantum Hall regime

Anomalous behavior of spin stiffness is revealed in ZnO-based two-dimensional electron systems (2DESs) with strong Coulomb interaction and Wigner-Seitz parameter ${r}_{s}>6$. The spin stiffness is extracted directly from the quadratic $k$ dispersion of spin excitons at $\ensuremath{\nu}=1$ probed by inelastic light scattering. The resulting values are found to be dramatically rescaled compared to the case of weakly interacting 2DESs---spin stiffness turned out to be of the order of the cyclotron energy with the effective mass of Fermi-liquid quasiparticles. This result is also confirmed by the exact diagonalization simulations.

Dynamic polaronic screening for anomalous exciton spin relaxation in two-dimensional lead halide perovskites.

Two-dimensional lead halide perovskites with confined excitons have shown exciting potentials in optoelectronic applications. It is intriguing but unclear how the soft and polar lattice redefines excitons in layered perovskites. Here, we reveal the intrinsic exciton properties by investigating exciton spin dynamics, which provides a sensitive probe to exciton coulomb interactions. Compared to transition metal dichalcogenides with comparable exciton binding energy, we observe orders of magnitude smaller exciton-exciton interaction and, counterintuitively, longer exciton spin lifetime at higher temperature. The anomalous spin dynamics implies that excitons exist as exciton polarons with substantially weakened inter- and intra-excitonic interactions by dynamic polaronic screening. The combination of strong light matter interaction from reduced dielectric screening and weakened inter-/intra-exciton interaction from dynamic polaronic screening explains their exceptional performance and provides new rules for quantum-confined optoelectronic and spintronic systems.

Transient circular dichroism and exciton spin dynamics in all-inorganic halide perovskites

All-inorganic metal halides perovskites (CsPbX3, X = Br or Cl) show strong excitonic and spin-orbital coupling effects, underpinning spin-selective excitonic transitions and therefore exhibiting great promise for spintronics and quantum-optics applications. Here we report spin-dependent optical nonlinearities in CsPbX3 single crystals by using ultrafast pump-probe spectroscopy. Many-body interactions between spin-polarized excitons act like a pseudo-magnetic field and thus lift the degeneracy of spin states resulting in a photoinduced circular dichroism. Such spontaneous spin splitting between “spin-up” and “spin-down” excitons can be several tens of milli-electron volts under intense excitations. The exciton spin relaxation time is ~20 picoseconds at very low pump fluence, the longest reported in the metal halides perovskites family at room temperature. The dominant spin-flip mechanism is attributed to the electron-hole exchange interactions. Our results provide essential understandings towards realizing practical spintronics applications of perovskite semiconductors.

Recombination and spin dynamics of excitons in thin (Ga,Al)(Sb,As)/AlAs quantum wells with an indirect band gap and type-I band alignment

The dynamics of exciton recombination and spin relaxation in thin (Ga,Al)(Sb,As)/AlAs quantum wells (QWs) with indirect band gap are studied. The band alignment in these QWs is identified as type I. The exciton recombination time exceeds hundreds of microseconds, while the spin relaxation times of the electron and the heavy hole in an exciton do not exceed hundreds of nanoseconds. The heavy-hole longitudinal $g$ factor is determined to be $+2.5$. Despite the long exciton lifetimes, the photoluminescence circular polarization degree induced by a magnetic field is unexpectedly small and does not exceed $25%$.

Entanglement robustness to excitonic spin precession in a quantum dot

A semiconductor quantum dot (QD) is an attractive resource to generate polarization-entangled photon pairs. We study the excitonic spin precession (flip-flop) in a family of QDs with different excitonic fine-structure splitting (FSS) and its impact on the entanglement of photons generated from the excitonic-biexcitonic radiative cascade. Our results reveal that coherent processes leave the time post-selected entanglement of QDs with finite FSS unaffected while changing the eigenstates of the system. The flip-flop's precession is observed via quantum tomography through anomalous oscillations of the coincidences in the rectilinear basis. A theoretical model is constructed with the inclusion of an excitonic flip-flop rate and is compared with a two-photon quantum tomography measurement on a QD exhibiting the spin flip-flop mechanism. A generalization of the theoretical model allows estimating the degree of entanglement as a function of the FSS and the spin-flip rate. For a finite temporal resolution, the negativity is found to be oscillating with respect to both the FSS and the spin-flip rate. This oscillatory behavior disappears for perfect temporal resolution and maximal entanglement is retrieved despite the flip-flop process.

Size effect of semiconductor quantum wells in excitonic spin generation under drift

The excitonic spin polarization in dependence of the size of semiconductor quantum well (QW) was investigated by observing the two different circular polarizations of photoluminescence (PL). From the measurements of PL in QWs, it was found that there is a difference between the two different polarization conditions, which is caused by spin-dependent phase-space filling. The PL spin polarization was estimated from the signals of the left and right circularly polarized PL and was found to depend on the size of the wells as well as on the strength of the bias field. The effects of the size of the well and applied electric field on the excitonic PL spin polarization were studied.

Anomalous Anti-Stokes Scattering Signal as an Indicator of Macrofilled Magnetoexciton Levels in the Quantum Hall Effect Regime

The Raman study of strongly interacting two-dimensional electron systems based on ZnO/MgZnO has revealed an anomalously intense spectral line of the anti-Stokes component of the spin exciton. This line is manifested near the filling factor v = 2 at the ferromagnetic ordering of the spin subsystem, whereas it is not observed at the paramagnetic ordering. It has been shown that this line can be attributed to the formation of an ensemble of long-lived collective excitations in the ferromagnetic phase at a filling factor of v = 2.

How Exciton Interactions Control Spin-Depolarization in Layered Hybrid Perovskites.

Using circularly polarized broadband transient absorption, time-resolved circular photoluminescence, and transient Faraday rotation spectroscopy, we report that spin-dependent interactions have a significant impact on exciton energies and spin depolarization times in layered Ruddlesden-Popper hybrid metal-halide perovskites. In BA2FAPb2I7, we report that room-temperature spin lifetimes are largest (3.2 ps) at a carrier density of ∼1017 cm-3 with increasing depolarization rates at higher exciton densities. This indicates that many-body interactions reduce spin-lifetimes and outcompete the effect of D'yakonov-Perel precessional relaxation that has been previously reported at lower carrier densities. We further observe a dynamic circular dichroism that arises from a photoinduced polarization in the exciton distribution between total angular momentum states. Our findings provide fundamental and application relevant insights into the spin-dependent exciton-exciton interactions in layered hybrid perovskites.

Spin-related optical behaviors of dilute magnetic semiconductor ZnSe:Ni(II) nanobelts

There are varied spin states in dilute magnetic semiconductors, and carriers are not the only elementary excitations that carry the spin. This article reports a study of spin interactions in excitons of ZnSe:NiI(II) nanostructures. High-quality ZnSe:NiI(II) nanobelts (NBs) prepared by chemical vapor deposition show a zinc blende structure by x-ray diffraction and Raman spectroscopy. The temperature-dependent photoluminescence spectra of doped NBs show independent free exciton (FX) and exciton magnetic polaron (EMP) peaks at room temperature with ferromagnetically coupled Ni ions. A single-mode lasing profile was obtained with femtosecond laser excitation due to condensation of EMPs over a threshold. The luminescence lifetimes at different pump powers indicated different relaxation profiles, confirming the formation of coherent EMP aggregates. At a slightly higher dopant concentration, a weak peak at the high-energy side of the FX peak showed up separately at low temperature; this should be the magnetic polaron emission band from the antiferromagnetically coupled Ni(II) pair binding with a FX (antiferromagnetic magnetic polaron). These results illustrate the typical spectroscopic characteristics of spin–spin magnetic coupling, exciton–spin or phonon interactions in dilute magnetic semiconductor nanostructures, showing that their different coupled spin types could work as exciton binders for their collective excitons, with possible use in spin nanophotonic devices and quantum modulations.