Phonon Effects Research Articles

Role of localized phonon vibration in luminescence performance of Pr doped Ba(Mg0.28Zr0.16Ta0.56)O3 transparent ceramics

Oxygen-assisted high temperature solid-state reaction approach was employed for the fabrication of Pr activated Ba(Mg0.28Zr0.16Ta0.56)O3 transparent ceramic phosphor. Retiveld refinement of X-ray diffraction pattern was carried out to reveal the lattice parameters and crystal structural information. Under the blue-light excitation of λex = 473 nm, the phosphor exhibits a sharp intense red emission centered at 645 nm, accompanied by several other weak peaks. PL evolution with temperature shows a significant luminescence quenching behavior, and the underlying multi-phonon interaction with optical center is revealed by proposing an unprecedent theoretical calculation work. Such a phonon effect is further confirmed from the red-shift of peak position with temperature, and the involved phonon energy of 50.7 meV is determined from Raman scattering measurement. More interestingly, the fitted results of transient-state PL spectra show a fluctuation of luminescence lifetime at various temperatures, further indicating a significant effect of phonon vibration in the system.

Strong reduction of quasiparticle fluctuations in a superconductor due to decoupling of the quasiparticle number and lifetime

We measure temperature dependent quasiparticle fluctuations in a small Al volume, embedded in a NbTiN superconducting microwave resonator. The resonator design allows for read-out close to equilibrium. By placing the Al film on a membrane, we enhance the fluctuation level and separate quasiparticle from phonon effects. When lowering the temperature, the recombination time saturates and the fluctuation level reduces a factor $\sim$100. From this we deduce that the number of free quasiparticles is still thermal. Therefore, the theoretical, inverse relation between quasiparticle number and recombination time is invalid in this experiment. This is consistent with quasiparticle trapping, where on-trap recombination limits the observed quasiparticle lifetime.

Deep insight into the luminescence performance of Li2MgSiO4:Mn2+ green phosphor synthesized by a sol-gel process

A sol-gel process together with a low-temperature sintering technique was applied for preparing Mn2+ activated Li2MgSiO4 green phosphor. Phase structure information was derived from the Rietveld refinement on its powder X-ray diffraction pattern. The luminescence performance was evaluated by characterizing the photoluminescence (PL) spectral evolution with Mn2+ concentration and in the temperature range of 300–500 K. The optimal Mn2+ doping level was 4 at% and the main PL quenching mechanism was identified to be the electric dipolar-dipolar interaction. The temperature-dependent PL spectra showed broad asymmetric line-profiles, and the underlying phonon effect was revealed from both experimental and theoretical works. The predominant phonon energy was determined to be 25 meV, and the luminescence quenching at high temperatures was mainly attributed to the six-phonon coupling interaction with the Mn2+ optical center, which was further confirmed from the simulation on PL spectral lineshape. These obtained results may provide us an unprecedented approach to study the phonon effect on the luminescence characteristic for the phosphors.

Exact solution of two simple non-equilibrium electron-phonon and electron-electron coupled systems: The atomic limit of the Holstein-Hubbard model and the generalized Hatsugai-Komoto model

One of the challenges in many-body physics is determining the effects of phonons on strongly correlated electrons. The difficulty arises from strong correlations at differing energy scales -- for band metals, Migdal-Eliashberg theory accurately determines electron-phonon coupling effects due to the absence of vertex corrections -- but strongly correlated electrons require a more complex description and the standard Migdal-Eliashberg approach does not necessarily apply. In this work, we solve for the atomic limit Green's function of the Holstein-Hubbard model with both time-dependent electron-electron and electron-phonon couplings. We then examine the photoemission spectra (PES) of this model in and out of equilibrium. Next we use similar methods to exactly solve an extended version of the Hatsugai-Komoto model, and examine its behavior in and out of equilibrium. These calculations lead us to propose using the first moment of the photoemission spectra to signal non-equilibrium changes in electron-electron and electron-phonon couplings.

Quantum transfer through small networks coupled to phonons: Effects of topology versus phonons.

Particle or energy transfer through quantum networks is determined by network topology and couplings to environments. This study examines the combined effect of topology and external couplings on the efficiency of directional quantum transfer through quantum networks. We consider a microscopic model of qubit networks coupled to external vibrations by Holstein and Peierls couplings. By treating the positions of the network sites and the site-dependent phonon frequencies as independent variables, we determine the Hamiltonian parameters corresponding to minimum transfer time by Bayesian optimization. The results show that Holstein couplings may accelerate transfer through suboptimal network configurations but cannot accelerate quantum dynamics beyond the limit of the transfer time in an optimal phonon-free configuration. By contrast, Peierls couplings distort the optimal networks to accelerate quantum transfer through configurations with less than six sites. However, the speed-up offered by Peierls couplings decreases with the network size and disappears for networks with more than seven sites. For networks with seven sites or more, Peierls couplings distort the optimal network configurations and change the mechanism of quantum transfer but do not affect the lower limit of the transfer time. The machine-learning approach demonstrated here can be applied to determine quantum speed limits in other applications.

Effect of density, phonon scattering and nanoporosity on the thermal conductivity of anisotropic cellulose nanocrystal foams

Anisotropic cellulose nanocrystal (CNC) foams with densities between 25 and 130 kg m−3 (CNC25 –CNC130) were prepared by directional ice-templating of aqueous dispersions. Estimates of the solid and gas conduction contributions to the thermal conductivity of the foams using a parallel resistor model showed that the relatively small increase of the radial thermal conductivity with increasing foam density can be attributed to interfacial phonon scattering. The foam wall nanoporosity and, to a lesser extent, the orientation of the CNC particles and alignment of the columnar macropores, also influence the insulation performance of the foams. The insight on the importance of phonon scattering for the thermal insulation properties of nanocellulose foams provides useful guidelines for tailoring nanofibrillar foams for super-insulating applications.

Ultrafast real-time tracing of surface electric field generated via hot electron transport in polar semiconductors

We trace an ultrafast real-space motion of photo-excited free carriers just near the surface of polar semiconductors GaAs and InAs by using the optical second-harmonic generation (SHG) technique. With a flat distribution of photo-carriers as an initial condition, ultrafast diffusion and drift motion followed by a rapid surface recombination develop a surface electric field which is efficiently probed by the electric-field-induced SHG. From the simulation based on the drift–diffusion equation combined with the ensemble Monte-Carlo approach, we could explain the experimental observation of the temporal evolution of the surface electric field, and extract time constants related to the hot electron cooling. Whereas the hot carrier cooling time is determined to be about 8 ps at room temperature for GaAs, it can be further extended to about 35 ps at 100 K due to the increase of the longitudinal optic phonon life time enhancing the hot phonon effect. Our work can be an important guide in designing optoelectronic nano-devices by providing a clear understanding of the ultrafast electron-hole separation near the surface of polar semiconductors in connection with the hot carrier cooling process.

Boundary element modeling of 3 T nonlinear transient magneto-thermoviscoelastic wave propagation problems in anisotropic circular cylindrical shells

The principle motivation behind this paper is to introduce boundary element modeling of three-temperature (3 T) nonlinear transient magneto-thermoviscoelastic wave propagation problems in anisotropic circular cylindrical shells under the effects of electron, ion, phonon, and total temperatures. The governing equations have solved using the boundary element method (BEM) to obtain the three-temperature, displacements and magneto-thermoviscoelastic stresses. The mathematical outcomes demonstrate that the impacts of three-temperature on the magneto-thermoviscoelastic stresses are extremely articulated. Additionally, these mathematical outcomes show the legitimacy and precision of the present mathematical strategy.

Photoexcited carrier dynamics of thin film Cd3As2 grown on a GaAs(111)B substrate by molecular beam epitaxy

The topological Dirac semimetal ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$ has drawn great attention for its novel physics and technical applications in optoelectronic devices operating in the infrared and THz regimes. Exploring the photoexcited carrier dynamics in ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$ is helpful to understand the transient carrier occupation and cooling processes that are closely associated with its unconventional band characteristic. Here, the photoexcited carrier dynamics in the ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$ thin film epitaxially grown on the $\mathrm{GaAs}(111)B$ substrate was investigated by employing the time-resolved midinfrared transient reflectance measurements, along with a theoretical modeling concerning the electron-polar optical ($e$-PO) phonon interaction. The measured photoexcited electron relaxation time of ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$ increases with the probe wavelength, and increases with temperature at temperatures higher than 30 K. Theoretical modeling under the framework of the two-temperature model can give qualitatively good description on both the temperature and probe wavelength dependence of the carrier relaxation time. Additionally, theoretical modeling shows that charge screening of the interaction of electrons with polar optical phonons can greatly reduce the hot carrier relaxation rate. The measured transient reflectance analyses indicate that the hot phonon effect plays a negligible role on the carrier relaxation in ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$. Our findings provide further insight into the photoexcited carrier dynamics in ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$ and valuable reference for developing its high-performance infrared optoelectronic devices.

Switching Behavior of a Heterostructure Based on Periodically Doped Graphene Nanoribbon

We theoretically propose a switching device that operates at room temperature. The device is an in-plane heterostructure based on a periodically boron-doped (nitrogen-doped) armchair graphene nanoribbon, which has been experimentally fabricated recently. The calculated $I$-$V$ curve shows that for a realistic device with interface width longer than $20$ nm, nonzero electric current occurs only in the region of bias voltage between $\ensuremath{-}0.22$ and $0.28$ V, which is beneficial to low-voltage operation. Furthermore, in this case, the electric current is robust against the change of the potential profile in the interface since the metallic impurity-induced sub-bands with delocalized wave functions contribute to the transmission exclusively. This also suggests the high response speed of the proposed device. We also discuss the temperature dependence, the output impedance, the effect of phonons, and the possible regimes to extend our work, which suggest that our model may have potential room-temperature nanoelectronics applications.

Effects of Bond Disorder and Surface Amorphization on Optical Phonon Lifetimes and Raman Peak Shape in Crystalline Nanoparticles

Optical phonons in nanoparticles with the randomness of interatomic bonds are considered both analytically and numerically. For weak dilute disorder two qualitatively different regimes of separated and overlapped levels are observed, resembling the case of random atomic masses investigated previously. At stronger and/or more dense disorder, the particles become essentially inhomogeneous, thus constituting the minimal model to describe an amorphous phase, where the picture of vibrational modes becomes more subtle. We concentrate here on the experimentally relevant case of strong disorder located near the particle surface and formulate the core-shell model aimed to describe the ubiquitous phenomenon of particle surface amorphization. We observe a peculiar effect of volume optical phonons "repelling" from the disordered shell. It results in the Raman spectrum in the form of a combination of narrow well-resolved peaks stemming from the quantized modes of a pure particle core (red-shifted due to its effective smaller size), and the noisy background signal from the disordered shell placed primarily to the right from the main Raman peak.

Coulomb interaction, phonons, and superconductivity in twisted bilayer graphene

The polarizability of twisted bilayer graphene, due to the combined effect of electron-hole pairs, plasmons, and acoustic phonons, is analyzed. The screened Coulomb interaction allows for the formation of Cooper pairs and superconductivity in a significant range of twist angles and fillings. The tendency toward superconductivity is enhanced by the coupling between longitudinal phonons and electron-hole pairs. Scattering processes involving large momentum transfers, Umklapp processes, play a crucial role in the formation of Cooper pairs. The magnitude of the superconducting gap changes among the different pockets of the Fermi surface.

Electronic, optical, elastic, mechanical and vibrational properties of hexagonal h-ZnS with density functional theory

In this work, we explored the electronic, optical, elastic and phonon effect in two-dimensional hexagonal Zinc Sulphide (h-ZnS) monolayer. We investigated which aspects of the orbitals of Zinc and Sulphur are the sources of core levels, valence band level and conduction band level in the bandstructure. We wrote the optical parameters in terms of dielectric functions. We observed that the absorption peak represents the optical bandgap. Using the linear response scheme, we determined the phonon dispersions and noticed the transverse-acoustic is the main source in precisely describing the phase transition from the bulk ZnS to h-ZnS monolayer. We also report that h-ZnS has a direct bandgap of 2.58 eV and the material is brittle, based on the B/G ratio. We notice, however, the elastic constants of the h-ZnS are somewhat different from the bulk. We further report that the use of the hybrid functionals is significant, while computationally demanding, in estimating the electronic bandstructure, compared to PBE-GGA, which overestimates the c axis and underestimates an axis.

Generation of entanglement between quantum dot molecule with the presence of phonon effects in a voltage-controlled junction

We investigate the generation of entanglement through a quantum dot molecule under the influence of vibrational phonon modes in a bias voltage junction. The molecular quantum dot system is realized by coupled quantum dots inside a suspended carbon nanotube. We consider the dynamical entanglement as a function of bias voltage and temperature by taking into account the electron-phonon interaction. In order to generate the robust entanglement between quantum dots and preserve it to reach the maximal achievable amount steadily, we introduce an asymmetric coupling protocol and apply the easy tunable bias voltage-driven field. For an oscillating bias voltage, the time-varying entanglement can periodically reach the maximum revival. In thermal entanglement dynamics, the phenomena of thermal entanglement degradation and thermal entanglement revival are observed which are intensively affected by the strength of phonon decoherence. The revival of entanglement shows a larger value for a higher phonon coupling.

Oscillations of the electron energy loss rate in two-dimensional transition-metal dichalcogenides in the presence of a quantizing magnetic field

We study the hot electron energy-loss rate (ELR) induced by acoustic ${P}^{\mathrm{ac}}$ and optical ${P}^{\mathrm{op}}$ phonons, in two-dimensional transition-metal dichalcogenides (TMDCs), in presence of quantizing magnetic field $B$, including the hot-phonon effect. At the low-temperature regime, the ELR is found to display a quantum oscillations with their amplitude being found to increase with the increase of the magnetic field. The unscreened TA phonon due to deformation potential (DP) coupling is dominant over the other screened acoustic phonon contributions. In the extreme Bloch-Gr\"uneisen (BG) region, the ELR displays a pronounced ${P}^{\mathrm{ac}}\ensuremath{\propto}{T}^{4}\phantom{\rule{0.16em}{0ex}}({T}^{6})$ temperature dependence for unscreened TA-DP phonons (other screened mechanisms). When the temperature increases, ${T}_{e}>{T}_{\mathrm{BG}}$, the ELR shows a linear ${P}^{\mathrm{ac}}\ensuremath{\propto}T$ behavior in the equipartition region. At higher temperatures, there is a crossover from ${P}^{\mathrm{ac}}$ dominated ELR to ${P}^{\mathrm{op}}$ by zeroth-order DP coupling dominated ELR with the cross-over temperature being about ${T}_{e}\ensuremath{\sim}50\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. The hot phonon effect is demonstrated to reduce ELR significantly. The effect of the magnetic field is found to enhance the ELR significantly, making $B$ as its another tuning knob. Among the four TMDC materials, ${\mathrm{MoS}}_{2}$ (${\mathrm{MoSe}}_{2}$) displays the biggest ELR due to acoustic (optical) phonon scattering while ${\mathrm{WSe}}_{2}$ (${\mathrm{WS}}_{2}$) shows the smallest ELR. Our results for the ${\mathrm{MoS}}_{2}$ material are compared with those of the zero-field ELR.

Giant phonon anomalies in the proximate Kitaev quantum spin liquid \u03b1-RuCl3

The Kitaev quantum spin liquid epitomizes an entangled topological state, for which two flavors of fractionalized low-energy excitations are predicted: the itinerant Majorana fermion and the Z2 gauge flux. It was proposed recently that fingerprints of fractional excitations are encoded in the phonon spectra of Kitaev quantum spin liquids through a novel fractional-excitation-phonon coupling. Here, we detect anomalous phonon effects in α-RuCl3 using inelastic X-ray scattering with meV resolution. At high temperature, we discover interlaced optical phonons intercepting a transverse acoustic phonon between 3 and 7 meV. Upon decreasing temperature, the optical phonons display a large intensity enhancement near the Kitaev energy, JK~8 meV, that coincides with a giant acoustic phonon softening near the Z2 gauge flux energy scale. These phonon anomalies signify the coupling of phonon and Kitaev magnetic excitations in α-RuCl3 and demonstrates a proof-of-principle method to detect anomalous excitations in topological quantum materials.

Spin-orbital coupling and slow phonon effects enabled persistent photoluminescence in organic crystal under isomer doping

When periodically packing the intramolecular donor-acceptor structures to form ferroelectric-like lattice identified by second harmonic generation, our CD49 molecular crystal shows long-wavelength persistent photoluminescence peaked at 542 nm with the lifetime of 0.43 s, in addition to the short-wavelength prompt photoluminescence peaked at 363 nm with the lifetime of 0.45 ns. Interestingly, the long-wavelength persistent photoluminescence demonstrates magnetic field effects, showing as crystalline intermolecular charge-transfer excitons with singlet spin characteristics formed within ferroelectric-like lattice based on internal minority/majority carrier-balancing mechanism activated by isomer doping effects towards increasing electron-hole pairing probability. Our photoinduced Raman spectroscopy reveals the unusual slow relaxation of photoexcited lattice vibrations, indicating slow phonon effects occurring in ferroelectric-like lattice. Here, we show that crystalline intermolecular charge-transfer excitons are interacted with ferroelectric-like lattice, leading to exciton-lattice coupling within periodically packed intramolecular donor-acceptor structures to evolve ultralong-lived crystalline light-emitting states through slow phonon effects in ferroelectric light-emitting organic crystal.

Non-Markovian perturbation theories for phonon effects in strong-coupling cavity quantum electrodynamics

Phonon interactions are inevitable in cavity quantum electrodynamical systems based on solid-state emitters or fluorescent molecules, where vibrations of the lattice or chemical bonds couple to the electronic degrees of freedom. Due to the non-Markovian response of the vibrational environment, it remains a significant theoretical challenge to describe such effects in a computationally efficient manner. This is particularly pronounced when the emitter-cavity coupling is comparable to or larger than the typical phonon energy range, and polariton formation coincides with vibrational dressing of the optical transitions. In this Article, we consider four non-Markovian perturbative master equation approaches to describe such dynamics over a broad range of light-matter coupling strengths and compare them to numerically exact reference calculations using a tensor network. The master equations are derived using different basis transformations and a perturbative expansion in the new basis is subsequently introduced and analyzed. We find that two approaches are particularly successful and robust. The first of these is suggested and developed in this Article and is based on a vibrational dressing of the exciton-cavity polaritons. This enables the description of distinct phonon-polariton sidebands that appear when the polariton splitting exceeds the typical phonon frequency scale in the environment. The second approach is based on a variationally optimized polaronic vibrational dressing of the electronic state. Both of these approaches demonstrate good qualitative and quantitative agreement with reference calculations of the emission spectrum and are numerically robust, even at elevated temperatures, where the thermal phonon population is significant.

Effects of the Interface between Inorganic and Organic Components in a Bi2Te3-Polypyrrole Bulk Composite on Its Thermoelectric Performance.

We provided a method to hybridize Bi2Te3 with polypyrrole, thus forming an inorganic/organic bulk composite (Bi2Te3–polypyrrole), in which the effects of energy band junction and phonon scattering were expected to occur at the interface of the two components. Bi2Te3–polypyrrole exhibited a considerably high Seebeck coefficient compared to pristine Bi2Te3, and thus it recorded a somewhat increased power factor despite the loss in electrical conductivity caused by the organic component, polypyrrole. Bi2Te3–polypyrrole also exhibited much lower thermal conductivity than pristine Bi2Te3 because of the phonon scattering effect at the interface. We successfully brought about the decoupling phenomenon of electrical and thermal properties by devising an inorganic/organic composite and adjusting its fabrication condition, thereby optimizing its thermoelectric performance, which is considered the predominant property for n-type binary Bi2Te3 reported so far.

Temperature-Dependent Phonon Shifts in van der Waals Crystals.

In recent years, there has been an explosive increase in the research on van der Waals (vdW) crystals because of their great potential applications in many optoelectronic devices. It is necessary to determine their temperature-dependent lattice vibration characteristics because their thermal and electrical transport are closely related to the anharmonic phonon effect, which will affect the performance of the devices. We review the temperature-dependent Raman spectroscopy of vdW crystals, systematically introduce the thermal behavior of optical phonons, and summarize their shift with temperature. Upon analyzing the theoretical models and summarizing the reported experimental data, it is found that the phonon shifts of vdW crystals have a "quasi-linear" relationship with temperature, which is widely described with first-order temperature (FOT) coefficients obtained through a linear fit. Thus, subsequently, the phonon shifts of monolayer materials, different-thickness crystals, suspended and supported samples, in-plane and out-of-plane modes in the same vdW materials, as well as heterostructures and alloys are discussed through comparative analysis of FOT coefficients.