Interacting Quantum Dot Research Articles

Charge susceptibility and conductances of a double quantum dot

We calculate the charge susceptibility and the linear and differential conductances of a double quantum dot coupled to two metallic reservoirs both at equilibrium and when the system is driven away from equilibrium. This work is motivated by recent progress in the realization of solid state spin qubits. The calculations are performed by using the Keldysh nonequilibrium Green function technique. In the noninteracting case, we give the analytical expression for the electrical current and deduce from there the linear conductance as a function of the gate voltages applied to the dots, leading to a characteristic charge stability diagram. We determine the charge susceptibility which also exhibits peaks as a function of gate voltages. We show how the study can be extended to the case of an interacting quantum dot.

Emission of an interacting quantum dot system embedded in an optical microcavity

In this work, we study the emission of an interacting quantum dots system embedded in an optical microcavity. We use a model that describes the quantum dots as two-level systems interacting through the Von Foerster mechanism, and also coupled to the cavity modes. Hamiltonian and dissipative dynamics are calculated for systems of microcavity-quantum dots with different spatial configurations, given by geometric arrangement of the quantum dots in the sample. Moreover, we obtained both first and second order correlation functions and the corresponding emission spectra. The results show that the statistical properties of the emitted light by a microcavity quantum dots system, are susceptible to the spatial configuration of the dots in the sample.

Effect of ZnO quantum dots on Escherichia coli global transcription regulator: A molecular investigation

ZnO quantum dots (QDs) are very well known for their antimicrobial activity against several bacteria, however, we still do not know any protein targets of ZnO QDs. In order to determine possible protein target, interaction of ZnO QDs was studied with CRP (Cyclic AMP Receptor Protein), a global transcription regulator protein. Binding between ZnO QDs and E. coli CRP was mainly studied by isothermal titration calorimetry (ITC), structural changes of protein were monitored by fluorescence and circular dichroism spectroscopy, and in-vitro transcription assay was used to asses CRP activity. Result shows that both electrostatic and hydrophobic interactions are involved in CRP-ZnO binding. Different spectroscopic investigation revealed that ZnO binding to CRP leads to extensive unfolding and destabilization, which ultimately leads to protein aggregation. It was also observed that in presence of ZnO dimerization ability of CRP was sharply reduced. In-vitro transcription assay also shows that CRP activity gets severely compromised on ZnO binding. All our data suggests that ZnO QD binding to CRP and consequent structural and functional changes most probably plays a crucial role in ZnO QD induced antimicrobial action.

FeOOH quantum dots coupled g-C3N4 for visible light driving photo- Fenton degradation of organic pollutants

Amorphous FeOOH quantum dots (QDs) were coupled with polymeric photocatalysts g-C3N4 which was developed as a visible light driving photo-Fenton catalyst. Highly dispersed FeOOH QDs anchored on g-C3N4 showed enhanced visible light driving photo-Fenton degradation of MO and phenol than that of pure g-C3N4 and mechanical mixture (FeOOH&g-C3N4). The mineralization efficiency on FeOOH/g-C3N4 is nearly 7 times higher than that on pure g-C3N4 which shows great potential in treatment of recalcitrant organic pollutants. XPS results indicated that extraneous carbon species were present in FeOOH/g-C3N4 which should be responsible for the electron transfer between FeOOH and g-C3N4. Based on the radical capture, electrochemical experiments and photoluminescence (PL) decay characterizations, we proposed that visible light excited the g-C3N4 to produce e−/h+ pairs and the e− participated the cycling of Fe(II)/Fe(III). The FeOOH/g-C3N4 showed high recycling stability without Fe leaching due to the interaction of FeOOH QDs and carbon species. The FeOOH QDs coupled g-C3N4 is a promising visible light driving photo-Fenton catalyst for organic pollutants treatment.

Dynamic analysis of the interactions between Si/SiO2 quantum dots and biomolecules for improving applications based on nano-bio interfaces

Due to their outstanding properties, quantum dots (QDs) received a growing interest in the biomedical field, but it is of major importance to investigate and to understand their interaction with the biomolecules. We examined the stability of silicon QDs and the time evolution of QDs – protein corona formation in various biological media (bovine serum albumin, cell culture medium without or supplemented with 10% fetal bovine serum-FBS). Changes in the secondary structure of BSA were also investigated over time. Hydrodynamic size and zeta potential measurements showed an evolution in time indicating the nanoparticle-protein interaction. The protein corona formation was also dependent on time, albumin adsorption reaching the peak level after 1 hour. The silicon QDs adsorbed an important amount of FBS proteins from the first 5 minutes of incubation that was maintained for the next 8 hours, and diminished afterwards. Under protein-free conditions the QDs induced cell membrane damage in a time-dependent manner, however the presence of serum proteins attenuated their hemolytic activity and maintained the integrity of phosphatidylcholine layer. This study provides useful insights regarding the dynamics of BSA adsorption and interaction of silicon QDs with proteins and lipids, in order to understand the role of QDs biocorona.

Emission Noise in an Interacting Quantum Dot: Role of Inelastic Scattering and Asymmetric Coupling to the Reservoirs.

A theory is developed for the emission noise at frequency ν in a quantum dot in the presence of Coulomb interactions and asymmetric couplings to the reservoirs. We give an analytical expression for the noise in terms of the various transmission amplitudes. Including the inelastic scattering contribution, it can be seen as the analog of the Meir-Wingreen formula for the current. A physical interpretation is given on the basis of the transmission of one electron-hole pair to the concerned reservoir where it emits an energy after recombination. We then treat the interactions by solving the self-consistent equations of motion for the Green functions. The results for the noise derivative versus eV show a zero value until eV=hν, followed by a Kondo peak in the Kondo regime, in good agreement with recent measurements in carbon nanotube quantum dots.

Nano interface potential influences in CdTe quantum dots and biolabeling

Nano interface influences in physiochemical properties of quantum dots (QDs) are the challenging approach to tailor its surface functionalities. In this study, a set of polar and non-polar solvents were selected to analyze the influences in solvent-based dynamic radius and surface potential of QDs. From the nano interface chemistry of polar and non-polar solvents, an appropriate mechanism of precipitation and hydrophobic ligand exchange strategy were elucidated by correlating Henry’s equation. Further, the in vitro cytotoxic potential and antimicrobial activity of QDs were assessed to perform biolabeling. From the observations, an appropriate dosage of QDs was fixed to label the animal ((RAW 264.7 cell lines) and bacterial cells (Escherichia coli) for effective cell attachment. Biolabeling was achieved by tailoring nano interface chemistry of QDs without additional support of biomolecules. Bacterial cell wall-based interaction of QDs was evaluated using SEM and EDAX analysis. Thus, provided clear insights into the nano interface chemistry in the development of highly photostable QDs will be helpful in biomedical applications.

Heat current through an artificial Kondo impurity beyond linear response

We investigate the heat current of a strongly interacting quantum dot in the presence of a voltage bias in the Kondo regime. Using the slave-boson mean-field theory, we discuss the behavior of the energy flow and the Joule heating. We find that both contributions to the heat current display interesting symmetry properties under reversal of the applied dc bias. We show that the symmetries arise from the behavior of the dot transmission function. Importantly, the transmission probability is a function of both energy and voltage. This allows us to analyze the heat current in the nonlinear regime of transport. We observe that nonlinearities appear already for voltages smaller than the Kondo temperature. Finally, we suggest to use the contact and electric symmetry coefficients as a way to measure pure energy currents.

Charge transfer between quasi-zero-dimensional nanostructures

In the present paper, we show the main features of the theoretical formula allowing us to understand the irreversible transfer of electrons or holes, as it may be observed in some electrically conducting (conjugated) polymers. The formula reported here is derived with the use of the nonequilibrium quantum transport theory. The key role in the formula is played by the electron–phonon interaction which is included in an approximation going beyond the limits of the finite order of the perturbation calculation. The transfer formula is developed for a simple model of the stacked conjugated polymer, which is represented here by two interacting quantum dots. The numerical calculations show the dependence of the charge carrier mobility on the charge carrier concentration and on the lattice temperature. A comparison with organic field-effect transistor experiments and with molecular-scale modeling on conjugated polymers is promising.

Using Surface Enhanced Raman Spectroscopy to Probe Single-Cell NF-kB Dynamics during TNF-α Stimulation

Surface-enhanced Raman spectroscopy (SERS) is an optical device that is complicated but fast, that deals with high precision cells, noninvasive and label-free. Tumor necrosis factor-alpha (TNF-α) is primarily produced by macrophages an inflammatory cytokine. When TNF-α binds to TNFR, it activates nuclear factor kappa B (NF-kB) transcript factors. This will lead to oscillation in nuclear NF-kB and steering gene expression by negative feedback loops. We applied biotin anti-human TNF-α antibody to bind with TNF-α proceeded by chemical bonding for streptavidin- Phycoerythrin (PE) to detect the space structure between TNF-α and TNFR. The intracellular p65 was labeled with GFP for NF-kB tracking. We indicated the probing of spatiotemporal interaction between binding of TNF-α to TNF-receptor. PE interacted with TNF-α on a ratio of 1:1 and 1:4. Quantum dots (QDs) with TNF-α at 1:1. The signal strength had decreased in the ratio 1:4. There was low bright field in QD interaction to TNF-α. We used real-time imaging for single TNF-α molecule on the living NIH-3T3 cell surface. The result showed the ligand-induced receptor dimerization and trimerization. The bioconjugation and diameter of fluorescent probes both affected the spatial binding of TNF-α to its receptor. Using real-time imaging of GFP-P65, we successfully visualized the intracellular NF-kB nuclear translocation. Our goal is to compare the results from fluorescence imaging to SERS experiment. SERS has the potential to analyze NF-kB. With this image, label-free SERS space detection and with potentially patentable novel gold nano-particles (Au NPs) it can be seen NF-kB activation in two hours. In addition, we can conduct a 96 or 384 test in parallel and increase the throughput by two or three orders by 100-1000 faults. This will be the ultimate goal to move this device into clinical application.

Facet-Specific Ligand Interactions on Ternary AgSbS2 Colloidal Quantum Dots.

Silver dimetal chalcogenide (Ag-V-VI2 ) ternary quantum dots (QDs) are emerging lead-free materials for optoelectronic devices due to their NIR band gaps, large absorption coefficients, and superior electronic properties. However, thin film-based devices of the ternary QDs still lag behind due to the lack of understanding of the surface chemistry, compared to that of lead chalcogenide QDs even with the same crystal structure. Herein the surface ligand interactions of AgSbS2 QDs, synthesized with 1-dodecanethiol used as a stabilizer, are studied. For nonpolar (1 0 0) surfaces, it is suggested that the thiolate ligands are associated with the crystal lattices, thus preventing surface oxidation by protecting sulfur after air-exposure, as confirmed through optical and surface chemical analysis. Otherwise, silver rich (1 1 1) surfaces are passivated by thiolate ligands, allowing ligand exchange processes for the conductive films. This in-depth investigation of the surface chemistry of ternary QDs will prompt the performance enhancement of their optoelectronic devices.

Effects of Direct Solvent-Quantum Dot Interaction on the Optical Properties of Colloidal Monolayer WS2 Quantum Dots.

Because of the absence of native dangling bonds on the surface of the layered transition metal dichalcogenides (TMDCs), the surface of colloidal quantum dots (QDs) of TMDCs is exposed directly to the solvent environment. Therefore, the optical and electronic properties of TMDCS QDs are expected to have stronger influence from the solvent than usual surface-passivated QDs due to more direct solvent-QD interaction. Study of such solvent effect has been difficult in colloidal QDs of TMDC due to the large spectroscopic heterogeneity resulting from the heterogeneity of the lateral size or (and) thickness in ensemble. Here, we developed a new synthesis procedure producing the highly uniform colloidal monolayer WS2 QDs exhibiting well-defined photoluminescence (PL) spectrum free from ensemble heterogeneity. Using these newly synthesized monolayer WS2 QDs, we observed the strong influence of the aromatic solvents on the PL energy and intensity of monolayer WS2 QD beyond the simple dielectric screening effect, which is considered to result from the direct electronic interaction between the valence band of the QDs and molecular orbital of the solvent. We also observed the large effect of stacking/separation equilibrium on the PL spectrum dictated by the balance between inter QD and QD-solvent interactions. The new capability to probe the effect of the solvent molecules on the optical properties of colloidal TMDC QDs will be valuable for their applications in various liquid surrounding environments.

Nonlinear electric and thermoelectric Andreev transport through a hybrid quantum dot coupled to ferromagnetic and superconducting leads

We discuss the nonlinear Andreev current of an interacting quantum dot coupled to spin-polarized and superconducting reservoirs when voltage and temperature biases are applied across the nanostructure. Due to the particle-hole symmetry introduced by the superconducting (S) lead, the subgap spin current vanishes identically. Nevertheless, the Andreev charge current depends on the degree of polarization in the ferromagnetic (F) contact since the shift of electrostatic internal potential of the conductor depends on spin orientation of the charge carrier. This spin-dependent potential shift characterizes nonlinear responses in our device. We show how the subgap current versus the bias voltage or temperature difference depends on the lead polarization in two cases, namely (i) S-dominant case, when the dot-superconductor tunneling rate ($\Gamma_R$) is much higher than the ferromagnet-dot tunnel coupling ($\Gamma_L$), and (ii) F-dominant case, when $\Gamma_L\gg \Gamma_R$. For the ferromagnetic dominant case the spin-dependent potential shows a nonmonotonic behavior as the dot level is detuned. Thus the subgap current can also exhibit interesting behaviors such as current rectification and the maximization of thermocurrents with smaller thermal biases when the lead polarization and the quantum dot level are adjusted.

Powerful Coulomb-drag thermoelectric engine

We investigate a thermoelectric nano-engine whose properties are steered by Coulomb interaction. The device whose design decouples charge and energy currents is made up of two interacting quantum dots connected to three different reservoirs. We show that, by tailoring the tunnel couplings, this setup can be made very attractive for energy-harvesting prospects, due to a delivered power that can be of the order of the quantum bound [R. S. Whitney, Phys. Rev. Lett. 112, 130601 (2014); Entropy 18, 208 (2016)], with a concomitant fair efficiency. To unveil its properties beyond the sequential quantum master equation, we apply a nonequilibrium noncrossing approximation in the Keldysh Green's function formalism, and a quantum master equation that includes cotunneling processes. Both approaches are rather qualitatively similar in a large operating regime where sequential tunneling alone fails.

Adverse effect of CdTe quantum dots on the cell membrane of Bacillus subtilis : Insight from microscopy

The aim of present work was to unveil the process of cell membrane disruption and analyze the adverse effect of CdTe quantum dots (QDs) on Bacillus subtilis isolated from soil. The minimum inhibitory concentration (MIC50) of CdTe was 0.45 μM. When bacterial cell was treated with CdTe QDs, firstly they interact with the cell and leads to membrane destabilization, as evident from the increase in anisotropy of treated cells. Confocal microscopy experiments reveal changes in the cell membrane integrity after 1 h of QD interaction, followed by internalization of the QDs after 2 h. Further, similar results were obtained by Atomic Force Microscopy, Scanning Electron Microscopy and Transmission Electron Microscopy. After internalization, the anti-oxidative defense system gets activated as sensed by elevated level of superoxide dismutase and catalase after 2 h of QD incubation with cells. Cell lysis occurs, when stress level increases beyond the capacity of anti-oxidative defense system.

Fate of the spin- 12 Kondo effect in the presence of temperature gradients

We consider a strongly interacting quantum dot connected to two leads held at quite different temperatures. Our aim is to study the behavior of the Kondo effect in the presence of large thermal biases. We use three different approaches, namely, a perturbation formalism based on the Kondo Hamiltonian, a slave-boson mean-field theory for the Anderson model at large charging energies and a truncated equation-of-motion approach beyond the Hartree-Fock approximation. The two former formalisms yield a suppression of the Kondo peak for thermal gradients above the Kondo temperature, showing a remarkably good agreement despite their different ranges of validity. The third technique allows us to analyze the full density of states within a wide range of energies. Additionally, we have investigated the quantum transport properties (electric current and thermocurrent) beyond linear response. In the voltage-driven case, we reproduce the split differential conductance due to the presence of different electrochemical potentials. In the temperature-driven case, we observe a strongly nonlinear thermocurrent as a function of the applied thermal gradient. Depending on the parameters, we can find nontrivial zeros in the electric current for finite values of the temperature bias. Importantly, these thermocurrent zeros yield direct access to the system's characteristic energy scales (Kondo temperature and charging energy).

Thermoelectric properties of an interacting quantum dot based heat engine

We study the thermoelectric properties and heat-to-work conversion performance of an interacting, multi-level quantum dot (QD) weakly coupled to electronic reservoirs. We focus on the sequential tunneling regime. The dynamics of the charge in the QD is studied by means of master equations for the probabilities of occupation. From here we compute the charge and heat currents in the linear response regime. Assuming a generic multi-terminal setup, and for low temperatures (quantum limit), we obtain analytical expressions for the transport coefficients which account for the interplay between interactions (charging energy) and level quantization. In the case of systems with two and three terminals we derive formulas for the power factor Q and the figure of merit ZT for a QD-based heat engine, identifying optimal working conditions which maximize output power and efficiency of heat-to-work conversion. Beyond the linear response we concentrate on the two-terminal setup. We first study the thermoelectric non-linear coefficients assessing the consequences of large temperature and voltage biases, focusing on the breakdown of the Onsager reciprocal relation between thermopower and Peltier coefficient. We then investigate the conditions which optimize the performance of a heat engine, finding that in the quantum limit output power and efficiency at maximum power can almost be simultaneously maximized by choosing appropriate values of electrochemical potential and bias voltage. At last we study how energy level degeneracy can increase the output power.

Enantioselective cytotoxicity of ZnS:Mn quantum dots in A549 cells.

Chirality strongly influences many biological properties of materials, such as cell accumulation, enzymatic activity, and toxicity. In the past decade, it has been shown that quantum dots (QDs), fluorescent semiconductor nanoparticles with unique optical properties, can demonstrate optical activity due to chiral ligands bound on their surface. Optically active QDs could find potential applications in biomedical research, therapy, and diagnostics. Consequently, it is very important to investigate the interaction of QDs capped with chiral ligands with living cells. The aim of our study was to investigate the influence of the induced chirality of Mn-doped ZnS QDs on the viability of A549 cells. These QDs were stabilized with D- and L-cysteine using a ligand exchange technique. The optical properties of QDs were studied using UV-Vis, photoluminescence (PL), and circular dichroism (CD) spectroscopy. The cytotoxicity of QDs was investigated by high content screening analysis. It was found that QDs stabilized by opposite ligand enantiomers, had identical PL and UV-Vis spectra and mirror-imaged CD spectra, but displayed different cytotoxicity: QDs capped with D-cysteine had greater cytotoxicity than L-cysteine capped QDs.

Nonlinear charge and energy dynamics of an adiabatically driven interacting quantum dot

We formulate a general theory to study the time-dependent charge and energy transport of an adiabatically driven interacting quantum dot in contact to a reservoir for arbitrary amplitudes of the driving potential. We study within this framework the Anderson impurity model with a local ac gate voltage. We show that the exact adiabatic quantum dynamics of this system is fully determined by the behavior of the charge susceptibility of the frozen problem. At $T=0$, we evaluate the dynamic response functions with the numerical renormalization group (NRG). The time-resolved heat production exhibits a pronounced feature described by an instantaneous Joule law characterized by an universal resistance quantum $R_0=h/(2 e^2)$ for each spin channel. We show that this law holds in non-interacting as well as in the interacting system and also when the system is spin-polarized. In addition, in the presence of a static magnetic field, the interplay between many-body interactions and spin polarization leads to a non-trivial energy exchange between electrons with different spin components.

Dynamical Coulomb blockade of thermal transport

The role of energy exchange between a quantum system and its environment is investigated from the perspective of the Onsager conductance matrix. We consider the thermoelectric linear transport of an interacting quantum dot coupled to two terminals under the influence of an electrical potential and a thermal bias. We implement in our model the effect of coupling to electromagnetic environmental modes created by nearby electrons within the P(E)-theory of dynamical Coulomb blockade. Our findings relate the lack of some symmetries among the Onsager matrix coefficients with an enhancement of the efficiency at maximum power and the occurrence of the heat rectification phenomenon.