The charge current pumped adiabatically through a deformable quantum dot is studied within the Green's function approach. Differently from the non-deformable case, the current shows an undefined parity with respect to the pumping phase ϕ. The unconventional current-phase relation, analyzed in the weak pumping regime, is due to a dynamical phase shift ϕ_D caused by the elastic deformations of the central region (classical phonons). The role of the quality factor Q of the oscillator, the effects induced by a mechanical resonance and the implications for current experiments on molecular systems are also discussed.
We propose schemes for generating spin currents into a semiconductor by adiabatic or non-adiabatic pumping of electrons through interacting quantum dots. The appeal of such schemes lies in the possibility to tune the pumping characteristics via gate voltages that control the properties of the quantum dot. The calculations are based on a systematic perturbation expansion in the tunnel-coupling strength and the pumping frequency, expressed within a diagrammatic real-time technique. Special focus is put on the possibility of pure spin pumping, i.e., of pumping spin currents without charge current…
We present a general formalism to study adiabatic pumping through interacting quantum dots. We derive a formula that relates the pumped charge to the local, instantaneous Green function of the dot. This formula is then applied to the infinite-U Anderson model both for weak and strong tunnel-coupling strengths.
We study non-adiabatic two-parameter charge and spin pumping through a single-level quantum dot with Coulomb interaction. For the limit of weak tunnel coupling and in the regime of pumping frequencies up to the tunneling rates, $Ω\lesssim Γ/\hbar$, we perform an exact resummation of contributions of all orders in the pumping frequency. As striking non-adiabatic signatures, we find frequency-dependent phase shifts in the charge and spin currents, which allow for an effective single-parameter pumping as well as pure spin without charge currents.
We study non-adiabatic charge pumping through single-level quantum dots taking into account Coulomb interactions. We show how a truncated set of equations of motion can be propagated in time by means of an auxiliary-mode expansion. This formalism is capable of treating the time-dependent electronic transport for arbitrary driving parameters. We verify that the proposed method describes very precisely the well-known limit of adiabatic pumping through quantum dots without Coulomb interactions. As an example we discuss pumping driven by short voltage pulses for various interaction strengths. Such…
We investigate the influence of the Coulomb interaction on the adiabatic pumping current through quantum dots. Using nonequilibrium Green's functions techniques, we derive a general expression for the current based on the instantaneous Green's function of the dot. We apply this formula to study the dependence of the charge pumped per cycle on the time-dependent pumping potentials. The possibility of charge quantization in the presence of a finite Coulomb repulsion energy is investigated in the light of recent experiments.
We analytically investigate the non-equilibrium pumping for a double quantum dots system on the basis of the quantum master equation (QME), where the double quantum dots are connected to two external leads by the spin coupling. Each of leads has two tunable parameters, temperature and chemical potential. Using QME formalism, we obtain an analytical expression of the Berry-like phase for eigenstate of the QME in the parameter space. We show that the Berry-like curvature is non zero in the whole region in the parameter space. We also show that the Berry-like curvature vanishes in the case of sin…
As an alternative to commonly used electrical methods, we have investigated the optical pumping of charged exciton complexes addressing impurity related transitions with photons of the appropriate energy. Under these conditions, we demonstrate that the pumping fidelity can be very high while still maintaining a switching behavior between the different excitonic species. This mechanism has been investigated for single quantum dots of different size present in the same sample and compared with the direct injection of spectator electrons from nearby donors.
We review spin properties of semiconductor quantum dots and their effect on optical spectra. Photoluminescence and other types of spectroscopy are used to probe neutral and charged excitons in individual quantum dots with high spectral and spatial resolution. Spectral fine structure and polarization reveal how quantum dot spins interact with each other and with their environment. By taking advantage of the selectivity of optical selection rules and spin relaxation, optical spin pumping of the ground state electron and nuclear spins is achieved. Through such mechanisms, light can be used to pro…
We derive a formula describing the adiabatically pumped charge through an interacting quantum dot within the scattering matrix and Green's function approach. We show that when the tunneling rates between the leads and the dot are varied adiabatically in time, both in modulus and phase, the current induced in the dot consists of two terms, the pumping current and a rectification-like term. The last contribution arises from the time-derivative of the tunneling phase and can have even or odd parity with respect to the pumping phase φ. The rectification-like term is also discussed in relation to s…
We investigate charge pumping in carbon nanotube quantum dots driven by the electric field of a surface acoustic wave. We find that at small driving amplitudes, the pumped current reverses polarity as the conductance is tuned through a Coulomb blockade peak using a gate electrode. We study the behavior as a function of wave amplitude, frequency and direction and develop a model in which our results can be understood as resulting from adiabatic charge redistribution between the leads and quantum dots on the nanotube.
The possibility of non-adiabatic electron pumping in the system of three coupled quantum dots attached to the leads is discussed. We have found out that periodical changing of energy level position in the middle quantum dot results in non zero mean tunneling current appeared due to non-adiabatic non-equilibrium processes. The same principle can be used for fabrication of a new class of semiconductor electronic devices based on non-stationary non-equilibrium currents. As an example we propose a nanometer quantum emitter with non-stationary inverse level occupation achieved by electron pumping.
In order to investigate the effects of interference and interaction in adiabatic pumping, we consider an Aharonov-Bohm (AB) interferometer with a quantum dot embedded either in one or in both arms. We employ a real-time formalism and we perform an expansion both in the tunnel-coupling strengths between dot and leads and in the pumping frequency, taking into account the Coulomb interaction non perturbatively. We find that pumping in a single-dot AB interferometer has a peristaltic but phase-coherent character. In a double-dot AB interferometer, we find a pumping mechanism that relies purely on …
We propose a random matrix theory to describe the influence of a time-dependent external field on electron transport through open quantum dots. We describe the generation of the current by an oscillating field for the dot, connected to two leads with equal chemical potentials. For low frequency fields our results correspond to adiabatic charge pumping. Finite current can be produced if the system goes along a closed loop in parameter space, which covers a finite area. At high frequency finite current is produced even if the loop is a line in parameter space. This result can be explained in the…
We propose a mechanism to explain the fluctuations of the ground state energy in quantum dots in the Coulomb blockade regime. Employing the random matrix theory we show that shape deformations may change the adjacent peak spacing distribution from Wigner-Dyson to nearly Gaussian even in the absence of strong charging energy fluctuations. We find that this distribution is solely determined by the average number of anti-crossings between consecutive conductance peaks and the presence or absence of a magnetic field. Our mechanism is tested in a dynamical model whose underlying classical dynamics …
Adiabatic quantum pumping in noninteracting, phase coherent quantum dots is elegantly described by Brouwer's formula. Interactions within the dot, while suppressing phase coherence, make Brouwer's formalism inapplicable. In this paper, we discuss the nature of the physical processes forcing a description of pumping beyond Brouwer's formula, and develop, using a controlled adiabatic expansion, a useful formalism to study the effect of interactions within a generic perturbative scheme. The pumped current consists of a first contribution, analogous to Brouwer's formula and accounting for the rema…
We study electron pumping through a system of barriers, whose heights are deformed adiabatically. We derive a simple formula for the pumped charge $Q$ in terms of the total reflection and transmission amplitudes and phases. The pumped charge increases with the number of barriers ($n_b$) and shows an interesting step-like behaviour, with the steps appearing at integer values of $Q$. The pumped charge also tends towards quantisation with the increase of the amplitude of the time-varying potential. The value of the quantised pumped charge is shown to be correlated to the discontinuity of the refl…
Nuclear spin polarization can be pumped into spin-blocked quantum dots by multiple Landau- Zener passages through singlet-triplet anticrossings. By numerical simulations of realistic systems including approximately $10^7$ nuclear spins during $10^5$ sweeps, we uncover a mechanism of dynamical self-quenching which results in a fast saturation of the nuclear polarization under stationary pumping. This is caused by screening of the field of the nuclear spins. In systems with moderate spin-orbit coupling, self-quenching also screens the spin-orbit interaction. The mechanism is generic and remains …
In a mesoscopic system, under zero bias voltage, a finite charge is transferred by quantum adiabatic pumping by adiabatically and periodically changing two or more control parameters. We obtained expressions for the pumped charge for a ring of three quantum dots (QDs) by choosing the magnetic flux penetrating the ring as one of the control parameters. We found that the pumped charge shows a steplike behavior with respect to the variance of the flux. The value of the step heights is not universal but depends on the trajectory of the control parameters. We discuss the physical origin of this beh…
We study conductance through a quantum dot under Coulomb blockade conditions in the presence of an external periodic perturbation. The stationary state is determined by the balance between the heating of the dot electrons by the perturbation and cooling by electron exchange with the cold contacts. We show that Coulomb blockade peak can have a peculiar shape if heating is affected by dynamic localization, which can be an experimental signature of this effect.
We consider adiabatic charge transport through an almost open quantum dot. We show that the charge transmitted in one cycle is quantized in the limit of vanishing temperature and one-electron mean level spacing in the dot. The explicit analytic expression for the pumped charge at finite temperature is obtained for spinless electrons. The pumped charge is produced by both non-dissipative and dissipative currents. The latter are responsible for the corrections to charge quantization which are expressed through the conductance of the system.
We demonstrate full charge control, narrow optical linewidths, and optical spin pumping on single self-assembled InGaAs quantum dots embedded in a $162.5\,\text{nm}$ thin diode structure. The quantum dots are just $88\,\text{nm}$ from the top GaAs surface. We design and realize a p-i-n-i-n diode that allows single-electron charging of the quantum dots at close-to-zero applied bias. In operation, the current flow through the device is extremely small resulting in low noise. In resonance fluorescence, we measure optical linewidths below $2\,μ\text{eV}$, just a factor of two above the transform l…
We propose a new mechanism for polarizing nuclear spins in quantum dots, based on periodic modulation of the hyperfine coupling by electric driving at the electron spin resonance frequency. Dynamical nuclear polarization results from resonant excitation rather than hyperfine relaxation mediated by a thermal bath, and thus is not subject to Overhauser-like detailed balance constraints. This allows polarization in the direction opposite to that expected from the Overhauser effect. Competition of the electrically-driven and bath assisted mechanisms can give rise to spatial modulation and sign rev…
In this work we study theoretically and experimentally the multi-particle structure of the so-called type-II quantum dots with spatially separated electrons and holes. Our calculations based on customarily developed full configuration interaction approach reveal that exciton complexes containing holes interacting with two or more electrons exhibit fairly large antibinding energies. This effect is found to be the hallmark of the type-II confinement. In addition, an approximate self-consistent solution of the multi-exciton problem allows us to explain two pronounced phenomena: the blue-shift of …
Precise manipulation of individual charge carriers in nanoelectronic circuits underpins practical applications of their most basic quantum property --- the universality and invariance of the elementary charge. A charge pump generates a net current from periodic external modulation of parameters controlling a nanostructure connected to source and drain leads; in the regime of quantized pumping the current varies in steps of $q_e f$ as function of control parameters, where $q_e$ is the electron charge and $f$ is the frequency of modulation. In recent years, robust and accurate quantized charge p…
We show that optical pumping of electron spins in individual InGaAs quantum dots leads to strong nuclear polarisation that we measure via the Overhauser shift (OHS) in magneto-photoluminescence experiments between 0 and 4T. We find a strongly non-monotonous dependence of the OHS on the applied magnetic field, with a maximum nuclear polarisation of 40% for intermediate magnetic fields. We observe that the OHS is larger for nuclear fields anti-parallel to the external field than in the parallel configuration. A bistability in the dependence of the OHS on the spin polarization of the optically in…
We investigate the statistical fluctuations of currents in chaotic quantum dots induced by pumping and rectification at finite temperature and in the presence of dephasing. In open quantum dots, dc currents can be generated by the action of two equal-frequency ac gate voltages. The adiabatic regime occurs when the driving frequency is smaller than the electron inverse dwell time. Using numerical simulations complemented by semiclassical calculations, we consider both limits of small and large number of propagating channels in the leads when time-reversal symmetry is fully broken. We find that …
We consider the adiabatic charge transport through zero-dimensional mesoscopic sample (quantum dot) caused by two periodically changing external perturbations. Both the magnitude and the sign of the transmitted charge are extremely sensitive to the configuration of the dot and to the magnetic field. We find the correlation function characterizing the random value of this pumped charge for arbitrary strength of the perturbation. In contrast to previous theoretical and experimental claims, the charge is found not to have any symmetry with respect to the inversion of magnetic field. At strong pum…
We derive the effective cavity pumping and decay rates for the master equation of a quantum dot-microcavity system in presence of $N$ weakly coupled dots. We show that the in-flow of photons is not linked to the out-flow by thermal equilibrium relationships.
We study adiabatic pumping of electrons through quantum dots attached to ferromagnetic leads. Hereby we make use of a real-time diagrammatic technique in the adiabatic limit that takes into account strong Coulomb interaction in the dot. We analyze the degree of spin polarization of electrons pumped from a ferromagnet through the dot to a nonmagnetic lead (N-dot-F) as well as the dependence of the pumped charge on the relative leads' magnetization orientations for a spin-valve (F-dot-F) structure. For the former case, we find that, depending on the relative coupling strength to the leads, spin …
We study conductance through a quantum dot under Coulomb blockade conditions in the presence of an external periodic perturbation. The stationary state is determined by the balance between the heating of the dot electrons by the perturbation and cooling. We analyze two cooling mechanisms: electron exchange with the cold contacts and emission of phonons. Together with the usual linear Ohmic heating of the dot electrons we consider possible effects of dynamic localization. The combination of the abovementioned factors may result in a drastic change of the shape of the Coulomb blockade peak with …
We analyze time-dependent transport through a quantum dot with electron-electron interaction that is statically tunable to both repulsive and attractive regimes, or even dynamically driven. Motivated by the recent experimental realization [Hamo et. al, Nature 535, 395 (2016)] of such a system in a static double quantum dot we compute the geometric pumping of charge in the limit of weak tunneling, high temperature and slow driving. We analyze the pumping responses for all pairs of driving parameters (gate voltage, bias voltage, tunnel coupling, electron-electron interaction). We show that the r…
We use exact techniques to demonstrate theoretically the pumping of fractional charges in a single-level non-interacting quantum dot, when the dot-reservoir coupling is adiabatically driven from weak to strong coupling. The pumped charge averaged over many cycles is quantized at a fraction of an electron per cycle, determined by the ratio of Lamb shift to level-broadening; this ratio is imposed by the reservoir band-structure. For uniform density of states, half an electron is pumped per cycle. We call this "adiabatic almost-topological pumping", because the pumping's Berry curvature is sharpl…
The interaction between electrons and the vibrational degrees of freedom of a molecular quantum dot can lead to an exponential suppression of the conductance, an effect which is commonly termed Franck-Condon blockade. Here, we investigate this effect in a quantum dot driven by time-periodic gate voltages and tunneling amplitudes using nonequilibrium Green's functions and a Floquet expansion. Building on previous results showing that driving can lift the Franck-Condon blockade, we investigate driving protocols which can be used to pump charge across the quantum dot. In particular, we show that …
We have investigated pumping in quantum dots from the perspective of non-Abelian (matrix) Berry phases by solving the time dependent Schr{ö}dinger equation exactly for adiabatic changes. Our results demonstrate that a pumped charge is related to the presence of a finite matrix Berry phase. When consecutive adiabatic cycles are performed the pumped charge of each cycle is different from the previous ones.
Semiconducting nanowires (NWs) are a versatile, highly tunable material platform at the heart of many new developments in nanoscale and quantum physics. Here, we demonstrate charge pumping, i.e., the controlled transport of individual electrons through an InAs NW quantum dot (QD) device at frequencies up to $1.3\,$GHz. The QD is induced electrostatically in the NW by a series of local bottom gates in a state of the art device geometry. A periodic modulation of a single gate is enough to obtain a dc current proportional to the frequency of the modulation. The dc bias, the modulation amplitude a…
We study experimentally the dependence of dynamic nuclear spin polarization on the power of non-resonant optical excitation in two types of individual neutral semiconductor quantum dots: InGaAs/GaAs and GaAs/AlGaAs. We show that the mechanism of nuclear spin pumping via second order recombination of optically forbidden (''dark'') exciton states recently reported in InP/GaInP quantum dots [Phys. Rev. B 83, 125318 (2011)] is relevant for material systems considered in this work. In the InGaAs/GaAs dots this nuclear spin polarization mechanism is particularly pronounced, resulting in Overhauser s…
We report optical pumping of neutral quantum dots leading to nuclear spin alignment with direction insensitive to polarization and wavelength of light. Measurements of photoluminescence of both "dark" and "bright" excitons in single dots reveal that nuclear spin pumping occurs via a virtual spin-flip transition between these states accompanied by photon emission. The sign of the nuclear spin polarization is determined by asymmetry in the exciton energy spectrum, rather than by the sign of the exciton spin polarization.
To understand and optimize optical spin initialization in room temperature CdSe nanocrystal quantum dots (NCQDs) we studied the dependence of the time-resolved Faraday rotation signal on pump energy $E_p$ in a series of NCQD samples with different sizes. In larger NCQDs, we observe two peaks in the spin signal vs. $E_p$, whereas in smaller NQCDs, only a single peak is observed before the signal falls to a low, broad plateau at higher energies. We calculate the spin-dependent oscillator strengths of optical transitions using a simple effective mass model to understand these results. The observe…
The photoluminescence polarizations of (In,Ga)As/GaAs quantum dots annealed at different temperatures are studied as a function of external magnetic field (Hanle curves). In these dependencies, remarkable resonant features appear due to all-optical nuclear magnetic resonances (NMR) for optical excitation with modulated circular polarization. Application of an additional radio-frequency field synchronously with the polarization modulation strongly modifies the NMR features. The resonances can be related to transitions between different nuclear spin states split by the strain-induced gradient of…
A theory of optical emission of quantum dot arrays in quantum microcavities is developed. The regime of the strong coupling between the quantum dots and photonic mode of the cavity is considered. The quantum dots are modeled as two-level systems. In the low pumping (linear) regime the emission spectra are mainly determined by the superradiant mode where the effective dipoles of the dots oscillate in phase. In the non-linear regime the superradiant mode is destroyed and the emission spectra are sensitive to the parity of quantum dot number. Further increase of the pumping results in the line wi…
We report on the spin properties of individual Mn atoms in II-VI semiconductor strain free quantum dots. Strain free Mn-doped CdTe quantum dots are formed by width fluctuations in thin quantum wells lattice matched on a CdTe substrate. These quantum dots permit to optically probe and address any spin state of a Mn atom in a controlled strain environment. The absence of strain induced magnetic anisotropy prevents an optical pumping of the Mn spin at zero magnetic field. Thus, a large photoluminescence is obtained under resonant optical excitation of the exciton-Mn complex. An efficient optical …
Spin inertia measurements are a novel experimental tool to study long-time spin relaxation processes in semiconductor nanostructures. We develop a theory of the spin inertia effect for resident electrons and holes localized in quantum dots. We consider the spin orientation by short optical pulses with arbitrary pulse area and detuning from the trion resonance. The interaction with an external longitudinal magnetic field and the hyperfine interaction with the nuclear spin bath is considered in both the ground and excited (trion) states of the quantum dots. We analyze how the spin inertia signal…
e study theoretically, the photoluminescence properties of a single quantum dot in a microcavity under incoherent excitation. We propose a microscopic quantum statistical approach providing a Lindblad (thus completely positive) description of pumping and decay mechanisms of the quantum dot and of the cavity mode. Our analytical results show that strong coupling (SC) and linewidths are largely independent on the pumping intensity (until saturation effects come into play), in contrast to previous theoretical findings. We shall show the reliable predicting character of our theoretical framework i…
We study geometric energy transport in a slowly driven single-level quantum dot weakly coupled to electronic contacts and with strong onsite interaction, which can be either repulsive or attractive. Exploiting a recently discovered fermionic duality for the evolution operator of the master equation, we provide compact and insightful analytic expressions of energy pumping curvatures for any pair of driving parameters. This enables us to systematically identify and explain the pumping mechanisms for different driving schemes, thereby also comparing energy and charge pumping. We determine the con…
We study adiabatic quantum pumping in the resonant tunneling regime of a nearly-closed quantum dot, which is coupled to two leads via tunneling barriers. Using small cyclic variations of the tunneling rates of the barriers as the pumping mechanism, a current is obtained which depends sensitively on the system parameters and exhibits peaks due to Coulomb blockade. The distribution of the peak heights is found for temperatures $\Gam \ll k_{B} T \ll Δ$, with $\Gam$ the total decay width into the leads and $Δ$ the single-particle level spacing of the dot, and their average height is predicted to i…
Single electron pumps are set to revolutionize electrical metrology by enabling the ampere to be re-defined in terms of the elementary charge of an electron. Pumps based on lithographically-fixed tunnel barriers in mesoscopic metallic systems and normal/superconducting hybrid turnstiles can reach very small error rates, but only at MHz pumping speeds corresponding to small currents of the order 1 pA. Tunable barrier pumps in semiconductor structures have been operated at GHz frequencies, but the theoretical treatment of the error rate is more complex and only approximate predictions are availa…
Nuclear polarization dynamics are measured in the nuclear spin bi-stability regime in a single optically pumped InGaAs/GaAs quantum dot. The controlling role of nuclear spin diffusion from the dot into the surrounding material is revealed in pump-probe measurements of the non-linear nuclear spin dynamics. We measure nuclear spin decay times in the range 0.2-5 sec, strongly dependent on the optical pumping time. The long nuclear spin decay arises from polarization of the material surrounding the dot by spin diffusion for long (>5sec) pumping times. The time-resolved methods allow the detection …
We address theoretically adiabatic regime of charge transport for a model of two tunnel-coupled quantum dots connected in series. The energy levels of the two dots are harmonically modulated by an external potential with a constant phase shift between the two. Motivated by recent experiments with surface-acoustic-wave excitation, we consider two situations: (a) pure pumping in the absence of external voltage (also at finite temperature), and (b) adiabatic modulation of the current driven by large external bias. In both cases we derive results consistent with published experimental data. For th…
Left-handedness with three zero-absorption windows tuned by the incoherent pumping field and inter-dot tunnelings in a GaAs/AlGaAs triple quantum dots system
We report on the dynamics of optically induced nuclear spin polarization in individual CdTe/ZnTe quantum dots loaded with one electron by modulation doping. The fine structure of the hot trion (charged exciton $X^-$ with an electron in the $P$-shell) is identified in photoluminescence excitation spectra. A negative polarisation rate of the photoluminescence, optical pumping of the resident electron and the built-up of dynamic nuclear spin polarisation (DNSP) are observed in time-resolved optical pumping experiments when the quantum dot is excited at higher energy than the hot trion triplet sta…
We demonstrate single-electron pumping in a gate-defined carbon nanotube double quantum dot. By periodic modulation of the potentials of the two quantum dots we move the system around charge triple points and transport exactly one electron or hole per cycle. We investigate the pumping as a function of the modulation frequency and amplitude and observe good current quantization up to frequencies of 18 MHz where rectification effects cause the mechanism to break down.
We present a diagrammatic real-time approach to adiabatic pumping of electrons through interacting quantum dots. Performing a systematic perturbation expansion in the tunnel-coupling strength, we compute the charge pumped through a single-level quantum dot per pumping cycle. The combination of Coulomb interaction and quantum fluctuations, accounted for in contributions of higher order in the tunnel coupling, modifies the pumping characteristics via an interaction-dependent renormalization of the quantum-dot level. The latter is even responsible for the {\em dominant} contribution to the pumped…
We study DC charge and spin transport through a weakly coupled quantum dot, driven by a non-adiabatic periodic change of system parameters. We generalize the model of Tien and Gordon to simultaneously oscillating voltages and tunnel couplings. When applying our general result to the two-parameter charge pumping in quantum dots, we find interference effects between the oscillations of the voltage and tunnel couplings. Furthermore, we discuss the possibility to electrically pump a spin current in presence of a static magnetic field.
We propose and analyze a new scheme of realizing both spin filtering and spin pumping by using ac-driven double quantum dots in the Coulomb blockade regime. By calculating the current through the system we demonstrate that the spin polarization of the current can be controlled by tuning the parameters (amplitude and frequency) of the ac field. We also discuss spin relaxation and decoherence effects in the pumped current.
We have investigated the spin preparation efficiency by optical pumping of individual Mn atoms embedded in CdTe/ZnTe quantum dots. Monitoring the time dependence of the intensity of the fluorescence during the resonant optical pumping process in individual quantum dots allows to directly probe the dynamics of the initialization of the Mn spin. This technique presents the convenience of including preparation and read-out of the Mn spin in the same step. Our measurements demonstrate that Mn spin initialization, at zero magnetic field, can reach an efficiency of 75% and occurs in the tens of \emp…
The electron-phonon coupling in self-assembled InGaAs quantum dots is relatively weak at low light intensities, which means that the zero-phonon line in emission is strong compared to the phonon sideband. However, the coupling to acoustic phonons can be dynamically enhanced in the presence of an intense optical pulse tuned within the phonon sideband. Recent experiments have shown that this dynamic vibronic coupling can enable population inversion to be achieved when pumping with a blue-shifted laser and for rapid de-excitation of an inverted state with red detuning. In this paper we confirm th…
