Nonresonant Optical Excitation Research Articles

Transient IR spectroscopy of optically centrifuged CO2 (R186-R282) and collision dynamics for the J = 244-282 states.

Collisions of optically centrifuged CO2 molecules with J = 244-282 (Erot = 22 800-30 300 cm-1) are investigated with high-resolution transient IR absorption spectroscopy to reveal collisional and orientational phenomena of molecules with hyper-thermal rotational energies. The optical centrifuge is a non-resonant optical excitation technique that uses ultrafast, 800 nm chirped pulses to drive molecules to extreme rotational states through sequential Raman transitions. The extent of rotational excitation is controlled by tuning the optical bandwidth of the excitation pulses. Frequencies of 30 R-branch ν3 fundamental IR probe transitions are measured for the J = 186-282 states of CO2, expanding beyond previously reported IR transitions up to J = 128. The optically centrifuged molecules have oriented angular momentum and unidirectional rotation. Polarization-sensitive transient IR absorption of individual rotational states of optically centrifuged molecules and their collision products reveals information about collisional energy transfer, relaxation kinetics, and dynamics of rotation-to-translation energy transfer. The transient IR probe also measures the extent of polarization anisotropy. Rotational energy transfer for lower energy molecules is discussed in terms of statistical models and a comparison highlights the role of increasing energy gap with J and angular momentum of the optically centrifuged molecules.

Enhanced coupling between ballistic exciton-polariton condensates through tailored pumping

We propose a method to enhance the spatial coupling between ballistic exciton-polariton condensates in a semiconductor microcavity based on available spatial light modulator technologies. Our method, verified by numerically solving a generalized Gross-Pitaevskii model, exploits the strong nonequilibrium nature of exciton-polariton condensation driven by localized nonresonant optical excitation. Tailoring the excitation beam profile from a Gaussian into a polygonal shape results in refracted and focused radial streams of outflowing polaritons from the excited condensate which can be directed towards nearest neighbors. Our method can be used to lower the threshold power needed to achieve polariton condensation and increase spatial coherence in extended systems, paving the way towards creating extremely large-scale quantum fluids of light.

Spin dynamics of positively charged excitons in Cr+ -doped quantum dots probed by resonant photoluminescence

We study the dynamics of the spin system that consists of a positively charged II-VI semiconductor quantum dot doped with a single ${\mathrm{Cr}}^{+}$ ion. The resonant photoluminescence (PL) of the positively charged exciton coupled with the ${\mathrm{Cr}}^{+}$ spin is used to analyze the main spin relaxation channels. The intensity of the resonant PL is reduced by an optical pumping of the spin of the resident hole-${\mathrm{Cr}}^{+}$ complex that can be seen as a nanomagnet. The spin memory can be partially erased by a nonresonant optical excitation. This leads to an increase of the resonant PL signal. The resonant PL is cocircularly polarized and corresponds to relaxation channels that conserve the ${\mathrm{Cr}}^{+}$ spin $|{S}_{z}|$. The observation in the resonant-PL excitation spectra of optical transitions with a change of the ${\mathrm{Cr}}^{+}$ spin permits to determine the magnetic anisotropy of the magnetic atom. Optical pumping, autocorrelation measurements, and the power dependence of the PL intensity distribution show that the effective temperature of the hole-${\mathrm{Cr}}^{+}$ spin system is affected by the optical excitation through the local generation of phonons.

Persistent Currents in Half-Moon Polariton Condensates

We create exciton-polariton condensates in half-moon shapes by the non-resonant optical excitation of GaAs-based cylindrical pillar microcavities. In this geometry, the π-jump of the phase of the c...

Influence of nonequilibrium phonons on the spin dynamics of a single Cr atom

We analyse the influence of optically generated non-equilibrium phonons on the spin relaxation and effective spin temperature of an individual Cr atom inserted in a quantum dot. Using a three pulses pump-probe technique, we show that the spin relaxation measured in resonant optical pumping experiments strongly depends on the optical excitation conditions. We observe for an isolated Cr in the dark a heating time shorter than a few hundreds $ns$ after an initial high power non-resonant excitation pulse. A cooling time larger than a few tens of $\mu s$, independent on the excitation, is obtained in the same experimental conditions. We show that a tunable spin-lattice coupling dependent on the density of non-equilibrium phonons can explain the observed dynamics. Low energy excitation conditions are found where the Cr spin states S$_z$=$\pm$1 can be efficiently populated by a non-resonant optical excitation, prepared and read-out by resonant optical pumping and conserved in the dark during a few $\mu$s.

Observation of nonequilibrium motion and equilibration in polariton rings

We present a study of the macroscopic dynamics of a polariton condensate formed by non-resonant optical excitation in a quasi-one-dimensional ring-shaped microcavity. The presence of a gradient in the cavity photon energy creates a macroscopic trap for the polaritons in which a single mode condensate is formed. With time- and energy-resolved imaging we show the role of interactions in the motion of the condensate as it undergoes equilibration in the ring. These experiments also give a direct measurement of the polariton-polariton interaction strength above the condensation threshold. Our observations are compared to the open-dissipative one-dimensional Gross-Pitaevskii equation which shows excellent qualitative agreement.

Polariton-enhanced exciton transport

The transport distance of excitons in exciton-polariton systems has previously been assumed to be very small ($\lesssim 1~\mu$m). The sharp spatial profiles observed when generating polaritons by non-resonant optical excitation show that this assumption is generally true. In this paper, however, we show that the transport distances of excitons in two-dimensional planar cavity structures with even a slightly polaritonic character are much longer than expected ($\approx 20~\mu$m). Although this population of slightly polaritonic excitons is normally small compared to the total population of excitons, they can substantially outnumber the population of the polaritons at lower energies, leading to important implications for the tailoring of potential landscapes and the measurement of interactions between polaritons.

Photon-Number-Resolved Measurement of an Exciton-Polariton Condensate.

We measure the full photon-number distribution emitted from a Bose condensate of microcavity exciton polaritons confined in a micropillar cavity. The statistics are acquired by means of a photon-number-resolving transition edge sensor. We directly observe that the photon-number distribution evolves with the nonresonant optical excitation power from geometric to quasi-Poissonian statistics, which is canonical for a transition from a thermal to a coherent state. Moreover, the photon-number distribution allows one to evaluate the higher-order photon correlations, shedding further light on the coherence formation and phase transition of the polariton condensate. The experimental data are analyzed in terms of thermal-coherent states, which gives direct access to the thermal and coherent fraction from the measured distributions. These results pave the way for a full understanding of the contribution of interactions in light-matter condensates in the coherence buildup at threshold.

Optical Bistability under Nonresonant Excitation in Spinor Polariton Condensates.

We realize bistability in the spinor of polariton condensates under nonresonant optical excitation and in the absence of biasing external fields. Numerical modeling of the system using the Ginzburg-Landau equation with an internal Josephson coupling between the two spin components of the condensate qualitatively describes the experimental observations. We demonstrate that polariton spin bistability strongly depends on the condensate's overlap with the exciton reservoir by tuning the excitation geometry and sample temperature. We obtain noncollapsing bistability hysteresis loops for a record range of sweep times, [10 μs, 1s], offering a promising route to spin switches and spin memory elements.

Room-Temperature Exciton-Polariton Condensation in a Tunable Zero-Dimensional Microcavity

We create exciton-polaritons in a zero-dimensional (0D) microcavity filled with organic ladder-type conjugated polymer in the strong light-matter interaction regime. Photonic confinement at wavelength scale is realized in the longitudinal direction by two dielectric Bragg mirrors and laterally by a sub-micron Gaussian-shaped defect. The cavity is separated into two parts allowing nanometer position control and enabling tuning of exciton and photon fractions of the polariton wavefunction. Polariton condensation is achieved with non-resonant, picosecond optical excitation at ambient conditions and evidenced by a threshold behavior with non-linear increase of the emission intensity, line narrowing and blue-shift of the emission peak. Furthermore, angular emission spectra show that condensation occurs in the ground state of the 0D-cavity, and first order coherence measurements reveal the coherent nature. These experiments open the door for polariton quantum fluids in complex external potentials at room temperature.

Room temperature strong coupling in a semiconductor microcavity with embedded AlGaAs quantum wells designed for polariton lasing.

We report a systematic study of the temperature and excitation density behavior of an AlAs/AlGaAs, vertically emitting microcavity with embedded ternary Al0.20Ga0.80As/AlAs quantum wells in the strong coupling regime. Temperature-dependent photoluminescence measurements of the bare quantum wells indicate a crossover from the type-II indirect to the type-I direct transition. The resulting mixing of quantum well and barrier ground states in the conduction band leads to an estimated exciton binding energy systematically exceeding 25 meV. The formation of exciton-polaritons is evidenced in our quantum well microcavity via reflection measurements with Rabi splittings ranging from (13.93 ± 0.15) meV at low temperature (30 K) to (8.58 ± 0.40) meV at room temperature (300 K). Furthermore, the feasibility of polariton laser operation is demonstrated under non-resonant optical excitation conditions at 20 K and emission around 1.835 eV.

Relaxation Oscillations and Ultrafast Emission Pulses in a Disordered Expanding Polariton Condensate

Semiconductor microcavities are often influenced by structural imperfections, which can disturb the flow and dynamics of exciton-polariton condensates. Additionally, in exciton-polariton condensates there is a variety of dynamical scenarios and instabilities, owing to the properties of the incoherent excitonic reservoir. We investigate the dynamics of an exciton-polariton condensate which emerges in semiconductor microcavity subject to disorder, which determines its spatial and temporal behaviour. Our experimental data revealed complex burst-like time evolution under non-resonant optical pulsed excitation. The temporal patterns of the condensate emission result from the intrinsic disorder and are driven by properties of the excitonic reservoir, which decay in time much slower with respect to the polariton condensate lifetime. This feature entails a relaxation oscillation in polariton condensate formation, resulting in ultrafast emission pulses of coherent polariton field. The experimental data can be well reproduced by numerical simulations, where the condensate is coupled to the excitonic reservoir described by a set of rate equations. Theory suggests the existence of slow reservoir temporarily emptied by stimulated scattering to the condensate, generating ultrashort pulses of the condensate emission.

A Yellow Polariton Condensate in a Dye Filled Microcavity

Polariton condensation in the yellow part of the visible spectrum from a planar organic semiconductor microcavity containing the molecular dye bromine‐substituted boron‐dipyrromethene is observed. This study provides experimental fingerprint of polariton condensation under nonresonant optical excitation, including the nonlinear dependence of the emission intensity and wavelength blueshift with increasing excitation density, single excitation pulse dispersion imaging, and real space interferometry. The latter two allow to visualize the collapse of the energy distribution and the long‐range coherence of the polariton condensate.

Valley polarized relaxation and upconversion luminescence from Tamm-plasmon trion–polaritons with a MoSe2 monolayer

Transition metal dichalcogenides represent an ideal testbed to study excitonic effects, spin-related phenomena and fundamental light-matter coupling in nanoscopic condensed matter systems. In particular, the valley degree of freedom, which is unique to such direct band gap monolayers with broken inversion symmetry, adds fundamental interest in these materials. Here, we implement a Tamm-plasmon structure with an embedded MoSe2 monolayer and study the formation of polaritonic quasi-particles. Strong coupling conditions between the Tamm-mode and the trion resonance of MoSe2 are established, yielding bright luminescence from the polaritonic ground state under non-resonant optical excitation. We demonstrate, that tailoring the electrodynamic environment of the monolayer results in a significantly increased valley polarization. This enhancement can be related to change in recombination dynamics shown in time-resolved photoluminescence measurements. We furthermore observe strong upconversion luminescence from resonantly excited polariton states in the lower polariton branch. This upconverted polariton luminescence is shown to preserve the valley polarization of the trion–polariton, which paves the way towards combining spin-valley physics and exciton scattering experiments.

Quantum interference of two photons emitted from a luminescence center in GaAs:N

The indistinguishability of photons emitted from a nitrogen luminescence center in GaAs is investigated by two-photon interference under nonresonant optical excitation. A clear dip is observed in a parallel polarization configuration for consecutively emitted two photons with a 2-ns time interval. The indistinguishability is approximately 0.24, and is found to be independent of the time interval between 2 ns and 4 ns. These results suggest the existence of a very fast dephasing mechanism within 2 ns.

Enhancement of Auger recombination induced by carrier localization in InGaN/GaN quantum wells

The origin of efficiency droop in state-of-the-art quality In GaN/GaN and GaN/AlGaN quantum wells (QWs) grown on various crystal planes is studied by means of time-resolved photoluminescence spectroscopy associated with a precise determination of the QW carrier density. In a first set of experiments, it is shown that a polar InGaN/GaN QW under nonresonant high optical excitation shows clear signatures of Auger loss mechanism and thus behaves quite differently compared to its binary based GaN/AlGaN QW counterpart, where no Auger signature is observed. In order to get rid of the impact of the built-in polarization field and illustrate the dominant role of carrier localization, similar experiments have been conducted on two m-plane In GaN/GaN QWs with similar In composition but a different degree of disorder. We demonstrate that carrier localization strongly enhances the Auger recombination process in nonpolar In GaN/GaN QWs. We also show that this effect may be further amplified by the presence of polarization fields on polar QWs. The relaxation of the k-selection rule during the Auger recombination process, resulting from QW potential disorder, can account for the enhancement of the efficiency droop in In GaN/GaN QWs.

Direct Observation of Ultrafast Exciton Formation in a Monolayer of WSe2.

Many of the fundamental optical and electronic properties of atomically thin transition metal dichalcogenides are dominated by strong Coulomb interactions between electrons and holes, forming tightly bound atom-like states called excitons. Here, we directly trace the ultrafast formation of excitons by monitoring the absolute densities of bound and unbound electron-hole pairs in single monolayers of WSe2 on a diamond substrate following femtosecond nonresonant optical excitation. To this end, phase-locked mid-infrared probe pulses and field-sensitive electro-optic sampling are used to map out the full complex-valued optical conductivity of the nonequilibrium system and to discern the hallmark low-energy responses of bound and unbound pairs. While the spectral shape of the infrared response immediately after above-bandgap injection is dominated by free charge carriers, up to 60% of the electron-hole pairs are bound into excitons already on a subpicosecond time scale, evidencing extremely fast and efficient exciton formation. During the subsequent recombination phase, we still find a large density of free carriers in addition to excitons, indicating a nonequilibrium state of the photoexcited electron-hole system.

Exciton Dipole-Dipole Interaction in a Single Coupled-Quantum-Dot Structure via Polarized Excitation.

We find that the exciton dipole-dipole interaction in a single laterally coupled GaAs/AlGaAs quantum dot structure can be controlled by the linear polarization of a nonresonant optical excitation. When the excitation intensity is increased with the linearly polarized light parallel to the lateral coupling direction [11̅0], excitons (X1 and X2) and local biexcitons (X1X1 and X2X2) of the two separate quantum dots (QD1 and QD2) show a redshift along with coupled biexcitons (X1X2), while neither coupled biexcitons nor a redshift are observed when the polarization of the exciting beam is perpendicular to the coupling direction. The polarization dependence and the redshift are attributed to an optical nonlinearity in the exciton Förster resonant energy transfer interaction, whereby exciton population transfer between the two quantum dots also becomes significant with increasing excitation intensity. We have further distinguished coupled biexcitons from local biexcitons by their large diamagnetic coefficient.

Dynamics of the Lowest-Energy Excitons in Single-Walled Carbon Nanotubes under Resonant and Nonresonant Optical Excitation

The dynamics of lowest-energy E11 excitons in undoped and hole-doped single-walled carbon nanotubes (SWCNTs) are investigated using transient absorption spectroscopy and theoretical calculations. In undoped SWCNT samples, E11 excitons under resonant E11 photoexcitation show faster decay than those under high-energy nonresonant photoexcitation. Doping SWCNTs with holes accelerates the E11 exciton decay through exciton-hole interactions; moreover, both resonant and nonresonant photoexcitation in hole-doped SWCNTs lead to nearly identical decay profiles. Theoretical calculations, which are based on a simple model that accounts for bright, dark, and charged exciton states, agree well with the experimental results. We ascribe the fast E11 exciton decay under the resonant E11 photoexcitation to the redistribution of exciton populations in the E11 bright exciton band, which includes optically accessible and inaccessible states; the rapid exciton redistribution is caused by exciton-hole scattering. Our study prov...

Polariton spin whirls

We report on the observation of spin whirls in a radially expanding polariton condensate formed under non-resonant optical excitation. Real space imaging of polarization- and time-resolved photoluminescence reveal a spiralling polarization pattern in the plane of the microcavity. Simulations of the spatiotemporal dynamics of a spinor condensate reveal the crucial role of polariton interactions with a spinor exciton reservoir. Harnessing spin dependent interactions between the exciton reservoir and polariton condensates allows for the manipulation of spin currents and the realization of dynamic collective spin effects in solid state systems.