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Topological materials for classical waves offer remarkable potential in applications such as sensing, waveguiding and signal processing, leveraging topological protection effects like strong robustness, immunity to backscattering and unidirectional transmission. This work presents the simultaneous inverse design of pseudospin-dependent topological edge states for acoustic and electromagnetic waves in two-dimensional $C_{\textrm{6v}}$ phoxonic crystals. The phoxonic crystals are created by arranging the silicon columns periodically in the air background. We propose a multi-objective optimization framework based on the NSGA-II collaborated with the finite element approach, where the bandgaps of acoustic and electromagnetic waves are treated separately as the objective values. The topological nature of bandgaps is determined by analyzing the positional relationships of paired degenerate modes through the modal field calculations, enabling the customization of one of the two bandgaps within the same unit cell. Unlike traditional approaches relying on the band inversion to induce topological phase transitions, the proposed approach directly generates a pair of unit cells with distinct topological properties for both wave types, achieving the maximum bandgap matching in each case. We further demonstrate the existence of the pseudospin-dependent topological edge states for both acoustic and electromagnetic waves, verifying their unidirectionality and robustness against backscattering and defects. This work establishes a systematic strategy for customizing phoxonic topological states, offering a new avenue for the inverse design of multi-functional devices based on both sound and light.

For different alternating-sign multi-pulse trains electric fields with oscillation, the effects of the electric field pulse number and the relative phase of the combined electric field on pair production are investigated by solving quantum Vlasov equation. It is found that the number density of created particles in the combined electric fields is increased by more than one order of magnitude compared to the results without oscillating structure for both zero transverse momentum and full momentum space. In the case of zero transverse momentum, the created particles longitudinal momentum spectrum are monochromatic for large pulse numbers and some suitable relative phases. The number density depends nonlinearly on the relative phase that enables the optimal relative phase parameters for the number density. Moreover, for the full momentum space, the created particles number density and momentum spectrum under different multi-pulse trains electric fields are given and discussed. We also find that the number density as a function of pulse number satisfies the power law with index 5.342 for the strong but slowly varying electric field with large pulse numbers., Comment: 24 pages, 14 figures

Reduced-dimensional CsPbBr$_3$ nanoplatelets (NPLs) are promising candidates for color-saturated blue emitters, yet their electroluminescence performance is hampered by non-radiative recombination, which is associated with bromine vacancies. Here, we show that a post-synthetic treatment of CsPbBr$_3$ NPLs with GdBr$_3$-dimethylformamide (DMF) can effectively eliminate defects while preserving the color. According to a combined experimental and theoretical study, Gd$^{3+}$ ions are less reactive with NPLs as a result of compact interaction between them and DMF, and this stable Gd$^{3+}$-DMF solvation structure makes Brions more available and allows them to move more freely. Consequently, defects are rapidly passivated and photoluminescence quantum yield increases dramatically (from 35 to ~100%), while the surface ligand density and emission color remain unchanged. The result is a remarkable electroluminescence efficiency of 2.4% (at 464 nm), one of the highest in pure blue perovskite NPL light-emitting diodes. It is noteworthy that the conductive NPL film shows a high photoluminescence quantum yield of 80%, demonstrating NPLs' significant electroluminescence potential with further device structure design.

Individual relaxation dynamics of electrons and holes in optically pumped semiconductors is rarely observed due to their overlap. Here we report the individual dynamics of long-lived (~200 mks) holes observed at room temperature in a 10 nm thick film of the 3D topological insulator (TI) Bi2Se3 coated with a 10 nm thick MgF2 layer using transient absorption spectroscopy in the UV-Vis region. The ultraslow hole dynamics was observed by applying multiphoton resonant pumping of massless Dirac fermions and bound valence electrons in Bi2Se3 at a certain wavelength sufficient for their photoemission and subsequent trapping at the Bi2Se3/MgF2 interface. The emerging deficit of electrons in the film makes it impossible for the remaining holes to recombine, thus causing their ultraslow dynamics measured at a specific probing wavelength. We also found an extremely long rise time (~600 ps) for this ultraslow optical response, which is due to the large spin-orbit coupling (SOC) splitting at the valence band maximum and the resulting intervalley scattering between the splitting components. The ultraslow hole dynamics in Bi2Se3 due to the presence of the Bi2Se3/MgF2 interface is nevertheless much faster than the known ultraslow electron dynamics at the Si/SiO2 interface, also induced by multiphoton excitation in Si. The observed dynamics of long-lived holes is gradually suppressed with decreasing Bi2Se3 film thickness for the 2D TI Bi2Se3 (film thickness 5, 4, and 2 nm) due to the loss of resonance conditions for multiphoton photoemission caused by the gap opening at the Dirac surface state nodes. This behavior indicates that the dynamics of massive Dirac fermions predominantly determines the relaxation of photoexcited carriers for both the 2D topologically nontrivial and 2D topologically trivial insulator phases.

It is often taken for granted that in pump-probe experiments on the topological insulator (TI) Bi2Se3 using IR pumping with a commercial Ti:Sapphire laser [~800 nm (1.55 eV photon energy)], the electrons are excited in the one-photon absorption regime, even when pumped with absorbed fluences in the mJ cm-2 range. Here, using UV-Vis transient absorption (TA) spectroscopy, we show that even at low-power IR pumping with absorbed fluences in the mkJ cm-2 range, the TA spectra of the TI Bi2Se3 extend across a part of the UV and the entire visible region. This observation suggests unambiguously that the two-photon pumping regime accompanies the usual one-photon pumping regime even at low laser powers applied. We attribute the high efficiency of two-photon pumping to the giant nonlinearity of Dirac fermions in the Dirac surface states (SS). On the contrary, one-photon pumping is associated with the excitation of bound valence electrons in the bulk into the conduction band. Two mechanisms of absorption bleaching were also revealed since they manifest themselves in different spectral regions of probing. These two mechanisms were assigned to the filling of the phase-space in the Dirac SS and bulk states and the corresponding Pauli blocking.

Ultrafast carrier relaxation in the 2D topological insulator (TI) Bi2Se3 [gapped Dirac surface states (SS)] and how it inherits ultrafast relaxation in the 3D TI Bi2Se3 (gapless Dirac SS) remains a challenge for developing new optoelectronic devices based on these materials. Here ultrashort (100 fs) pumping pulses of ~340 nm wavelength (~3.65 eV photon energy) were applied to study ultrafast electron relaxation in the 2D TI Bi2Se3 films with a thickness of 2 and 5 quintuple layers (~2 and ~5 nm, respectively) using transient absorption (TA) spectroscopy in the ultraviolet-visible spectral region (1.65 - 3.85 eV). The negative and positive contributions of TA spectra were attributed to absorption bleaching that mostly occur in the bulk states and to the inverse bremsstrahlung type free carrier absorption in the surface states, respectively. Owing to this direct and selective access to the bulk and surface carrier dynamics, we were able to monitor coherent longitudinal optical (LO) phonon oscillations, which were successively launched in the bulk and surface states by the front of the relaxing electron population within the LO-phonon cascade emission. We have also recognized the coherent surface-to-bulk vibrational coupling that appears through the phase-dependent amplitude variations of coherent LO-phonon oscillations. This unique behavior manifests itself predominantly for the topologically trivial insulator phase of the 2D TI Bi2Se3 (2 nm thick film) in the photon energy range (~2.0 - 2.25 eV) where efficient energy exchange between the bulk and surface states occurs. We also found that the coherent surface-to-bulk vibrational coupling significantly weakens with increasing both the Bi2Se3 film thickness and pumping power.

Optical control of Dirac surface states (SS) in topological insulators (TI) remains one of the most challenging problems governing their potential applications in novel electronic and spintronic devices. Here, using visible-range transient absorption spectroscopy exploiting ~340 nm (~3.65 eV) pumping, we provide evidence for dynamic opening of a gap in Dirac SS of the thin-film 3D TI Bi2Se3, which has been induced by the dynamic Rashba effect occurring in the film bulk with increasing optical pumping power (photoexcited carrier density). The observed effect appears through the transient absorption band associated with inverse-bremsstrahlung-type free carrier absorption in the gapped Dirac SS. We have also recognized experimental signatures of the existence of the higher energy Dirac SS in the 3D TI Bi2Se3 (in addition to those known as SS1 and SS2) with energies of ~2.7 and ~3.9 eV (SS3 and SS4). It is evidenced that the dynamic gap opening has the same effect on the Dirac SS occurring at any energy.

Ultrafast carrier dynamics in the topological insulator Bi2Se3 have recently been intensively studied using a variety of techniques. However, we are not aware of any successful experiments exploiting transient absorption (TA) spectroscopy for these purposes. Here we demonstrate that if the ~730 nm wavelength pumping (~1.7 eV photon energy) is applied to ultrathin Bi2Se3 films, TA spectra cover the entire visible region, thus unambiguously pointing to two-photon excitation (~3.4 eV). The carrier relaxation dynamics is found to be governed by the polar optical phonon cascade emission occurring in both the bulk states and the Dirac surface states (SS), including SS-bulk-SS vertical electron transport and being also exclusively influenced by whether the Dirac point is presented between the Dirac cones of the higher energy (~1.5 eV) Dirac SS (known as SS2). We have recognized that SS2 act as a valve substantially slowing down the relaxation of electrons when the gap between Dirac cones exceeds the polar optical phonon and resonant defects energies. The resulting progressive accumulation of electrons in the gapped SS2 becomes detectable through the inverse bremsstrahlung type free carrier absorption.

Hybrid plasmonic nanoemitters based on the combination of quantum dot emitters (QD) and plasmonic nanoantennas open up new perspectives in the control of light. However, precise positioning of any active medium at the nanoscale constitutes a challenge. Here, we report on the optimal overlap of antenna's near-field and active medium whose spatial distribution is controlled via a plasmon-triggered 2-photon polymerization of a photosensitive formulation containing QDs. Au nanoparticles of various geometries are considered. The response of these hybrid nano-emitters is shown to be highly sensitive to the light polarization. Different light emission states are evidenced by photoluminescence measurements. These states correspond to polarization-sensitive nanoscale overlap between the exciting local field and the active medium distribution. The decrease of the QD concentration within the monomer formulation allows trapping of a single quantum dot in the vicinity of the Au particle. The latter objects show polarization-dependent switching in the single-photon regime.

Although the structural phase transitions in single-crystal hybrid methyl-ammonium (MA) lead halide perovskites (MAPbX3, X = Cl, Br, I) are common phenomena, they have never been observed in the corresponding nanocrystals. Here we demonstrate that two-photon-excited photoluminescence (PL) spectroscopy is capable of monitoring the structural phase transitions in MAPbX3 nanocrystals because nonlinear susceptibilities govern the light absorption rates. We provide experimental evidence that the orthorhombic-to-tetragonal structural phase transition in a single layer of 20-nm-sized 3D MAPbBr3 nanocrystals is spread out within the 70 - 140 K range. This structural phase instability range arises because, unlike in single-crystal MAPbX3, free rotations of MA ions in the corresponding nanocrystals are no longer restricted by a long-range MA dipole order. The resulting configurational entropy loss can be even enhanced by the interfacial electric field arising due to charge separation at the MAPbBr3/ZnO heterointerface, extending the orthorhombic-to-tetragonal structural phase instability range from 70 to 230 K. We conclude that the weak sensitivity of conventional one-photon-excited PL spectroscopy to the structural phase transitions in 3D MAPbX3 nanocrystals results from the structural phase instability providing negligible distortions of PbX6 octahedra. In contrast, the intensity of two-photon-excited PL and electric-field-induced one-photon-excited PL still remains sensitive enough to weak structural distortions due to the higher rank tensor nature of nonlinear susceptibilities involved. We also show that room-temperature PL originates from the radiative recombination of the optical-phonon vibrationally excited polaronic quasiparticles with energies might exceed the ground-state Frohlich polaron and Rashba energies due to optical-phonon bottleneck.

This paper reviews recent progress in the synthesis of near-infrared (NIR) lead chalcogenide (PbX; PbX=PbS, PbSe, PbTe) quantum dots (QDs) and their applications in NIR QDs based light emitting diodes (NIR-QLEDs). It summarizes the strategies of how to synthesize high efficiency PbX QDs and how to realize high performance PbX based NIR-QLEDs., Comment: 25 pages, 16 figures, review

The dynamical and static Rashba effects in hybrid methylammonium (MA) lead halide perovskites have recently been theoretically predicted. However, only the static effect was experimentally confirmed so far. Here we report on the dynamical Rashba effect observed using snapshot transient absorption spectral imaging with 400 nm pumping for a fully encapsulated film of 20-nm-sized 3D MAPbBr3 nanocrystals. The effect causes a 240 meV splitting of the lowest-energy absorption bleaching band, initially appearing over sub-ps timescale and progressively stabilizing to 60 meV during 500 ps. The integrated intensities of the split subbands demonstrate a photon-helicity-dependent asymmetry, thus proving the Rashba-type splitting and providing direct experimental evidence for the Rashba spin-split edge states in lead halide perovskite materials. The ultrafast dynamics is governed by the relaxation of two-photon-excited electrons in the Rashba spin-split system caused by a built-in electric field originating from dynamical charge separation in the entire MAPbBr3 nanocrystal., Comment: Under consideration at Nature Communications