Quantum spin fluctuations provide a unique way to study spin dynamics without system perturbation. Here we put forward an optical resonance shift spin noise spectroscopy as a powerful tool to measure the spin noise of various systems from magnetic impurities in solids to free atoms and molecules. The quantum spin fluctuations in these systems can shift the optical resonances by more than the homogeneous linewidth and produce huge Faraday rotation noise. We demonstrate, that the resonance shift spin noise spectroscopy gives access to the high order spin correlators, which contain complete information about the spin dynamics in contrast with the second order correlator measured by conventional Pauli-blocking spin noise spectroscopy. The high order quantum spin correlators manifest themselves as a comb of peaks in the Faraday rotation noise spectra in transverse magnetic field. This effect is closely related with the multispin flip Raman scattering observed in the Mn-doped nanostructures.
We present a new method for high-resolution nanoscale magnetic resonance imaging (nano-MRI) that combines the high spin sensitivity of nanowire-based magnetic resonance detection with high spectral resolution nuclear magnetic resonance (NMR) spectroscopy. By applying NMR pulses designed using optimal control theory, we demonstrate a factor of $500$ reduction of the proton spin resonance linewidth in a $(50\text{-nm})^{\text{3}}$ volume of polystyrene and image proton spins in one dimension with a spatial resolution below $2~\text{nm}$.
X-band electron spin resonance (ESR) spectroscopy has been performed for gold nanorods (AuNRs) of four different sizes covered with a diamagnetic stabilizing component, cetyltrimethylammmonium bromide. The ESR spectra show ferromagnetic features such as hysteresis and resonance field shift, depending on the size of the AuNRs. In addition, the ferromagnetic transition is indicated by an abrupt change in the spectra of the two smallest AuNRs studied. A large g-value in the paramagnetic region suggests that the ferromagnetism in the AuNRs originates from strong spin-orbit interaction.
We have measured the electronic energy spectra of nm-scale Au particles using a new tunneling spectroscopy configuration. The particle diameters ranged from 5nm to 9nm, and at low energies the spectrum is discrete, as expected by the electron-in-a-box model. The density of tunneling resonances increases rapidly with energy, and at higher energies the resonances overlap forming broad resonances. Near the Thouless energy, the broad resonances merge into a continuum. The tunneling resonances display Zeeman splitting in a magnetic field. Surprisingly, the g-factors (~0.3) of energy levels in Au na…
We perform polarization-resolved Raman spectroscopy on graphene in magnetic fields up to 45T. This reveals a filling-factor-dependent, multi-component anticrossing structure of the Raman G peak, resulting from magnetophonon resonances between magnetoexcitons and E$_{2g}$ phonons. This is explained with a model of Raman scattering taking into account the effects of spatially inhomogeneous carrier densities and strain. Random fluctuations of strain-induced pseudo-magnetic fields lead to increased scattering intensity inside the anti-crossing gap, consistent with the experiment.
Spin noise spectroscopy is a method of magnetic resonance widely used, nowadays, in atomic and semiconductor research. Classical objects of the EPR spectroscopy - dielectrics with paramagnetic impurities - seemed to be unsuitable for this technique because of large widths of allowed optical transitions and, therefore, low specific Faraday rotation (FR). We show, however, that the FR noise detected at the wavelength of a weak optical transition (with low regular FR) may increase by many orders of magnitude as its homogeneous width decreases. This spin-noise gain effect, numerically described by…
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…
Resonant optical excitation of few-level quantum systems enables coherent quantum control, resonance fluorescence, and direct characterization of dephasing mechanisms. Experimental demonstrations have been achieved in a variety of atomic and solid-state systems. An alternative but intriguing quantum photonic platform is based on single layer transition metal chalcogenide semiconductors, which exhibit a direct band-gap with optically addressable exciton valley-pseudospins in a uniquely two-dimensional form. Here we perform resonance and near-resonance excitation of three-dimensionally confined …
Molecular vibrational spectroscopy with the scanning tunneling microscope is feasible but usually detects few vibrational modes. We harness sharp Yu-Shiba-Rusinov (YSR) states observed from molecules on a superconductor to significantly enhance the vibrational signal. From a lead phthalocyanin molecule 46 vibrational peaks are resolved enabling a comparison with calculated modes. The energy resolution is improved beyond the thermal broadening limit and shifts induced by neighbor molecules or the position of the microscope tip are determined. Vice versa, spectra of vibrational modes are used to…
The optically induced polarization of localized electron spins in an ensemble of quantum dots (QDs) dephases due to the interaction with the surrounding nuclear spins. Despite this dephasing, the spins in the QDs can be controlled to respond coherently by applying periodic laser pulses, leading to a revival of the spin polarization before each pulse. This effect, known as spin mode locking, strongly depends on an emerging selection of certain polarizations of the nuclear spin bath which is driven to a steady state far from equilibrium. We investigate the influence of the nuclear composition in…
In the scanning tunnelling microscope, the many-body Kondo effect leads to a zero-bias feature of the differential conductance spectra of magnetic adsorbates on surfaces. The intrinsic line shape of this Kondo resonance and its temperature dependence in principle contain valuable information. We use measurements on a molecular Kondo system, all-trans retinoic acid on Au(111), and model calculations to discuss the role of instrumental broadening. The modulation voltage used for the lock-in detection, noise on the sample voltage, and the temperature of the microscope tip are considered. These so…
Raman measurements are performed on defect-free wurzite GaP nanowires. Resonance Raman measurements are carried out over the excitation energy range between 2.19 and 2.71 eV. Resonances at 2.38 eV and 2.67 eV of the E1(LO) mode and at 2.67 eV of the A1(LO) are observed. The presence of these intensity resonances clearly demonstrates the existence of energy states with Gamma_9hh and Gamma_7V (Gamma_7C) symmetries of the valence (conduction) band and allows to measure WZ phase GaP band energies at the Gamma point. In addition, we have investigated temperature dependent resonant Raman measurement…
A nitrogen-vacancy (NV) center in diamond is a promising sensor for nanoscale magnetic sensing. Here we report electron spin resonance (ESR) spectroscopy using a single NV center in diamond. First, using a 230 GHz ESR spectrometer, we performed ensemble ESR of a type-Ib sample crystal and identified a substitutional single nitrogen impurity as a major paramagnetic center in the sample crystal. Then, we carried out free-induction decay and spin echo measurements of the single NV center to study static and dynamic properties of nanoscale bath spins surrounding the NV center. We also measured ESR…
We present the new optically-detected magnetic resonance (ODMR) technique which reveals single point defects in silicon quantum wells embedded in microcavities within frameworks of the excitonic normal-mode coupling (NMC) without the external cavity and the hf source.
Origin of shifts in the surface plasmon resonance (SPR) frequency for noble metal (Au, Ag) nanoclusters are discussed in this book chapter. Spill out of electron from the Fermi surface is considered as the origin of red shift. On the other hand, both screening of electrons of the noble metal in porous media and quantum effect of screen surface electron are considered for the observed blue shift in the SPR peak position.
The surface quantum Hall state, magneto-electric phenomena and their connection to axion electrodynamics have been studied intensively for topological insulators. One of the obstacles for observing such effects comes from nonzero conductivity of the bulk. To overcome this obstacle we propose to use an external magnetic field to suppress the conductivity of the bulk carriers. The magnetic field dependence of galvanomagnetic and electromagnetic responses of the whole system shows anomalies due to broken time-reversal symmetry of the surface quantum Hall state, which can be used for its detection…
Nuclear magnetic resonance (NMR) spectroscopy has approached the limit of single molecule sensitivity, however the spectral resolution is currently insufficient to obtain detailed information on chemical structure and molecular interactions. Here we demonstrate more than two orders of magnitude improvement in spectral resolution by performing correlation spectroscopy with shallow nitrogen-vacancy (NV) magnetic sensors in diamond. In principle, the resolution is sufficient to observe chemical shifts in $\sim$1 T magnetic fields, and is currently limited by molecular diffusion at the surface. We…
We report electron spin resonance measurements of donors in silicon at millikelvin temperatures using a superconducting $LC$ planar micro-resonator and a Josephson Parametric Amplifier. The resonator includes a nanowire inductor, defining a femtoliter detection volume. Due to strain in the substrate, the donor resonance lines are heavily broadened. Single-spin to photon coupling strengths up to $\sim 3~\text{kHz}$ are observed. The single shot sensitivity is $120 \pm 24~$spins/Hahn echo, corresponding to $\approx 12 \pm 3$~spins$/\sqrt{\text{Hz}}$ for repeated acquisition.
Nonlinear manipulation of nuclear and electron spins is the basis for all advanced methods in magnetic resonance including multidimensional nuclear magnetic and electron spin resonance spectroscopies, magnetic resonance imaging, and in recent years, quantum control over individual spins. The methodology is facilitated by the ease with which the regime of strong coupling can be reached between radiofrequency or microwave magnetic fields and nuclear or electron spins respectively, typified by sequences of magnetic pulses that control the magnetic moment directions. The capabilities meet a bottle…
We report electron spin resonance spectroscopy measurements performed at millikelvin temperatures in a custom-built spectrometer comprising a superconducting micro-resonator at $7$ GHz and a Josephson parametric amplifier. Owing to the small ${\sim}10^{-12}λ^3$ magnetic resonator mode volume and to the low noise of the parametric amplifier, the spectrometer sensitivity reaches $260\pm40$ spins$/$echo and $65\pm10$ $\mathrm{spins}/\sqrt{\text{Hz}}$, respectively.
Quantum sensing exploits fundamental features of quantum mechanics and quantum control to realise sensing devices with potential applications in a broad range of scientific fields ranging from basic science to applied technology. The ultimate goal are devices that combine unprecedented sensitivity with excellent spatial resolution. Here, we propose a new platform for all-electric nanoscale quantum sensing based on a carbon nanotube double quantum dot. Our analysis demonstrates that the platform can achieve sensitivities that allow for the implementation of single-molecule magnetic resonance sp…
Quantum sensing based on nitrogen-vacancy (NV) centers in diamond has been developed as a powerful tool for microscopic magnetic resonance. However, the reported sensor-to-sample distance is limited within tens of nanometers because the signal of spin fluctuation decreases cubically with the increasing distance. Here we extend the sensing distance to tens of micrometers by detecting spin polarization rather than spin fluctuation. We detected the mesoscopic magnetic resonance spectra of polarized electrons of a pentacene-doped crystal, measured its two typical decay times and observed the optic…
Using p-aminothiophenol (PATP) molecules on a gold substrate as prototypical examples and high vacuum tip-enhanced Raman spectroscopy (HV-TERS), we show that the vibrational spectra of those molecules are distinctly different from those in typical surface-enhanced Raman spectroscopy. Detailed first-principles calculations help to assign the Raman peaks in the TERS measurements as Raman active and infrared (IR) active vibrational modes of dimercaptoazobenzene (DMAB), thus providing strong spectroscopic evidence for the conversion of PATP dimerization to DMAB. The activation of the IR active mod…
Backscattering Raman spectroscopic investigations were performed on an yttrium-iron garnet single crystal using linearly and circularly polarized light. A terahertz (THz) magnon of the Kaplan-Kittel (KK) exchange resonance was discovered, which had been regarded as unobservable via optical methods. The KK exchange resonance had a 7.8-THz frequency at 80 K, and the polarization selection rule led to an antisymmetric Raman tensor of the $A_{2}$ mode. Moreover, the assignment of all the Raman-active phonon modes, $3A_{1g}$, $8E_{g}$, and $14T_{2g}$, was proposed. This study will stimulate further…
We present a simplified yet sophisticated variation to localised surface plasmon resonance spectroscopy, which makes use of naked or non-functionalised, nanoparticle templates. These nanoparticle templates, produced with a rapid and scalable process, namely laser annealing, were used as a highly sensitive surface sensor to monitor the adsorption of both metallic lead and a lead salt from aqueous solutions, showing a measurable optical response due to a surface abundance of lead as low as 100 ppm from 0.3 ml of Pb2SO4 solutions, with concentrations less than 20 ppm. This proposed method enables…
Scanning tunneling spectroscopic studies of Bi2Se3 epitaxial films on Si (111) substrates reveal highly localized unitary impurity resonances associated with non-magnetic quantum impurities. The strength of the resonances depends on the energy difference between the Fermi level ({E_F}) and the Dirac point ({E_D}) and diverges as {E_F} approaches {E_D}. The Dirac-cone surface state of the host recovers within ~ 2Å spatial distance from impurities, suggesting robust topological protection of the surface state of topological insulators against high-density impurities that preserve time reversal s…
The nitrogen-vacancy (NV) center has enabled widespread study of nanoscale nuclear magnetic resonance (NMR) spectroscopy at low magnetic fields. NMR spectroscopy at high magnetic fields significantly improves the technique's spectral resolution, enabling clear identification of closely related chemical species. However, NV-detected NMR is typically performed using AC sensing through electron spin echo envelope modulation (ESEEM), a hyperfine spectroscopic technique that is not feasible at high magnetic fields. Within this paper, we have explored an NV-detected NMR technique for applications of…
We use a laser-driven single (In,Ga)As quantum dot (QD) in the dressed state regime of resonance fluorescence ($T = 4$ K) to observe the four $D_1$-transition lines of alkali atomic cesium ($Cs$) vapor at room temperature. We tune the frequency of the dressing continuous-wave laser in the vicinity of the bare QD resonance $\sim 335.116$ THz ($\sim 894.592$ nm) at constant excitation power and thereby controllably tune the center and side channel frequencies of the probe light, i.e. the Mollow triplet. Resonances between individual QD Mollow triplet lines and the atomic hyperfine-split transiti…
Nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) spectroscopy of bulk quantum materials have provided insight into phenomena such as quantum phase criticality, magnetism, and superconductivity. With the emergence of nanoscale 2-D materials with magnetic phenomena, inductively-detected NMR and NQR spectroscopy are not sensitive enough to detect the smaller number of spins in nanomaterials. The nitrogen-vacancy (NV) center in diamond has shown promise in bringing the analytic power of NMR and NQR spectroscopy to the nanoscale. However, due to depth-dependent formation effi…
We report the magnetic field-dependent far-infrared reflectivity of polycrystalline bismuth. We observe four distinct absorptions that we attribute to magnetoplasmon resonances, which are collective modes of an electron-hole liquid in magnetic field and become optical and acoustic resonances of the electron-hole system in the small-field limit. The acoustic mode is expected only when the masses of distinct components are very different, which is the case in bismuth. In a polycrystal, where the translational symmetry is broken, a big shift of spectral weight to acoustic plasmon is possible. Thi…
We performed magnetic field and frequency tunable electron paramagnetic resonance spectroscopy of an Er$^{3+}$ doped Y$_2$SiO$_5$ crystal by observing the change in flux induced on a direct current-superconducting quantum interference device (dc-SQUID) loop of a tunable Josephson bifurcation amplifer. The observed spectra show multiple transitions which agree well with the simulated energy levels, taking into account the hyperfine and quadrupole interactions of $^{167}$Er. The sensing volume is about 0.15 pl, and our inferred measurement sensitivity (limited by external flux noise) is approxim…
We investigate the rotational properties of molecular hydrogen and its isotopes physisorbed on the surfaces of graphene and hexagonal boron nitride ($h$-BN), grown on Ni(111), Ru(0001), and Rh(111), using rotational excitation spectroscopy (RES) with the scanning tunneling microscope. The rotational thresholds are in good agreement with $ΔJ=2$ transitions of freely spinning para-H$_2$ and ortho-D$_2$ molecules. The line shape variations in RES for H$_2$ among the different surfaces can be traced back and naturally explained by a resonance mediated tunneling mechanism. RES data for H$_2$/$h$-BN…
Significant attention has been recently focused on the realization of high precision nano-thermometry using the spin-resonance temperature shift of the negatively charged nitrogen-vacancy (NV-) center in diamond. However, the precise physical origins of the temperature shift is yet to be understood. Here, the shifts of the center's optical and spin resonances are observed and a model is developed that identifies the origin of each shift to be a combination of thermal expansion and electron-phonon interactions. Our results provide new insight into the center's vibronic properties and reveal imp…
We report on the structural and optical properties of individual bowtie nanoantennas both on glass and semiconducting GaAs substrates. The antennas on glass (GaAs) are shown to be of excellent quality and high uniformity reflected by narrow size distributions with standard deviations for the triangle and gap size of $σ_s^{glass}=4.5nm$ ($σ_s^{GaAs}=2.6nm$) and $σ_g^{glass}=5.4nm$ ($σ_g^{GaAs}=3.8nm$), respectively. The corresponding optical properties of individual nanoantennas studied by differential reflection spectroscopy show a strong reduction of the localised surface plasmon polariton re…
We present combined experimental and numerical work on light-matter interactions at nanometer length scales. We report novel numerical simulations of near-field infrared nanospectroscopy that consider, for the first time, detailed tip geometry and have no free parameters. Our results match published spectral shapes of amplitude and phase measurements even for strongly resonant surface phonon-polariton (SPhP) modes. They also verify published absolute scattering amplitudes for the first time. A novel, ultrabroadband light source enables near-field amplitude and phase acquisition into the far-in…
A periodically driven quantum system with avoided-level crossing experiences both non-adiabatic transitions and wave-function phase changes. These result in coherent interference fringes in the system's occupation probabilities. For qubits, with repelling energy levels, such interference, named after Landau-Zener-Stuckelberg-Majorana, displays arc-shaped resonance lines. We demonstrate that in the case of a multi-level system with an avoided-level crossing of the two lower levels, the shape of the resonances can change from convex arcs to concave heart-shaped and harp-shaped resonance lines. I…
High resolution coherent nonlinear optical spectroscopy of an ensemble of red-emitting InGaN quantum dots in GaN nanowires is reported. The data show a pronounced atom-like interaction between resonant laser fields and quantum dot excitons at low temperature that is difficult to observe in the linear absorption spectrum due to inhomogeneous broadening from indium fluctuation effects. We find that the nonlinear signal persists strongly at room temperature. The robust atom-like room temperature response indicates the possibility that this material could serve as the platform for proposed exciton…
Quantum sensors based on nitrogen-vacancy centers in diamond have emerged as a promising detection modality for nuclear magnetic resonance (NMR) spectroscopy owing to their micron-scale detection volume and non-inductive based detection. A remaining challenge is to realize sufficiently high spectral resolution and concentration sensitivity for multidimensional NMR analysis of picoliter sample volumes. Here, we address this challenge by spatially separating the polarization and detection phases of the experiment in a microfluidic platform. We realize a spectral resolution of 0.65 +/- 0.05 Hz, a…
We consider an open (scattering) quantum system under the action of a perturbation of its closed counterpart. It is demonstrated that the resulting shift of resonance widths is a sensitive indicator of the non-orthogonality of resonance wavefunctions, being zero only if those were orthogonal. Focusing further on chaotic systems, we employ random matrix theory to introduce a new type of parametric statistics in open systems, and derive the distribution of the resonance width shifts in the regime of weak coupling to the continuum.
