Photodetection is an indispensable function of optoelectronic devices in modern communication and sensing systems. Contrary to the near-infrared/visible regions, the fast and sensitive photodetectors operated at room temperature for the far-infrared/terahertz regions are not well developed despite a possibly vast range of applications. The bulk photovoltaic effect (BPVE) in single-phase noncentrosymmetric materials based on the shift current mechanism enables less-dissipative energy conversion endowed with instantaneous responsivity owing to the quantum-mechanical geometric phase of electronic states. Nevertheless, the small-band-gap material for the low-energy BPVE inevitably suffers from the thermal noise due to the intrinsically high conductivity. Here, we demonstrate the shift current induced by soft-phonon excitations without creation of electron-hole pairs in the archetypal ferroelectric BaTiO3 by using the terahertz light, whose energy scale is three orders of magnitude smaller than the electronic band gap. At and above room temperature, we observe appreciable photocurrents caused by the soft-phonon excitation as large as that for electronic excitation and their strong phonon-mode dependence. The observed phonon-driven BPVE can be well accounted for by the shift current model considering the electron-phonon coupling in the displacement-type ferroelectrics as supported by the first-principles calculation. Our findings establish the efficient quantum BPVE arising from low-energy elementary excitations, suggesting the novel principle for the high-performance terahertz photodetectors.
Solid systems with strong correlations and interactions under light illumination have the potential for exhibiting interesting bulk photovoltaic behavior in the non-perturbative regime, which has remained largely unexplored in the past theoretical studies. We investigate the bulk photovoltaic response of a perovskite manganite with strongly coupled electron-spin-lattice dynamics, using real-time simulations performed with a tight-binding model. The transient changes in the band structure and the photoinduced phase transitions, emerging from spin and phonon dynamics, result in a nonlinear curre…
Solar cells based on conventional semiconductors have low efficiency in converting solar energy into electricity because the excess energy beyond the gap of an incident solar photon is converted into heat by phonons. Here we show by ab initio methods that the presence of strong Coulomb interactions in strongly correlated insulators (SCI) causes the highly photo-excited electron-hole pair to decay fast into multiple electron-hole pairs via impact ionization (II). We show that the II rate in the insulating $M_1$ phase of vanadium dioxide (chosen for this study as it is considered a prototypical …
We study a model for photovoltaic energy collection consisting of a Mott insulating layer in presence of acoustic phonons, coupled to two wide-band fermion leads at different chemical potentials and driven into a nonequilibrium steady state by a periodic electric field. We treat electron correlations with nonequilibrium dynamical mean-field theory (DMFT) using the so-called auxiliary master equation approach as impurity solver and include dissipation by acoustic phonons via the Migdal approximation. For a small hybridization to the leads, we obtain a peak in the photocurrent as a function of t…
Role of Ward-Takahashi identity in an electron-phonon coupled system -- Revisiting phonon shift current
The University of Tokyo（东京大学）；RIKEN Center for Emergent Matter Science (CEMS)（理化学研究所涌现物质科学中心）；Fundamental Quantum Science Program (FQSP), TRIP Headquarters, RIKEN（理化学研究所基础量子科学项目（FQSP）TRIP总部）
Interactions with electronic excitations can soften and/or broaden phonons. They are greatly amplified at wavevectors Q+- that connect parallel (nested) sheets of the Fermi surface. In such a case, called a Kohn anomaly, the phonon dispersion sharply dips and its linewidth has a maximum at Q+-. Here we present results of inelastic x-ray scattering measurements that uncovered soft phonons in chromium far from Q+-. They appear in addition to the previously reported soft phonons at Q+-. Calculations in the local density approximation (LDA) show that the new anomalies originate from enhanced elect…
We report high-resolution inelastic x-ray measurements of the soft phonon mode in the charge-density-wave compound TiSe$_2$. We observe a complete softening of a transverse optic phonon at the L point, i.e. q = (0.5, 0, 0.5), at T ~ T_{CDW}. Renormalized phonon energies are observed over a large wavevector range $(0.3, 0, 0.5) \le \mathbf{q} \le (0.5, 0, 0.5)$. Detailed ab-initio calculations for the electronic and lattice dynamical properties of TiSe2 are in quantitative agreement with experimental frequencies for the phonon branch involving the soft mode. The observed broad range of renormal…
We study spin dynamics of a spin-Peierls chain with nearest-neighbor and next-nearest-neighbor Heisenberg spin exchange interactions together with a gapped and dispersionless phonon. The dynamical spin correlation function and phonon excitation spectrum are calculated at zero temperature by using dynamical density-matrix renormalization-group method. We find a new spin excitation assisted by non-softening phonon. The excitation is located above phonon in energy and shows a dispersive feature with strong intensity near the momentum $π$. The phonon excitation spectrum is also influenced by the s…
We use variable-temperature x-ray thermal diffuse scattering and inelastic scattering to investigate the lattice dynamics in single crystals of multiferroic CaMn7O12 which undergo a series of orbital and magnetic transitions at low temperatures. Upon approaching the charge and orbital ordering temperature To=250 K from above, we observe intense diffuse scattering features and a pronounced optical phonon softening centered around the superstructure reflections of the incommensurately modulated structure. The phonon anomaly appears well above To and continuously increases upon cooling, following…
We performed ultrasonic measurements on (Ta$_{0.952}$V$_{0.048}$)$_2$NiSe$_5$ to investigate the contribution of acoustic phonons at the zone center to structural and possible excitonic transitions. The transverse elastic constant $C_{55}$ with irreducible representation $B_\mathrm{2g}$ exhibits softening over 90\% above a transition temperature of $T_\mathrm{s} = 280$ K, indicating the soft mode of corresponding TA phonons. Our analysis based on the quadrupole response indicates that the electron-phonon interaction contributes to the excitonic transition in addition to the hybridization betwe…
We investigate the effect of local electron-phonon coupling on nonlinear optical conductivity in an interacting ferroelectric system. Using real-time simulations, we show an enhancement in nonlinear conductivity under linearly-polarized light due to generation of the phonon-assisted ballistic-current in addition to the injection-current generated by electron-hole pairs. The optically excited phonon modes generate an asymmetric carrier distribution that causes a strong directional ballistic-current. The ballistic-current enhances the photocurrent several times at above band-gap excitation frequ…
We investigate the influence of the electron-phonon coupling in the one-dimensional spinless Holstein model at half-filling using both a recently developed projector-based renormalization method (PRM) and an refined exact diagonalization technique in combination with the kernel polynomial method. At finite phonon frequencies the system shows a metal-insulator transition accompanied by the appearance of a Peierls distorted state at a finite critical electron-phonon coupling. We analyze the opening of a gap in terms of the (inverse) photoemission spectral functions which are evaluated in both ap…
We present an investigation of the lattice dynamics of the charge-density-wave compound 2H-NbSe2. We analyze the precise nature of the wave vector dependent electron-phonon coupling (EPC) and derive the bare dispersion of the charge-density-wave (CDW) soft phonon mode using inelastic x-ray scattering combined with ab-initio calculations. Experimentally, phonon modes along the Γ - M line, i.e. q = (h, 0, 0) with 0 <= h <= 0.5, with the same longitudinal symmetry (Σ1) as the CDW soft mode were investigated up to 32 meV. In agreement with our calculations we observe significant EPC in the optic m…
We have studied the S=1/2 quasi-one-dimensional antiferromagnet TiOCl using single crystal x-ray diffraction and inelastic x-ray scattering techniques. The Ti ions form staggered spin chains which dimerize below Tc1 = 66 K and have an incommensurate lattice distortion between Tc1 and Tc2 = 92 K. Based on our measurements of the intensities, wave vectors, and harmonics of the incommensurate superlattice peaks, we construct a model for the incommensurate modulation. The results are in good agreement with a soliton lattice model, though some quantitative discrepancies exist near Tc2. The behavior…
Electronic tuning of the soft-phonon transport anomaly in Ta$_2$Ni(S$_x$Se$_{1-x}$)$_5$
Max Planck Institute for Solid State Research（马克斯·普朗克固体研究所）；Institute for Functional Matter and Quantum Technologies, University of Stuttgart（斯图加特大学功能物质与量子技术研究所）；National Institute for Materials Science（国立材料研究所）
We study the symmetric Anderson-Holstein (AH) model at zero temperature with Wilson's numerical renormalization group (NRG) technique to study the interplay between the electron-electron and electron-phonon interactions. An improved method for calculating the phonon propagator using the NRG technique is presented, which turns out to be more accurate and reliable than the previous works in that it calculates the phonon renormalization explicitly and satisfies the boson sum rule better. The method is applied to calculate the renormalized phonon propagators along with the electron propagators as …
The complex coupling between charge carriers and phonons is responsible for diverse phenomena in condensed matter. We apply ultrafast electron diffuse scattering to unravel electron-phonon coupling phenomena in 1T-TiSe$_2$ in both momentum and time. We are able to distinguish effects due to the real part of the many-body bare electronic susceptibility, $\Re\left[χ_0(\mathbf{q})\right]$, from those due to the electron-phonon coupling vertex, $g_{\mathbf{q}}$, by following the response of semi-metallic (normal phase) 1T-TiSe$_2$ to the selective photo-doping of carriers into the electron pocket …
We investigate electron-phonon coupling in many-electron systems using dynamical mean-field theory in combination with the numerical renormalization group. This non-perturbative method reveals significant precursor effects to the gap formation at intermediate coupling strengths. The emergence of a soft phonon mode and very strong lattice fluctuations can be understood in terms of Kondo-like physics due to the development of a double-well structure in the effective potential for the ions.
Phonon softening is a ubiquitous phenomenon in condensed matter systems which is often associated with charge density wave (CDW) instabilities and anharmonicity. The interplay between phonon softening, CDW and superconductivity is a topic of intense debate. In this work, the effects of anomalous soft phonon instabilities on superconductivity are studied based on a recently developed theoretical framework that accounts for phonon damping and softening within the Migdal-Eliashberg theory. Model calculations show that the phonon softening in the form of a sharp dip in the phonon dispersion relati…
Phonons in nearly optimally doped HgBa$_2$CuO$_{4+δ}$ were studied by inelastic X-ray scattering. The dispersion of the low energy modes is well described by a shell model, while the Cu-O bond stretching mode at high energy shows strong softening towards the zone boundary, which deviates strongly from the model. This seems to be common in the hole-doped high-$T_\mathrm{c}$ superconducting cuprates, and, based on this work, not related to a lattice distortion specific to each material.
We measured phonon dispersion in single crystal EuTiO$_3$ using inelastic x-ray scattering. A structural transition to an antiferrodistortive phase was found at a critical temperature $T_0$=287$\pm$1 K using powder and single-crystal x-ray diffraction. Clear softening of the zone boundary \emph{R}-point \textbf{q}=(0.5 0.5 0.5) acoustic phonon shows this to be a displacive transition. The mode energy plotted against reduced temperature could be seen to nearly overlap that of $\rm SrTiO_3$, suggesting a universal scaling relation. Phonon dispersion was measured along $Γ$-$X$ (0 0 0)$\rightarrow…
We use diffuse and inelastic x-ray scattering to study the formation of an incommensurate charge-density-wave (I-CDW) in BaNi$_2$As$_2$, a candidate system for charge-driven electronic nematicity. Intense diffuse scattering is observed around the modulation vector of the I-CDW, $Q_{I-CDW}$. It is already visible at room temperature and collapses into superstructure reflections in the long-range ordered state where a small orthorhombic distortion occurs. A clear dip in the dispersion of a low-energy transverse optical phonon mode is observed around $Q_{I-CDW}$. The phonon continuously softens u…
Soft Phonon Charge-Density Wave Formation in the Kagome Metal KV$_3$Sb$_5$
Zhejiang University（浙江大学）；Hangzhou Normal University（杭州师范大学）；University of Science and Technology of China（中国科学技术大学）；Zhejiang University of Technology（浙江工业大学）；Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China（中国科学院微观尺度物理科学合肥国家研究中心，中国科学技术大学）
Monoclinic crystal structure of the undoped BaBiO3 can be described as a cubic perovskite distorted by a frozen breathing and tilting phonon modes of BiO6 octahedra. The phonon mode softening is experimentally observed [M. Braden et al., Europhysics Letters (EPL) 34, 531 (1996)] in Ba1-xKxBiO3 through potassium doping followed by a transition into an ideal cubic perovskite structure at x = 0.37 close to the appearance of superconductivity. In our previous paper [D. Korotin et al., Journal of Physics: Condensed Matter 24, 415603 (2012)] we demonstrated that it is necessary to take into account …
The quasi-skutterudite superconductors $A_3T_4$Sn$_{13}$ ($A$=Sr, Ca; $T$=Ir, Rh, Co) are highly tunable featuring a structural quantum critical point. We construct a temperature-lattice constant phase diagram for these isovalent compounds, establishing Ca$_{3}$Rh$_4$Sn$_{13}$ and Ca$_{3}$Co$_4$Sn$_{13}$ as members close to and far away from the structural quantum critical point, respectively. Deconvolution of the lattice specific heat and the electrical resistivity provide an approximate phonon density of states $F(ω)$ and the electron-phonon transport coupling function $α_{tr}^2F(ω)$ for Ca$…
