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Pavel A. Frantsuzov

Publications and source records attributed to Pavel A. Frantsuzov.

9 recordsLinked to original sources

To Blink or Not to Blink? A New Criterion to Quantify Luminescence Blinking

Colloidal semiconductor quantum dots are promising materials for numerous applications due to their tunable emission and high quantum yields. However, emission instability in the form of luminescence blinking remains a significant obstacle to their practical implementation. While recent advances in synthesis and surface engineering have demonstrated partial or complete blinking suppression, the quantitative assessment of the "quality" of this suppression remains challenging. Existing criteria typically rely on threshold-based classification into ON and OFF states, which becomes inherently ambiguous owing to the continuous distribution of emission intensities in single quantum dots. Here, we propose a threshold-free two-dimensional quantitative criterion based on the variance of the recombination rate and the relative quantum yield, both of which can be extracted from standard time-correlated single-photon counting measurements. We validate the criterion using simulated blinking trajectories covering all major blinking mechanisms and demonstrate that it cleanly separates them into distinct regions of the two-dimensional parameter space while providing a quantitative measure of the degree of suppression. This approach directly quantifies the temporal stability of emission without requiring arbitrary state definitions, thereby providing a robust metric for comparing different blinking suppression strategies.

cond-mat.mes-hall↗

Quantum field theory approach for multistage chemical kinetics in liquids

Reaction-diffusion processes play an important role in a variety of physical, chemical, and biological systems. Conventionally, the kinetics of these processes are described by the law of mass action. However, there are various cases where these equations are insufficient. A fundamental challenge lies in accurately accounting for the microscopic correlations that inevitably arise in bimolecular reactions. While approaches to describe microscopic correlations in many specific cases exist, no general theory for multistage reactions has been established. In this article, we apply the quantum field theory approach to derive kinetic equations for general multistage reactive systems termed CMET (complete modified encounter theory). CMET can be formulated as a set of coupled partial differential equations that can be easily integrated numerically, thereby serving as a versatile tool for investigating reaction-diffusion processes. Across multiple case studies, we demonstrated that CMET reproduces the kinetics predicted by many other theories within their respective scopes of applicability.

physics.chem-ph↗

Model of luminescence and delayed luminescence correlated blinking in single CsPbBr$_3$ nanocrystals

Cesium lead halide nanocrystals and quantum dots are prominent materials for different types of applications because of their remarkable photophysical properties. However, they are also known to exhibit the same effects observed for non-perovskite colloidal semiconductor quantum dots such as blinking, photobleaching, delayed luminescence, etc. In this study we reveal the correlations between fast and delayed emission components for both the intensity and characteristic decay time for single CsPbBr$_3$ nanocrystals. In order to explain the phenomena observed, we propose a novel model of single CsPbBr$_3$ nanocrystals luminescence blinking based on the hypothesis of slow variations in the electron-phonon coupling.

cond-mat.mtrl-sci↗

The model of photoswitching in lead-halide perovskite microcrystals

A theoretical model for the recently discovered effect of all-optical photoswitching in lead tribromide perovskite single microcrystals is proposed. The model takes into account the spatially distributed kinetics of the charge carrier recombination and the creation/destruction of trap states. It successfully reproduces the key features of the photoswitching phenomenon.

cond-mat.mtrl-sci↗

Contribution of electron-phonon coupling to the luminescence spectra of single colloidal quantum dots

Luminescence spectroscopy experiments were realized for single colloidal quantum dots CdSe/ZnS in a broad temperature range above room temperature in a nitrogen atmosphere. Broadening and shifts of spectra due to the temperature change as well as due to spectral diffusion processes were detected and analyzed. A linear correlation between the positions of maxima and the squared linewidths of the spectra was found. This dependence was explained by a model which takes into account the slow variation of the electron-phonon coupling strength.

cond-mat.mes-hall↗

Models of semiconductor quantum dots blinking based on spectral diffusion

Three models of single colloidal quantum dot emission fluctuations (blinking) based on spectral diffusion were considered analytically and numerically. It was shown that the only one of them, namely the Frantsuzov and Marcus model reproduces the key properties of the phenomenon. The other two models, the Diffusion-Controlled Electron Transfer (DCET) model and the Extended DCET model predict that after an initial blinking period, most of the QDs should become permanently bright or permanently dark which is significantly different from the experimentally observed behavior.

cond-mat.stat-mech↗

Model of fluorescence intermittency of single colloidal semiconductor quantum dots using multiple recombination centers

We present a new physical model resolving a long-standing mystery of the power-law distributions of the blinking times in single colloidal quantum dot fluorescence. The model considers the non-radiative relaxation of the exciton through multiple recombination centers. Each center is allowed to switch between two quasi-stationary states. We point out that the conventional threshold analysis method used to extract the exponents of the distributions for the on-times and off-times has a serious flaw: The qualitative properties of the distributions strongly depend on the threshold value chosen for separating the on and off states. Our new model explains naturally this threshold dependence, as well as other key experimental features of the single quantum dot fluorescence trajectories, such as the power-law power spectrum (1/f noise).

cond-mat.stat-mech↗

Explanation of quantum dot blinking without long-lived trap hypothesis

A simple model explaining the experimental data on QDs luminescence blinking is suggested. The model does not assume the presence of the long-lived electron traps. The bleaching of the QD luminescence is a result of the Auger assisted radiationless relaxation of the excitation through the deep surface states. Possible ways of the experimental verification of the model are discussed.

cond-mat.mes-hall↗

Thermodynamics and equilibrium structure of Ne_38 cluster: Quantum Mechanics versus Classical

The equilibrium properties of classical LJ_38 versus quantum Ne_38 Lennard-Jones clusters are investigated. The quantum simulations use both the Path-Integral Monte-Carlo (PIMC) and the recently developed Variational-Gaussian-Wavepacket Monte-Carlo (VGW-MC) methods. The PIMC and the classical MC simulations are implemented in the parallel tempering framework. The VGW method is used to locate and characterize the low energy states of Ne_38, which are then further refined by PIMC calculations. Unlike the classical case, the ground state of Ne_38 is a liquid-like structure. Among the several liquid-like states with energies below the two symmetric states (O_h and C_5v), the lowest two exhibit strong delocalization over basins associated with at least two classical local minima. Because the symmetric structures do not play an essential role in the thermodynamics of Ne_38, the quantum heat capacity is a featureless curve indicative of the absence of any structural transformations. Good agreement between the two methods, VGW and PIMC, is obtained.

physics.chem-ph↗