Phonon Absorption Research Articles

Electron–photon–phonon interactions in Dirac semimetals: Magneto-optical absorption and mobility analysis

We study the magneto-optical properties of Dirac semimetal (DSM) slabs with particular emphasis on Cd3As2 through electron–photon–phonon interactions, focusing on the magneto-optical absorption coefficient (MOAC) and full-width at half maximum (FWHM). Studying the Landau level (LL) energy of DSMs in the (xy) plane and the z-direction revealed a unique deviation from the square root dependence on the magnetic field, distinguishing DSMs from other semiconductors. At high magnetic fields, the electron–hole symmetry in the LL spectrum is broken, indicating a topological phase in DSMs. For undoped DSMs, MOAC is driven by interband transitions, with peaks from one-photon absorption being smaller and positioned to the left of two-photon ones. Increasing the magnetic field increases peak values. FWHM for one- and two-photon processes increases with the magnetic field and follows a T dependence on temperature. In doped DSMs, both intraband and interband transitions occur, with new interband peaks emerging at higher temperatures near the Fermi energy. Increased electron density shifts the peak position slightly toward higher energy. Peaks from optical phonon emission are consistently higher and located to the right of those from optical phonon absorption, indicating a stronger emission process. The FWHM data allow for the estimation of electron mobilities, and using a reasonable broadening parameter, our predicted mobility values agree with experimental results.

Germanium Single Crystals for Photonics

Germanium (Ge) is a system-forming material of IR photonics for the atmospheric transparency window of 8–14 µm. For optics of the 3–5 µm range, more widespread silicon (Si), which has phonon absorption bands in the long-wave region, is predominantly used. A technology for growing Ge single crystals has been developed, allowing the production of precision optical parts up to 500 mm in diameter. Ge is used primarily for the production of transparent optical parts for thermal imaging devices in the 8–14 µm range. In addition, germanium components are widely used in a large number of optical devices where such properties as mechanical strength, good thermal properties, and climatic resistance are required. A very important area of application of germanium is nonlinear optics, primarily acousto-optics. The influence of doping impurities and temperature on the absorption of IR radiation in germanium is considered in detail. The properties of germanium photodetectors are reported, primarily on the effect of photon drag of holes. Optical properties in the THz range are considered. The features of optical properties for all five stable isotopes of germanium are studied. The isotopic shift of absorption bands in the IR region, caused by phonon phenomena, which was discovered by the authors for the first time, is considered.

Two stage decoherence of optical phonons in long oligomers.

Molecular vibrations are generally responsible for chemical energy transport and dissipation in molecular systems. This transport is fast and efficient if energy is transferred by optical phonons in periodic oligomers, but its efficiency is limited by decoherence emerging due to anharmonic interactions with acoustic phonons. Using a general theoretical model, we show that in the most common case of the optical phonon band being narrower than the acoustic bands, decoherence takes place in two stages. The faster stage involves optical phonon multiple forward scattering due to absorption and emission of transverse acoustic phonons, i.e., collective bending modes with a quadratic spectrum; the transport remains ballistic and the speed can be altered. The subsequent slower stage involves phonon backscattering in multiphonon processes involving two or more acoustic phonons resulting in a switch to diffusive transport. If the initially excited optical phonon possesses a relatively small group velocity, then it is accelerated in the first stage due to its transitions to states propagating faster. This theoretical expectation is consistent with the recent measurements of optical phonon transport velocity in alkane chains, increasing with increasing the chain length.

Effects of hydrostatic pressure, aluminium composition, and external magnetic field on intersubband and intrasubband transitions characteristics in symmetric potential quantum wells

Aluminium composition (λ), magnetic field (B), and hydrostatic pressure (P) influences on magneto-optical (MO) properties of intra- and inter-subband transitions in GaAs/AlλGa1−λAs symmetric QWs for four models of confined optic phonons are studied and compared. The findings indicate: the MO characteristics of intra- and inter-subband transitions are significantly influenced by B, λ, and P for phonon absorption and emission. The e–p interaction intensity decreases as P increases, whereas it increases as λ increases. The influences of λ and P on phonon absorption are more significant than those on emission. E–p interaction intensity dependence on λ and P for intra-subband transitions is stronger than that for inter-subband ones. The e–p interaction in QWs is well described by Knipp–Reinecke and Huang–Zhu models. To reduce the influence of P on MO properties, we can increase T and λ or decrease B. At T≈600 K, the influence of P is insignificant and can be neglected.

Integration of Heterogeneous Interfaces and Multi‐Dimensional Encapsulation Structure in Fe2N@CNTs Enabling Highly Efficient Thermal Management and Microwave Absorption

AbstractThe opposing effects of interface effect on phonon heat conduction and microwave absorption hinder the integration of thermal conduction with microwave absorption. Reconciling this contradiction by rationally optimizing the material structure remains a challenge. Herein, Fe2N@CNTs with heterogeneous interfaces and multi‐dimensional encapsulated structures are fabricated through in situ chemical vapor deposition (CVD) to realize excellent thermal conductivity and microwave absorption. When the mass fraction of active material is 40 wt.%, the thermal conductivity (λ//) of Fe2N@CNTs composite films is 6.69 W m−1 K−1. The minimum reflection loss (RLmin) is up to −54.55 dB at a thickness of 3.43 mm, and the effective absorption bandwidth (EAB) is 5.52 GHz at 1.82 mm. The well‐designed Fe2N@CNTs is an ideal model for gaining insight into electron transportation and phonon multi‐dimensional heat transport. Heterogeneous interface improves the dielectric loss and facilitates microwave and phonon absorption and conversion. The multi‐dimensional encapsulation structure increases the electron transport path and phonon heat transport paths making axial and radial co‐transfer possible. The multi‐dimensional encapsulation structure demonstrates extremely high microwave absorption and thermal management capabilities, which open up new possibilities for multifunctional applications in host materials with internal hollows.

Heavy dark matter in white dwarfs: multiple-scattering capture and thermalization

We present an improved treatment for the scattering of heavy dark matter from the ion constituents of a white dwarf. In the heavy dark matter regime, multiple collisions are required for the dark matter to become gravitationally captured. Our treatment incorporates all relevant physical effects including the dark matter trajectories, nuclear form factors, and radial profiles for the white dwarf escape velocity and target number densities. Our capture rates differ by orders of magnitude from previous estimates, which have typically used approximations developed for dark matter scattering in the Earth.We also compute the time for the dark matter to thermalize in the center of the white dwarf, including in-medium effects such as phonon emission and absorption from the ionic lattice in the case where the star has a crystallized core. We find much shorter thermalization timescales than previously estimated, especially if the white dwarf core has crystallized.We illustrate the importance of our improved approach by determining the cross section required for accumulated asymmetric dark matter to self-gravitate.

Enhancement of vibrationally assisted energy transfer by proximity to exceptional points, probed by fluorescence-detected vibrational spectroscopy

Emulation of energy transfer processes in natural systems on quantum platforms can further our understanding of complex dynamics in nature. One notable example is the demonstration of vibrationally assisted energy transfer (VAET) on a trapped-ion quantum emulator, which offers insights for the energetics of light harvesting. In this work, we expand the study of VAET simulation with trapped ions to a non-Hermitian quantum system comprising a PT-symmetric chromophore dimer weakly coupled to a vibrational mode. We first characterize exceptional points (EPs) and non-Hermitian features of the excitation energy transfer processes in the absence of the vibration, finding a degenerate pair of second-order EPs. Exploring the non-Hermitian dynamics of the whole system including vibrations, we find that energy transfer accompanied by absorption of phonons from a vibrational mode can be significantly enhanced near such a degenerate EP. Our calculations reveal a unique spectral feature accompanying the coalescing of eigenstates and eigenenergies that provides a unique approach to probe the degenerate EP by fluorescence-detected vibrational spectroscopy. Enhancement of the VAET process near the EP is found to be due to maximal favorability of phonon absorption at the degenerate EP, enabling multiple simultaneous excitations. Our work on improving VAET processes in non-Hermitian quantum systems paves the way for leveraging non-Hermiticity in quantum dynamics related to excitation energy transfer. Published by the American Physical Society 2024

Use of rational approximations for phonon density of states in evaluation of neutron thermal scattering law

We propose and explore a new analytical formulation for evaluation of Thermal Scattering Law (TSL) using continuous phonon spectra for neutron inelastic scattering. It involves approximating Phonon Density of States (PDOS) in terms of rational approximations in energy transfer. Debye Waller coefficient calculated with these forms are in reasonable agreement with LEAPR calculated values. TSL can be expanded as a power series, each term of which can be integrated analytically. The method leads to TSL being a series of exponential cosine integrals which again have closed rational forms in energy transfer. Their shapes are analogous to asymmetric resonance line shapes and show maxima for certain values of energy transfer which could correspond to phonon emission or absorption. The series is shown to be convergent and easy to compute as it does not involve any numerical integration. The approach is applied to Beryllium metal and Graphite which have vastly different PDOS shapes, and is shown to be capable of giving most of the trends shown by TSL and cross section results from NJOY nuclear code processing system, even with smaller number of power series terms. Since TSL can be calculated for both negative and positive energy transfer with equal ease, one can easily check for the validity of the approximation obeying Principle of Detailed Balance (PDB). The results overall have shown promise of our formulation in making a case for rapid calculations of TSL and also for using the rational forms in energy transfer for analysis of experimental/calculated PDOS data.

Bond theory, vibrational spectroscopy, and dielectric responses of trirutile ATa2O6 (A = Mg, Ni) microwave ceramics

This study established the connection between structure and dielectric responses by synergistically evaluating the chemical bond characteristics and lattice vibrational spectroscopies of trirutile ATa2O6 (A = Mg, Ni) microwave ceramics. The MgTa2O6 ceramic exhibits a uniform grain size distribution and a dense microstructure, with dielectric characteristics at microwave range of a εr value of 27.27, a high Q×f value of 109,203 GHz (8.73 GHz), and a τf of approximately 53.38 ppm/°C when sintered at 1300 °C, while the NiTa2O6 ceramic presents a smaller average grain size and minor micropores, with dielectric characteristics at microwave range of εr = 24.58, Q×f = 27,610 GHz (9.25 GHz), and τf = 33.94 ppm/°C, sintered at 1250 °C. The structural refinement and atomic arrangements confirm a trirutile structure along the [001], [100], and [3 3‾1‾] zone axes. Ta–O bonds are found to contribute the most to the ionic character of a bond, bond susceptibility, lattice stability, thermal expansion behaviors, and strength of bonding ability, indicating their significant influence on dielectric polarization, lattice stability, and temperature coefficient of resonant frequency. Raman scattering spectra analysis reveals that the A1g mode near 700 cm−1 mainly controls the Raman vibrational behaviors. The theoretical dielectric properties calculated from the infrared spectrum and dielectric properties analysis consistent with the measured dielectric performances, suggesting that the dielectric characteristics at the microwave range are mainly determined by the oscillatory absorption of structural phonons, with the first two modes at 210.48 cm−1 and 232.87 cm−1 contributing 72.02% to the εr value and 90.45% to the tanδ value, respectively.

Transform-Limited Photon Emission from a Lead-Vacancy Center in Diamond above 10K.

Transform-limited photon emission from quantum emitters is essential for high-fidelity entanglement generation. In this Letter, we report the coherent optical property of a single negatively charged lead-vacancy (PbV) center in diamond. Photoluminescence excitation measurements reveal stable fluorescence with a linewidth of 39MHz at 6K, close to the transform limit estimated from the lifetime measurement. We observe 4 orders of magnitude different linewidths of the two zero-phonon lines, and find that the phonon-induced relaxation in the ground state contributes to this huge difference in the linewidth. Because of the suppressed phonon absorption in the PbV center, we observe nearly transform-limited photon emission up to 16K, demonstrating its high temperature robustness compared to other color centers in diamond.

Phosphides‐Based Terahertz Quantum‐Cascade Laser

Due to their high optical phonon energies GaInP/AlGaInP heterostructures are a promising active medium to solve the problem of creating compact semiconductor sources with an operating frequency range of 5.5–7 THz. In this work, the temperature dependences of gain and absorption at 6.4–6.9 THz have been calculated for a GaInP/AlGaInP‐based quantum‐cascade laser (QCL) with two quantum wells in the cascade and a metal–metal waveguide. The dielectric function and mode losses for a 10 μm thick Au–Au waveguide, based on ternary InGaP and quaternary AlGaInP semiconductors, have been investigated in details. A laser structure that provides a mode gain of over 100 cm−1 with a maximum operating temperature about 100 K is proposed. The results of this study open the way to the development of a QCL for operation in a significant part of the GaAs phonon absorption band region, which is inaccessible for existing QCLs.

Ionic organic terahertz crystals: a perspective on design and solid-state phonon absorption

This perspective discusses various design strategies for high-performance ionic organic nonlinear optical crystals, their solid-state molecular phonon vibrations, as well as their influence on THz optical properties and THz applications.

Intersystem crossing as vibronically induced phonon emission and absorption processes: a unified view of nonradiative transitions in a molecule

Abstract An analytical expression for the nonradiative rate constant is derived based on Fermi's golden rule within the mixed-spin crude adiabatic (CA) approximation. The mixed-spin CA basis is defined by a set of eigenstates for the electronic Hamiltonian that comprises the nonrelativistic electronic Hamiltonian and spin-orbit coupling clumped at the reference nuclear configuration. The mixed-spin basis differs from the pure-spin basis defined by a set of eigenstates for the nonrelativistic electronic Hamiltonian. The mixed-spin CA representation provides a unified view of the nonradiative transitions; both internal conversion and intersystem crossing (ISC) are regarded as vibronically induced phonon emission and absorption processes. The analytical expression enables us to determine important vibrational modes that are responsible for phonon emission/absorption (promoting modes) and accepting excitation energy (accepting modes) according to the selection rule of vibronic coupling. An advantage of the CA representation is that the spatial distribution of vibronic coupling is elucidated based on its density form, i.e. vibronic coupling density, which can be applied to theoretical molecular designs with controlled nonradiative processes. The calculated ISC rate constant for tetracene reproduces the experimental result well.

Single site-controlled inverted pyramidal InGaAs QD–nanocavity operating at the onset of the strong coupling regime

Precise positioning of single site-controlled inverted pyramidal InGaAs quantum dots (QDs) at the antinode of a GaAs photonic crystal cavity with nanometer-scale accuracy holds unique advantages compared to self-assembled QDs and offers great promise for practical on-chip photonic quantum information processing. However, the strong coupling regime in this geometry has not yet been achieved due to the low cavity Q-factor based on the (111)B-oriented membrane structures. Here, we reveal the onset of phonon-mediated coherent exciton–photon interaction on our tailored single site-controlled InGaAs QD–photonic crystal cavity. Our results present the Rabi-like oscillation of luminescence intensity between excitonic and photonic components correlated with their energy splitting pronounced at small detuning. Such Rabi-like oscillation is well reproduced by modeling the coherent exchange of the exciton-photon population. The modeling further reveals an oscillatory two-time covariance at QD-cavity resonance, which indicates that the system operates at the onset of the strong coupling regime. Moreover, by using the cavity mode as a probe of the virtual state of the QD induced by phonon scattering, it reveals an increase in phonon scattering rates near the QD–cavity resonance and asymmetric phonon emission and absorption rate of even around 50 K.

Infrared dielectric function of GaAs1−xPx semiconductor alloys near the reststrahlen bands

The infrared dielectric function of thick GaAs1−xPx alloy layers grown on (001) GaAs substrates by hydride vapor phase epitaxy was investigated in the reststrahlen region using Fourier-transform infrared ellipsometry. The spectra are influenced by the Berreman artifact at the longitudinal optical phonon frequency of the GaAs substrate and by interference fringes due to the finite layer thickness. The ellipsometric angles were analyzed to determine the dielectric function of the alloy layer. Two-mode behavior, including strong GaAs-like and GaP-like optical phonons, was observed, confirming the results of Verleur and Barker [Phys. Rev. 149, 715 (1966)]. Due to the increased sensitivity of ellipsometry in the reststrahlen region, several weak phonon features could also be seen. The lattice absorption peaks are asymmetric and show side bands at the lower and higher frequencies. A single additional peak, as suggested by the percolation model, does not describe the spectra. The cluster model proposed by Verleur and Barker is a better fit to the data. Due to the broadening of the phonon absorption peaks, the authors were unable to find a unique decomposition into multiple components.

Rate equations description of the asymmetric double barrier electronic cooler

Recent experimental results showed that an electron gas in an asymmetrical double barrier heterostructure can be effectively cooled down under resonant tunneling condition, thus leading to the realization of an electronic cooler. The cooling process is a multi-parameters phenomenon and it is desirable to handle this problem through a reasonably simple approach, in order to understand the role of each parameter. To this end, we present a rate equation modeling of the electron cooling. We model the resonant tunnel injection of the electrons in the well and their thermionic emission assisted by Longitudinal Optical (LO) phonons absorption and emission. The influence of several parameters on the electronic temperature is discussed. This simple model compares rather well to the predictions of non-equilibrium Green function approach and to the experiments.

Practical approach to thermal conductivity calculations of small SiO2 samples

We compute the thermal conductivity of amorphous SiO2 combining density functional theory calculations and lifetime models. The supercell we use to represent amorphous SiO2 is small, 78 atoms. We show that this rudimentary model is nevertheless sufficient to reproduce the temperature dependence of the thermal conductivity from 0.1 K to 1000 K if we use a lifetime model at low frequencies accounting for Rayleigh scattering, the absorption of phonons by two levels systems and structural relaxations. The necessary conditions needed to observe the plateau in the thermal conductivity around 10 K are also discussed according to this model.

Phonon dichroism in proximitized graphene

We systematically investigate the phonon dichroism in proximitized graphene with broken time-reversal symmetry. We find that in the absence of any type of spin–orbit coupling, phonon dichroism vanishes. Linear and circular phonon dichroism occur in the presence of uniform (staggered) intrinsic spin–orbit coupling and ferromagnetic (antiferromagnetic) exchange coupling. All these situations can be distinguished by their specific behaviors of phonon absorption at the transition point. Our finding provides new possibilities to use phonon dichroism to identify the form of spin–orbit coupling and exchange coupling in proximitized graphene on various magnetic substrates.

Maximum propagation speed and Cherenkov effect in optical phonon transport through periodic molecular chains.

Optical phonons serve as the fast and efficient carriers of energy across periodic polymers due to their delocalization, large group velocity because of covalent bonding, and large energy quantum compared to that for acoustic phonons as it was observed in a number of recent measurements in different oligomers. However, this transport is dramatically sensitive to anharmonic interactions, including the unavoidable interaction with acoustic phonons responsible for transport decoherence, suppressing ballistic transport at long distances. Here, we show that this decoherence is substantially suppressed if the group velocity of optical phonons is less than the sound velocity of acoustic phonons; otherwise, ballistic transport is substantially suppressed by a Cherenkov-like emission of acoustic phonons. This conclusion is justified considering energy and momentum conservation during phonon absorption or emission and supported by the numerical evaluation of the lifetimes of the optical phonons. It is also consistent with the recent experimental investigations of ballistic optical phonon transport in oligomers with the minor exception of relatively short oligophenylenes.

The impact of phonon-assisted tunneling on optical and quantum characteristics of a coupled two-quantum dot system

This work investigates the impact of decoherence induced by pure dephasing and phonon-assisted tunneling mechanisms on the optical and quantum properties of two quantum dots. Special attention is given to the density matrix at steady state, and a detailed analysis of populations, coherences, optical transitions and the emission spectrum is performed. Additionally, we study the influence of both phonon-decoherence mechanisms on bipartite entanglement and the degree of mixedness of the system. In particular, our findings indicate that the phonon-assisted tunneling mechanism partially affects the coherences of the system and quantum properties when the imbalance of phonon absorption and emission is significant. Conversely, the pure dephasing mechanism does not affect the populations but strongly entangles the quantum dots and the reservoir, inducing maximally mixed states and significantly reducing the spectral splitting in the emission spectrum of the system.