Spectroscopic studies of semiconductor quantum dots (SQDs) addressing the problem of non-radiative carrier losses is vital for the improvement in the efficiency of various light-emitting devices. Various designs of SQDs emitter like doping, forming core-shell and alloying has been attempted to suppress non-radiative recombination. In this article, we show that forming a hybrid with metal nanoparticles (MNP) having localized surface plasmon resonance overlapped with the emission spectrum of SQD, the non-radiative carrier loss via Auger recombination can be mitigated. Using steady-state and time-resolved photoluminescence, it has been shown that when such hybrid is selectively excited well above the bandgap without exciting plasmon, the contribution to fast decay time reduces along with an increase in contributions to longer decay times. A completely reverse kinetics is observed when exciton and plasmon are simultaneously excited. Such control of photoluminescence kinetics by placing MNP near SQD opens up a new method for designing hybrid materials that are well suited for light-emitting devices.
In semiconductor nanostructures nonradiative Auger recombination is enhanced by the presence of boundaries which relax the momentum conservation and thereby removes the threshold reduction for these processes. We propose a method to strongly reduce the Auger recombination rate by injecting spin-polarized carriers. Our method is illustrated on the example of a quantum well in which the spin-orbit coupling of conduction band is negligible as compared to valence band and thus holes can be considered as spin-unpolarized. The suppression factor of the Auger recombination is determined by the two-di…
The fast nonradiative decay of multiexcitonic states via Auger recombination is a fundamental process affecting a variety of applications based on semiconductor nanostructures. From a theoretical perspective, the description of Auger recombination in confined semiconductor nanostructures is a challenging task due to the large number of valance electrons and exponentially growing number of excited excitonic and biexcitonic states that are coupled by the Coulomb interaction. These challenges have restricted the treatment of Auger recombination to simple, noninteracting electron-hole models. Here…
Modern materials science requires efficient processing and characterization techniques for low dimensional systems. Raman spectroscopy is an important non-destructive tool, which provides enormous information on these materials. This understanding is not only interesting in its own right from a physicist's point of view, but can also be of considerable importance in optoelectronics and device applications of these materials in nanotechnology. The commercial Raman spectrometers are quite expensive. In this article, we have presented a relatively less expensive set-up with home-built collection …
Carrier dynamics in metallic nanostructures is strongly influenced by their confining dimensions. Gold nanoparticles of size $\sim 2$ nm lie at the boundary separating metallic and non-metallic behavior. In this work, we report carrier dynamics in high aspect ratio ultrathin gold nanowires (Au-UNWs) of average diameter $\sim$2 nm using pump (3.1 eV) and coherent white light continuum as probe in the spectral range of 1.15 eV to 2.75 eV. The transient carrier dynamics in Au-UNWs under extreme excitation regime is slower than predicted by the often used two temperature model. We identify Auger-a…
We present a theory of highly excited interacting carriers confined in a semiconductor nanostructure, incorporating Auger coupling between excited states with different number of excitations. The Coulomb matrix elements connecting exciton, bi-exciton and tri-exciton complexes are derived and an intuitive picture of breaking neutral multi-exction complexes into positively and negatively charged multi-exciton complexes is given. The general approach is illustrated by analyzing the coupling of biexciton and exciton in CdSe spherical nanocrystals. The electron and hole states are computed using at…
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…
Metal photoluminescence (MPL) originates from radiative recombination of photoexcited core holes and conduction band electrons. In metal nanostructures, MPL is enhanced due to the surface plasmon local field effect. We identify another essential process in plasmon-assisted MPL - excitation of Auger plasmons by core holes - that hinders MPL from small nanostructures. We develop a microscopic theory of plasmon-enhanced MPL that incorporates both plasmon-assisted enhancement and suppression mechanisms and derive the enhancement factor for MPL quantum efficiency. Our numerical calculations of MPL …
Origin of room temperature visible photoluminescence (PL) from defect free germanium (Ge) nanoparticles have been discussed here. The Ge nanoparticles produced by laser-induced etching technique show broad visible PL around 2.0 - 2.2 eV at room temperature. Size dependent PL peak shift in Ge nanoparticles has been explained in terms of quantum confinement. Theoretical calculations of radiative lifetime using oscillator strength, which is closely related to the size of the nanostructures, suggests that the PL is originating from a radiative recombination process in quantum confined Ge nanostruc…
We study the dependence of the quantum yield of photoluminescence of a dense, periodic array of semiconductor nanocrystals (NCs) on the level of doping and NC size. Electrons introduced to NCs via doping quench photoluminescence by the Auger process, so that practically only NCs without electrons contribute to the photoluminescence. Computer simulation and analytical theory are used to find a fraction of such empty NCs as a function of the average number of donors per NC and NC size. For an array of small spherical NCs, the quantization gap between 1S and 1P levels leads to transfer of electro…
The rate at which excited charge carriers relax to their equilibrium state affects many aspects of the performance of nanoscale devices, including switching speed, carrier mobility and luminescent efficiency. Better understanding of the processes that govern carrier relaxation therefore has important technological implications. A significant increase in carrier-carrier interactions caused by strong spatial confinement of electronic excitations in semiconductor nanostructures leads to a considerable enhancement of Auger effects, which can further result in unusual, Auger-process-controlled reco…
We have analyzed the energetics of decay of the X^- trion (exciton + electron) on the assumption that the exciton and trion are independent excitations of a single two-dimensional semiconducting quantum well. For the first time, it has been shown that in filling a well with electrons from a selective donor-doped matrix, the binding energy of the trion (of the electron with the exciton) increases linearly with a shift of the Fermi level into the depth of the c band. This agrees with the well-known experimental data on the low-temperature radiative decay (photoluminescence) of trions in the hete…
In surface-enhanced Raman scattering experiments that use plasmonic nanostructures as substrates, the scattering spectrum contains a broad background usually associated with photoluminescence. This background exists above and below the frequency of the incident wave. The low-frequency part of this background is similar to the scattering spectrum of a plasmon nanoparticle, while the high-frequency part follows the Gibbs distribution. We develop a theory that explains experimentally observed features in both the high- and low-frequency parts of the photoluminescence spectrum from a unified point…
In a multi-electron atom, an excited electron can decay by emitting a photon. Typically, the leftover electrons are in their ground state. In a radiative Auger process, the leftover electrons are in an excited state and a redshifted photon is created. In a semiconductor quantum dot, radiative Auger is predicted for charged excitons. Here we report the observation of radiative Auger on trions in single quantum dots. For a trion, a photon is created on electron-hole recombination, leaving behind a single electron. The radiative Auger process promotes this additional (Auger) electron to a higher …
Achieving tunability of two dimensional (2D) transition metal dichalcogenides (TMDs) functions calls for the introduction of hybrid 2D materials by means of localized interactions with zero dimensional (0D) materials. A metal-semiconductor interface, as in gold (Au) - molybdenum disulfide (MoS2), is of great interest from the standpoint of fundamental science as it constitutes an outstanding platform to investigate plasmonic-exciton interactions and charge transfer. The applied aspects of such systems introduce new options for electronics, photovoltaics, detectors, gas sensing, catalysis, and …
Experimental results obtained previously for the photoluminescence efficiency (PL$_{eff}$) of Ge quantum dots (QDs) are theoretically studied. A $\log$-$\log$ plot of PL$_{eff}$ versus QD diameter ($D$) resulted in an identical slope for each Ge QD sample only when $E_{G}\sim (D^2+D)^{-1}$. We identified that above $D\approx$ 6.2 nm: $E_{G}\sim D^{-1}$ due to a changing effective mass (EM), while below $D\approx$ 4.6 nm: $E_{G}\sim D^{-2}$ due to electron/ hole confinement. We propose that as the QD size is initially reduced, the EM is reduced, which increases the Bohr radius and interface sca…
The interpretation of the electronic kinetic processes in the quantum zero dimensional nanostructures is considered. The main mechanism of the processes is supposed to be the interaction of electrons with the optical phonons. An emphasis is put on the recently measured effect of the long-time photoluminescence of quantum dot samples, which is observed to occur after an illumination of the sample by a laser pulse. In addition to this, an attention is devoted to the possible origin of the optical effect of the blinking (intermittence) of the optical emission of certain quantum dot samples under …
Continuous and concerted development of colloidal quantum-dot light-emitting diodes over the past two decades has established them as a bedrock technology for the next generation of displays. However, a fundamental issue that limits the performance of these devices is the quenching of photoluminescence due to excess charges from conductive charge transport layers. Although device designs have leveraged various workarounds, doing so often comes at the cost of limiting efficient charge injection. Here we demonstrate that high-field terahertz (THz) pulses can dramatically brighten quenched QDs on…
We demonstrate how the controlled positioning of a plasmonic nanoparticle modifies the photoluminescence of a single epitaxial GaAs quantum dot. The antenna particle leads to an increase of the luminescence intensity by about a factor of eight. Spectrally and temporally resolved photoluminescence measurements prove an increase of the quantum dot's excitation rate. The combination of stable epitaxial quantum emitters and plasmonic nanostructures promises to be highly beneficial for nanoscience and quantum optics.
The Jaynes-Cummings model, describing the interaction between a single two-level system and a photonic mode, has been used to describe a large variety of systems, ranging from cavity quantum electrodynamics, trapped ions, to superconducting qubits coupled to resonators. Recently there has been renewed interest in studying the quantum strong-coupling (QSC) regime, where states with photon number greater than one are excited. This regime has been recently achieved in semiconductor nanostructures, where a quantum dot is trapped in a planar microcavity. Here we study the quantum strong-coupling re…
Previous single-particle spectroscopic studies of colloidal quantum dots have indicated a significant spread in biexciton lifetimes across an ensemble of nominally identical nanocrystals. It has been speculated that in addition to dot-to-dot variation in physical dimensions, this spread is contributed to by variations in the structure of the quantum dot interface, which controls the shape of the confinement potential. Here we directly evaluate the effect of the composition of the core-shell interface on single- and multi-exciton dynamics via side-by-side measurements of individual core-shell C…
We present experimental and theoretical investigation of exciton recombination dynamics and the related polarization of emission in highly in-plane asymmetric nanostructures. Considering general asymmetry- and size-driven effects, we illustrate them with a detailed analysis of InAs/AlGaInAs/InP elongated quantum dots. These offer a widely varied confinement characteristics tuned by size and geometry that are tailored during the growth process, which leads to emission in the application-relevant spectral range of 1.25-1.65 μm. By exploring the interplay of the very shallow hole confining potent…
Time resolved photoluminescence is a powerful technique to study the collective dynamics of excitons and polaritons in semiconductor nanostructures. We present a two excitation pulses technique to induce the ultrafast and controlled quenching of the exciton emission in a quantum well. The depth of the dip is given by the magnitude of the warming of the carriers induced by the arrival of a laser pulse when an exciton population is already present in the sample. We use this technique to study the relaxation mechanisms of polaritons in semiconductor microcavities, which are of great importance to…
A magnetophotoluminescence study of the carrier transfer with hybrid InAs/GaAs quantum dot(QD)-InGaAs quantum well (QW) structures is carried out where we observe an unsual dependence of the photoluminescence (PL) on the GaAs barrier thickness at strong magnetic field and excitation density. For the case of a thin barrier the QW PL intensity is observed to increase at the expense of a decrease in the QD PL intensity. This is attributed to changes in the interplane carrier dynamics in the QW and the wetting layer (WL) resulting from increasing the magnetic field along with changes in the coupli…
We investigate spin properties of a Fe2+ dopant, known for having single nondegenerate ground state in bulk host semiconductor. Due to zero magnetic moment such a ground state is of little use for spintronics and solotronics. We show that this well-established picture of Fe2+ spin configuration can be contradicted by subjecting the Fe2+ ion to sufficiently high strain, e.g., resulting from lattice mismatched epitaxial heterostructures. Our analysis reveals that high strain induces qualitative change in the ion energy spectrum and results in doubly degenerate ground state with spin projection S…
The fine structure of the exciton spectrum, containing optically allowed (bright) and forbidden (dark) exciton states, determines the radiation efficiency in nanostructures. We study time-resolved micro-photoluminescence in MoS$_2$ monolayers and bilayers, both unstrained and compressively strained, in a wide temperature range (10-300 K) to distinguish between exciton states optically allowed and forbidden, both in spin and momentum, as well as to estimate their characteristic decay times and contributions to the total radiation intensity. The decay times were found to either increase or decre…
Transients of upconverted photoluminescence (UPL) from molecular beam epitaxy (MBE) grown InAs quantum structures have been obtained. The results indicate the importance of spatial energy transfer cross section in the upconversion processes. The time constants determined suggest that several monolayer (ML) thick InAs quantum structures are the origin of upconversion. Both the time resolved and continuous wave data allow for the discussion of the dynamic balance between a local process (for example excitonic Auger process) and non-local process (for example two-step two-photon-absorption proces…
In semiconductors, quantum confinement can greatly enhance the interaction between band carriers (electrons and holes) and dopant atoms. One manifestation of this enhancement is the increased stability of exciton magnetic polarons in magnetically-doped nanostructures. In the limit of very strong 0D confinement that is realized in colloidal semiconductor nanocrystals, a single exciton can exert an effective exchange field $B_{\rm{ex}}$ on the embedded magnetic dopants that exceeds several tesla. Here we use the very sensitive method of resonant photoluminescence (PL) to directly measure the pre…
The plasmon-mediated manipulation of light-matter interaction in two-dimensional atomically transition-metal dichalcogenides (TMDs) critically depends on the design of plasmonic nanostructures to achieve the maximum optical field in TMDs. Here, a metal-isolator-metal Salisbury-type perfect absorber was fabricated to serve as a generator of the localized surface plasmons. The significant photoluminescence (PL) enhancement up to 60-fold was observed experimentally in the monolayer (ML) MoS2 on the top of this gold plasmonic hybrid nanostructures. Furthermore, the PL linear polarization can appro…
Despite showing great promise for optoelectronics, the commercialization of halide perovskite nanostructure-based devices is hampered by inefficient electrical excitation and strong exciton binding energies. While transport of excitons in an energy-tailored system via Förster resonance energy transfer (FRET) could be an efficient alternative, halide ion migration makes the realization of cascaded structures difficult. Here, we show how these could be obtained by exploiting the pronounced quantum confinement effect in two dimensional CsPbBr3 based nanoplatelets (NPls). In thin films of NPls of …
Time-resolved and temperature-dependent photoluminescence measurements on one-dimensional sexithiophene lattices reveal intrinsic branching of photoexcitations to two distinct species: self-trapped excitons and dark charge-transfer excitons (CTX; > 5% yield), with radii spanning 2-3 sites. The significant CTX yield results from the strong charge-transfer character of the Frenkel exciton band due to the large free exciton bandwidth (~400 meV) in these supramolecular nanostructures.
Although the field of 2D materials has democratized materials science by making high quality samples accessible cheaply, due to the atomically thin nature of these systems, an integration with nanostructures is almost always required to obtain a significant optical response. Traditionally, these nanostructures are fabricated via electron beam lithography or focused ion beam milling, which are expensive and large area fabrication can be further time consuming. In order to overcome this problem, we report the integration of 2D semiconductors on a cost-effective and large area fabricated nanocone…
Metallic nanostructures can support so-called plasma oscillations (plasmons). Plasmons allow for the concentration of the energy from light, down to sizes well below the conventional diffraction limit known from optics. Plasmonics thus allows for a plethora of new optical applications at the nanoscale. In this thesis, we have investigated the optical and plasmonic properties of semi-continuous gold films (also called percolation films). These films consist of complex tortuous fractal patterns on the nanoscale. They are an easy, fast, and scalable method to fabricate metallic nanostructures. We…
