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Physical review. B./Physical review. B

Weak probe readout of coherent impurity orbital superpositions in silicon

K. L. Litvinenko, P. Thornton Greenland, Britta Redlich, C. R. Pidgeon, G. Aeppli, Benedict N Murdin

Published Dec 20, 2016• 2 citations
Publisher

Abstract

Pump-probe spectroscopy is the most common time-resolved technique for investigation of electronic dynamics, and the results provide the incoherent population decay time ${T}_{1}$. Here we use a modified pump-probe experiment to investigate coherent dynamics, and we demonstrate this with a measurement of the inhomogeneous dephasing time ${T}_{2}^{*}$ for phosphorus impurities in silicon. The pulse sequence produces the same information as previous coherent all-optical (photon-echo-based) techniques but is simpler. The probe signal strength is first order in the pulse area but its effect on the target state is only second order, meaning that it does not demolish the quantum information. We propose simple extensions to the technique to measure the homogeneous dephasing time ${T}_{2}$, or to perform tomography of the target qubit.

DOI
10.1103/physrevb.94.235207

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Pump-probe spectroscopy is the most common time-resolved technique for investigation of electronic dynamics, and the results provide the incoherent population decay time T1{T}_{1}T1​. Here we use a modified pump-probe experiment to investigate coherent dynamics, and we demonstrate this with a measurement of the inhomogeneous dephasing time T2∗{T}_{2}^{*}T2∗​ for phosphorus impurities in silicon. The pulse sequence produces the same information as previous coherent all-optical (photon-echo-based) techniques but is simpler. The probe signal strength is first order in the pulse area but its effect on the target state is only second order, meaning that it does not demolish the quantum information. We propose simple extensions to the technique to measure the homogeneous dephasing time T2{T}_{2}T2​, or to perform tomography of the target qubit.
The coherence spike observed in the transmitted probe intensity decay curve in pump–probe experiments is analyzed with a model which depends explicitly upon the population decay and dephasing rate constants. Using this model and simple pulse shape functions a series of decay curves are calculated throughout the range of wide to narrow pulse widths relative to the dephasing time. These calculations suggest that the coherence spike may be used to obtain information about the phase coherence in the electronic or vibrational transition being investigated, when the pulse width is comparable to or smaller than the dephasing time. Methods of extracting T2 from the coherence spike are also discussed.
It has long been known that shallow donors such as phosphorous and the other group-V elements, have a hydrogen-like optical spectrum. The main difference is that while the spectrum of atomic hydrogen lies in the visible band, the spectrum of shallow donors in silicon is downshifted to the THz frequency band. This is a direct consequence of the reduced Coulomb attraction seen by the loosely bound electron because the core electrons shield the positive donor atom nucleus, and because the electron is now moving in a dielectric material. While spectroscopy has already revealed much about the energy level structure, very little was known about the temporal dynamics of the system until now. We have used THz pulses from the FELIX free electron laser to probe these hydrogen-like levels. By exploiting the well-known pump-probe technique we have measured the characteristic lifetimes of the excited Rydberg states and found them to be of the order 200 ps. Then, by making subtle changes to the geometry of the pump-probe experimental setup we demonstrate the existence of a THz photon echo. The photon echo is a purely quantum phenomenon with no classical analogue, and it allows us to study the quantum state of the donor electron. We then show, using the photon echo, that it is possible to create a coherent superposition of the ground and excited state of the donor. Measuring the photon echo is important because it can also be used to measure a second important characteristic lifetime of the silicon-donor system, the phase decoherence time.
The electrical detection of spin echoes via echo tomography is used to observe coherent processes associated with the electrical readout of the spin state of phosphorus donor electrons in silicon near a SiO2 interface. Using the Carr-Purcell pulse sequence, an echo decay with a time constant of 1.7+/-0.2 micros is observed and discussed in terms of decoherence and recombination times. Electrical spin echo tomography thus can be used to study the dynamics of the spin-dependent transport processes, e.g., in realistic spin qubit devices for quantum information processing.
We perform femtosecond spectrally resolved pump-probe differential reflectivity measurements on excitons in GaAs quantum wells in both coherent and incoherent regimes. The spectral signal is nonzero and oscillatory at $\ensuremath{-}\mathrm{ve}$ delay up to a few ps indicating persistent coherence between excitonic polarization induced by the probe pulse and the delayed pump pulse. The signal for small +ve+ve+ve and $\ensuremath{-}\mathrm{ve}$ delay $(\ensuremath{\tau})$ shows modulation caused by quantum beats due to coexcitation of heavy and light hole excitons. The rise of the signal with $\ensuremath{\tau}$ for $\ensuremath{\tau}<0$ is rather nonexponential and is sensitive to detuning of the detection energy with respect to the exciton energy. The signal decay with $\ensuremath{\tau}$ for small +ve+ve+ve $\ensuremath{\tau}$ shows dependence on pump-probe relative polarization. The excitonic reflectivity shows a large reduction caused by excitonic absorption saturation for both +ve+ve+ve and $\ensuremath{-}\mathrm{ve}$ $\ensuremath{\tau}$ when the pump pulse intensity is increased to large values. To compare the experimental results with theory, we obtain an expression for the PPDR signal in terms of the third order excitonic polarization. This has an additional term not considered earlier to describe pump-probe experiments. The calculations are performed using optical Bloch equations, modified to incorporate exciton inhomogeneous broadening, quantum beats, and many body effects such as local field, excitation induced energy shift, and dephasing. These effects are found essential in explaining the observed PPDR spectral data. The delay dependence of the signal near the exciton energy is mainly controlled by inhomogeneous broadening for $\ensuremath{-}\mathrm{ve}$ $\ensuremath{\tau}.$ The signal decay for large +ve+ve+ve $\ensuremath{\tau}$ has an exponential behavior determined by the lifetime of incoherent excitons. Experiments for collinear polarization reveal an additional exponential component for small +ve+ve+ve delay. Theoretically, this is found to be related to exciton dephasing and is present only when many body effects are included.
We demonstrate an entirely new method to probe quantum measurement phenomena in semiconductor quantum dot (QD) spin qubits [1]. In addition to providing direct evidence for the quantum nature of solid state qubits, we show that our method has practical importance since it provides a completely alternative route for measuring ensemble and quantum dephasing times, T2* and T2, using only repeated projective measurements and without the need for coherent spin control. Our approach is based on measuring time-correlators of a spin qubit in an optically active QD beyond the second order. We utilize a quantum dot spin-storage structure to initialize a single electron spin in a quantum dot subject to a magnetic field applied in Voigt geometry through tunnel ionization and perform repeated projective measurements of the spin at times t1 and t2. This measurement is repeated, corresponding to ensemble averaging, and the resulting third-order time correlations reveals rich physics: For times t1 or t2 < T2* Larmor precession is observed which reveals the ensemble dephasing time T2*. Importantly, even though the time-correlators were obtained through averaging many measurements for times t1 and t2 > T2* oscillations are observed that decay with the dephasing time T2 and allow its determination even without the need for coherent spin control. Finally, combining the third-order time correlator with the second-order time correlator allows to demonstrate a violation of Leggett-Garg type inequalities for certain times providing clear evidence for the quantum nature of the quantum dot spin. [1] A. Bechtold et al. Phys. Rev. Lett. 117, 027402 (2016)
Two-dimensional electronic spectroscopy (2DES) can be implemented with different geometries, e.g., BOXCARS, collinear, and pump-probe geometries. The pump-probe geometry has the advantage of overlapping only two beams and reducing phase cycling steps. However, its applications are typically limited to observing the dynamics with single-quantum coherence and population, leaving the challenge to measure the dynamics of the double-quantum (2Q) coherence, which reflects the many-body interactions. We demonstrate an experimental technique in 2DES under pump-probe geometry with a designed pulse sequence and the signal processing method to extract 2Q coherence. In the designed pulse sequence, with the probe pulse arriving earlier than the pump pulses, our measured signal includes the 2Q signal as well as the zero-quantum signal. With phase cycling and data processing using causality enforcement, we extract the 2Q signal. The proposal is demonstrated with rubidium atoms. We observe the collective resonances of two-body dipole-dipole interactions in both the D1 and D2 lines.