High resolution two-dimensional optical spectroscopy of electron spins

Abstract

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.

11 pages, 6 figures

References in corpus (7)

• Coherent Population Trapping of an Electron Spin in a Single Negatively Charged Quantum Dot
• Pump-Probe Faraday Rotation and Ellipticity in an Ensemble of Singly Charged Quantum Dots
• Spin coherence of a two-dimensional electron gas induced by resonant excitation of trions and excitons in CdTe/(Cd,Mg)Te quantum wells
• Environment-assisted quantum control of a solid-state spin via coherent dark states
• Multi-Wave Coherent Control of a Solid State Single Emitter
• Electromagnetically Induced Transparency with an Ensemble of Donor-Bound Electron Spins in a Semiconductor
• Transient photon echoes from donor-bound excitons in ZnO epitaxial layers

Cited by in corpus (8)

• Damping of Rabi oscillations in intensity-dependent photon echoes from exciton complexes in a CdTe/(Cd,Mg)Te single quantum well
• Microscopic dynamics of electron hopping in a semiconductor quantum well probed by spin-dependent photon echoes
• Controlled Coherent Coupling in a Quantum Dot Molecule Revealed by Ultrafast Four-Wave Mixing Spectroscopy
• The in-plane anisotropy of the hole $g$ factor in CdTe/(Cd,Mg)Te quantum wells studied by spin-dependent photon echoes
• Dark-state and loss-induced phenomena in the quantum-optical regime of $\Lambda$-type three-level systems
• Quantum beats in the polarization of the spin-dependent photon echo from donor-bound excitons in CdTe/(Cd,Mg)Te quantum wells
• Long-living dark coherence brought to light by magnetic-field controlled photon echo
• Polarimetry of photon echo on charged and neutral excitons in CdTe/(Cd,Mg)Te quantum wells