Ultrafast energy relaxation of quantum dot-generated 2D hot electrons
Dongsung T. Park, Dongkun Kim, Uhjin Kim, Hwanchul Jung, Juho Choi, Cheolhee Han, Yunchul Chung, H. -S. Sim, V. Umansky, Hyoungsoon Choi, Hyung Kook Choi
Through a series of transverse magnetic focusing experiments, we show that hot electrons in a two-dimensional electron gas system undergo an ultrafast relaxation when generated by a quantum dot (QD) instead of a quantum point contact (QPC). We find here that QPC hot electrons were well described by the non-interacting Fermi gas model for excitations up to 1.5 meV above the Fermi level of 7.44 meV, whereas QD hot electrons exhibited an energy loss quadratic to the excitation. The energy relaxation was a sizeable fraction of the tested excitations, up to about 55%. With the proposal that the hot electrons are relaxed by the QD immediately after emission, we present a toy model in which a capacitive coupling between the QD and its leads results in a finite, ultrafast energy relaxation.
Employing the ultrafast control of electronic states of a semiconductor quantum dot in a cavity, we introduce a novel approach to achieve on-demand emission of single photons with almost perfect indistinguishability and photon pairs with near ideal entanglement. Our scheme is based on optical excitation off-resonant to a cavity mode followed by ultrafast control of the electronic states using the time-dependent quantum-confined Stark effect, which then allows for cavity-resonant emission. Our theoretical analysis takes into account cavity-loss mechanisms, the Stark effect, and phonon-induced d…
Harvesting non-equilibrium hot carriers from photo-excited metal nanoparticles has enabled plasmon-driven photochemical transformations and tunable photodetection with resonant nanoantennas. Despite numerous studies on the ultrafast dynamics of hot electrons, to date, the temporal evolution of hot holes in metal-semiconductor heterostructures remains unknown. An improved understanding of the carrier dynamics in hot-hole-driven systems is needed to help expand the scope of hot-carrier optoelectronics beyond hot-electron-based devices. Here, using ultrafast transient absorption spectroscopy, we …
We study theoretically the fluctuation properties of acoustic phonons created in a semiconductor quantum dot after ultrafast optical excitation. An excitation with a single ultrafast pulse creates an exciton confined to the quantum dot, which is coupled to longitudinal acoustic phonons. This leads to the formation of a polaron in the quantum dot accompanied by the emission of a phonon wave packet. We show that the fluctuations of the lattice displacement associated with the wave packet after a single laser pulse excitation in resonance with the exciton transition are always larger than their r…
We demonstrate ultrafast incoherent depopulation of a quantum dot from above to below the transparency point using LA-phonon-assisted emission stimulated by a redshifted laser pulse. The QD is turned from a weakly vibronic system into a strongly vibronic one by laser driving which enables the phonon-assisted relaxation between the excitonic components of two dressed states. The depopulation is achieved within a laser pulse-width-limited time of 20 ps and exhibits a broad tuning range of a few meV. Our experimental results are well reproduced by path-integral calculations.
We have studied theoretically the possibility of ultra-fast manipulation of a single electron spin in 2D semiconductor quantum dots, by means of high-frequency time-dependent electric fields. The electron spin degree of freedom is excited through spin-orbit coupling, and the procedure may be enhanced by the presence of a static magnetic field. We use quantum optimal control theory to tailor the temporal profile of the electric field in order to achieve the most effective manipulation. The scheme predicts significant control over spin operations in times of the order of picoseconds -- an ultraf…
We study, by means of a Monte Carlo simulator, the hot phonon effect on the relaxation dynamics in photoexcited graphene and its quantitative impact as compared to considering an equilibrium phonon distribution. Our multi-particle approach indicates that neglecting the hot phonon effect significantly underestimates the relaxation times in photoexcited graphene. The hot phonon effect is more important for a higher energy of the excitation pulse and photocarrier densities between $1$ and $3\times 10^{12} \mathrm{~cm}^{-2}$. Acoustic intervalley phonons play a non-negligible role, and emitted pho…
We analyze ultrafast electron dynamics in the time domain upon optical excitation of propagating surface plasmon-polaritons (SPs) in metal-dielectric heterostructures. Developing a kinetic model where both local and non-local electron relaxation in metals are included, we identify relevant timescales and extend the existing non-equilibrium electron dynamics framework onto the case of collective electronic excitations. The experimental data obtained in two distinct series of pump-probe measurements (with varied pump wavelength and angle of incidence) demonstrate SP-driven, one order of magnitud…
We consider a double quantum dot system with two embedded and non-aligned spin impurities to manipulate the magnitude and polarization of the electron spin density. The device is attached to semi-infinite one-dimensional leads which are treated exactly. We provide a real-time description of the electron spin dynamics when a sequence of ultrafast voltage pulses acts on the device. The numerical simulations are carried out using a spin generalized and modified version of a recently proposed algorithm for the time propagation of open systems [Phys. Rev. B {\bf 72}, 035308 (2005)]. Time-dependent …
Coherent manipulation of quantum bits (qubits) on time scales much shorter than the coherence time is a key prerequisite for quantum information processing. Electron spins in quantum dots (QDs) are particularly attractive for implementations of qubits. Efficient optical methods for initialization and readout of spins have been developed in recent years. Spin coherence times in the microsecond range have been demonstrated, so that spin control by picosecond optical pulses would be highly desirable. Then a large number of spin rotations could be performed while coherence is maintained. A major r…
Efficient operation of electronic nanodevices at ultrafast speeds requires understanding and control of the currents generated by femtosecond bursts of light. Ultrafast laser-induced currents in metallic nanojunctions can originate from photo-assisted hot electron tunneling or lightwave-induced tunneling. Both processes can drive localized photocurrents inside a scanning tunneling microscope (STM) on femto- to attosecond time scales, enabling ultrafast STM with atomic spatial resolution. Femtosecond laser excitation of a metallic nanojunction, however, also leads to the formation of a transien…
We demonstrate the all-optical ultrafast manipulation and read-out of optical transitions in a single negatively charged self-assembled InAs quantum dot, an important step towards ultrafast control of the resident spin. Experiments performed at zero magnetic field show the excitation and decay of the trion (negatively charged exciton) as well as Rabi oscillations between the electron and trion states. Application of a DC magnetic field perpendicular to the growth axis of the dot enables observation of a complex quantum beat structure produced by independent precession of the ground state elect…
We propose a fast and accurate spin initialization method for a single electron trapped in an electrostatic quantum dot. The dot is created in a nanodevice composed of a catalytically grown indium antimonide (InSb) nanowire and nearby gates to which control voltages are applied. Initially we insert a single electron of arbitrary spin into the wire. Operations on spin are performed using the Rashba spin-orbit interaction induced by an electric field. First, a single pulse of voltages applied to lateral gates is used to split the electron wavepacket into two parts with opposite spin orientations…
We demonstrate three-photon excitation in quantum dots with a mode-locked fiber laser operating in the telecommunications band. We compare spectra and intensity dependence of fluorescence from one- and three-photon excitation of commercially available 640 nm quantum dots, using a 372 nm diode laser for one-photon excitation and 116 fs pulses from a mode-locked fiber laser with a center wavelength of 1575 nm for three-photon excitation.
Using ultrafast pump-probe reflectivity with 3.1 eV pump and coherent white light probe (1.1 to 2.6 eV), we show that graphene on gold nanostructures exhibits a strong coupling to the plasmonic resonances of the ordered lattice hole array, thus injecting a high density of hot carriers in graphene through plasmons. The system being studied is single-layer graphene on ultrathin film of gold with periodic arrangements of holes showing anomalous transmission. A comparison is made with gold film with and without hole array. By selectively probing transient carrier dynamics in the spectral regions c…
When a two-level quantum dot and a plasmonic metal nanoantenna are resonantly coupled by the electromagnetic near field, the system can exhibit a Fano resonance, resulting in a transparency dip in the optical spectrum of the coupled system. We calculate the nonlinear response of such a system, for illumination both by continuous-wave and ultrafast pulsed lasers, using both a cavity quantum electrodynamics and a semiclassical coupled-oscillator model. For the experimentally relevant case of meV thermal broadening of the quantum-dot transition, we predict that femtosecond pulsed illumination can…
We employ a quantum master equations approach based on a vectorial Maxwell-pseudospin model to compute the quantum evolution of the spin populations and coherences in the fundamental singlet trion transition of a negatively charged quantum dot embedded in a micropillar cavity. Excitation of the system is achieved through an ultrashort, either circularly or linearly polarised resonant pulse. By implementing a realistic micropillar cavity geometry, we numerically demonstrate a giant optical phase shift ($\sim \pm π/2$) of a resonant circularly polarised pulse in the weak-coupling regime. The pha…
A quantum-kinetic approach to the ultrafast dynamics of carrier multiplication in semiconductor quantum dots is presented. We investigate the underlying dynamics in the electronic subband occupations and the time-resolved optical emission spectrum, focusing on the interplay between the light-matter and the Coulomb interaction. We find a transition between qualitatively differing behaviors of carrier multiplication, which is controlled by the ratio of the interaction induced time scale and the pulse duration of the exciting light pulse. On short time scales, i.e., before intra-band relaxation, …
We report on the impulsive generation of coherent optical phonons in CdTe0.68Se0.32 nanocrystallites embedded in a glass matrix. Pump probe experiments using femtosecond laser pulses were performed by tuning the laser central energy to resonate with the absorption edge of the nanocrystals. We identify two longitudinal optical phonons, one longitudinal acoustic phonon and a fourth mode of a mixed longitudinal-transverse nature. The amplitude of the optical phonons as a function of the laser central energy exhibits a resonance that is well described by a model based on impulsive stimulated Raman…
Hole spin qubits in planar Ge heterostructures are one of the frontrunner platforms for scalable quantum computers. In these systems, the spin-orbit interactions permit efficient all-electric qubit control. We propose a minimal design modification of planar devices that enhances these interactions by orders of magnitude and enables low power ultrafast qubit operations in the GHz range. Our approach is based on an asymmetric potential that strongly squeezes the quantum dot in one direction. This confinement-induced spin-orbit interaction does not rely on microscopic details of the device such a…
The interaction between two quantum bits enables entanglement, the two-particle correlations that are at the heart of quantum information science. In semiconductor quantum dots much work has focused on demonstrating single spin qubit control using optical techniques. However, optical control of entanglement of two spin qubits remains a major challenge for scaling from a single qubit to a full-fledged quantum information platform. Here, we combine advances in vertically-stacked quantum dots with ultrafast laser techniques to achieve optical control of the entangled state of two electron spins. …
Phonon-Bottleneck-Governed Ultrafast Hot-Carrier Super-Diffusion in Transition Metal Dichalcogenides
Key Laboratory of Quantum Materials and Devices of Ministry of Education, School of Physics, Southeast University（东南大学物理学院教育部量子材料与器件重点实验室）；School of Electronic Science and Engineering, Southeast University（东南大学电子科学与工程学院）
We employ ultrafast pump-probe spectroscopy to directly monitor electron tunneling between discrete orbital states in a pair of spatially separated quantum dots. Immediately after excitation, several peaks are observed in the pump-probe spectrum due to Coulomb interactions between the photo-generated charge carriers. By tuning the relative energy of the orbital states in the two dots and monitoring the temporal evolution of the pump-probe spectra the electron and hole tunneling times are separately measured and resonant tunneling between the two dots is shown to be mediated both by elastic and…
Pauli blockade occurs when the excited electrons fill up the states near the conduction bands and block subsequent absorption in semiconductors, and has been widely applied in mode-locking for passively-pulsed-laser systems. In this letter, we report the first direct observation that the Pauli blockade is broken by ultrafast cooling of hot electrons in optically-pumped graphene. With femtosecond spectroscopy, we demonstrate that the time scale to excite an electron (~100 fs) is of the same order as that of the electron decay via electron-electron scattering, which allows the electron excitatio…
We investigate the hot carrier dynamics of ZrTe$_5$ by ultrafast time-resolved optical reflectivity. Our results reveal a phonon-mediated across-gap recombination, consistent with its temperature-dependent gap nature as observed previously by photoemission. In addition, two distinct relaxations with a kink feature right after initial photoexcitation are well resolved, suggesting the complexity of electron thermalization process. Our findings indicate that correlated many-body effects play important role for the transient dynamics of ZrTe$_5$.
Operation speed and coherence time are two core measures for the viability of a qubit. Strong spin-orbit interaction (SOI) and relatively weak hyperfine interaction make holes in germanium (Ge) intriguing candidates for spin qubits with rapid, all-electrical coherent control. Here we report ultrafast single-spin manipulation in a hole-based double quantum dot in a germanium hut wire (GHW). Mediated by the strong SOI, a Rabi frequency exceeding 540 MHz is observed at a magnetic field of 100 mT, setting a record for ultrafast spin qubit control in semiconductor systems. We demonstrate that the s…
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…
We present results on both the intensity and phase-dynamics of the transient non-linear optical response of a single quantum dot (SQD). The time evolution of the Four Wave Mixing (FWM) signal on a subpicosecond time scale is dominated by biexciton effects. In particular, for the cross-polarized excitation case a biexciton bound state is found. In this latter case, mean-field results are shown to give a poor description of the non-linear optical signal at small times. By properly treating exciton-exciton effects in a SQD, coherent oscillations in the FWM signal are clearly demonstrated. These o…
We study the ultrafast structural dynamics, in response to electronic excitations, in heterostructures composed of Au$_{923}$ nanoclusters on thin-film substrates with the use of femtosecond electron diffraction. Various forms of atomic motion, such as thermal vibrations, thermal expansion and lattice disordering, manifest as distinct and quantifiable reciprocal-space observables. In photo-excited, supported nanoclusters thermal equilibration proceeds through intrinsic heat flow, between their electrons and their lattice, and extrinsic heat flow between the nanoclusters and their substrate. Fo…
Physical implementations of large-scale quantum processors based on solid-state platforms benefit from realizations of quantum bits positioned in regular arrays. Self-assembled quantum dots are well-established as promising candidates for quantum optics and quantum information processing, but they are randomly positioned. Site-controlled quantum dots, on the other hand, are grown in pre-defined locations, but have not yet been sufficiently developed to be used as a platform for quantum information processing. In this letter we demonstrate all-optical ultrafast complete coherent control of a qu…
An ultrafast spin current can be induced by femtosecond laser excitation in a ferromagnetic (FM) thin film in contact with a nonmagnetic (NM) metal. The propagation of an ultrafast spin current into NM metal has recently been found in experiments to generate transient spin accumulation. Unlike spin accumulation in equilibrium NM metals that occurs due to spin transport at the Fermi energy, transient spin accumulation involves highly nonequilibrium hot electrons well above the Fermi level. To date, the diffusion and dissipation of this transient spin accumulation has not been well studied. Usin…
We investigate the usefulness and viability of the scheme developed by Viola and Lloyd [Phys. Rev. A 58, 2733 (1998)] to control dephasing in the context of exciton-based quantum computation with self-assembled quantum dots. We demonstrate that optical coherence of a confined exciton qubit exposed to phonon-induced dephasing can be substantially enhanced through the application of a simple periodic sequence of control pulses. The shape of the quantum dot has a significant effect on the dephasing properties. Remarkably, we find that quantum dots with parameters optimized for implementing quantu…
We use optimal control theory to construct external electric fields which coherently transfer the electronic charge in a double quantum-dot system. Without truncation of the eigenstates we operate on desired superpositions of the states in order to prepare the system to a localized state and to coherently transfer the charge from one well to another. Within a fixed time interval, the optimal processes are shown to occur through several excited states. The obtained yields are generally between 99% and 99.99% depending on the field constraints, and they are not dramatically affected by strict fr…
Hot electron effects in graphene are significant because of graphene's small electronic heat capacity and weak electron-phonon coupling, yet the dynamics and cooling mechanisms of hot electrons in graphene are not completely understood. We describe a novel photocurrent spectroscopy method that uses the mixing of continuous-wave lasers in a graphene photothermal detector to measure the frequency dependence and nonlinearity of hot-electron cooling in graphene as a function of the carrier concentration and temperature. The method offers unparalleled sensitivity to the nonlinearity, and probes the…
Plasmonic nanoparticles hold great promise as photon handling elements and as channels for coherent transfer of energy and information in future all-optical computing devices. Coherent energy oscillations between two spatially separated plasmonic entities via a virtual middle state exemplify electron-based population transfer, but their realization requires precise nanoscale positioning of heterogeneous particles. Here, we show the assembly and optical analysis of a triple particle system consisting of two gold nanoparticles with an inter-spaced silver island. We observe strong plasmonic coupl…
Using ultrafast optical pump-probe spectroscopy, we study the relaxation dynamics of hot optical phonons in few-layer and multi-layer graphene films grown by epitaxy on silicon carbide substrates and by chemical vapor deposition on nickel substrates. In the first few hundred femtoseconds after photoexcitation, the hot carriers lose most of their energy to the generation of hot optical phonons which then present the main bottleneck to subsequent carrier cooling. Optical phonon cooling on short time scales is found to be independent of the graphene growth technique, the number of layers, and the…
We describe a theoretical approach for spin-polarized hot-electron transport, as it occurs after excitation by ultrafast optical pulses in heterostructures formed by ferromagnetic and normal metals. We formulate a spin-dependent particle-in-cell model that solves the Boltzmann equation for excited electrons. It includes lifetimes and transmission coefficients as parameters, which can be taken from ab-initio calculations or experiment, and can be easily extended to multilayer systems. This approach is capable of describing electron transport in the ballistic, super-diffusive and diffusive regim…
We investigate the influence of exciton-phonon coupling on the dynamics of a strongly coupled quantum dot-photonic crystal cavity system and explore the effects of this interaction on different schemes for non-classical light generation. By performing time-resolved measurements, we map out the detuning-dependent polariton lifetime and extract the spectrum of the polariton-to-phonon coupling with unprecedented precision. Photon-blockade experiments for different pulse-length and detuning conditions (supported by quantum optical simulations) reveal that achieving high-fidelity photon blockade re…
We perform a femtosecond-THz optical pump-probe spectroscopy to investigate the cooling dynamics of hot carriers in quasi-free standing bilayer epitaxial graphene. We observed longer decay time constants, in the range of 2.6 to 6.4 ps, compared to previous studies on monolayer graphene, which increase nonlinearly with excitation intensity. The increased relaxation times are due to the decoupling of the graphene layer from the SiC substrate after hydrogen intercalation which increases the distance between graphene and substrate. Furthermore, our measurements do not show that the supercollision …
We investigate waveguide-integrated plasmonic graphene photodetector operating based on the hot carrier photo-bolometric effect, which is characterized simultaneously by high responsivity on the scale of hundreds of AW-1 and high speed on the scale of 100s of GHz. We develop a theory of bolometric effect originating from the band nonparabolicity of graphene and estimate responsivity due to bolometric effect is shown to significantly surpass the responsivity of co-existing photo-conductive effect thus convincingly demonstrating the dominance of bolometric effect. Based on the theory we propose …
A hot-spot of high local field can be created in between two closely placed metal nanoparticles by irradiating them with an appropriate wavelength and polarization of incident light. The strength of the field at the hot-spot is expected to get enhanced by even up to six orders of magnitude than that of the applied field. Placing a semiconductor quantum dot or an analyte molecule at the hot-spot is an essential step towards harnessing the enhanced field for applications. In this article, we show that it is possible to position a CdTe quantum dot (QD) between two larger silver nanospheres in col…
The effects of spin-orbit (SO) coupling arising from the confinement potential in single and two vertically-coupled quantum dots have been investigated. Our work indicates that a dot containing a single electron shows the lifting of the degeneracy of dipole-allowed transitions at B=0 due to the SO coupling which disappears for a dot containing two electrons. For coupled dots with one electron in each dot, the optical spectra is not affected by the coupling and is the same as the dot containing one electron. However, for the case of two coupled dots where one partner dot has two interacting ele…
We examine the multiple exciton population dynamics in PbS quantum dots by ultrafast spectrally-resolved supercontinuum transient absorption (SC-TA). We simultaneously probe the first three excitonic transitions over a broad spectral range. Transient spectra show the presence of first order bleach of absorption for the 1S_h-1S_e transition and second order bleach along with photoinduced absorption band for 1P_h-1P_e transition. We also report evidence of the one-photon forbidden 1S_{h,e}-1P_{h,e} transition. We examine signatures of carrier multiplication (multiexcitons for the single absorbed…
We monitor the dynamics of hot carriers in InSe by means of two photons photoelectron spectroscopy (2PPE). The electrons excited by photons of 3.12 eV experience a manifold relaxation. First, they thermalize to the electronic states degenerate with the $\bar M$ valley. Subsequently, the electronic cooling is dictated by Fröhlich coupling with phonons of small momentum transfer. Ab-initio calculations predict cooling rates that are in good agreement with the observed dynamics. We argue that electrons accumulating in states degenerate with the $\bar M$ valley could travel through a multilayer fl…
Cubic boron arsenide (BAs) is promising for microelectronics thermal management due to its high thermal conductivity. Recently, its potential as an optoelectronic material is also being explored. However, it remains challenging to measure its photocarrier transport properties due to small sizes of available high-quality crystals. Here, we use scanning ultrafast electron microscopy (SUEM) to directly visualize the diffusion of photoexcited charge carriers in BAs single crystals. Surprisingly, we observed ambipolar diffusion at low optical fluence with persistent hot carrier dynamics for above 2…
A new generalised group-theoretical approach, based on master Maxwell-pseudospin equations, is proposed to explain recently observed enhanced circular dichroism in the excited state emission from p-doped quantum dot ensembles under resonant circularly polarised excitation into hot trion states, herein referred to as "spin-filtering effect". The theory agrees remarkably well with polarised time-resolved photoluminescence experiments, yielding largely unknown inter- and intra-shell spin relaxation time scales. This approach allows to predict optimum pulse parameters for control of spin dynamics,…
We report a computational theoretical investigation of electron spin-flip scattering induced by the electron-phonon interaction in the transition-metal ferromagnets bcc Fe, fcc Co and fcc Ni. The Elliott-Yafet electron-phonon spin-flip scattering is computed from first-principles, employing a generalized spin-flip Eliashberg function as well as ab initio computed phonon dispersions. Aiming at investigating the amount of electron-phonon mediated demagnetization in femtosecond laser-excited ferromagnets, the formalism is extended to treat laser-created thermalized as well as nonequilibrium, nont…
Magneto photoluminescence and excitation spectroscopy are used to probe the excited state spectrum of negatively charged trions in a InGaAs quantum dot. A single dot optical charging device allows us to selectively prepare specific few (1e, 2e) electron states and stabilize hot trions against decay via electron tunnelling from excited orbital states. The spin structure of the excited state results in the formation of metastable trions with strong optical activity that are directly observed in luminescence. Excitation spectroscopy is employed to map the excited singlet and triplet states of the…
Using the ultrafast pump-probe transient absorption spectroscopy, the femtosecond-resolved plasmon-exciton interaction of graphene-Ag nanowire hybrids is experimentally investigated, in the VIS-NIR region. The plasmonic lifetime of Ag nanowire is about 150 femtosecond (fs). For a single layer of graphene, the fast dynamic process at 275 fs is due to the excitation of graphene excitons, and the slow process at 1.4 picosecond (ps) is due to the plasmonic hot electron interaction with phonons of graphene. For the graphene-Ag nanowire hybrids, the time scale of the plasmon-induced hot electron tra…
The fast decay of carrier inversion in photoexcited graphene has been attributed to optical phonon emission and Auger recombination. Plasmon emission provides another pathway that, as we show here, drives the carrier relaxation dynamics on ultrafast timescales. In studying the nonequilibrium relaxation dynamics we find that plasmon emission effectively converts inversion into hot carriers, whose energy is then extracted by optical phonon emission. This mechanism not only explains the observed fs-lifetime of inversion but also offers the prospect for atomically thin ultrafast plasmon emitters.
The ultrafast dynamics of excited carriers in graphene is closely linked to the Dirac spectrum and plays a central role for many electronic and optoelectronic applications. Harvesting energy from excited electron-hole pairs, for instance, is only possible if these pairs can be separated before they lose energy to vibrations, merely heating the lattice. While the hot carrier dynamics in graphene could so far only be accessed indirectly, we here present a direct time-resolved view on the Dirac cone by angle-resolved photoemission (ARPES). This allows us to show the quasi-instant thermalisation o…
