Polaron System Research Articles

Anomalous Polarons in Two-Dimensional Organometallic Perovskite Ferroelectric.

The concept of ferroelectric polarons is proposed to partially explain the exceptional optoelectronic properties observed in lead halide perovskites (LHPs). It is intriguing but unclear how this proposal, which involves local or transient polarizations, applies in general to 2D LHPs with long-range ferroelectricity. Here, this work presents a pioneering time-domain experimental investigation of polarons in ferroelectric (IA)2(MA)2Pb3Br10 (IMPB; IA is isoamylammonium and MA is methylammonium) using transient absorption spectroscopy. Compared to non-ferroelectric LHPs, IMPB exhibits several distinct polaronic properties closely associated with macroscopic polarizations of ferroelectricity, including a prolonged polaron formation time (≈1.1ps), a Stark splitting of the bleaching (≈63 meV), and a giant polaron Mott density (≈7.6 × 1018 cm-3). These findings broaden the realm of 2D polaron systems and reveal the decisive role of static/unidirectional polarizations on polaron physics in 2D LHPs.

Scaling Behavior in the Spectral and Power Density Dependent Photovoltaic Response of Hot Polaronic Heterojunctions

AbstractStrongly correlated manganites can be considered as model systems for the study of photovoltaic harvesting of hot polarons that can be excited from the electronically ordered ground state. In order to gain basic understanding of hot polaron harvesting, the deviations of the photovoltaic response of a heterojunction with polaronic absorber from a conventional semiconductor are analyzed. Specifically, the spectral and photon power density dependence of the open circuit voltage Uoc and the short circuit current density Jsc in heterojunctions consisting of orbital ordered Pr1‐xCaxMnO3 (x = 0.1, PCMO) thin films epitaxially grown on single crystalline (100) SrTiO3 (STO) and Nb‐doped (100) SrTiO3 (STNO) substrates are investigated. The observed behavior is fundamentally different from conventional solar cells, in which Uoc is limited by fast carrier relaxation to the band edges. Whereas the spectral and photon power dependence of Uoc of conventional semiconductor junctions is well described by the Shockley‐Queisser (SQ) theory, the hot polaron junctions surprisingly show a scaling law behavior of Uoc. Such scaling laws otherwise apply to equilibrium order parameters in second‐order phase transitions. It is concluded that its physical origin is the unique dependence of the quasi‐Fermi level splitting on temperature, photon energy, and power density in a hot polaron system.

Tensor-Train Format Hierarchical Equations of Motion Formalism: Charge Transfer in Organic Semiconductors via Dissipative Holstein Models.

Hierarchical Equations of Motion (HEOM) in the Tensor-Train (TT) representation is applied to study the charge-transfer dynamics in organic semiconductors (OSCs). The theoretical formulation as well as the basic computational aspects of HEOM-TT are discussed in detail. Charge transfer in OSCs is modeled using dissipative polaronic models that incorporate the effects of both high- and low-frequency molecular vibrations, and it is simulated in a fully quantum and nonperturbative manner, which has not been studied intensively. The capability of treating complex electron-vibrational systems is examined by analyzing and comparing the numerical behavior of the time-dependent variational approach and the time-Alternating Minimal Energy methods and by calculating the current autocorrelation function and diffusivity across various models. Our results indicate that the HEOM-TT framework offers a robust tool for the detailed analysis of complex polaronic systems, suggesting its potential for broader applications.

A multiferroic coupling mechanism in the polar interface region of GaN-ZnO heterojunction: A first-principle study

In this paper, the electronic structure and ferroelectric-ferromagnetic coupling properties of Y-doped and vacancy-containing GaN-ZnO heterojunctions are systematically investigated by using the generalized gradient approximation + U (GGA + U) method within the framework of density functional theory. The results reveal that in systems with vacancy defects, the magnetism is generated by the spin polarization of unpaired electrons induced by cationic vacancies, and the magnetic moment of the system is related to the number of unpaired electrons. However, in systems containing interstitial Y-doping, the s-state and d-state electrons of the Y-doped elements are coupled by orbital hybridization to form bound magnetic polarons. Compared with the system containing vacancies, the bound magnetic polaron systems have better stability, although the magnetic moments are relatively small and the total magnetic moment is limited by the concentration of bound magnetic polarons. And the modulation of different magnetic changes can be achieved in different polar interfaces by adjusting the electric polarization intensity of the bound magnetic polaron systems.

Universal many-body properties of one-dimensional mass-imbalanced highly polarized Fermi gases

We investigate the universal properties of mass-imbalanced highly polarized Fermi gases in one-dimensional scenarios. By treating the mass ratio as a parameter, we delve into the binding energy, quasiparticle residue, and correlation functions of the systems. We provide a thorough momentum distribution for impurities and spin-up atoms within the Fermi sea. When the impurity mass is infinite, we discover that the quasiparticle residue approaches to zero and the systems exhibit the signature of the Anderson orthogonality catastrophe in strong coupling regime. We observe an increase in Tan contact under large mass ratios and study density correlations by applying Fourier transform. Crucially, we demonstrate the existence of the molecular state in one-dimensional polaron system with strong attractive interactions, unlike previous conclusions.

Polaronic state of conducting oligomer as a new approach to design non-lieaner optical materials: A case study of oligofurans

The geometric, electronic and nonlinear optical properties of neutral and polaron based oligofurans are studied comparatively. We have reported the role of polaron to trigger the nonlinear optical response of oligofurans (nFu). The polaron based oligomers show excellent opto-electronic properties. The effect of polaron on nFu* chains is measured by electronic properties i.e (ionization energy, electron affinity, band gap) and global reactivity descriptors like softness, hardness and chemical potential than their neutral counterpart. An interesting trends of reactivity descriptors have been observed. Lower band gaps (EH-L = 4.66 and 4.41 eV) are observed for polaronic systems as compared to their neutral counterpart. On the other hand, the TD-DFT study further demonstrated that, as the size of chain increases, the absorption maxima (λmax) also increases with significant reduction in excitation energies (ΔE). Furthermore, the nonlinear optical response is confirmed through the linear polarizability (αo), static first order hyperpolarizability (βo) and dynamic (frequency denepndent) hyperpolarizability. Electric filed induced second harmonic generation (EFISHG) and electro-optic pockle effect (EOPE) at 532 nm and 1064 nm, commonly used lasers frequencies have also been employed. Our results showed that the maximum hyperpolarizabilities are observed for polaron based 7Fu* and 9Fu* i.e 1.3 × 104, and 3.1 × 104 au. This study concluded that these polaron based organic polymers (nFu*) are useful as an efficient NLO material with vast applications in different fields.

Correlation functions and polaron-molecule crossover in one-dimensional attractive Fermi gases

We study the correlation functions in a one-dimensional attractive Fermi polaron system of spin-1/2 Fermi gas with one flipped spin as an impurity immersed in the fully polarized spin-up media. By means of the exact Bethe ansatz wave function with string solutions for the momentum, we manage to explicitly deduce the asymptotic form of the correlation functions in the infinite attractive limit and show that the system undergoes a polaron-molecule crossover when the attraction grows. The correlation functions in the infinite attractive limit can be decomposed into the free fermion term with the number of particles reduced by one and the molecular term indicated by the emergence of a sharp peak or dip in the central area of the correlation. These analytical results are checked by the numerical Monte Carlo methods for multiple integrals. The calculation is further extended to the excited states, i.e., the super-Tonks-Girardeau gas, and there is no peak or dip found in the vicinity of the correlation center. Tan contact is found to be proportional to the cubic of the interaction strength and the total energy is verified to satisfy the Tan adiabatic theorem in the strong attraction regime.

Models of Polaron Transport in Inorganic and Hybrid Organic-Inorganic Titanium Oxides.

Polarons are a type of localized excess charge in materials and often form in transition metal oxides. The large effective mass and confined nature of polarons make them of fundamental interest for photochemical and electrochemical reactions. The most studied polaronic system is rutile TiO2 where electron addition results in small polaron formation through the reduction of Ti(IV) d0 to Ti(III) d1 centers. Using this model system, we perform a systematic analysis of the potential energy surface based on semiclassical Marcus theory parametrized from the first-principles potential energy landscape. We show that F-doped TiO2 only binds polaron weakly with effective dielectric screening after the second nearest neighbor. To tailor the polaron transport, we compare TiO2 to two metal-organic frameworks (MOFs): MIL-125 and ACM-1. The choice of MOF ligands and connectivity of the TiO6 octahedra largely vary the shape of the diabatic potential energy surface and the polaron mobility. Our models are applicable to other polaronic materials.

Engineering coexistence between free and trapped carriers via extrinsic polarons

The transition between delocalized and localized electronic configurations is a characteristic property of all small-polaron systems. In this study, we explore a doping approach by which the coexistence between delocalized and localized electronic states may be precisely tuned within extrinsic polaron systems. Through comprehensive ab initio calculations employing hybrid functionals, for which Ti-doped ${\mathrm{SnO}}_{2}$ is selected as a model system, it is demonstrated how strain and alloying can be utilized to achieve a high degree of control over the activation energetics separating localized and delocalized electronic states. By means of a phenomenological tight-binding analysis of our ab initio results, it is shown that two physical parameters play a dominant role in the associated transition physics: (1) the dopant electronic offset ${\mathrm{\ensuremath{\Delta}}}_{a}$, and (2) the dopant bandwidth $W$. Overall, this study presents an exciting route toward tailoring the coexistence between delocalized and localized states with a potentially much greater degree of control than is currently possible in intrinsic materials.

Electron removal spectral function of a polaron coupled to dispersive optical phonons

We explore the ground state and thermodynamic properties of the polaron coupled to quantum dispersive optical phonons in one spatial dimension. Calculations are performed using the finite--temperature Lanczos method augmented by a highly efficient construction of the variational Hilbert space. We focus on the electron removal spectral function as relevant for the angle-resolved photoemission experiments. We show that photoemission spectroscopy can be used to measure the phonon dispersion relation in a dilute system of polarons. The spectral weight of observed phonon bands is proportional to the phonon contribution to the wavefunction at finite phonon momentum. In addition, we demonstrate that when removing an electron from a polaron ground state, the polaron band does not appear in the spectral function. The latter becomes observable only at elevated temperatures.

Ultrafast Spontaneous Localization of a Jahn-Teller Exciton Polaron in Two-Dimensional Semiconducting CrI3 by Symmetry Breaking.

The excited state species and properties in low-dimensional semiconductors can be completely redefined by electron-lattice coupling or a polaronic effect. Here, by combining ultrafast broadband pump-probe spectroscopy and first-principles GW and Bethe-Salpeter equation calculations, we show semiconducting CrI3 as a prototypical 2D polaronic system with characteristic Jahn-Teller exciton polaron induced by symmetry breaking. A photogenerated electron and hole in CrI3 localize spontaneously in ∼0.9 ps and pair geminately to a Jahn-Teller exciton polaron with elongated Cr-I octahedra, large binding energy, and an unprecedentedly small exciton-exciton annihilation rate constant (∼10-20 cm3 s-1). Coherent phonon dynamics indicates the localization is mainly triggered by the coherent nuclear vibration of the I-Cr-I out-of-plane stretch mode at 128.5 ± 0.1 cm-1. The excited state Jahn-Teller exciton polaron in CrI3 broadens the realm of 2D polaron systems and reveals the decisive role of coupled electron-lattice motion on excited state properties and exciton physics in 2D semiconductors.

Magnetic barrier and temperature effects on optical and dynamic properties of exciton-polaron in monolayers transition metal dichalcogenides

We theoretically investigate the properties of exciton-polaron moving through a magnetic barrier in monolayers (1Ls) transition metal dichalcogenides (TMDs): MoS 2 , WS 2 , MoSe 2 , and WSe 2 . We find that the exciton-polaron has the highest ground state energy in WS 2 and the lowest one in MoSe 2 . It is seen that the magnetic barrier stabilizes the excitonic polaron system subjected to thermal perturbation. We demonstrate that the entropy of the system is very sensitive to the type of monolayers TMDs, the length scale of the barrier, the temperature. We observe that the higher the magnetic length, the greater the disorder in exciton-polaron system and the highest entropy is in MoSe 2 . Also, the mobility and the lifetime of exciton-polaron decrease with the enhancement of the magnetic length. We observe the highest mobility and lifetime in WS 2 . Moreover, We show that the optical absorption appears when the photon energy is more than twice phonon energy and the absorption coefficient is higher when the incident photon induces an in plane field. MoS 2 presents the highest amplitude of optical absorption. • Amount the selected TMD the MoS 2 presents the highest amplitude of optical absorption. The exciton-polaron has the highest ground state energy in WS 2 and the lowest one in MoSe 2 . • The magnetic barrier stabilizes the exciton-polaron system subjected to thermal perturbation. • The entropy of the system is very sensitive to the type of monolayers TMDs, the length scale of the barrier and the temperature. • The higher the magnetic length, the greater the disorder in exciton-polaron system and the highest entropy is in MoSe 2 . • The mobility and the lifetime of exciton-polaron decrease with the enhancement of the magnetic length,these two parameters are stronger in WS 2. .

Coherent interaction and action–counteraction theory in small polaron systems, and ground state properties

Based on the coherent interaction and action–counteraction principles, we investigate the ground state properties for small polaron systems, the coherent-squeezed fluctuation correction, and the anomalous lattice quantum fluctuation, with the new variational generator containing correlated squeezed-coherent coupling and quantum entanglement. Noting that −2t is the T.B.A. energy, for the coherent interaction effect, we find the ground-state energy E 0 to be −2.428t, in which the coherent squeezed fluctuation correction −A 0 t is −0.463t (where t is the hopping integral, ω is the phonon frequency), with the electron–one-phonon coupling constant g = 1 and the electron–two-phonon coupling constant g 1 = −0.1. However, as a result of the action–counteraction effect, is −2.788t, but is −0.735t. As to the polaron binding energy (E P), for the coherent interaction effect, E P is −1.38ω, but for the action–counteraction effect, is −1.88ω. In particular, the electron–two-phonon interaction noticeably enlarges the coherent interaction and the coherent squeezed quantum fluctuation correction. By intervening with the quantum entanglement, the evolutions of the squeezed coherent state and the lattice quantum fluctuation begin to take control. At that time, we encounter a new quantum phase coherence phenomenon — the collapse and revival of inversion repeatedly for the coherent state in the entangled evolution.

Pattern Formation in One-Dimensional Polaron Systems and Temporal Orthogonality Catastrophe

Recent studies have demonstrated that higher than two-body bath-impurity correlations are not important for quantitatively describing the ground state of the Bose polaron. Motivated by the above, we employ the so-called Gross Ansatz (GA) approach to unravel the stationary and dynamical properties of the homogeneous one-dimensional Bose-polaron for different impurity momenta and bath-impurity couplings. We explicate that the character of the equilibrium state crossovers from the quasi-particle Bose polaron regime to the collective-excitation stationary dark-bright soliton for varying impurity momentum and interactions. Following an interspecies interaction quench the temporal orthogonality catastrophe is identified, provided that bath-impurity interactions are sufficiently stronger than the intraspecies bath ones, thus generalizing the results of the confined case. This catastrophe originates from the formation of dispersive shock wave structures associated with the zero-range character of the bath-impurity potential. For initially moving impurities, a momentum transfer process from the impurity to the dispersive shock waves via the exerted drag force is demonstrated, resulting in a final polaronic state with reduced velocity. Our results clearly demonstrate the crucial role of non-linear excitations for determining the behavior of the one-dimensional Bose polaron.

Quasiparticle Nature of the Bose Polaron at Finite Temperature.

The Bose polaron has attracted theoretical and experimental interest because the mobile impurity is surrounded by a bath that undergoes a superfluid-to-normal phase transition. Although many theoretical works have studied this system in its ground state, only a few analyze its behavior at finite temperature. We have studied the effect of temperature on a Bose polaron system performing abinitio path integral MonteCarlo simulations. This method is able to approach the critical temperature without losing accuracy, in contrast with perturbative approximations. We have calculated the polaron energy for the repulsive and attractive branches and we have observed an asymmetric behavior between the two branches. When the potential is repulsive, the polaron energy decreases when the temperature increases, and contrariwise for the attractive branch. Our results for the effective mass and the dynamical structure factor of the polaron show unambiguously that its quasiparticle nature disappears close to the critical temperature, in agreement with recent experimental findings. Finally, we have also estimated the fraction of bosons in the condensate as well as the superfluid fraction, and we have concluded that the impurity hinders the condensation of the rest of bosons.

Nature of the polaron-molecule transition in Fermi polarons

In this work, we explore the polaron and molecule physics by utilizing a unified variational ansatz with up to two particle-hole(p-h) excitations(V-2ph). We confirm the existence of a first-order transition in 3D and 2D Fermi polarons, and show that the nature of such transition lies in an energy competition between systems with different momenta ${\mathbf Q}=0$ and $|{\mathbf Q}|=k_F$, here ${\mathbf Q}$ is defined as the momentum of Fermi polaron system with respect to the Fermi sea of majority fermions (with Fermi momentum $k_F$). The literally proposed molecule ansatz is identified as an asymptotic limit of $|{\mathbf Q}|=k_F$ state in strong coupling regime, which implies a huge $SO(3)$(for 3D) or $SO(2)$ (for 2D) ground state degeneracy in this regime. The recognization of such degeneracy is crucially important for evaluating the molecule occupation in realistic systems with finite impurity density and at finite temperature. To compare with recent experiment of 3D Fermi polarons, we have calculated various physical quantities under the V-2ph framework and obtained results that are in good agreements with experimental data in the weak coupling and near resonance regime. Further, to check the validity of our conclusion in 2D, we have adopted a different variational method based on the Gaussian sample of high-order p-h excitations(V-Gph), and found the same conclusion on the nature of polaron-molecule transition therein. For 1D system, the V-2ph method predicts no sharp transition and the ground state is always at ${\mathbf Q}=0$ sector, consistent with exact Bethe ansatz solution. The presence/absence of polaron-molecule transition is analyzed to be closely related to the interplay effect of Pauli-blocking and p-h excitations in different dimensions.

Thermodynamic Properties and Optical Absorption of Polaron in Monolayer Graphene Under Laser Field

In this work, we use the variational method to investigate thermal properties and optical absorption of polaron in monolayer graphene under laser field. We have shown that the energies and the optical absorption of the system strongly depend on laser parameters and graphene characteristics. We found that the simple model adopted to calculate the optical absorption is enough accurate and interesting to investigate the optical absorption coefficient of the polarons in graphene. We observe that the laser assists the polaron in the optical absoprtion phenomenon. We observe that temperature, the coupling between electron and quantum of lattice vibration, laser parameters and wave number affect the disorder in the system. Contrary to temperature, the laser increases the disorder in the system. At low temperature, the polaronic system becomes decoherent for low values of wave number and gains coherency for high values of wave number. In addition, the coherence of the system is not significantly affected by the laser field but there is a considerable change at higher temperatures. We also observed that laser increases the capacity of system to store energy.

Analysis for vortex superposition state evolution of microcavity exciton polariton excited by ring-shaped pump

Owing to its light effective mass, polariton can easily realize Bose-Einstein condensates (BEC) and can also produce gyro effect under external drive. Therefore, it has a promising application prospect. Based on the Gross-Pitaevskii equation, the evolution of the exciton polaron BEC system in the annular microcavity is studied. Two key parameters affecting the characteristics of the exciton polaron system, namely the size of the microcavity and the configuration of the ring-shaped pumped beam, are investigated. The size of microcavity often directly affects the volume and power consumption of integrated devices. In addition, the number of coherent petals of exciton polariton superposition state matter wave propagated in microcavity is closely related to the precision and sensitivity of gyro, and the size of microcavity has a direct effect on the number of coherent petals. At the same time, whether the pumping region is continuous or not also has a key effect on the evolution of the system, and different pump configurations will affect the evolutions of the system. We find that in the microcavity radius on a micron scale, the annular microcavity can excite the petal of vortex superposition state when pumped by pumping light, and the petals can be stable, but circular cavity with a certain radius can “accommodate” a limited vortex quantum number, when vortex quantum number is too large, the system will be unstable and unable to support the formation of stable petals. However, with the increase of the radius of the annular microcavity, the superposition petal number of the exciton polariton system contained in the annular region will also increase, and the maximum petal number contained in the exciton polariton system has a positive linear correlation with the inner radius of the annular microcavity. At the same time, we find that when the pump laser configuration is changed, the system will evolve into a special form of steady state. The calculation results show that when microcavity parameters are the same but for only changing the radial width of single pump, the number of petals obtained is three times that before changing the radial width. In such a case, the number of superposition petals not only exceeds the previously calculated maximum number of petals accommodated by the annular cavity under the radius but also there appear the multiple petals combined radially. Under the double-ring pump system, changing the width of the hollow ring may produce not only the new exciton polariton condensation in the hollow ring, but also vortex states in the original petal. Under each of the three-ring and four-ring pumping condition, the evolution of the system finally presents a multi-petal state in the radial direction. Because these vortex superposition states contain the information about the density and the phase, it has important guiding significance for designing the new system of gyroscope. Therefore, these special evolutionary results open a new direction for studying the new system gyroscope.

Fractons from polarons

Fractons are a type of emergent quasiparticle which cannot move freely in isolation, but can easily move in bound pairs. Similar phenomenology is found in boson-affected hopping models, encountered in the study of polaron systems and hole-doped Ising antiferromagnets, in which motion of a particle requires the creation or absorption of bosonic excitations. We show that boson-affected hopping models can provide a natural realization of fractons, either approximately or exactly, depending on the details of the system. We first consider a generic one-dimensional boson-affected hopping model, in which we show that single particles move only at sixth order in perturbation theory, while motion of bound states occurs at second order, allowing for a broad parameter regime exhibiting approximate fracton phenomenology. We explicitly map the model onto a fracton Hamiltonian featuring conservation of dipole moment via integrating out the mediating bosons. We then consider a special type of boson-affected hopping models with mutual hard-core repulsion between particles and bosons, accessible in hole-doped mixed-dimensional Ising antiferromagnets, in which the hole motion is one dimensional in an otherwise two-dimensional antiferromagnetic background. We show that this system, which is within the current reach of ultracold-atom experiments, exhibits perfect fracton behavior to all orders in perturbation theory, thereby enabling the experimental study of dipole-conserving field theories. We further discuss diagnostic signatures of fractonic behavior in these systems. In studying these models, we also identify simple effective one-dimensional microscopic Hamiltonians featuring perfect fractonic behavior, paving the way to future studies on fracton physics in lower dimensions.

Polaronic effects in one-dimensional Fermi gas

Using the variational method and exact Bethe ansatz (BA) method, we studied the effects of an impurity immersed in a one-dimensional (1D) Fermi sea. With attractive interactions between them, the impurity is dressed up by surrounding particles in Fermi sea and forms a polaron. For equal masses and heavy polaron systems, we calculated the binding energy, effective mass, momentum distribution and Tan contact. In the strongly attractive limit, the impurity forms a dimer with inner fermion in Fermi sea which just accords with the highly imbalanced 1D Fulde–Ferrell–Larkin–Ovchinnikov (FFLO) state in experiment. We find that the heavy impurity is dressed more deeply with Fermi sea in whole interaction regime. Furthermore, we explore the complete influence of particle-hole excitation in Fermi polaron system in 1D. We find a shocking phenomenon that the hole term in Fermi sea has a great influence on the Tan relation even in the attractive interaction regime.