Semiconductor spin noise spectroscopy (SNS) has emerged as a unique experimental tool that utilizes spin fluctuations to provide profound insight into undisturbed spin dynamics in doped semiconductors and semiconductor nanostructures. The technique maps ever present stochastic spin polarization of free and localized carriers at thermal equilibrium via the Faraday effect onto the light polarization of an off-resonant probe laser and was transferred from atom optics to semiconductor physics in 2005. The inimitable advantage of spin noise spectroscopy to all other probes of semiconductor spin dynamics lies in the fact that in principle no energy has to be dissipated in the sample, i.e., SNS exclusively yields the intrinsic, undisturbed spin dynamics and promises optical non-demolition spin measurements for prospective solid state based optical spin quantum information devices. SNS is especially suitable for small electron ensembles as the relative noise increases with decreasing number of electrons. In this review, we first introduce the basic principles of SNS and the difference in spin noise of donor bound and of delocalized conduction band electrons. We continue the introduction by discussing the spectral shape of spin noise and prospects of spin noise as a quantum interface between light and matter. In the main part, we give a short overview about spin relaxation in semiconductors and summarize corresponding experiments employing SNS. Finally, we give in-depth insight into the experimental aspects and discuss possible applications of SNS.
The intrinsic spin Hall effect in semiconductors has developed to a remarkably lively and rapidly growing branch of research in the field of semiconductor spintronics. In this article we give a pedagogical overview on both theoretical and experimental accomplishments and challenges. Emphasis is put on the the description of the intrinsic mechanisms of spin Hall transport in III-V zinc-blende semiconductors, and on the effects of dissipation.
We describe recent experimental efforts to perform polarization-resolved optical spectroscopy of monolayer transition-metal dichalcogenide semiconductors in very large pulsed magnetic fields to 65 tesla. The experimental setup and technical challenges are discussed in detail, and temperature-dependent magneto-reflection spectra from atomically thin tungsten disulphide (WS$_2$) are presented. The data clearly reveal not only the valley Zeeman effect in these 2D semiconductors, but also the small quadratic exciton diamagnetic shift from which the very small exciton size can be directly inferred.…
Two-dimensional correlation spectroscopy (2DCS) based on the nonlinear optical response of excitons to sequences of ultrafast pulses, has the potential to provide some unique insights into carrier dynamics in semiconductors. The most prominent feature of 2DCS, cross peaks, can best be understood using a sum-over-states picture involving the many-body eigenstates. However, the optical response of semiconductors is usually calculated by solving truncated equations of motion for dynamical variables, which result in a quasiparticle picture. In this work we derive Green's function expressions for t…
We report the implementation of energy dispersive X-ray spectroscopy for layered semiconductors in the form of atomically thin transition metal dichalcogenides. The technique is based on a scanning electron microscope equipped with a silicon drift detector for energy dispersive X-ray analysis. By optimizing operational parameters in numerical simulations and experiments, we achieve layer-resolving sensitivity for few-layer crystals down to the monolayer limit and demonstrate elemental composition profiling in vertical and lateral heterobilayers of transition metal dichalcogenides. The techniqu…
The effects of electron-electron interaction of a two-electron nanoring on the energy levels and far-infrared (FIR) spectroscopy have been investigated based on a model calculation which is performed within the exactly numerical diagonalization. It is found that the interaction changes the energy spectra dramatically, and also shows significant influence on the FIR spectroscopy. The crossings between the lowest spin-singlet and triplet states induced by the coulomb interaction are clearly revealed. Our results are related to the experiment recently carried out by A. Lorke et al. [Phys. Rev. Le…
We investigated low-frequency current fluctuations, i.e. noise, in the quasi-two-dimensional (2D) van der Waals antiferromagnetic semiconductor FePS3 with the electronic bandgap of 1.5 eV. The electrical and noise characteristics of the p-type, highly resistive, thin films of FePS3 were measured at different temperatures. The noise spectral density was of the 1/f - type over most of the examined temperature range but revealed well-defined Lorentzian bulges, and increased strongly near the Neel temperature of 118 K (f is the frequency). Intriguingly, the noise spectral density attained its mini…
Reliable and precise measurements of the relative energy of band edges in semiconductors are needed to determine band gaps and band offsets, as well as to establish the band diagram of devices and heterostructures. These measurements are particularly important in the field of two-dimensional materials, in which many new semiconducting systems are becoming available through exfoliation of bulk crystals. For two-dimensional semiconductors, however, commonly employed techniques suffer from difficulties rooted either in the physics of these systems, or of technical nature. The very large exciton b…
Photocurrent spectroscopy is a versatile technique to identify and understand the optoelectronic dynamics occurring in semiconductor nanowires. Conventional photocurrent spectroscopy allows to explore the morphology and material properties of nanowires as well as their contact interfaces. Using time-resolved photocurrent spectroscopy one gets additional information on the multiple photocurrent generation mechanisms and their respective timescales. This chapter discusses various aspects of the photocurrent spectroscopy and it summarizes the physical mechanisms behind the photocurrent and photoc…
Optical excitations of BiTeI with large Rashba spin splitting have been studied in an external magnetic field ($B$) applied parallel to the polar axis. A sequence of transitions between the Landau levels (LLs), whose energies are in proportion to $\sqrt{B}$ were observed, being characteristic of massless Dirac electrons. The large separation energy between the LLs makes it possible to detect the strongest cyclotron resonance even at room temperature in moderate fields. Unlike in 2D Dirac systems, the magnetic field induced rearrangement of the conductivity spectrum is directly observed.
Utilizing three-terminal tunnel emission of ballistic electrons and holes, we have developed a method to self-consistently measure the bandgap of semiconductors and band discontinuities at semiconductor heterojunctions without any prerequisite material parameter. Measurements are performed on lattice-matched GaAs/AlxGa1-xAs and GaAs/(AlxGa1-x)0.51In0.49P single-barrier heterostructures. The bandgaps of AlGaAs and AlGaInP are measured with a resolution of several meV at 4.2 K. For the GaAs/AlGaAs interface, the measured Gamma band offset ratio is 60.4:39.6 (+/-2%). For the GaAs/AlGaInP interfac…
We demonstrate how dynamic correlations of heavy-hole and light-hole excitons in semiconductor quantum wells may be investigated by two dimensional correlation spectroscopy (2DCS). The coherent response to three femtosecond optical pulses is predicted to yield cross (off-diagonal) peaks that contain direct signatures of many-body two-exciton correlations. Signals generated at various phase-matching directions are compared.
A three-terminal spectroscopy that probes both subsurface energy barriers and interband optical transitions in a semiconductor heterostructure is demonstrated. A metal-base transistor with a unipolar p-type semiconductor collector embedding InAs/GaAs quantum dots (QDs) is studied. Using minority/majority carrier injection, ballistic electron emission spectroscopy and its related hot-carrier scattering spectroscopy measures barrier heights of a buried AlxGa1-xAs layer in conduction band and valence band respectively, the band gap of Al0.4Ga0.6As is therefore determined as 2.037 +/- 0.009 eV at …
Transport studies of Andreev bound states (ABSs) are complicated by the interplay of charging effects and superconductivity. Here, we compare transport approaches to ABS spectroscopy in a semiconductor-superconductor island to a charge-sensing approach based on an integrated radio-frequency single-electron transistor. Consistency of the methods demonstrates that fast, non-invasive charge sensing allows accurate quantitative measurement of ABSs while eluding some complexities of transport.
We report shot noise spectroscopy on a semiconductor quantum dot in a cotunneling regime. The DC conductance measurements show clear signatures of both elastic and inelastic cotunneling transport inside a Coulomb diamond. We observed Poissonian shot noise with the Fano factor $F\approx 1$ in the elastic cotunneling regime, and super-Poissonian Fano factor $1<F<3$ in the inelastic cotunneling regime. The differences in the value of the Fano factor between elastic and inelastic processes reveal the microscopic mechanisms involved in the cotunneling transport.
Semiconductors in the proximity of superconductors have been proposed to support phases hosting Majorana bound states. When the systems undergo a topological phase transition towards the Majorana phase, the spectral gap closes, then reopens, and the quasiparticle band spin polarization is inverted. We focus on two paradigmatic semiconductor-superconductor heterostructures and propose an all-electrical spectroscopic probe sensitive to the spin inversion at the topological transition. Our proposal relies on the indirect coupling of a time-dependent electric field to the electronic spin due to th…
We propose a three-pulse coherent ultrafast optical technique that is particularly sensitive to two-exciton correlations. Two Liouville-space pathways for the density matrix contribute to this signal which reveals double quantum coherences when displayed as a two-dimensional correlation plot. Two-exciton couplings spread the cross peaks along both axes, creating a characteristic highly resolved pattern. This level of detail is not available from conventional one-dimensional four-wave mixing or other two-dimensional correlation spectroscopy signals such as the photo echo, in which two-exciton c…
A particular difficulty in studying many-body interactions in a solid is the absence of an experimental technique that can directly probe their key characteristics. We show that 2D Fourier spectroscopy provides an efficient tool for the measurement of critical parameters describing the effect of many-body interactions on the optical response of semiconductors. We develop the basic microscopic theory of 2D Fourier spectroscopy of semiconductors in the framework of the three-band model (heavy holes, light holes, and electrons). The theory includes many-body correlations nonperturbatively and can…
Organic light emitting devices and solar cells are machines that create, manipulate and destroy excited states in organic semiconductors. It is crucial to characterize these excited states, or excitons, to optimize device performance in applications like displays and solar energy harvesting. This is complicated if the excited state is a triplet because the electronic transition is dark with a vanishing oscillator strength. As a consequence, triplet state spectroscopy must usually be performed at cryogenic temperatures to reduce competition from non-radiative rates. Here, we control non-radiati…
We consider terahertz absorption and gain in a single miniband of semiconductor superlattice subject to a bichromatic electric field in the most general case of commensurate frequencies of the probe and pump fields. Using an exact solution of Boltzmann transport equation, we show that in the small-signal limit the formulas for absorption always contain two distinct terms related to the parametric and incoherent interactions of miniband electrons with the alternating pump field. It provides a theoretical background for a control of THz gain without switching to the negative differential conduct…
We report on the design of loop-gap resonators (LGR) operating in the frequency range 34-36 GHz with the goal to achieve single electron spin resonance (ESR) in quantum dot nanostructures. We present a comprehensive study of the magnetic field strength and the spatial distribution of the electric and magnetic fields in the resonator by means of experiments and numerical simulations.
Making use of self-assembly techniques, we demonstrate the realization of nanoscopic semiconductor quantum rings in which the electronic states are in the true quantum limit. We employ two complementary spectroscopic techniques to investigate both the ground states and the excitations of these rings. Applying a magnetic field perpendicular to the plane of the rings, we find that when approximately one flux quantum threads the interior of each ring, a change in the ground state from angular momentum $\ell = 0$ to $\ell = -1$ takes place. This ground state transition is revealed both by a drasti…
The optical response of semiconducting monolayer transition-metal dichalcogenides (TMDCs) is dominated by strongly bound excitons that are stable even at room temperature. However, substrate-related effects such as screening and disorder in currently available specimens mask many anticipated physical phenomena and limit device applications of TMDCs. Here, we demonstrate that that these undesirable effects are strongly suppressed in suspended devices. Extremely robust (photogain >1,000) and fast (response time <1ms) photoresponse combined with the high quality of our devices allow us to study, …
Using previously developed exciton scattering model accounting for the interband, i.e., exciton-biexciton, Coulomb interactions in semiconductor nanocrystals (NCs), we derive a closed set of equations for 2D double-quantum coherence signal. The signal depends on the Liouville space pathways which include both the interband scattering processes and the inter- and intraband optical transitions. These processes correspond to the formation of different cross-peaks in the 2D spectra. We further report on our numerical calculations of the 2D signal using reduced level scheme parameterized for PbSe N…
We propose a method of two-beam spin noise spectroscopy to test the spin transport at equilibrium via analysis of correlations between time-shifted spin fluctuations at different space locations. This method allows one to determine the strength of spin-orbit interaction and spin relaxation time and separate spin noise of conducting electrons from the background noise of localized electrons. We formulate a theory of two-beam spin noise spectroscopy in semiconductor wires with Bychkov-Rashba spin-orbit interaction taking into account several possible spin relaxation channels and finite size of l…
We perform a magneto-infrared spectroscopy study of the semiconductor to semimetal transition of InAs/GaSb double quantum wells from the normal to the inverted state. We show that owing to the low carrier density of our samples (approaching the intrinsic limit), the magneto-absorption spectra evolve from a single cyclotron resonance peak in the normal state to multiple absorption peaks in the inverted state with distinct magnetic field dependence. Using an eight-band Pidgeon-Brown model, we explain all the major absorption peaks observed in our experiment. We demonstrate that the semiconductor…
The electronic properties of ultrathin crystals of molybdenum disulfide consisting of N = 1, 2, ... 6 S-Mo-S monolayers have been investigated by optical spectroscopy. Through characterization by absorption, photoluminescence, and photoconductivity spectroscopy, we trace the effect of quantum confinement on the material's electronic structure. With decreasing thickness, the indirect band gap, which lies below the direct gap in the bulk material, shifts upwards in energy by more than 0.6 eV. This leads to a crossover to a direct-gap material in the limit of the single monolayer. Unlike the bulk…
In semiconductor physics, many essential optoelectronic material parameters can be experimentally revealed via optical spectroscopy in sufficiently large magnetic fields. For monolayer transition-metal dichalcogenide semiconductors, this field scale is substantial --tens of teslas or more-- due to heavy carrier masses and huge exciton binding energies. Here we report absorption spectroscopy of monolayer MoS$_2$, MoSe$_2$, MoTe$_2$, and WS$_2$ in very high magnetic fields to 91~T. We follow the diamagnetic shifts and valley Zeeman splittings of not only the exciton's $1s$ ground state but also …
Semiconductor devices continue to press into the nanoscale regime, and new applications have emerged for which the quantum properties of dopant atoms act as the functional part of the device, underscoring the necessity to probe the quantum structure of small numbers of dopant atoms in semiconductors[1-3]. Although dopant properties are well-understood with respect to bulk semiconductors, new questions arise in nanosystems. For example, the quantum energy levels of dopants will be affected by the proximity of nanometer-scale electrodes. Moreover, because shallow donors and acceptors are analogo…
We probe local charge fluctuations in a semiconductor via laser spectroscopy on a nearby self-assembled quantum dot. We demonstrate that the quantum dot is sensitive to changes in the local environment at the single charge level. By controlling the charge state of localized defects, we are able to infer the distance of the defects from the quantum dot with +-5 nm resolution. The results identify and quantify the main source of charge noise in the commonly-used optical field-effect devices. Based on this understanding we achieve routinely close-totransform-limited quantum dot optical linewidths…
We address the low-energy effective Hamiltonian of electron doped d0 perovskite semiconductors in cubic and tetragonal phases using the k*p method. The Hamiltonian depends on the spin-orbit interaction strength, on the temperature-dependent tetragonal distortion, and on a set of effective-mass parameters whose number is determined by the symmetry of the crystal. We explain how these parameters can be extracted from angle resolved photo-emission, Raman spectroscopy, and magneto-transport measurements and estimate their values in SrTiO3.
Multi-electron semiconductor quantum dots have found wide application in qubits, where they enable readout and enhance polarizability. However, coherent control in such dots has typically been restricted to only the lowest two levels, and such control in the strongly interacting regime has not been realized. Here we report quantum control of eight different resonances in a silicon-based quantum dot. We use qubit readout to perform spectroscopy, revealing a dense set of energy levels with characteristic spacing far smaller than the single-particle energy. By comparing with full configuration in…
The superconducting proximity effect in semiconductor nanowires has recently enabled the study of new superconducting architectures, such as gate-tunable superconducting qubits and multiterminal Josephson junctions. As opposed to their metallic counterparts, the electron density in semiconductor nanosystems is tunable by external electrostatic gates providing a highly scalable and in-situ variation of the device properties. In addition, semiconductors with large $g$-factor and spin-orbit coupling have been shown to give rise to exotic phenomena in superconductivity, such as $φ_0$ Josephson jun…
Motivated by recent transport experiments and proposed atomic-scale semiconductor devices, we present measurements that extend the reach of scanned-probe methods to discern the properties of individual dopants tens of nanometers below the surface of a silicon sample. Using a capacitance-based approach, we have both spatially-resolved individual subsurface boron acceptors and detected spectroscopically single holes entering and leaving these minute systems of atoms. A resonance identified as the B+ state is shown to shift in energy from acceptor to acceptor. We examine this behavior with respec…
Spin noise (SN) spectroscopy measurements on delicate semiconductor spin systems, like single InGaAs quantum dots, are currently not limited by optical shot noise but rather by the electronic noise of the detection system. Here, we report a realization of homodyne SN spectroscopy enabling shot noise limited SN measurements. The proof-of-principle measurements on impurities in an isotopically enriched rubidium atom vapor show that homodyne SN spectroscopy can be utilized even in the low frequency spectrum which facilitates advanced semiconductor spin research like higher order SN measurements o…
Beginning with the 'conventional' two-dimensional (2D) quantum wells (QWs) based on III-V and II-VI semiconductors in the 1970s, to the recent atomically-thin sheets of van der Waals materials such as 2D semiconducting transition metal dichalcogenides (TMDCs) and 2D magnets, the research in 2D materials is continuously evolving and providing new challenges. Magnetooptical spectroscopy has played a significant role in this area of research, both from fundamental physics and technological perspectives. A major challenge in 2D semiconductors such as TMDCs is to understand their spin-valley-resolv…
Optical spectroscopy and quantum control of semiconductor quantum dots has become a vivid field of research. The recent progress in both theory and experiment is reviewed, with emphasis on theoretical and computational concepts.
The magneto-phonon resonance or MPR occurs in semiconductor materials when the energy spacing between Landau levels is continuously tuned to cross the energy of an optical phonon mode. MPRs have been largely explored in bulk semiconductors, in two-dimensional systems and in quantum dots. Recently there has been significant interest in the MPR interactions of the Dirac fermion magnetoexcitons in graphene, and a rich splitting and anti-crossing phenomena of the even parity E2g long wavelength optical phonon mode have been theoretically proposed and experimentally observed. The MPR has been found…
Semiconductor microcavities can exhibit various macroscopic quantum phenomena, including Bose-Einstein condensation of polaritons, Bardeen-Cooper-Schrieffer (BCS) states of polaritons, and photon lasing (lasing with negligible Coulombic exciton effects). An important aspect of possible experimental identification of these states is a gap in the excitation spectrum (the BCS gap in the case of a polaritonic BCS state). Similar to the polaritonic BCS gap, a light-induced gap can exist in photon lasers. Although polaritonic BCS states have been observed on the basis of spectroscopy in the vicinity…
Rephasing and non-rephasing two-dimensional coherent spectra map the anti-crossing associated with normal-mode splitting in a semiconductor microcavity. For a 12-meV detuning range near zero detuning, it is observed that there are two diagonal features related to the intra-action of exciton-polariton branches and two off-diagonal features related to coherent interaction between the polaritons. At negative detuning, the lineshape properties of the diagonal intra-action features are distinguishable and can be associated with cavity-like and exciton-like modes. A biexcitonic companion feature is …
Controlling doping is essential for a successful integration of semiconductor materials into device technologies. However, the assessment of doping levels and the distribution of charge carriers in carbon nanotubes or other nanoscale semiconductor materials is often either limited to a qualitative attribution of being 'high' or 'low' or it is entirely absent. Here, we describe efforts toward a quantitative characterization of doping in redox- or electrochemically doped semiconducting carbon nanotubes (s-SWNTs) using VIS-NIR absorption spectroscopy. We discuss how carrier densities up to about …
Combining monolayers of different two-dimensional (2D) semiconductors into heterostructures opens up a wealth of possibilities for novel electronic and optical functionalities. Exploiting them hinges on accurate measurements of the band parameters and orbital hybridization in separate and stacked monolayers, many of which are only available as small samples. The recently introduced technique of angle-resolved photoemission spectroscopy with submicron spatial resolution (μ-ARPES) offers the capability to measure small samples, but the energy resolution obtained for such exfoliated samples to da…
We investigate equilibrium and non-equilibrium charge-transfer processes by performing high-resolution transport spectroscopy. Using electrostatically defined quantum dots for energy-selective emission and detection, we achieved unprecedented spectral resolution and a high degree of tunability of relevant experimental parameters. Most importantly, we observe that the spectral width of elastically transferred electrons can be substantially smaller than the linewidth of a thermally broadened Coulomb peak. This finding indicates that the charge-transfer process is fast compared to the electron--p…
The Cooper-pair transistor (CPT), a small superconducting island enclosed between two Josephson weak links, is the atomic building block of various superconducting quantum circuits. Utilizing gate-tunable semiconductor channels as weak links, the energy scale associated with the Josephson tunneling can be changed with respect to the charging energy of the island, tuning the extent of its charge fluctuations. Here, we directly demonstrate this control by mapping the energy level structure of a CPT made of an indium arsenide nanowire (NW) with a superconducting aluminum shell. We extract the dev…
Understanding the movement of charge within organic semiconducting films is crucial for applications in photo-voltaics and flexible electronics. We study the sensitivity of the electrical conductance of a silicon nanowire to changes of charge states within an organic semiconductor physisorbed on the surface of the nanowire. Elastic scattering caused by motion of charge carriers near the nanowire modifies the mean-free path for backscattering of electrons propagating within it, which we have mathematically expressed in terms of the causal Green's functions. The scattering potential has been com…
Spectroscopy With Intelligent Feature Tracking for automated characterization of excited-state structure in semiconductor quantum dot devices
University of Wisconsin-Madison（威斯康星大学麦迪逊分校）；University of Maryland（马里兰大学）；Joint Center for Quantum Information and Computer Science（量子信息与计算科学联合中心）；National Institute of Standards and Technology（美国国家标准与技术研究院）；Massachusetts Institute of Technology（麻省理工学院）；QuTech and Kavli Institute of Nanoscience, Delft University of Technology（代尔夫特理工大学奎泰克与卡弗里纳米科学研究所）
QuTech and Kavli Institute of Nanoscience, Delft University of Technology（代尔夫特理工大学量子技术与卡弗里纳米科学研究所）；Netherlands Organisation for Applied Scientific Research (TNO)（荷兰应用科学研究组织）
The electronic band structure of complex nanostructured semiconductors has a considerable effect on the final electronic and optical properties of the material and, ultimately, on the functionality of the devices incorporating them. Valence electron energy-loss spectroscopy (VEELS) in the transmission electron microscope (TEM) provides the possibility of measuring this property of semiconductors with high spatial resolution. However, it still represents a challenge for narrow-bandgap semiconductors, since an electron beam with low energy spread is required. Here we demonstrate that by means of…
Frequency-resolved decoherence spectroscopy of a semiconductor charge qubit coupled to a high-impedance resonator
ETH Zurich（苏黎世联邦理工学院）；École Polytechnique Fédérale de Lausanne (EPFL)（洛桑联邦理工学院）；Microsoft Quantum Lab Delft（微软量子实验室代尔夫特）；Lund University（隆德大学）；Delft University of Technology（代尔夫特理工大学）；Leiden University（莱顿大学）；Norwegian University of Science and Technology（挪威科技大学）
We report magneto-transport measurements of quasi-1-dimensional (1D) Al-InAs nanowires produced via etching of a hybrid superconductor-semiconductor two-dimensional electron gas (2DEG). Tunnel spectroscopy measurements above the superconducting gap provide a means of identifying the 1D sub-bands associated with the confined 1D region. Fitting the data to a model that includes the different components of the spin-orbit interaction (SOI) reveals their strength, of interest for evaluating the suitability of superconductor-semiconductor 2DEG for realizing Majorana qubits.
