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Register a new userHigh resolution two-dimensional optical spectroscopy of electron spins
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Multidimensional coherent optical spectroscopy is one of the most powerful tools for investigating complex quantum mechanical systems. While it was conceived decades ago in magnetic resonance spectroscopy using micro- and radio-waves, it has recently been extended into the visible and UV spectral range. However, resolving MHz energy splittings with ultrashort laser pulses has still remained a challenge. Here, we analyze two-dimensional Fourier spectra for resonant optical excitation of resident electrons to localized trions or donor-bound excitons in semiconductor nanostructures subject to a transverse magnetic field. Particular attention is devoted to Raman coherence spectra which allow one to accurately evaluate tiny splittings of the electron ground state and to determine the relaxation times in the electron spin ensemble. A stimulated step-like Raman process induced by a sequence of two laser pulses creates a coherent superposition of the ground state doublet which can be retrieved only optically due to selective excitation of the same sub-ensemble with a third pulse. This provides the unique opportunity to distinguish between different complexes that are closely spaced in energy in an ensemble. The related experimental demonstration is based on photon echo measurements in an n-type CdTe/(Cd,Mg)Te quantum well structure detected by a heterodyne technique. The difference in the sub-$mu$eV range between the Zeeman splittings of donor-bound electrons and electrons localized at potential fluctuations can be resolved even though the homogeneous linewidth of the optical transitions is larger by two orders of magnitude.
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Spectroscopic methods involving the sudden injection or ejection of electrons in materials are a powerful probe of electronic structure and interactions. These techniques, such as photoemission and tunneling, yield measurements of the single particle density of states (SPDOS) spectrum of a system. The SPDOS is proportional to the probability of successfully injecting or ejecting an electron in these experiments. It is equal to the number of electronic states in the system able to accept an injected electron as a function of its energy and is among the most fundamental and directly calculable quantities in theories of highly interacting systems. However, the two-dimensional electron system (2DES), host to remarkable correlated electron states such as the fractional quantum Hall effect, has proven difficult to probe spectroscopically. Here we present an improved version of time domain capacitance spectroscopy (TDCS) that now allows us to measure the SPDOS of a 2DES with unprecedented fidelity and resolution. Using TDCS, we perform measurements of a cold 2DES, providing the first direct measurements of the single-particle exchange-enhanced spin gap and single particle lifetimes in the quantum Hall system, as well as the first observations of exchange splitting of Landau levels not at the Fermi surface. The measurements reveal the difficult to reach and beautiful structure present in this highly correlated system far from the Fermi surface.
Quantum sensors have recently achieved to detect the magnetic moment of few or single nuclear spins and measure their magnetic resonance (NMR) signal. However, the spectral resolution, a key feature of NMR, has been limited by relaxation of the sensor to a few kHz at room temperature. The spectral resolution of NMR signals from single nuclear spins can be improved by, e.g., using quantum memories, however at the expense of sensitivity. Classical signals on the other hand can be measured with exceptional spectral resolution by using continuous measurement techniques, without compromising sensitivity. To apply these techniques to single-spin NMR, it is critical to overcome the impact of back action inherent of quantum measurements. Here we report sequential weak measurements on a single $^{13}$C nuclear spin. The back-action of repetitive weak measurements causes the spin to undergo a quantum dynamics phase transition from coherent trapping to coherent oscillation. Single-spin NMR at room-temperature with a spectral resolution of 3.8 Hz is achieved. These results enable the use of measurement-correlation schemes for the detection of very weakly coupled single spins.
We report on precise localization spectroscopy experiments of individual 13C nuclear spins near a central electronic sensor spin in a diamond chip. By detecting the nuclear free precession signals in rapidly switchable external magnetic fields, we retrieve the three-dimensional spatial coordinates of the nuclear spins with sub-Angstrom resolution and for distances beyond 10 Angstroms. We further show that the Fermi contact contribution can be constrained by measuring the nuclear g-factor enhancement. The presented method will be useful for mapping the atomic-scale structure of single molecules, an ambitious yet important goal of nanoscale nuclear magnetic resonance spectroscopy.
In this paper we use electrically detected optical excitation spectroscopy of individual erbium ions in silicon to determine their optical and paramagnetic properties simultaneously. We demonstrate that this high spectral resolution technique can be exploited to observe interactions typically unresolvable in silicon using conventional spectroscopy techniques due to inhomogeneous broadening. In particular, we resolve the Zeeman splitting of the 4I15/2 ground and 4I13/2 excited state separately and in strong magnetic fields we observe the anti-crossings between Zeeman components of different crystal field levels. We discuss the use of this electronic detection technique in identifying the symmetry and structure of erbium sites in silicon.
Strain in two-dimensional (2D) transition metal dichalcogenide (TMD) has led to localized states with exciting optical properties, in particular in view of designing one photon sources. The naturally formed of the MoS2 monolayer deposed on hBN substrate leads to a reduction of the bandgap in the strained region creating a nanobubble. The photogenerated particles are thus confined in the strain-induced potential. Using numerical diagonalization, we simulate the spectra of the confined exciton states, their oscillator strengths and radiative lifetimes. We show that a single state of the confined exciton is optically active, which suggests that the MoS2/hBN nanobubble is a good candidate for the realisation of single-photon sources. Furthermore, the exciton binding energy, oscillator strength and radiative lifetime are enhanced due to the confinement effect.
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