Polarization-resolved Photoluminescence Measurements Research Articles

Robust valley quantum coherence in synthetic 3R-phase MoS2: A material for future valley based devices

Two-dimensional layered transition metal dichalcogenides (TMDCs) offer the ideal platform to optically initialize the qubits utilizing the superposition of valley polarized photons. However, in the commonly available 2H phase TMDCs, thickness sensitive crystal inversion symmetry demands the precise control over the number of layers, which makes the study of valley physics challenging. On the other hand, 3R-polymorphic phase TMDCs are non-centrosymmetric irrespective of the number of layers and therefore retain valley degree of freedom for all the thicknesses. Here, using polarization resolved photoluminescence measurements under linearly polarized excitations, we demonstrate the coherent superposition of the valley photons (known as valley coherence) in synthetic 3R-phase MoS2 with different numbers of layers ranging from 3 layers to 11 layers. With near-resonant excitation (633 nm for AX0), the degree of linear polarization (a measure of the valley coherence) is observed up to 70% at 80 K measurement temperatures and is found to be layer thickness independent. Robust valley coherence is attributed to the high optical quality and the 3R crystal symmetry of the MoS2. Using angle resolved polarization dependent measurements, it is established that the net dipolar emission aligns with the polarization orientations of the incident laser, which signifies the valley coherence to be independent of the crystal orientation. This study paves the way toward using 3R-phase MoS2 as a key material for the development of future quantum technologies utilizing valley polarized photons.

Polarization anisotropy and valence band ordering in semipolar (112¯2) AlInN/GaN heterostructures

Semipolar $(11\overline{2}2)$ AlInN/GaN heterostructures on GaN templates were studied using photoluminescence (PL) spectroscopy both at 15 K and at room temperature. The polarization-resolved PL measurements revealed a dominant polarization along the $[11\overline{2}\overline{3}] {c}^{\ensuremath{'}}$ and a weaker signal along the $[1\overline{1}00] m$-direction, i.e., the two in-plane directions of the semipolar $(11\overline{2}2)$ growth plane. We observed slightly different polarization degrees of $0.34\ifmmode\pm\else\textpm\fi{}0.01, 0.25\ifmmode\pm\else\textpm\fi{}0.02$, and $0.20\ifmmode\pm\else\textpm\fi{}0.01$ at room temperature, respectively, depending on the degree of strain relaxation in the $[1\overline{1}00]$ direction. From a theoretical model based on a $\mathbf{k}\ifmmode\cdot\else\textperiodcentered\fi{}\mathbf{p}$ calculation, we find that the transition from the conduction band (CB) to the uppermost valence band (VB) is C for AlInN similar to AlN, followed by the transition A from the CB to the second VB, for a wide range of compositions. Thus, the in-plane transition matrix elements from the CB to the two topmost VBs near the $\mathrm{\ensuremath{\Gamma}}$ point of the Brillouin zone are dominated by ${M}_{[11\overline{2}\overline{3}]}$ for the C transition and by ${M}_{[1\overline{1}00]}$ for the A transition. For the samples under consideration with an energy splitting of about $18\ifmmode\pm\else\textpm\fi{}1\phantom{\rule{4pt}{0ex}}\mathrm{meV}$, there is sizable thermal occupation of the second VB at room temperature, reasonably explaining the experimental results. The results show that AlInN possesses a band structure similar to AlN, which might explain the strong Stokes shift and the large variation in the band-gap values reported previously.

Highly linear polarized emission at telecom bands in InAs/InP quantum dot-nanowires by geometry tailoring.

Nanowire (NW)-based opto-electronic devices require certain engineering in the NW geometry to realize polarized-dependent light sources and photodetectors. We present a growth procedure to produce InAs/InP quantum dot-nanowires (QD-NWs) with an elongated top-view cross-section relying on the vapor-liquid-solid method using molecular beam epitaxy. By interrupting the rotation of the sample during the radial growth sequence of the InP shell, hexagonal asymmetric (HA) NWs with long/short cross-section axes were obtained instead of the usual symmetrical shape. Polarization-resolved photoluminescence measurements have revealed a significant influence of the asymmetric shaped NWs on the InAs QD emission polarization with the photons being mainly polarized parallel to the NW long cross-section axis. A degree of linear polarization (DLP) up to 91% is obtained, being at the state of the art for the reported DLP values from QD-NWs. More importantly, the growth protocol herein is fully compatible with the current applications of HA NWs covering a wide range of devices such as polarized light emitting diodes and photodetectors.

Effects of thermal annealing on localization and strain in core/multishell GaAs/GaNAs/GaAs nanowires

Core/shell nanowire (NW) heterostructures based on III-V semiconductors and related alloys are attractive for optoelectronic and photonic applications owing to the ability to modify their electronic structure via bandgap and strain engineering. Post-growth thermal annealing of such NWs is often involved during device fabrication and can also be used to improve their optical and transport properties. However, effects of such annealing on alloy disorder and strain in core/shell NWs are not fully understood. In this work we investigate these effects in novel core/shell/shell GaAs/GaNAs/GaAs NWs grown by molecular beam epitaxy on (111) Si substrates. By employing polarization-resolved photoluminescence measurements, we show that annealing (i) improves overall alloy uniformity due to suppressed long-range fluctuations in the N composition; (ii) reduces local strain within N clusters acting as quantum dot emitters; and (iii) leads to partial relaxation of the global strain caused by the lattice mismatch between GaNAs and GaAs. Our results, therefore, underline applicability of such treatment for improving optical quality of NWs from highly-mismatched alloys. They also call for caution when using ex-situ annealing in strain-engineered NW heterostructures.

Anisotropic dependence of light extraction behavior on propagation path in AlGaN-based deep-ultraviolet light-emitting diodes.

The anisotropic extraction dependence of polarized light on propagation path in AlGaN-based deep-ultraviolet (DUV) light-emitting diodes (LEDs) is investigated by simulations and photoluminescence (PL) measurements. Theoretical calculations based on k⋅p approximation and Monte Carol ray tracing indicate that there are two kinds of polarized sources with different angular distributions in ~280 nm AlGaN-based LEDs, s-polarized (spherical-shaped) and p-polarized (dumbbell-shaped) sources, which have different extraction behaviors. It is found that the total light extraction intensities are improved with decreasing the propagation path, and the lateral surface extraction gradually becomes dominant. Moreover, the extraction intensity of s-polarized light improves more than that of p-polarized light when the propagation path decreases, leading to a greater polarization degree. Polarization-resolved PL measurements show that the polarization degree of extracted light from lateral facet of the AlGaN multiple quantum well sample can be enhanced from 1% to 17% as the average propagation path reduces by 0.6 mm, which is consistent with the simulation results of the anisotropic dependence of light extraction on propagation path. Our results are significant for understanding and modulating the anisotropic extraction behavior of polarized light to realize high efficiency AlGaN-based DUV LEDs.

A- and B-exciton photoluminescence intensity ratio as a measure of sample quality for transition metal dichalcogenide monolayers

The photoluminescence (PL) in monolayer transition metal dichalcogenides (TMDs) is dominated by the recombination of electrons in the conduction band with holes in the spin-orbit split valence bands, and there are two distinct emission features referred to as the A-peak (ground state exciton) and B-peak (higher spin-orbit split state). The intensity ratio of these two features varies widely, and several contradictory interpretations have been reported. In this work, we analyze the room temperature PL from MoS2, MoSe2, WS2, and WSe2 monolayers and identify the underlying cause of observed variations in emission profile. We determine that PL variations arise from differences in the non-radiative recombination associated with defect densities. Therefore, the relative intensities of the A- and B-emission features can be used to qualitatively assess the non-radiative recombination and a low B/A ratio is indicative of low defect density and high sample quality. We also performed polarization-resolved PL measurements. Emission from TMD monolayers is governed by unique optical selection rules which make them promising materials for valleytronic operations. We observe a notably higher valley polarization in the B-exciton relative to the A-exciton. The high polarization is a consequence of the shorter B-exciton lifetime resulting from rapid relaxation of excitons from the B-exciton to the A-exciton of the valence band. Our work clarifies disparities reported in the literature relating to the emission profile and provides a straightforward means to assess sample quality.

Phonon Interaction and Phase Transition in Single Formamidinium Lead Bromide Quantum Dots.

Formamidinium lead bromide (FAPbBr3) quantum dots (QDs) are promising materials for light emitting applications in the visible spectral region because of their high photoluminescence (PL) quantum yield (QY) and the enhanced chemical stability as compared to, for instance, methylammonium based analogues. Toward practical harnessing of their compelling optical characteristics, the exciton recombination process, and in particular the exciton-phonon interaction and the impact of crystal phase transition, has to be understood in detail. This is addressed in this contribution by PL studies on single colloidal FAPbBr3 QDs. Polarization-resolved PL measurements reveal a fine structure splitting of excitonic transitions due to the Rashba effect. Distinct phonon replica have been observed within energetic distances of 4.3 ± 0.5, 8.6 ± 0.9, and 13.2 ± 1.1 meV from the zero phonon line, which we attribute to vibrational modes of the lead bromide lattice. Additional vibrational modes of 18.6 ± 0.3 and 38.8 ± 1.1 meV are found and related to liberation modes of the formamidinium (FA) cation. Temperature-dependent PL spectra reveal a line broadening of the emission caused by exciton phonon interaction as well an unusual energy shift which is attributed to a crystal phase transition within the single QD.

Anisotropic visible photoluminescence from thermally annealed few-layer black phosphorus

Black phosphorus, a two-dimensional material, with high carrier mobility, tunable direct bandgap and anisotropic electronic properties has attracted enormous research interest towards potential application in electronic, optoelectronic and optomechanical devices. The bandgap of BP is thickness dependent, ranging from 0.3 eV for bulk to 1.3 eV for monolayer, while lacking in the visible region, a widely used optical regime for practical optoelectronic applications. In this work, photoluminescence (PL) centered at 605 nm is observed from the thermally annealed BP with thickness ≤20 nm. This higher energy PL is most likely the consequence of the formation of higher bandgap phosphorene oxides and suboxides on the surface BP layers as a result of the enhanced rate of oxidation. Moreover, the polarization-resolved PL measurements show that the emitted light is anisotropic when the excitation polarization is along the armchair direction. However, if excited along zigzag direction, the PL is nearly isotropic. Our findings suggest that the thermal annealing of BP can be used as a convenient route to fill the visible gap of the BP-based optoelectronic and optomechanical devices.

Optical polarization in mono and bilayer MoS2

Optical anisotropy in monolayer- and bilayer-MoS2 was investigated by polarization resolved photoluminescence measurements. The photoluminescence of monolayer-MoS2 is found to be partially polarized at 4.2 K and maintains this polarization characteristic up to room temperature, while the photoluminescence of bilayer-MoS2 shows no obvious polarization. This polarization anisotropy is due to strain effects at the interface between the MoS2 layer and the SiO2 substrate, causing symmetry breaking of the MoS2 charge distribution. Calculations using density functional theory of the electron density distribution of the monolayer- and bilayer-MoS2 in the in-plane direction are also presented, giving support to our qualitative analysis.

Excitonic structure and pumping power dependent emission blue-shift of type-II quantum dots

In this work we study theoretically and experimentally the multi-particle structure of the so-called type-II quantum dots with spatially separated electrons and holes. Our calculations based on customarily developed full configuration interaction ap- proach reveal that exciton complexes containing holes interacting with two or more electrons exhibit fairly large antibinding energies. This effect is found to be the hallmark of the type-II confinement. In addition, an approximate self-consistent solution of the multi-exciton problem allows us to explain two pronounced phenomena: the blue-shift of the emission with pumping and the large inhomogeneous spectral broadening, both of those eluding explanation so far. The results are confirmed by detailed intensity and polarization resolved photoluminescence measurements on a number of type-II samples.

Phonon symmetries in hexagonal boron nitride probed by incoherent light emission

Layered compounds are stacks of weakly bound two-dimensional atomic crystals, with a prototypal hexagonal structure in graphene, transition metal dichalcogenides and boron nitride. This crystalline anisotropy results in vibrational modes with specific symmetries depending on the in-plane or out-of-plane atomic displacements. We show that polarization-resolved photoluminescence measurements in hexagonal boron nitride reflect the phonon symmetries in this layered semiconductor. Experiments performed with a detection on the sample edge, perpendicular to the c-axis, reveal the strong polarization-dependence of the emission lines corresponding to the recombination assisted by the three acoustic phonon modes. We elucidate the dipole orientation of the fundamental indirect exciton. We demonstrate evidence of the so-far missing phonon replica due to the optical out-of-plane phonon mode.

Robust room temperature valley polarization in monolayer and bilayer WS2.

We report robust room temperature valley polarization in chemical-vapor-deposition (CVD) grown monolayer and bilayer WS2via polarization-resolved photoluminescence measurements using excitation below the bandgap. We show that excitation with energy slightly below the bandgap of the multi-valleyed transition metal chalcogenides can effectively suppress the random redistribution of excited electrons and, thereby, greatly enhance the efficiency of valley polarization at room temperature. Compared to mechanically exfoliated WS2, our CVD grown WS2 films also show enhancement in the coupling of spin, layer and valley degree of freedom and, therefore, provide improved valley polarization. At room temperature, using below-bandgap excitation and CVD grown monolayer and bilayer WS2, we have reached a record-high valley polarization of 35% and 80%, respectively, exceeding the previously reported values of 10% and 65% for mechanically exfoliated WS2 layers using resonant excitation. This observation provides a new direction to enhance valley control at room temperature.

Polarization anisotropy of the emission from type-II quantum dots

We study the polarization response of the emission from type-II GaAsSb capped InAs quantum dots. The theoretical prediction based on the calculations of the overlap integrals of the single-particle states obtained in the k.p framework is given. This is verified experimentally by polarization resolved photoluminescence measurements on samples with the type-II confinement. We show that the polarization anisotropy might be utilized to find the vertical position of the hole wavefunction and its orientation with respect to crystallographic axes of the sample. A proposition for usage in the information technology as a room temperature photonic gate operating at the communication wavelengths as well as a simple model to estimate the energy of fine-structure splitting for type-II GaAsSb capped InAs QDs are given.

Highly anisotropic and robust excitons in monolayer black phosphorus.

Semi-metallic graphene and semiconducting monolayer transition-metal dichalcogenides are the most intensively studied two-dimensional materials of recent years. Lately, black phosphorus has emerged as a promising new two-dimensional material due to its widely tunable and direct bandgap, high carrier mobility and remarkable in-plane anisotropic electrical, optical and phonon properties. However, current progress is primarily limited to its thin-film form. Here, we reveal highly anisotropic and strongly bound excitons in monolayer black phosphorus using polarization-resolved photoluminescence measurements at room temperature. We show that, regardless of the excitation laser polarization, the emitted light from the monolayer is linearly polarized along the light effective mass direction and centres around 1.3 eV, a clear signature of emission from highly anisotropic bright excitons. Moreover, photoluminescence excitation spectroscopy suggests a quasiparticle bandgap of 2.2 eV, from which we estimate an exciton binding energy of ∼0.9 eV, consistent with theoretical results based on first principles. The experimental observation of highly anisotropic, bright excitons with large binding energy not only opens avenues for the future explorations of many-electron physics in this unusual two-dimensional material, but also suggests its promising future in optoelectronic devices.

Integration of multiple site-controlled pyramidal quantum dot systems with photonic-crystal membrane cavities

We describe the fabrication, epitaxial growth and photoluminescence (PL) spectra of systems of site-controlled pyramidal quantum dots (QDs) integrated with photonic crystal (PhC) membrane cavities. The spectra of the individual QDs are characterized by scanning micro-PL spectroscopy, and the cavity modes are identified by polarization-resolved PL measurements and modeling. Weak coupling of systems incorporating up to four identifiable QDs with single modes of the PhC cavities is demonstrated.

Anomalously robust valley polarization and valley coherence in bilayer WS2.

We report the observation of anomalously robust valley polarization and valley coherence in bilayer WS2. The polarization of the photoluminescence from bilayer WS2 follows that of the excitation source with both circular and linear polarization, and remains even at room temperature. The near-unity circular polarization of the luminescence reveals the coupling of spin, layer, and valley degree of freedom in bilayer system, and the linearly polarized photoluminescence manifests quantum coherence between the two inequivalent band extrema in momentum space, namely, the valley quantum coherence in atomically thin bilayer WS2. This observation provides insight into quantum manipulation in atomically thin semiconductors.

A direct comparison of CVD-grown and exfoliated MoS2 using optical spectroscopy

MoS2 is a highly interesting material, which exhibits a crossover from an indirect band gap in the bulk crystal to a direct gap for single layers. Here, we perform a direct comparison between large-area MoS2 films grown by chemical vapor deposition (CVD) and MoS2 flakes prepared by mechanical exfoliation from mineral bulk crystal. Raman spectroscopy measurements show differences between the in-plane and out-of-plane phonon mode positions in CVD-grown and exfoliated MoS2. Photoluminescence (PL) mapping reveals large regions in the CVD-grown films that emit strong PL at room-temperature, and low-temperature PL scans demonstrate a large spectral shift of the A exciton emission as a function of position. Polarization-resolved PL measurements under near-resonant excitation conditions show a strong circular polarization of the PL, corresponding to a valley polarization.

Spin–layer locking effects in optical orientation of exciton spin in bilayer WSe2

Monolayer and few-layer materials present interesting spin and pseudospin states. A study of the coupling between spin, valley and layer degrees of freedom in bilayer WSe2 reveals coherent superpositions of distinct valley configurations and suggests the possibility of electrical control of the spin states. Coupling degrees of freedom of distinct nature plays a critical role in numerous physical phenomena1,2,3,4,5,6,7,8,9,10. The recent emergence of layered materials11,12,13 provides a laboratory for studying the interplay between internal quantum degrees of freedom of electrons14,15. Here we report new coupling phenomena connecting real spin with layer pseudospins in bilayer WSe2. In polarization-resolved photoluminescence measurements, we observe large spin orientation of neutral and charged excitons by both circularly and linearly polarized excitation, with the trion spectrum splitting into a doublet at large vertical electrical field. These observations can be explained as a locking of spin and layer pseudospin in a given valley15, where the doublet implies an electrically induced spin splitting. The observed distinctive behaviour of the trion doublet under polarized excitation further provides spectroscopic evidence of interlayer and intralayer trion species, a promising step towards optical manipulation in van der Waals heterostructures16 through interlayer excitons.

Telecom-wavelength (1.5 μm) single-photon emission from InP-based quantum dots

We demonstrate pronounced single-photon emission from InAs/AlGaInAs/InP quantum dots (QDs) at wavelengths above 1.5 μm that are compatible with standard long-distance fiber communication. The QDs are grown by molecular beam epitaxy on distributed Bragg reflectors. A low QD density of about 5 × 108 cm−2 was obtained using optimized growth conditions. Low-temperature micro-photoluminescence spectroscopy exhibits sharp excitonic emission lines from single QDs without the necessity of further processing steps. The combination of excitation power-dependent and polarization-resolved photoluminescence measurements reveal a characteristic exciton-biexciton behavior with biexciton binding energies that range from 3.5 to 4 meV and fine-structure splitting values down to 20 μeV.

Quantum Efficiency Analysis of Near-Ultraviolet Emitting AlGaN and AlInGaN Structures

The quantum efficiency of c-plane AlxGa1-xN and AlxInyGa1-x-yN structures (x = 0.06–0.21, y = 0.015–0.05) emitting in the UV spectral range between 320 and 350 nm was analyzed using temperature-dependent and polarization-resolved photoluminescence measurements. We found increasing bandgap fluctuation and charge carrier localization in case of higher aluminum or higher indium content. Improved suppression of nonradiative recombination was observed only in case of indium incorporation. The light polarization changed from E⊥c to E∥c with increasing aluminum content in AlGaN. It switched back to E⊥c by the incorporation of indium in AlInGaN. Light polarization significantly contributes to the photoluminescence intensity measured from the top, and the degree of light polarization decreases with increasing temperature. Thus, temperature-dependent photoluminescence measured via the c-plane surface was found to depend both on internal quantum efficiency and on extraction efficiency.