Tommaso Venanzi, Himani Arora, Stephan Winnerl, Alexej Pashkin, Phanish Chava, Amalia Patanè, Zakhar D. Kovalyuk, Zalhar R. Kudrynskyi, Kenji Watanabe, Takashi … 展开作者
Tommaso Venanzi, Himani Arora, Stephan Winnerl, Alexej Pashkin, Phanish Chava, Amalia Patanè, Zakhar D. Kovalyuk, Zalhar R. Kudrynskyi, Kenji Watanabe, Takashi Taniguchi, Artur Erbe, Manfred Helm, Harald Schneider
备注：
The manuscript will be published in the journal Physical Review Materials. Copyright 2011 by American Physical Society (https://journals.aps.org/prmaterials/)
We study the optical properties of thin flakes of InSe encapsulated in hBN. More specifically, we investigate the photoluminescence (PL) emission and its dependence on sample thickness and temperature. Through the analysis of the PL lineshape, we discuss the relative weights of the exciton and electron-hole contributions. Thereafter we investigate the PL dynamics. Two contributions are distinguishable at low temperature: direct bandgap electron-hole and defect-assisted recombination. The two recombination processes have lifetime of $τ_1 \sim 8\;$ns and $τ_2 \sim 100\;$ns, respectively. The relative weights of the direct bandgap and defect-assisted contributions show a strong layer dependence due to the direct-to-indirect bandgap crossover. Electron-hole PL lifetime is limited by population transfer to lower-energy states and no dependence on the number of layers was observed. The lifetime of the defect-assisted recombination gets longer for thinner samples. Finally, we show that the PL lifetime decreases at high temperatures as a consequence of more efficient non-radiative recombinations.
Layered III-chalcogenide compounds belong to a variety of layered crystals that can be implemented in van der Waals heterostructures. Here we report an optical study of the stability of two of these compounds: indium selenide (InSe) and gallium selenide (GaSe). Micro-photoluminescence (PL) and Raman spectroscopy are used to determine how the properties of thin films of these materials change when they are exposed to air at room temperature. We find that in GaSe films, PL signal decreases on average below 50% over 24 (72) hours of exposure for films with thicknesses 10-25 (48-75) nm. In contras…
Phosphorene is a new family member of two-dimensional materials. We observed strong and highly layer-dependent photoluminescence in few-layer phosphorene (2 to 5 layers). The results confirmed the theoretical prediction that few-layer phosphorene has a direct and layer-sensitive band gap. We also demonstrated that few-layer phosphorene is more sensitive to temperature modulation than graphene and MoS2 in Raman scattering. The anisotropic Raman response in few-layer phosphorene has enabled us to use an optical method to quickly determine the crystalline orientation without tunneling electron mi…
Electron spin polarization up to 100% has been observed in type-II narrow-gap heterostructures with ultrathin InSb insertions in an InAs matrix via investigation of circularly polarized photoluminescence in an external magnetic field applied in Faraday geometry. The polarization degree decreases drastically, changes its sign, and saturates finally at the value of 10% in the limit of either high temperature or strong excitation. The observed effect is explained in terms of strong Zeeman splitting of the electron conduction band in the InAs matrix and a heavy-hole state confined in the InSb inse…
We report the exotic photoluminescence (PL) behaviour of 3D topological insulator Bi2Te3 single crystals grown by customized self-flux method and mechanically exfoliated few layers (18 plus minus 2 nm)/thin flakes obtained by standard scotch tape method from as grown Bi2Te3 crystals.The experimental PL studies on bulk single crystal and mechanically exfoliated few layers of Bi2Te3 evidenced a broad red emission in the visible region. These findings are in good agreement with our theoretical results obtained using the ab initio density functional theory framework.
In this paper we investigate the structural and optical properties of few strain-unbalanced multiple Ge/GeSi quantum wells pseudomorphically grown on GeSi reverse-graded substrates. The obtained high epitaxial quality demonstrates that strain symmetrization is not a mandatory requirement for few quantum-well repetitions. Photoluminescence data, supported by a thorough theoretical modeling, allow us to unambiguously disentangle the spectral features of the quantum wells from those originating in the virtual substrate and to evaluate the impact on the optical properties of key parameters, such a…
Charged magneto-excitons X- in a dilute 2D electron gas in narrow and symmetric quantum wells are studied using exact diagonalization techniques. An excited triplet X- state with a binding energy of about 1 meV is found. This state and the singlet are the two optically active states observed in photoluminescence (PL). The interaction of X-'s with electrons is shown to have short range, which effectively isolates bound X- states from a dilute e-h plasma. This results in the insensitivity of PL to the filling factor nu. For the "dark" triplet X- ground state, the oscillator strength decreases ex…
We used the theory of finite periodic systems to explain the photoluminescence spectra dependence on the average diameter of nanocrystals embedded in oxide matrices. Because of the broad matrix band gap, the photoluminescence response is basically determined by isolated nanocrystals and sequences of a few of them. With this model we were able to reproduce the shape and displacement of the experimentally observed photoluminescence spectra.
Few-layer InSe draws tremendous research interests owing to the superior electronic and optical properties. It exhibits high carrier mobility up to more than 1000 cm2/Vs at room temperature. The strongly layer-tunable band gap spans a large spectral range from near-infrared to the visible. In this perspective, we systematically review the optical properties of few-layer InSe. Firstly, the intrinsic optical and electronic properties are introduced. Compared to other two-dimensional (2D) materials, the light-matter interaction of few-layer InSe is unusual. The band gap transition is inactive or …
A decade of intense research on two-dimensional (2D) atomic crystals has revealed that their properties can differ greatly from those of the parent compound. These differences are governed by changes in the band structure due to quantum confinement and are most profound if the underlying lattice symmetry changes. Here we report a high-quality 2D electron gas in few-layer InSe encapsulated in hexagonal boron nitride under an inert atmosphere. Carrier mobilities are found to exceed 1,000 and 10,000 cm2/Vs at room and liquid-helium temperatures, respectively, allowing the observation of the fully…
We quantitatively study the Raman and photoluminescence (PL) emission from single layer molybdenum disulfide (MoS2) on dielectric (SiO2, hexagonal boron nitride, mica and the polymeric dielectric Gel-Film) and conducting substrates (Au and few-layer graphene). We find that the substrate can affect the Raman and PL emission in a twofold manner. First, the absorption and emission intensities are strongly modulated by the constructive/destructive interference within the different substrates. Second, the position of the A1g Raman mode peak and the spectral weight between neutral and charged excito…
The possibility of spatially resolving the optical properties of atomically thin materials is especially appealing as they can be modulated at the micro- and nanoscale by reducing their thickness, changing the doping level or applying a mechanical deformation. Therefore, optical spectroscopy techniques with high spatial resolution are necessary to get a deeper insight into the properties of two-dimensional materials. Here we study the optical absorption of single- and few-layer molybdenum disulfide (MoS2) in the spectral range from 1.24 eV to 3.22 eV (385 nm to 1000 nm) by developing a hypersp…
Due to the strong quantum confinement effect, few-layer γ-InSe exhibits a layer-dependent bandgap, spanning the visible and near infrared regions, and thus recently draws tremendous attention. As a two-dimensional material, the mechanical flexibility provides an additional tuning knob for the electronic structure. Here, for the first time, we engineer the band structures of few-layer and bulk-like InSe by uniaxial tensile strain, and observe salient shift of photoluminescence (PL) peaks. The shift rate of the optical gap is approximately 90-100 meV per 1% strain for 4- to 8-layer samples, whic…
InSe, a newly rediscovered two-dimensional (2D) semiconductor, possesses superior electrical and optical properties as a direct bandgap semiconductor with high mobility from bulk to atomically thin layers, drastically different from transition metal dichalcogenides (TMDCs) in which the direct bandgap only exists at the single layer limit. However, absorption in InSe is mostly dominated by an out-of-plane dipole contribution which results in the limited absorption of normally incident light which can only excite the in-plane dipole at resonance. To address this challenge, we have explored a uni…
We present a detailed spectroscopic study of the photoluminescence quenching in an epitaxial structures containing CdSe/ZnSe quantum dots doped with low concentration of Mn$^{2+}$ ions. Our time-resolved and time-integrated experiments reveal the origin of the quenching observed in macro-photoluminescence studies of ensembles of such dots. We show that incorporation of even a few ions to an individual dot does not quench its luminescence effectively, although some fingerprints of expected spin-dependent quenching are visible. At the same time, the presence of Mn$^{2+}$ ions in the sample signi…
InSe, a member of the layered materials family, is a superior electronic and optical material which retains a direct bandgap feature from the bulk to atomically thin few-layers and high electronic mobility down to a single layer limit. We, for the first time, exploit strain to drastically modify the bandgap of two-dimensional (2D) InSe nanoflakes. We demonstrated that we could decrease the bandgap of a few-layer InSe flake by 160 meV through applying an in-plane uniaxial tensile strain to 1.06% and increase the bandgap by 79 meV through applying an in-plane uniaxial compressive strain to 0.62%…
Atomically thin, two-dimensional (2D) indium selenide (InSe) has attracted considerable attention due to large tunability in the band gap (from 1.4 to 2.6 eV) and high carrier mobility. The intriguingly high dependence of band gap on layer thickness may lead to novel device applications, although its origin remains poorly understood, and generally attributed to quantum confinement effect. In this work, we demonstrate via first-principles calculations that strong interlayer coupling may be mainly responsible for this phenomenon, especially in the fewer-layer region, and it could also be an esse…
Resonant Photoluminescence of Quantum Incompressible Liquids
Institute of Solid State Physics named after Yu. A. Osipyan, Russian Academy of Sciences（俄罗斯科学院奥西普扬固体物理研究所）；Moscow Institute of Physics and Technology（莫斯科物理技术学院）；Braun Center for Submicron Research, Weizmann Institute of Science（魏茨曼科学研究所微纳研究中心）
Yb3+-doped inorganic metal-halide perovskites (Yb3+:CsPbX3, X = Cl, Br) have recently been discovered to display highly efficient quantum cutting, in which the energy from individual blue or UV photons absorbed by the material is re-emitted in the form of pairs of near-infrared photons by Yb3+ dopants. Experimental photoluminescence quantum yields approaching 200{%} have been reported. As the first quantum-cutting materials that combine such high photoluminescence quantum yields with strong, broadband absorption in the visible, these materials offer unique opportunities for enhancing the effic…
Two-dimensional semiconductors - atomic layers of materials with covalent intra-layer bonding and weak (van der Waals or quadrupole) coupling between the layers - are a new class of materials with great potential for optoelectronic applications. Among those, a special position is now being taken by post-transition metal chalcogenides (PTMC), InSe and GaSe. It has recently been found that the band gap in 2D crystals of InSe more than doubles in the monolayer compared to thick multilayer crystals, while the high mobility of conduction band electrons is promoted by their light in-plane mass. Here…
Layered transition metal dichalcogenides (TMDCs) host a variety of strongly bound exciton complexes that control the optical properties in these materials. Apart from spin and valley, layer index provides an additional degree of freedom in a few-layer thick film. Here we show that in a few-layer TMDC film, the wavefunctions of the conduction and valence band edge states contributing to the K (K') valley are spatially confined in the alternate layers - giving rise to direct (quasi-)intra-layer bright exciton and lower-energy inter-layer dark excitons. Depending on the spin and valley configurat…
We review vibrational and electronic properties of single and a few layer MoS$_2$ relevant to understand their resonant and non-resonant Raman scattering results. In particular, the optical modes and low frequency shear and layer breathing modes show significant dependence on the number of MoS$_2$ layers. Further, the electron doping of the MoS$_2$ single layer achieved using top-gating in a field effect transistor renormalizes the two optical modes A$_{1g}$ and E$^1_{2g}$ differently due to symmetry-dependent electron-phonon coupling. The issues related to carrier mobility, the Schottky barri…
The vibrational and electronic properties of 2-dimensinal (2D) materials can be efficiently tuned by external strain due to their good stretchability. Resonant Raman spectroscopy is a versatile tool to study the physics of phonons, electrons and their interactions simultaneously, which is particularly useful for the investigation of strain effect on 2D materials. Here, for the first time, we report the resonant Raman study of strained few-layer InSe (γ-phase). Under ~ 1% of uniaxial tensile strain, one order of magnitude enhancement of Raman intensity for longitudinal optical (LO) phonon is ob…
We measure the photoluminescence spectra for an array of modulation doped, T-shaped quantum wires as a function of the 1d density n_e which is modulated with a surface gate. We present self-consistent electronic structure calculations for this device which show a bandgap renormalization which, when corrected for excitonic energy and its screening, are largely insensitive to n_e and which are in quantitatively excellent agreement with the data. The calculation (cf. cond-mat/9908349) shows the importance of including orthogonality between the screening electrons and the electron(s) bound to the …
We show that spin-orbit coupling (SOC) in InSe enables the optical transition across the principal band gap to couple with in-plane polarized light. This transition, enabled by $p_{x,y}\leftrightarrow p_z$ hybridization due to intra-atomic SOC in both In and Se, can be viewed as a transition between two dominantly $s$- and $p_z$-orbital based bands, accompanied by an electron spin-flip. Having parametrized $\mathbf{k\cdot p}$ theory using first principles density functional theory we estimate the absorption for $σ^{\pm}$ circularly polarized photons in the monolayer as $\sim 1.5\%$, which satu…
Optical properties of thin layers of rhenium diselenide (ReSe$_2$) with thickness ranging from mono- (1 ML) to nona-layer (9 MLs) are demonstrated. The photoluminescence (PL) and Raman scattering were measured at low ($T$=5 K) and room ($T$=300 K) temperature, respectively. The PL spectra of ReSe$_2$ layers display two well-resolved emission lines, which blueshift by about 120 meV when the layer thickness decreases from 9 MLs to a monolayer. A rich structure of the observed low-energy Raman scattering modes can be explained within a linear chain model. The two phonon modes of intralayer vibrat…
We demonstrate electrical control of the A-exciton interband transition in mono- and few-layer $MoS_{2}$ crystals embedded into photocapacitor devices via the DC Stark effect. Electric field dependent low-temperature photoluminescence spectroscopy reveals a significant tuneability of the A-exciton transition energy, up to $\sim 16 meV$, from which we extract the mean DC exciton polarisability $<\barβ>_{N} = (0.58 \pm 0.25) \cdot 10^{-8} DmV^{-1}$. The exciton polarisability is shown to be layer-independent, indicating a strong localisation of both electron and hole wave functions in each indiv…
We present a comprehensive optical study of thin films of tungsten disulfide (WS$_2$) with layer thicknesses ranging from mono- to octalayer and in the bulk limit. It is shown that the optical band-gap absorption of monolayer WS$_2$ is governed by competing resonances arising from one neutral and two distinct negatively charged excitons whose contributions to the overall absorption of light vary as a function of temperature and carrier concentration. The photoluminescence response of monolayer WS$_2$ is found to be largely dominated by disorder/impurity- and/or phonon-assisted recombination pr…
We present a tight-binding (TB) model and $\mathbf{k\cdot p}$ theory for electrons in monolayer and few-layer InSe. The model is constructed from a basis of all $s$ and $p$ valence orbitals on both indium and selenium atoms, with tight-binding parameters obtained from fitting to independently computed density functional theory (DFT) band structures for mono- and bilayer InSe. For the valence and conduction band edges of few-layer InSe, which appear to be in the vicinity of the $Γ$ point, we calculate the absorption coefficient for the principal optical transitions as a function of the number o…
The electronic structure of few-layer(FL) black phosphorus(BP) sensitively depends on the sample thickness, strain and doping. In this paper, we show that it is also vulnerable to air-exposure. The oxidation of BP caused by air-exposure gives several optical signatures, including the broadening of resonance peaks and increased Stokes shift between infrared (IR) absorption and photoluminescence (PL) peaks. More importantly, air exposure causes blue shifts of all resonance peaks in IR absorption and PL spectra, with more prominent effects for thinner samples and higher order subband transitions.…
We report highly efficient non-radiative energy transfer from cadmium selenide (CdSe) quantum dots to monolayer and few-layer molybdenum disulfide (MoS2). The quenching of the donor quantum dot photoluminescence increases as the MoS2 flake thickness decreases, with the highest efficiency (>95%) observed for monolayer MoS2. This counterintuitive result arises from reduced dielectric screening in thin layer semiconductors having unusually large permittivity and a strong in-plane transition dipole moment, as found in MoS2. Excitonic energy transfer between a 0D emitter and a 2D absorber is fundam…
Understanding broadband photoconductive behaviour in two dimensional layered materials are important in order to utilize them for a variety of opto-electronic applications. Here we present our results of photocurrent spectroscopy measurements performed on few layer Indium Selenide (InSe) flakes. Temperature (T) dependent (40 K < T < 300 K) photocurrent spectroscopy was performed in order to estimate the band-gap energies E_g(T) of InSe at various temperatures. Our measurements indicate that room temperature E_g value for InSe flake was ~ 1.254 eV, which increased to a value of ~ 1.275 eV at lo…
Charge doping in transition metal dichalcogenide is currently a subject of high importance for future electronic and optoelectronic applications. Here we demonstrate chemical doping in CVD grown monolayer (1L) of WS2 by a few commonly used laboratory solvents by investigating the room temperature photoluminescence (PL). The appearance of distinct trionic emission in the PL spectra and quenched PL intensities suggest n-type doping in WS2. The temperature-dependent PL spectra of the doped 1L-WS2 reveal significant enhancement of trion emission intensity over the excitonic emission at low tempera…
Indium selenide, a post-transition metal chalcogenide, is a novel two-dimensional (2D) semiconductor with interesting electronic properties. Its tunable band gap and high electron mobility have already attracted considerable research interest. Here we demonstrate strong quantum confinement and manipulation of single electrons in devices made from few-layer crystals of InSe using electrostatic gating. We report on gate-controlled quantum dots in the Coulomb blockade regime as well as one-dimensional quantization in point contacts, revealing multiple plateaus. The work represents an important mi…
We perform a $\mathbf{k \cdot p}$ theory analysis of the spectra of the lowest energy and excited states of the excitons in few-layer atomically thin films of InSe taking into account in-plane electric polarizability of the film and the influence of the encapsulation environment. For the thinner films, the lowest-energy state of the exciton is weakly indirect in momentum space, with its dispersion showing minima at a layer-number-dependent wave number, due to an inverted edge of a relatively flat topmost valence band branch of the InSe film spectrum and we compute the activation energy from th…
Atomically-thin films of phosphorene (also known as black phosphorus) are a low dimensional optical material with direct exciton emission, whose wavelength is tunable by controlling the number of layers. In addition to this excitonic emission, recent works revealed the existence of emissions from defect states and described new methods to manipulate them. Monolayer phosphorene exhibits emission from localized defect states at wavelengths near 920 nm. Increasing the number of layers should shift the defect emission to longer wavelengths, enabling the material to span a broader spectral range. H…
Strong Coulomb interaction in atomically-thin transition metal dichalcogenides makes these systems particularly promising for studies of excitonic physics. Of special interest are the manifestations of the charged excitons, also known as trions, in the optical properties of two-dimensional semiconductors. In order to describe the optical response of such a system, the exciton interaction with resident electrons should be explicitly taken into account. In this paper we demonstrate that this can be done both in the trion (essentially, few-particle) and Fermi-polaron (many-body) approaches, which…
The electronic properties of quasi two-dimensional multicomponent systems are investigated in the presence of a perpendicular magnetic field. The effects of the presence of a few valence band holes on the properties of quantum Hall systems are examined by analyzing the results of exact numerical diagonalization of small electron-hole systems confined to the spherical surface. The novel type of elementary excitations, the angular momenta, binding energies, interaction pseudopotentials, and effects on the photoluminescence spectrum are presented.
We report on the dynamics of optically induced nuclear spin polarization in individual CdTe/ZnTe quantum dots loaded with one electron by modulation doping. The fine structure of the hot trion (charged exciton $X^-$ with an electron in the $P$-shell) is identified in photoluminescence excitation spectra. A negative polarisation rate of the photoluminescence, optical pumping of the resident electron and the built-up of dynamic nuclear spin polarisation (DNSP) are observed in time-resolved optical pumping experiments when the quantum dot is excited at higher energy than the hot trion triplet sta…
Two-dimensional (2D) materials beyond graphene such as transition metal dichalcogenides (TMDs) have unique mechanical, optical and electronic properties with promising applications in flexible devices, catalysis and sensing. Optical imaging of TMDs using photoluminescence and Raman spectroscopy can reveal the effects of structure, strain, doping, defects, edge states, grain boundaries and surface functionalization. However, Raman signals are inherently weak and so far have been limited in spatial resolution in TMDs to a few hundred nanometres which is much larger than the intrinsic scale of th…
Spin-orbit interaction in a quantum dot couples far infrared radiation to non center of mass excitation modes, even for parabolic confinement and dipole approximation. The intensities of the absorption peaks satisfy the optical sum rule, giving direct information on the total number of electrons inside the dot. In the case of a circularly polarized radiation the sum rule is insensitive to the strength of a Rashba spin-orbit coupling due to an electric field orthogonal to the dot plane, but not to other sources of spin-orbit interaction, thus allowing to discriminate between the two.
