Ultrafast dynamic conductivity and scattering rate saturation of photoexcited charge carriers in silicon investigated with a midinfrared continuum probe
Fanqi Meng, Mark D. Thomson, Bo E. Sernelius, Michael Jörger, Hartmut G. Roskos
We employ ultra-broadband terahertz-midinfrared probe pulses to characterize the optical response of photoinduced charge-carrier plasmas in high-resistivity silicon in a reflection geometry, over a wide range of excitation densities (10^{15}-10^{19} cm^{-3}) at room temperature. In contrast to conventional terahertz spectroscopy studies, this enables one to directly cover the frequency range encompassing the resultant plasma frequencies. The intensity reflection spectra of the thermalized plasma, measured using sum-frequency (up-conversion) detection of the probe pulses, can be modeled well by a standard Drude model with a density-dependent momentum scattering time of approx. 200 fs at low densities, reaching approx. 20 fs for densities of approx. 10^{19} cm^{-3}, where the increase of the scattering rate saturates. This behavior can be reproduced well with theoretical results based on the generalized Drude approach for the electron-hole scattering rate, where the saturation occurs due to phase-space restrictions as the plasma becomes degenerate. We also study the initial sub-picosecond temporal development of the Drude response, and discuss the observed rise in the scattering time in terms of initial charge-carrier relaxation, as well as the optical response of the photoexcited sample as predicted by finite-difference time-domain simulations.
We calculate the ferroelectric polarization dynamics induced by a femtosecond midinfrared pulse as measured in the recent experiment by R. Mankowsky et al., Phys. Rev. Lett. 118, 197601 (2017). It is due to the nonlinear coupling of the excited infrared-active phonon with the ferroelectric mode or to the excitation of the ferroelectric mode itself depending on the pulse frequency. To begin with, we write the LiNbO$_3$ crystal symmetry invariant thermodynamic potential including electric field and nonlinear phonon coupling terms. We solve the equations of motion determined by this potential for…
The electromagnetic response of Dirac semimetals in the infrared and terahertz frequency ranges is attracting growing interest for potential applications in optoelectronics and nonlinear optics. The interplay between the free-carrier response and interband transitions in the gapless, linear dispersion relation plays a key role in enabling novel functionalities. Here we investigate ultrafast dynamics in thin films of a photoexcited Dirac semimetal Cd$_3$As$_2$ by probing the broadband response functions as complex quantities in the multiterahertz region (10-45 THz, 40-180 meV, or 7-30 $μ$m), wh…
We report results from ultrafast two-color optical pump-probe spectroscopy on bulk $β$-Ga$_2$O$_3$. A two-photon absorption scheme is used to photoexcite carriers with the pump pulse and free-carrier absorption of the probe pulse is used to record the subsequent dynamics of the photoexcited carriers. Our results are consistent with carrier recombination via defect-assisted processes. We also observe transient polarization-selective optical absorption of the probe pulse by defect states under nonequilibrium conditions. A rate equation model for electron and hole capture by defects is proposed a…
We theoretically study the dynamic time evolution following laser pulse pumping in an antiferromagnetic insulator Cr$_{2}$O$_{3}$. From the photoexcited high-spin quartet states to the long-lived low-spin doublet states, the ultrafast demagnetization processes are investigated by solving the dissipative Schrödinger equation. We find that the demagnetization times are of the order of hundreds of femtosecond, in good agreement with recent experiments. The switching times could be strongly reduced by properly tuning the energy gaps between the multiplet energy levels of Cr$^{3+}$. Furthermore, th…
There is growing interest in using ultrafast light pulses to drive functional materials into nonequilibrium states with novel properties. The conventional wisdom is that above gap photoexcitation behaves similarly to raising the electronic temperature and lacks the desired selectivity in the final state. Here we report a novel nonthermal lattice instability induced by ultrafast above-gap excitation in SnSe, a representative of the IV-VI class of semiconductors that provides a rich platform for tuning material functionality with ultrafast pulses due to their multiple lattice instabilities. The …
Ultrafast electron dynamics of solids after an absorption of femtosecond laser pulse is governed by electron-electron, electron-phonon, phonon-electron, and phonon-phonon collisions. It is of importance to construct a framework for interpreting experimental observations correctly. In this paper we review recent developments of modeling the relaxation dynamics of solids. We discuss the ultrafast relaxation in respect to the effective temperature dynamics and the excess energy dynamics.
We present a first-principles method for the calculation of the temperature-dependent relaxation of symmetry-breaking atomic driving forces in photoexcited systems. We calculate the phonon-assisted decay of the photoexcited force on the low-symmetry $E_g$ mode following absorption of an ultrafast pulse in the prototypical group-V semimetals, Bi, Sb and As. The force decay lifetimes for Bi and Sb are of the order of $10$ fs and in good agreement with recent experiments, demonstrating that electron-phonon scattering is the dominant mechanism relaxing the symmetry-breaking forces. Calculations fo…
In order to determine the role of non-thermal transport of hot carriers which is decisive for the dissipation of energy in condensed matter we performed time-resolved broadband femtosecond transient reflectivity measurements on $7-197 \mathrm{nm}$ thick Bi(111) films epitaxially grown on Si(111). We monitored the behavior of the Fourier amplitude and the central frequency of the coherent $A_\mathrm{1g}$ phonon mode as function of the incident fluence, film thickness, and probe wavelength in the range of $580 -700 \mathrm{nm}$. The frequency redshift that follows photoexcitation was used as a r…
The perturbation of a semiconductor from the thermodynamic equilibrium often leads to the display of nonlinear dynamics and formation of spatiotemporal patterns due to the spontaneous generation of competing processes. Here, we describe the ultrafast imaging of nonlinear carrier transport in silicon, excited by an intense femtosecond laser pulse. We use scanning ultrafast electron microscopy (SUEM) to show that, at a sufficiently high excitation fluence, the transport of photoexcited carriers slows down by turning into an oscillatory process. We attribute this nonlinear response to the electri…
We present a complementary experimental and theoretical investigation of relaxation dynamics in the charge-density-wave (CDW) system TbTe$_3$ after ultrafast optical excitation. Using time- and angle-resolved photoemission spectroscopy, we observe an unusual transient modulation of the relaxation rates of excited photocarriers. A detailed analysis of the electron self-energy based on a nonequilibrium Green's function formalism reveals that the phase space of electron-electron scattering is critically modulated by the photoinduced collective CDW excitation, providing an intuitive microscopic un…
We present a constrained density functional perturbation theory scheme for the calculation of structural and harmonic vibrational properties of insulators in the presence of an excited and thermalized electron-hole plasma. The method is ideal to tame ultrafast light induced structural transitions in the regime where the photocarriers thermalize faster than the lattice, the electron-hole recombination time is longer than the phonon period and the photocarrier concentration is large enough to be approximated by an electron-hole plasma. The complete derivation presented here includes total energy…
The element specificity of soft X-ray spectroscopy makes it an ideal tool for analyzing the microscopic origin of ultrafast dynamics induced by localized optical excitation in metal-insulator heterostructures. Using [Fe/MgO]$_n$ as a model system, we perform ultraviolet pump/soft X-ray probe experiments, which are sensitive to all constituents of these heterostructures, to probe both electronic and lattice excitations. Complementary ultrafast electron diffraction experiments independently analyze the lattice dynamics of the Fe constituent, and together with ab initio calculations yield compreh…
Simultaneous measurements of transient transmission and reflectivity were performed in the unintentionally doped InN film to reveal ultrafast optical bleaching and its recovery behavior under intense laser irradiation. The optical bleaching is attributed to Pauli blocking due to the occupation of photoexcited electrons at the probing energy level. The time constant for the transition from the excitation state to the conduction band edge is $\sim$260 fs. The interplay between band filling and band gap renormalization caused by electron-hole and electron-electron interactions gives rise to compl…
Tuning of Photoexcited Electron Dynamics at Monolayer h-BN/Metal Interfaces by Corrugation
Osaka Metropolitan University（大阪公立大学）；Institute for Molecular Science, National Institutes of Natural Sciences（国立自然科学院分子科学研究所）；Friedrich Schiller University Jena（耶拿弗里德里希·席勒大学）
A Route to Nonrelativistic Altermagnetic Spin Splitting via Ultrafast Light
State Key Laboratory of Semiconductor Physics and Chip Technologies, Institute of Semiconductors, Chinese Academy of Sciences（中国科学院半导体研究所半导体物理与芯片技术国家重点实验室）；Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences（中国科学院大学材料科学与光电工程技术中心）；Department of Materials Science and Engineering, Northwestern University（西北大学材料科学与工程系）
We use time- and angle-resolved photoemission spectroscopy (tr-ARPES) to investigate ultrafast charge transfer in an epitaxial heterostructure made of monolayer WS$_2$ and graphene. This heterostructure combines the benefits of a direct gap semiconductor with strong spin-orbit coupling and strong light-matter interaction with those of a semimetal hosting massless carriers with extremely high mobility and long spin lifetimes. We find that, after photoexcitation at resonance to the A-exciton in WS$_2$, the photoexcited holes rapidly transfer into the graphene layer while the photoexcited electro…
Hybrid quantum dot (QD) / transition metal dichalcogenide (TMD) heterostructures are attractive components of next generation optoelectronic devices, which take advantage of the spectral tunability of QDs and the charge and exciton transport properties of TMDs. Here, we demonstrate tunable electronic coupling between CdSe QDs and monolayer WS$_2$ using variable length alkanethiol ligands on the QD surface. Using femtosecond time-resolved second harmonic generation (SHG) microscopy, we show that electron transfer from photoexcited CdSe QDs to single-layer WS$_2$ occurs on ultrafast (50 fs - 1 p…
In hybrid lead halide perovskites, the coupling between photogenerated charges and the ionic degrees of freedom plays a crucial role in defining the intrinsic limit of carrier mobility and lifetime. However, direct investigation of this fundamental interaction remains challenging because its relevant dynamics occur on ultrashort spatial and ultrafast temporal scales. Here, we unveil the coupled electron-lattice dynamics of a CH3NH3PbI3 single crystal upon intense photoexcitation through a unique combination of ultrafast electron diffraction, time-resolved photoelectron spectroscopy, and time-d…
Charge transfer between photoexcited quantum dots and molecular acceptors is one of the key limiting processes in most applications of colloidal nanostructures, most prominently in photovoltaics. An atomistic detailed description of this process would open new ways to optimize existing and create new structures with targeted properties. We achieve a one-to-one comparison between ab-initio non-adiabatic molecular dynamics calculations and transient absorption spectroscopy experiments, which allows us to draw a comprehensive atomistic picture of the charge transfer process, following the time ev…
Photoinduced phase transition (PIPT) is always treated as a coherent process, but ultrafast disordering in PIPT is observed in recent experiments. Utilizing the real-time time-dependent density functional theory (rt-TDDFT) method, here, we track the motion of individual vanadium (V) ions during PIPT in VO2 and uncover that their coherent or disordered dynamics can be manipulated by tuning the laser fluence. We find that the photoexcited holes generate a force on each V-V dimer to drive their collective coherent motion, in competing with the thermal-induced vibrations. If the laser fluence is s…
Recently, the switching between the different charge-ordered phases of 1T-TaS2 has been probed by ultrafast techniques, revealing unexpected phenomena such as "hidden" metastable states and peculiar photoexcited charge patterns. Here, we apply broadband pump-probe spectroscopy with varying excitation energy to study the ultrafast optical properties of 1T-TaS2 in the visible regime. By scanning the excitation energy in the near-IR region we unravel the coupling between different charge excitations and the low-lying charge-density wave state. We find that the amplitude mode of the charge-density…
Fast carrier cooling is important for high power graphene based devices. Strongly Coupled Optical Phonons (SCOPs) play a major role in the relaxation of photoexcited carriers in graphene. Heterostructures of graphene and hexagonal boron nitride (hBN) have shown exceptional mobility and high saturation current, which makes them ideal for applications, but the effect of the hBN substrate on carrier cooling mechanisms is not understood. We track the cooling of hot photo-excited carriers in graphene-hBN heterostructures using ultrafast pump-probe spectroscopy. We find that the carriers cool down f…
Recent years have seen the rapid discovery of solids whose low-energy electrons have a massless, linear dispersion, such as Weyl, line-node, and Dirac semimetals. The remarkable optical properties predicted in these materials show their versatile potential for optoelectronic uses. However, little is known of their response in the picoseconds after absorbing a photon. Here we measure the ultrafast dynamics of four materials that share non-trivial band structure topology but that differ chemically, structurally, and in their low-energy band structures: ZrSiS, which hosts a Dirac line node and Di…
Laser-induced nonthermal melting in semiconductors has been studied over the last four decades, but the underlying mechanism is still under debate. Here, by utilizing an advanced real-time time-dependent density functional theory simulation, we reveal that the photoexcitation-induced ultrafast nonthermal melting in silicon occurs via homogeneous nucleation with random seeds originating from a self-amplified local dynamic instability at the photoexcited states rather than by simultaneously breaking of all bonds, as suggested by the inertial model, phonon instability, or Coulombic repulsion mech…
We use an x-ray free-electron laser to study the ultrafast lattice dynamics following above band-gap photoexcitation of the incipient ferroelectric potassium-tantalate, \kto. % We use ultrafast near-UV (central wavelength 266\,nm and 50 fs pulse duration) laser light to photoexcite charge carriers across the gap and probe the ultrafast lattice dynamics by recording the x-ray diffuse intensity throughout multiple Brillouin zones using pulses from the Linac Coherent Light Source (LCLS) (central wavelength 1.3\,Å\, and $< 10$~fs pulse duration). We observe changes in the diffuse intensity that we…
