Interacting Quantum Dot Research Articles

Thermoelectric cooling of a finite reservoir coupled to a quantum dot

We investigate nonequilibrium transport of charge and heat through an interacting quantum dot coupled to a finite electron reservoir. Both the quantum dot and the finite reservoir are coupled to conventional electric contacts, i.e., infinite electron reservoirs, between which a bias voltage can be applied. We develop a phenomenological description of the system, combining a rate equation for transport through the quantum dot with standard expressions for bulk transport between the finite and infinite reservoirs. The finite reservoir is assumed to be in a quasiequilibrium state with a time-dependent chemical potential and temperature which we solve for self-consistently. We show that the finite reservoir can have a large impact on the stationary state transport properties, including a shift and broadening of the Coulomb diamond edges. We also demonstrate that there is a region around the conductance lines where a heat current flows out of the finite reservoir. Our results reveal the dependence of the temperature that can be reached by this thermoelectric cooling on the system parameters, in particular the coupling between the finite and infinite reservoirs and additional heat currents induced by electron-phonon couplings, and can thus serve as a guide for experiments on quantum-dot-enabled thermoelectric cooling of finite electron reservoirs. Finally, we study the full dynamics of the system, with a particular focus on the timescales involved in the thermoelectric cooling. Published by the American Physical Society 2024

Manipulation of defect state emission in Zn chalcogenide quantum dots and their effects on chlorophyll spectral response

Water soluble Zn based quantum dots (QDs) are of interest due to their biocompatibility and less toxic features. They have been frequently used in studies related to biotechnology, especially in agriculture studies. However, to control the optical properties of Zn based QDs has still been a challenge. In this work, the defect state emission of ZnSe QDs was successfully controlled through two different routes; 1) By creating a sulfur rich outer region around the Se rich core 2) By changing the capping agent. Gradient alloyed ZnSeS QDs with Se rich core and S rich outer region were successfully synthesized with two different capping agents; N-Acetyl-L-Cysteine (NAC) and 3-Mercaptopropionic Acid (3-MPA). The contribution of emission originated from surface-defects almost disappeared in NAC capped ZnSeS QDs, with causing a significant increase in photoluminescence quantum yield. The interaction between Zn based QDs with chlorophyll molecules was also investigated. The absorption capacity of chlorophylls significantly enhanced upon interaction with 3-MPA capped ZnSeS QDs. Also, the spectral response of chlorophylls could be modulated through interaction with 3-MPA capped ZnSeS QDs, which could be manipulated by using ZnSeS QDs with different chemical composition. Our results indicated that ZnSeS QDs have potential to be used in agriculture, which could act as a modulator of light-harvesting capacity of chlorophylls. The ability to modulate chlorophyll spectral responses through QD interaction opens new possibilities for optimizing light utilization in photosynthetic organisms, thereby contributing to enhanced crop yields and more efficient use of light energy in natural and artificial ecosystems.

Josephson current through the SYK model

We calculate the equilibrium Josephson current through a disordered interacting quantum dot described by a Sachdev-Ye-Kitaev model fully contacted by two BCS superconductors, such that all modes of the dot contribute to the coupling, which encodes hopping and spin-flip processes. We show that, at zero temperature and at the conformal limit, i.e. in the strong interacting limit, the Josephson current is suppressed by UU, the strength of the interaction, as ln(U)/U and becomes universal, namely it gets independent on the superconducting gap. At finite temperature, instead, it depends on the ratio between the gap and the temperature. A proximity effect exists but the self-energy corrections induced by the coupling with the superconducting leads seem subleading as compared to the interaction self-energy and the tunneling matrix for large number of particles. Finally we compare the results of the original four-fermion model with those obtained considering zero interaction, two-fermions and a generalized qq-fermion model.

Ligand Controls Excited Charge Carrier Dynamics in Metal-Rich CdSe Quantum Dots: Computational Insights.

Small metal-rich semiconducting quantum dots (QDs) are promising for solid-state lighting and single-photon emission due to their highly tunable yet narrow emission line widths. Nonetheless, the anionic ligands commonly employed to passivate these QDs exert a substantial influence on the optoelectronic characteristics, primarily owing to strong electron-phonon interactions. In this work, we combine time-domain density functional theory and nonadiabatic molecular dynamics to investigate the excited charge carrier dynamics of Cd28Se17X22 QDs (X = HCOO-, OH-, Cl-, and SH-) at ambient conditions. These chemically distinct but regularly used molecular groups influence the dynamic surface-ligand interfacial interactions in Cd-rich QDs, drastically modifying their vibrational characteristics. The strong electron-phonon coupling leads to substantial transient variations at the band edge states. The strength of these interactions closely depends on the physicochemical characteristics of passivating ligands. Consequently, the ligands largely control the nonradiative recombination rates and emission characteristics in these QDs. Our simulations indicate that Cd28Se17(OH)22 has the fastest nonradiative recombination rate due to the strongest electron-phonon interactions. Conversely, QDs passivated with thiolate or chloride exhibit considerably longer carrier lifetimes and suppressed nonradiative processes. The ligand-controlled electron-phonon interactions further give rise to the broadest and narrowest intrinsic optical line widths for OH and Cl-passivated single QDs, respectively. Obtained computational insights lay the groundwork for designing appropriate passivating ligands on metal-rich QDs, making them suitable for a wide range of applications, from blue LEDs to quantum emitters.

Formation of hybrid nanostructures based on Zn0.5Cd0.5S quantum dots and silver nanoparticles for nonlinear optical applications in the near ultraviolet

The goal of this study was to establish optimal conditions for the formation of hybrid nanostructures based on quantum dots and metal nanoparticles with a nonlinear optical response in the near ultraviolet. The relevance of this study is confirmed by the need to create passive devices for controlling the parameters of laser radiation in the presence of semiconductor colloidal quantum dots (QDs) and plasmonic nanoparticles (NPs). Manifestations of interaction in the nonlinear optical response of Zn0.5Cd0.5S QDs and spherical Ag NPs (10 nm) in the field of laser pulses of 10 ns duration at a probing radiation wavelength of 355 nm have been established using the Z-scan method. Manifestations of the formation of hybrid nanostructures have been established using transmission electron microscopy and optical absorption and luminescence spectroscopy. The interaction of colloidal QDs and NPs was manifested as the recombination luminescencequenching of the former with a peak at a wavelength of 450-480 nm. For ensembles of colloidal Zn0.5Cd0.5S QDs with an average size (2.0, 2.2, 2.4 nm), nonlinear refraction (defocusing) of 10 ns laser pulses in the near ultraviolet (355 nm) was established, the coefficient of which increased with increase in QDs. It has been established that during the interaction of Zn0.5Cd0.5S QDs with Ag NPs, the suppression of nonlinear refraction was observed against the background of a twelvefold increase in the nonlinear absorption coefficient. It was concluded that the most probable reason for the observed changes in the nonlinear optical response is the polarizing effect of plasmonic Ag NPs

Conductance and thermopower fluctuations in interacting quantum dots

Conductance and thermopower fluctuations in interacting quantum dots

Hidden Symmetry in Interacting-Quantum-Dot-Based Multiterminal Josephson Junctions.

We study a multiterminal Josephson junction based on an interacting quantum dot coupled to n superconducting BCS leads. Using an Anderson type model of a local level with an arbitrary on-site Coulomb repulsion, we uncover its surprising equivalence with an effective two-terminal junction with symmetric couplings to appropriately phase-biased leads. Regardless of the strength of the Coulomb interaction, this hidden symmetry enables us to apply well-established numerical and theoretical tools for exact evaluation of various physical quantities, and imposes strict relations among them. Focusing on three-terminal devices, we then demonstrate several phenomena such as the existence of the finite energy band crossings and superconducting transistor and diode effects, as well as current phase relation modulation.

Modulating spectral response of raw photosynthetic pigments via ternary cadmium chalcogenide quantum dots: simultaneous enhancement at green spectrum and inhibition at UV region.

Photosynthesis relies on the absorption of sunlight by photosynthetic pigments (PPs) such as chlorophylls and carotenoids. While these pigments are outstanding at harvesting light, their natural structure restricts their ability to harvest light at specific wavelengths. In this study, Oleic acid-capped CdSeS and CdTeS ternary quantum dots (QDs) were synthesized using a novel two-phase synthesis method. Then, these QDs were used to interact with raw PPs, a mixture of chlorophylls and carotenoids isolated from spinach. Our findings revealed the following: (1) Interacting QDs with raw PPs effectively inhibited the chlorophyll fluorescence of the pigments upon excitation in UV light region (250-400nm) without causing any damage to their structure. (2) By forming an interaction with QDs, the chlorophyll fluorescence of raw PPs could be induced through excitation with green-light spectrum. (3) The composition of the QDs played a fundamental role in their interaction with PPs. Our study demonstrated that the photophysical properties of isolated PPs could be modified by using cadmium-based QDs by preserving the structure of the pigments themselves.

Quantum dots interacting with a non-classical field under Kerr-phase modulation as a resource for repeatable quantum algorithms

An analytical solution describing the dynamics of a hybrid system comprising an interacting quantum dot and a quantum electromagnetic field in the presence of Kerr nonlinearity is obtained. A completely new regime of interaction is found. It provides stable periodically repeating dynamics for the total bipartite system and for the quantum dot excitation, accompanied by full and pure revivals. This is even observed when the initial field state is in a squeezed vacuum. Periodical strong entanglement and full disentanglement between the interacting subsystems are demonstrated. The obtained regime forms the basis for the development of quantum information algorithms and photon–matter interfaces involving these hybrid systems. The formation of non-Gaussian field states is revealed. Methods to control and manage the specific features of the found pure and mixed states of the considered subsystems are developed.

Effective spin filtering in correlated semiconductor nanostructures

A new theoretical concept of an electrically controllable single-electron spin filter (polarizator) based on the exchange interaction in the system of interacting quantum dots or impurity atoms is proposed. The sign of the spin polarization of the current flowing through the device can be effectively controlled in two ways (i) by changing the applied bias and (ii) by tuning the tunnel coupling via an external gate. The minimal realization involves three bound state levels coupled to the contact leads. One of these levels is occupied by a single electron with a certain spin and the two-electron occupation is prohibited by a strong on-site Coulomb repulsion. Interestingly, while the spin polarization of this state is fixed, the sign of the single-electron current spin polarization flowing between the contacts through two consistent bound state levels can be switched.

Electrical and Thermal Bias‐Driven Negative Magnetoresistance Effect in an Interacting Quantum Dot

Spin‐dependent electron transport is theoretically studied for a system with an interacting quantum dot sandwiched between a pair of ferromagnetic electrodes. By separately applying an electrical bias or a temperature gradient across the junction, a spin‐polarized current can be obtained and controlled by tuning the gate voltage. Interestingly, regardless of whether the electron transport is driven by the bias voltage or temperature difference, the current in the device always exhibits negative magnetoresistance under the control of the gate voltage. Such magnetoresistance anomalies in the current profile originate from the spin‐selective tunneling channels in quantum dots, which have been proven experimentally feasible. This device scheme is compatible with current technologies and has potential applications in spintronics or spin caloritronics.

Transient transport spectroscopy of an interacting quantum dot proximized by a superconductor: Charge and heat currents after a switch

Transient transport spectroscopy of an interacting quantum dot proximized by a superconductor: Charge and heat currents after a switch

Spin diode and spin valve based on an interacting quantum dot coupled with nonmagnetic electrodes

How to control the charge and spin in nanodevices is an important topic in spintronics. In this letter, we theoretically propose a spin diode and spin valve (SV) device controlled by all-electrical means, which is composed of a quantum dot (QD) coupled to a pair of nonmagnetic electrodes. When both electric charge bias and spin bias exist within the device, the I–V curves of this device exhibit an asymmetric distribution, and this asymmetry can be manipulated by the gate voltage. More interestingly, if we apply an external magnetic field on the QD, we can observe significant high- and low-resistance state switching with respect to the magnetic field, which can function as a SV device. This device scheme can be compatible with current technologies and has potential applications in spintronics or quantum processing.

Quantum Dot Metal Salt Interactions Unraveled by the Sphere of Action Model.

Postsynthetic metal salt treatments are frequently employed in the luminescence enhancement of quantum dots (QDs); however, its microscopic picture remains unclear. CsPbBr3-QDs, featuring strong excitonic absorption and high photoluminescence (PL) quantum yield, are ideal QDs to unravel the intricate interaction between QDs and such surface-bound metal salts. Herein, we study this interaction based on the controlled PL quenching of CsPbBr3-QDs with BiBr3. Upon the addition of BiBr3, an instant and complete PL quenching is observed, which can be fully recovered after the addition of an excess of PbBr2. This, together with the complete preservation of the excitonic absorption suggests a surface-driven adsorption equilibrium. Additionally, time-resolved studies reveal a non-homogeneous surface trap formation. Based on the so-called sphere of action model for the adsorption process, we show that already a single BiBr3 adsorption suffices to completely quench a QD's luminescence. This approach is expanded to analyze size-, ligand-, and metal-dependent quenching dynamics. Facet junctions are identified as regions of enhanced surface reactivity. A Langmuir-type ligand coverage is exposed with a strong impact on adsorption. Our results provide a detailed mechanistic insight into postsynthetic interaction of QDs with metal salts, opening pathways for future surface manipulations.

Quantum thermodynamics with fast driving and strong coupling via the mesoscopic leads approach

Understanding the thermodynamics of driven quantum systems strongly coupled to thermal baths is a central focus of quantum thermodynamics and mesoscopic physics. A variety of different methodological approaches exist in the literature, all with their own advantages and disadvantages. The mesoscopic leads approach was recently generalised to steady state thermal machines and has the ability to replicate Landauer B\"uttiker theory in the non-interacting limit. In this approach a set of discretised lead modes, each locally damped, provide a markovian embedding for the baths. In this work we further generalise this approach to incorporate an arbitrary time dependence in the system Hamiltonian. Following a careful discussion of the calculation of thermodynamic quantities we illustrate the power of our approach by studying several driven mesoscopic examples coupled to finite temperature fermionic baths, replicating known results in various limits. In the case of a driven non interacting quantum dot we show how fast driving can be used to induce heat rectification.

Thermoelectric efficiency in multiterminal quantum thermal machines from steady-state density functional theory

The multi-terminal generalization of the steady-state density functional theory for the description of electronic and thermal transport (iq-DFT) is presented. The linear response regime of the framework is developed leading to exact expressions for the many-body transport coefficients and thermoelectric efficiency purely in terms of quantities accessible to the framework. The theory is applied to a multi-terminal interacting quantum dot in the Coulomb blockade regime for which accurate parametrizations of the exchange-correlation kernel matrix are given. The thermoelectric efficiency and output power of the multi-terminal system are studied. Surprisingly, the strong-interaction limit of these quantities can be understood in terms of the non-interacting one.

Solution of master equations by fermionic-duality: Time-dependent charge and heat currents through an interacting quantum dot proximized by a superconductor

We analyze the time-dependent solution of master equations by exploiting fermionic duality, a dissipative symmetry applicable to a large class of open systems describing quantum transport. Whereas previous studies mostly exploited duality relations after partially solving the evolution equations, we here systematically exploit the invariance under the fermionic duality mapping from the very beginning when setting up these equations. Moreover, we extend the resulting simplifications -so far applied to the local state evolution- to non-local observables such as transport currents. We showcase the exploitation of fermionic duality for a quantum dot with strong interaction -covering both the repulsive and attractive case- proximized by contact with a large-gap superconductor which is weakly probed by charge and heat currents into a wide-band normal-metal electrode. We derive the complete time-dependent analytical solution of this problem involving non-equilibrium Cooper pair transport, Andreev bound states and strong interaction. Additionally exploiting detailed balance we show that even for this relatively complex problem the evolution towards the stationary state can be understood analytically in terms of the stationary state of the system itself via its relation to the stationary state of a dual system with inverted Coulomb interaction, superconducting pairing and applied voltages.

Photoinduced Modulation of the Dielectric Permittivity in a System of Interacting Quantum Dots in an External Electric Field

Photoinduced Modulation of the Dielectric Permittivity in a System of Interacting Quantum Dots in an External Electric Field

The Effects of 2D Dissipative Tunneling for the Recombination Radiation Spectra of Interacting Quantum Dots in an External Electric Field

The Effects of 2D Dissipative Tunneling for the Recombination Radiation Spectra of Interacting Quantum Dots in an External Electric Field

Thermoelectric Rectification and Amplification in Interacting Quantum-Dot Circuit-Quantum-Electrodynamics Systems.

Thermoelectric rectification and amplification were investigated in an interacting quantum-dot circuit-quantum-electrodynamics system. By applying the Keldysh nonequilibrium Green's function approach, we studied the elastic (energy-conserving) and inelastic (energy-nonconserving) transport through a cavity-coupled quantum dot under the voltage biases in a wide spectrum of electron-electron and electron-photon interactions. While significant charge and Peltier rectification effects were found for strong light-matter interactions, the dependence on electron-electron interaction could be nonmonotonic and dramatic. Electron-electron interaction-enhanced transport was found under certain resonance conditions. These nontrivial interaction effects were found in both linear and nonlinear transport regimes, which manifested in charge and thermal currents, rectification effects, and the linear thermal transistor effect.