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arXiv:cond-mat/0412370 · Physical Review B

Microscopic approach to spin dynamics: Meaning of spin-relaxation times

C. Lechner, U. Rößler

Published Jul 7, 2005• 7 citations
arXivHTMLPDF

Abstract

We present an approach to spin dynamics by extending the optical Bloch equations for the driven two-level system to derive microscopic expressions for the transverse and longitudinal spin-relaxation times. This is done for the six-level system of electron and hole subband states in a semiconductor or a semiconductor quantum structure to account for the degrees of freedom of the carrier spin and the polarization of the exciting light and includes the scattering between carriers and lattice vibrations on a microscopic level. For the subsystem of the spin-split electron subbands we treat the electron-phonon interaction in second order and derive a set of equations of motion for the $2\ifmmode\times\else\texttimes\fi{}2$ spin-density matrix, which describes the electron spin dynamics and contains microscopic expressions for the longitudinal $({T}_{1})$ and transverse $({T}_{2})$ spin-relaxation times. Their meaning will be discussed in relation to experimental investigations of these quantities.

DOI
10.1103/physrevb.72.045311

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The Density Matrix

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We present an approach to spin dynamics by extending the optical Bloch equations for the driven two-level system to derive microscopic expressions for the transverse and longitudinal spin-relaxation times. This is done for the six-level system of electron and hole subband states in a semiconductor or a semiconductor quantum structure to account for the degrees of freedom of the carrier spin and the polarization of the exciting light and includes the scattering between carriers and lattice vibrations on a microscopic level. For the subsystem of the spin-split electron subbands we treat the electron-phonon interaction in second order and derive a set of equations of motion for the 2\ifmmode×\else\texttimes\fi22\ifmmode\times\else\texttimes\fi{}22\ifmmode×\else\texttimes\fi2 spin-density matrix, which describes the electron spin dynamics and contains microscopic expressions for the longitudinal (T1)({T}_{1})(T1​) and transverse (T2)({T}_{2})(T2​) spin-relaxation times. Their meaning will be discussed in relation to experimental investigations of these quantities.
We present a theoretical approach to spin dynamics in semiconductors and semiconductor heterostructures based on the density matrix formalism. It consists in an extension of the coherent Semiconductor Bloch equations for the two‐level system to a six‐level system which accounts for the spin and polarization degrees‐of‐freedom and includes carrier‐carrier scattering beyond the Hartree‐Fock truncation. This extension provides the concept to formulate spin dynamics including spin relaxation and dephasing times on a microscopic level.
The quantum dynamics of many-electron spin systems is investigated using a reduced-density-matrix description. Applications of interest include trapped atomic systems in optical lattices, semiconductor quantum dots, and vacancy defect centers in solids. Complimentary time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are self-consistently developed. The general non-perturbative and non-Markovian formulations provide a fundamental framework for systematic evaluations of corrections to the standard Born (lowest-order-perturbation) and Markov (short-memory-time) approximations. Particular attention is given to decoherence and relaxation processes, together with spectral-line broadening phenomena, that are induced by interactions of many-electron spin systems with photons, phonons, nuclear spins, external electric, magnetic, and electromagnetic fields. Within the framework of a quantum-open-systems (reduced-density-operator) approach, these processes are treated either as coherent interactions or as environmental interactions. The environmental interactions are incorporated by means of the general expressions that are derived for the time-domain and frequency-domain Liouville-space self-energy operators, for which the tetradic-matrix elements are explicitly evaluated in the diagonal-resolvent, lowest-order, and Markov (short-memory time) approximations.
Understanding the effect of vibrations on the relaxation process of individual spins is crucial for implementing nanosystems for quantum information and quantum metrology applications. In this work, we present a theoretical microscopic model to describe the spin-lattice relaxation of individual electronic spins associated to negatively charged nitrogen-vacancy centers in diamond, although our results can be extended to other spin-boson systems. Starting from a general spin-lattice interaction Hamiltonian, we provide a detailed description and solution of the quantum master equation of an electronic spin-one system coupled to a phononic bath in thermal equilibrium. Special attention is given to the dynamics of one-phonon processes below 1 K where our results agree with recent experimental findings and analytically describe the temperature and magnetic-field scaling. At higher temperatures, linear and second-order terms in the interaction Hamiltonian are considered and the temperature scaling is discussed for acoustic and quasilocalized phonons when appropriate. Our results, in addition to confirming a T5{T}^{5}T5 temperature dependence of the longitudinal relaxation rate at higher temperatures, in agreement with experimental observations, provide a theoretical background for modeling the spin-lattice relaxation at a wide range of temperatures where different temperature scalings might be expected.
Using laser pulses of duration comparable to semiconductor relaxation and dephasing times, the coherent phenomena common to two-level systems have been demonstrated in II-VI and III-V semiconductors. These light-matter interactions are characterized by electrons and holes in their initially excited states and/or a macroscopic polarization that persists after the excitation. A nonthermal carrier distribution was observed in bulk CdSe, demonstrating the extremely fast energy relaxation possible when carrier-LO-phonon scattering is included. Quantum-confined CdSe microcrystallites were then employed to limit the available decay avenues. The one and two-pair transitions were characterized, and using spectral hole-burning, energy relaxation was shown to be substantially slower than in bulk. Dipole dephasing remained very rapid. Persistent macroscopic polarization was demonstrated in semiconductors through pump and probe experiments conducted on time scales faster than the inverse linewidth of the exciton. In the first set of experiments, it was found that the exciton optical Stark shift deviates from that predicted by a steady-state theory. The shift is smaller than expected and lasts longer than the pump pulse. Both effects are explained by free evolution of the exciton's polarization. Transient exciton bleaching is observed and shown to be a result of adiabatic following. In a second study of coherent polarization, spectral oscillations at negative delay times were studied. Oscillations were measured in a wide variety of semiconductors, temporally preceding several different pump-probe phenomena. By comparison with a semiclassical theory, it was shown that spectral oscillations in the spectral region of the exciton are evidence of persistent exciton polarization. Oscillations in the band are due to four wave mixing of the pump and probe beams.
The dynamics of electrons and holes in semiconductors and semiconductor heterostructures have been extensively discussed in the literature, and are governed by their mutual Coulomb interaction, by their interaction with lattice vibrations (phonons) and by their radiative recombination (for an overview see e.g. Ref. [1]). A powerful technique to study the carrier dynamics in semiconductors utilizes short optical pulses to photoexcite electrons from the valence to the conduction band (i.e. to create electron-hole pairs) that subsequently relax until the photon energy stored in the medium is dissipated and the system has recovered the thermal equilibrium. The dynamics of the carriers photoexcited by the short optical pulse can be followed by monitoring two main optical observables: the interband population difference and the induced polarization. Both quantities decay with time after the photoexcitation due to the carrier dynamics. While the induced polarization (which is an ensemble average over many photoexcited dipole moments) is sensitive to scattering events that break the phase relationship among the individual dipoles and/or with the light field creating them (dephasing processes), the population difference is sensitive only to events that change the energy state of the carriers. Transient coherent optical spectroscopy addresses the time-evolution of the induced polarization in the time-regime during and immediately following the photoexcitation by a short laser pulse, in which the photoexcited dipoles have retained a defined phase relationship among each other and with the exciting coherent radiation.
The density matrix is a useful concept which will allow one to deal with a large collection of spinors with a statistical distribution at time t = 0 and follow their time evolution by tracking the time evolution of a new operator (the density matrix). This will require the extension of the Bloch sphere to the Bloch ball concept, in which the vector representing the collection of spinors will be able to reach points in the interior of the Bloch sphere as a function of time. This requires the inclusion of damping and scattering mechanisms representing interactions among spinors, and also their interactions with the environment. The phenomenological equations allowing a description of these relaxation mechanisms are known as Bloch’s equations. They are introduced here through a connection to the Bloch sphere and Bloch ball concepts. The longitudinal and transverse relaxation times, T1 and T2, respectively, are also introduced and some numerical examples (results of Monte-Carlo simulations) are presented to illustrate their physical meaning.