The bulk photovoltaic effect is an example of a non-linear optical response that leads to a DC current that is relevant for photo-voltaic applications. In this work, we theoretically study this effect in the presence of electron-phonon interactions. Using the response function formalism we find that the non-linear optical response, in general, contains three operator correlation functions, one of which is not ordered in time. This latter correlator cannot be computed from equilibrium field theory. Using a semiclassical approach instead, we show that the bulk photovoltaic effect can be attributed to the dipole moment of the generated excitons. We then confirm the validity of the semiclassical result (which agrees with the non-interacting result) for non-linear DC response from a quantum master equation approach. From this formalism we find that, in contrast to usual linear response, the scattering rate has a strong implicit effect on the non-linear DC response. Most interestingly, the semiclassical treatment shows that the non-linear DC response for spatially inhomogeneous excitation profiles is strongly non-local and must involve the aforementioned out-of-time-ordered correlators that cannot be computed by equilibrium field theory.
Broadband, efficient and fast conversion of light to electricity is crucial for sensing and clean energy. Here we reveal the largest observed bulk photo-voltaic effect (BPVE), an intrinsic mechanism predicted to be ultrafast and exceed the Shockley-Quiesser limit. This discovery results from combining recent developments in the connection of BPVE to topology, Weyl semimetals and focused-ion beam fabrication. Our room temperature observation of the first BPVE in the mid-IR, is enabled by microscopic devices of the Weyl semimetal TaAs. Detailed symmetry analysis enables unambiguous separation of…
Successful incorporation of the spin degree of freedom in semiconductor technology requires the development of a new paradigm allowing for a scalable, non-destructive electrical detection of the spin-polarization of injected charge carriers as they propagate along the semiconducting channel. In this paper we report the observation of a spin-injection Hall effect (SIHE) which exploits the quantum-relativistic nature of spin-charge transport and which meets all these key requirements on the spin detection. The two-dimensional electron-hole gas photo-voltaic cell we designed to observe the SIHE a…
Non-equilibrium transport properties and energy conversion performance of a molecular photo-voltaic cell are analyzed using the Lindblad master equation within the open quantum systems approach. The method allows us to calculate the dynamics of a system driven by several non-equilibrium sources (a situation we call "strong non-equilibrium"), which is the natural operating condition of photovoltaic cells. We include both coherent and incoherent processes and treat electrons, photon, and phonons on an equal footing. We find that decoherence plays a crucial role in determining both the overall ef…
This paper presents a study of dc photocurrents in biased insulators to the third order in the electric field. We find three photocurrents which are characterized by physical divergences of the third-order free-electron polarization susceptibility. In the absence of momentum relaxation and saturation effects, these dc photocurrents grow as $t^n$ $(n=2,1,0)$ with illumination time. The photocurrents are dubbed \textit{jerk}, third-order injection, and third-order shift current, respectively, and are generalizations of the second-order injection and shift currents of the bulk photovoltaic effect…
We study theoretically 2D HgTe/CdTe quantum well topological insulator (TI) illuminated by circularly polarized light with frequencies higher than the difference between the equilibrium Fermi level and the bottom of the conduction band (THz range). We show that electron-hole asymmetry results in spin-dependent electric dipole transitions between edge and bulk states, and we predict an occurrence of a circular photocurrent. If the edge state is tunnel-coupled to a conductor, then the photocurrent can be detected by measuring an electromotive force (EMF) in the conductor, which is proportional t…
The surface Fermi arc, as a hallmark of Weyl semimetals (WSMs), has been well known in current research, but it remains a challenge to unveil novel phenomena associated with the Fermi arc. Here, we predict a heretofore unrecognized process in WSMs, namely, the photoinduced transition between the bulk states and the Fermi arc. We find this process is significant and can lead to a large effective three-dimensional shift current on the boundaries with the Fermi arc in wide terahertz range. Moreover, due to the low symmetry of the boundaries, the surface photogalvanic effect predicted here can app…
The circular photon drag effect is observed in a bulk semiconductor. The photocurrent caused by a transfer of both translational and angular momenta of light to charge carriers is detected in tellurium in the mid-infrared frequency range. Dependencies of the photocurrent on the light polarization and on the incidence angle agree with the symmetry analysis of the circular photon drag effect. Microscopic models of the effect are developed for both intra- and inter-subband optical absorption in the valence band of tellurium. The shift contribution to the circular photon drag current is calculated…
Topological insulators possess completely different spin-orbit coupled bulk and surface electronic spectra that are each predicted to exhibit exotic responses to light. Here we report time-resolved fundamental and second harmonic optical pump-probe measurements on the topological insulator Bi2Se3 to independently measure its photo-induced charge and spin dynamics with bulk and surface selectivity. Our results show that a transient net spin density can be optically induced in both the bulk and surface, which may drive spin transport in topological insulators. By utilizing a novel rotational ani…
Models of organic bulk heterojunction photovoltaics which include the effect of spatially varying composition of donor/acceptor materials are developed and analyzed. Analytic expressions for the current-voltage relation in simplified cases show that the effect of varying blend composition on charge transport is minimal. Numerical results for various blend compositions, including the experimentally relevant composition of a donor-rich region near the cathode (a "skin layer" of donor material), show that the primary effect of this variation on device performance derives from its effect on photoc…
We investigate the Terahertz(THz)-response of a square antidot superlattice by means of photoconductivity measurements using a Fourier-transform-spectrometer. We detect, spectrally resolved, the cyclotron resonance and the fundamental magnetoplasmon mode of the periodic superlattice. In the dissipative transport regime both resonances are observed in the photoresponse. In the adiabatic transport regime, at integer filling factor $ν=2$, only the cyclotron resonance is observed. From this we infer that different mechanisms contribute to converting the absorption of THz-radiation into photoconduc…
We study the low-frequency properties of the bulk photovoltaic effect in topological semimetals. The bulk photovoltaic effect is a nonlinear optical effect that generates DC photocurrents under uniform irradiation, allowed by noncentrosymmetry. It is a promising mechanism for a terahertz photodetection based on topological semimetals. Here, we systematically investigate the low-frequency behavior of the second-order optical conductivity in point-node semimetals. Through symmetry and power-counting analysis, we show that Dirac and Weyl points with tilted cones show the leading low-frequency div…
We investigate the bulk photovoltaic effect, which rectifies light into electric current, in a collective quantum state with correlation driven electronic ferroelectricity. We show via explicit real-time dynamical calculations that the effect of the applied electric field on the electronic order parameter leads to a strong enhancement of the bulk photovoltaic effect relative to the values obtained in a conventional insulator. The enhancements include both resonant enhancements at sub-band-gap frequencies, arising from excitation of optically active collective modes, and broadband enhancements …
As the responsivity (R) of a thin film photo detector is proportional to the product of the photo-induced carrier density (n) and mobility (u) (Z. Sun, Z. Liu, J. Li, G.-a. Tai, S. Lau and F. Yan, Adv. Mater., 24, 5878, 2012), which of the types is conducive to photo detection, choosing between layer-heterojunction (LH) and bulk-heterojunction (BH) field effect phototransistors (FEpTs), is still unknown. A comparison study is performed based on an MEH-PPV and PbS QDs hybrid.
Spin current generators are critical components for spintronics-based information processing. In this work, we theoretically and computationally investigate the bulk spin photovoltaic (BSPV) effect for creating DC spin current under light illumination. The only requirement for BPSV is inversion symmetry breaking, thus it applies to a broad range of materials and can be readily integrated with existing semiconductor technologies. The BSPV effect is a cousin of the bulk photovoltaic (BPV) effect, whereby a DC charge current is generated under light. Thanks to the different selection rules on spi…
We investigate the shift current bulk photovoltaic response of materials close to a band inversion topological phase transition. We find that the bulk photocurrent reverses direction across the band inversion transition, and that its magnitude is enhanced in the vicinity of the phase transition. These results are demonstrated with first principles DFT calculations of BiTeI and CsPbI$_3$ under hydrostatic pressure, and explained with an analytical model, suggesting that this phenomenon remains robust across disparate material systems.
Optical injection and detection of charge currents can complement conventional transport and photoemission measurements without the necessity of invasive contact that may disturb the system being examined. This is a particular concern for the surface states of a topological insulator. In this work one- and two-color sources of photocurrents are examined in epitaxial, thin films of Bi2Se3. We demonstrate that optical excitation and terahertz detection simultaneously captures one- and two- color photocurrent contributions, as previously not required in other material systems. A method is devised…
We investigate the non-linear response and energy absorption in bulk silicon irradiated by intense 12-fs near-infrared laser pulses. Depending on the laser intensity, we distinguish two regimes of non-linear absorption of the laser energy: for low intensities, energy deposition and photoionization involve perturbative three-photon transition through the direct bandgap of silicon. For laser intensities near and above 10$^{14}$ W/cm$^2$, corresponding to photocarrier density of order 10$^{22}$ cm$^{-3}$, we find that absorption at near-infrared wavelengths is greatly enhanced due to excitation o…
We compute the electric spin susceptibility of Bloch electrons with spin-orbit coupling to second order. We find that it is possible to generate a nonequilibrium spin polarization in the bulk of non-magnetic inversion-symmetric materials using linearly polarized electric fields, but the process depends on interband coherence and produces heating. It may be possible to avoid heating with circular polarization in certain scenarios. The standard Edelstein effect and spin orientation effects are recovered in appropriate limits within the formalism. Finally, the electric spin susceptibility of meta…
Effects of interface regularity on the bulk-edge correspondence in continuum photonic systems
University of Chicago（芝加哥大学）；Committee on Computational and Applied Mathematics, University of Chicago（芝加哥大学计算与应用数学委员会）；Departments of Mathematics and Statistics, University of Chicago（芝加哥大学数学与统计系）
We study ultrafast photocurrents in thin films of a model ferromagnetic metal with broken bulk inversion symmetry, the half-metallic Heusler compound NiMnSb, following excitation with an optical pump pulse with photon energy 1.55 eV. Remarkably, in terms of the direction of the sample magnetization M, all photocurrents are found to be a superposition of a component with Rashba- and Dresselhaus-type symmetry. We explain the Dresselhaus bulk photocurrent as follows: Pump-induced electron heating induces an excess of spin μ_s||M, which transfers spin angular momentum into states with Dresselhaus-…
A hallmark of topological band theory in periodic media is that bulk properties are not affected by boundary conditions. Remarkably, in certain non-Hermitian lattices the bulk properties are largely affected by boundaries, leading to such major effects as the non-Hermitian skin effect and violation of the bulk-boundary correspondence. Here we unveil that non-unitary discrete-time quantum walks of photons in systems involving gain and loss show rather generally non-Bloch parity-time ($\mathcal{PT}$) symmetry breaking phase transitions, and suggest a bulk probing method to detect such boundary-d…
Direct spatiotemporal imaging of carriers reveals a long-lived bulk photovoltaic mechanism
Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST（加泰罗尼亚纳米科学与纳米技术研究所）；TU Eindhoven（埃因霍温理工大学）；University of Pennsylvania（宾夕法尼亚大学）；SPEC, CEA, CNRS, Université Paris-Saclay（巴黎萨克雷大学）；ICREA - Institució Catalana de Recerca i Estudis Avançats（加泰罗尼亚研究与高级研究学院）
