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S. A. Crooker

Publications and source records attributed to S. A. Crooker.

At least 37 records · Page 2Linked to original sources

Unusual thickness dependence of exciton characteristics in 2D perovskite quantum wells

Understanding the nature and energy distribution of optical resonances is of central importance in low-dimensional materials$^{1-4}$ and its knowledge is critical for designing efficient optoelectronic devices. Ruddlesden-Popper halide perovskites are 2D solution-processed quantum wells with a general formula A$_2$A'$_{n-1}$M$_n$X$_{3n+1}$, where optoelectronic properties can be tuned by varying the perovskite layer thickness (n value), and have recently emerged as efficient semiconductors with technologically relevant stability. However, fundamental questions concerning the nature of optical resonances (excitons or free-carriers) and the exciton reduced mass, and their scaling with quantum well thickness remains unresolved. Here, using optical spectroscopy and 60-Tesla magneto-absorption supported by modelling, we unambiguously demonstrate that the optical resonances arise from tightly bound excitons with unexpectedly high exciton reduced mass (0.20 m0) and binding energies varying from 470 meV to 125 meV with increasing thickness from n=1 to 5. Our work demonstrates the dominant role of Coulomb interactions in 2D solution-processed quantum wells and presents unique opportunities for next-generation optoelectronic and photonic devices.

cond-mat.mtrl-sci↗

Direct Measurements of Magnetic Polarons in Cd$_{1-x}$Mn$_x$Se Nanocrystals from Resonant Photoluminescence

In semiconductors, quantum confinement can greatly enhance the interaction between band carriers (electrons and holes) and dopant atoms. One manifestation of this enhancement is the increased stability of exciton magnetic polarons in magnetically-doped nanostructures. In the limit of very strong 0D confinement that is realized in colloidal semiconductor nanocrystals, a single exciton can exert an effective exchange field $B_{\rm{ex}}$ on the embedded magnetic dopants that exceeds several tesla. Here we use the very sensitive method of resonant photoluminescence (PL) to directly measure the presence and properties of exciton magnetic polarons in colloidal Cd$_{1-x}$Mn$_x$Se nanocrystals. Despite small Mn$^{2+}$ concentrations ($x$=0.4-1.6\%), large polaron binding energies up to $\sim$26~meV are observed at low temperatures via the substantial Stokes shift between the pump laser and the resonant PL maximum, indicating nearly complete alignment of all Mn$^{2+}$ spins by $B_{\rm{ex}}$. Temperature and magnetic field-dependent studies reveal that $B_{\rm{ex}} \approx$ 10~T in these nanocrystals, in good agreement with theoretical estimates. Further, the emission linewidths provide direct insight into the statistical fluctuations of the Mn$^{2+}$ spins. These resonant PL studies provide detailed insight into collective magnetic phenomena, especially in lightly-doped nanocrystals where conventional techniques such as nonresonant PL or time-resolved PL provide ambiguous results.

cond-mat.mes-hall↗

Gate controlled spin-valley locking of resident carriers in WSe2 monolayers

Using time-resolved Kerr rotation, we measure the spin/valley dynamics of resident electrons and holes in single charge-tunable monolayers of the archetypal transition-metal dichalcogenide (TMD) semiconductor WSe2. In the n-type regime, we observe long (70 ns) polarization relaxation of electrons that is sensitive to in-plane magnetic fields $B_y$, indicating spin relaxation. In marked contrast, extraordinarily long (2 microsecond) polarization relaxation of holes is revealed in the p-type regime, that is unaffected by $B_y$, directly confirming long-standing expectations of strong spin-valley locking of holes in the valence band of monolayer TMDs. Supported by continuous-wave Kerr spectroscopy and Hanle measurements, these studies provide a unified picture of carrier polarization dynamics in monolayer TMDs, which can guide design principles for future valleytronic devices.

cond-mat.mes-hall↗

Higher order spin noise spectroscopy of atomic spins in fluctuating external fields

We discuss the effect of external noisy magnetic fields on mesoscopic spin fluctuations that can be probed in semiconductors and atomic vapors by means of optical spin noise spectroscopy (SNS). We show that conventional arguments of the law of large numbers do not apply to spin correlations induced by external fields, namely, the magnitude of the 4th order spin cumulant grows as $\sim N^2$ with the number $N$ of observed spins, i.e. it is not suppressed in comparison to the 2nd order cumulant. This allows us to design a simple experiment to measure the 4th order cumulant of spin fluctuations in an atomic system near thermodynamic equilibrium and develop quantitative theory that explains all observations.

cond-mat.mes-hall↗

Spectrally-resolved hyperfine interactions between polaron and nuclear spins in organic light emitting diodes: Magneto-EL studies

We use spectrally-resolved magneto-electroluminescence (EL) measurements to study the energy dependence of hyperfine interactions between polaron and nuclear spins in organic LEDs. Using layered devices based on Bphen/MTDATA -- a well-known exciplex emitter -- we show that the increase in EL emission intensity $I$ due to small applied magnetic fields of order 100 mT is markedly larger at the high-energy blue end of the EL spectrum (dI/I ~11%) than at the low-energy red end (~4%). Concurrently, the widths of the magneto-EL curves increase monotonically from blue to red, revealing an increasing hyperfine coupling between polarons and nuclei and directly providing insight into the energy-dependent spatial extent and localization of polarons.

cond-mat.mtrl-sci↗

Revealing Optically Induced Magnetization in SrTiO$_3$ using Optically Coupled SQUID Magnetometry and Magnetic Circular Dichroism

In this work, we study the time- and temperature-dependence of optically induced magnetization in bulk crystals of slightly oxygen-deficient SrTiO$_{3-δ}$ using an optically coupled SQUID magnetometer. We find that a weak ($\sim$5$\times$10$^{-7}$~emu) but extremely long-lived (hours) magnetic moment can be induced in SrTiO$_{3-δ}$ at zero magnetic field by circular-polarized sub-bandgap light. We utilize this effect to demonstrate that SrTiO$_{3-δ}$ crystals can be used as an optically addressable magnetic memory by writing and subsequently reading magnetic patterns with light. The induced magnetization is consistent with that of a polarized ensemble of independent oxygen-vacancy-related complexes, rather than from collective or long-range magnetic order.

cond-mat.mtrl-sci↗

Two-color spin noise spectroscopy: Using spin fluctuation correlations to reveal homogeneous linewidths within quantum dot ensembles

"Spin noise spectroscopy" (SNS) is a powerful optical technique for probing electron and hole spin dynamics that is based on detecting their intrinsic and random fluctuations while in thermal equilibrium, an approach guaranteed by the fluctuation-dissipation theorem. Because SNS measures fluctuation properties rather than conventional response functions, we show that fluctuation \emph{correlations} can be exploited in multi-probe noise studies to reveal information that in general cannot be accessed by conventional linear optical spectroscopy, such as the underlying homogeneous linewidths of individual constituents within inhomogeneously-broadened systems. This is demonstrated in an ensemble of singly-charged (In,Ga)As quantum dots using two weak probe lasers: When the two lasers have the same wavelength, they are sensitive to the same QDs in the ensemble and their spin fluctuation signals are correlated. In contrast, two probe lasers that are widely detuned from each other measure different subsets of QDs, leading to uncorrelated fluctuations. Measuring the noise correlation versus laser detuning directly reveals the QD homogeneous linewidth even in the presence of a strong inhomogeneous broadening. Such noise-based correlation techniques are not limited to semiconductor spin systems, but can be widely applied to any system in which intrinsic fluctuations are measurable.

cond-mat.mes-hall↗

Spin noise spectroscopy beyond thermal equilibrium and linear response

Per the fluctuation-dissipation theorem, the information obtained from spin fluctuation studies in thermal equilibrium is necessarily constrained by the system's linear response functions. However, by including weak radiofrequency magnetic fields, we demonstrate that intrinsic and random spin fluctuations even in strictly unpolarized ensembles \emph{can} reveal underlying patterns of correlation and coupling beyond linear response, and can be used to study non-equilibrium and even multiphoton coherent spin phenomena. We demonstrate this capability in a classical vapor of $^{41}$K alkali atoms, where spin fluctuations alone directly reveal Rabi splittings, the formation of Mollow triplets and Autler-Townes doublets, ac Zeeman shifts, and even nonlinear multiphoton coherences.

physics.atom-ph↗

Persistent Optically Induced Magnetism in Oxygen-Deficient Strontium Titanate

Strontium titanate (SrTiO$_3$) is a foundational material in the emerging field of complex oxide electronics. While its electronic and optical properties have been studied for decades, SrTiO$_3$ has recently become a renewed materials research focus catalyzed in part by the discovery of magnetism and superconductivity at interfaces between SrTiO$_3$ and other oxides. The formation and distribution of oxygen vacancies may play an essential but as-yet-incompletely understood role in these effects. Moreover, recent signatures of magnetization in gated SrTiO$_3$ have further galvanized interest in the emergent properties of this nominally nonmagnetic material. Here we observe an optically induced and persistent magnetization in oxygen-deficient SrTiO$_{3-δ}$ using magnetic circular dichroism (MCD) spectroscopy and SQUID magnetometry. This zero-field magnetization appears below ~18K, persists for hours below 10K, and is tunable via the polarization and wavelength of sub-bandgap (400-500nm) light. These effects occur only in oxygen-deficient samples, revealing the detailed interplay between magnetism, lattice defects, and light in an archetypal oxide material.

cond-mat.mes-hall↗

Role of Nuclear Quadrupole Coupling on Decoherence and Relaxation of Central Spins in Quantum Dots

Strain-induced gradients of local electric fields in semiconductor quantum dots can couple to the quadrupole moments of nuclear spins. We develop a theory describing the influence of this quadrupolar coupling (QC) on the spin correlators of electron and hole "central" spins localized in such dots. We show that when the QC strength is comparable to or larger than the hyperfine coupling strength between nuclei and the central spin, the relaxation rate of the central spin is strongly enhanced and can be exponential. We demonstrate a good agreement with recent experiments on spin relaxation in hole-doped (In,Ga)As self-assembled quantum dots.

cond-mat.mes-hall↗

A cascade of magnetic field induced spin transitions in LaCoO3

We present magnetization and magnetostriction studies of the insulating perovskite LaCoO3 in magnetic fields approaching 100 T. In marked contrast with expectations from single-ion models, the data reveal two distinct first-order spin transitions and well-defined magnetization plateaux. The magnetization at the higher plateau is only about half the saturation value expected for spin-1 Co3+ ions. These findings strongly suggest collective behavior induced by strong interactions between different electronic -- and therefore spin -- configurations of Co3+ ions. We propose a model of these interactions that predicts crystalline spin textures and a cascade of four magnetic phase transitions at high fields, of which the first two account for the experimental data.

cond-mat.str-el↗

Intrinsic spin fluctuations reveal the dynamical response function of holes coupled to nuclear spin baths in (In,Ga)As quantum dots

The problem of how single "central" spins interact with a nuclear spin bath is essential for understanding decoherence and relaxation in many quantum systems, yet is highly nontrivial owing to the many-body couplings involved. Different models yield widely varying timescales and dynamical responses (exponential, power-law, Gaussian, etc). Here we detect the small random fluctuations of central spins in thermal equilibrium (holes in singly-charged (In,Ga)As quantum dots) to reveal the timescales and functional form of bath-induced spin relaxation. This spin noise indicates long (400 ns) spin correlation times at zero magnetic field, that increase to $\sim$5 $μ$s as hole-nuclear coupling is suppressed with small (100 G) applied fields. Concomitantly, the noise lineshape evolves from Lorentzian to power-law, indicating a crossover from exponential to inverse-log dynamics.

cond-mat.mes-hall↗

Circular-Polarization Dependent Cyclotron Resonance in Large-Area Graphene in Ultrahigh Magnetic Fields

Using ultrahigh magnetic fields up to 170 T and polarized midinfrared radiation with tunable wavelengths from 9.22 to 10.67 um, we studied cyclotron resonance in large-area graphene grown by chemical vapor deposition. Circular-polarization dependent studies reveal strong p-type doping for as-grown graphene, and the dependence of the cyclotron resonance on radiation wavelength allows for a determination of the Fermi energy. Thermal annealing shifts the Fermi energy to near the Dirac point, resulting in the simultaneous appearance of hole and electron cyclotron resonance in the magnetic quantum limit, even though the sample is still p-type, due to graphene's linear dispersion and unique Landau level structure. These high-field studies therefore allow for a clear identification of cyclotron resonance features in large-area, low-mobility graphene samples.

cond-mat.mes-hall↗

Spin-polarized Mn$^{2+}$ emission from Manganese-doped colloidal nanocrystals

We report magneto-photoluminescence studies of strongly quantum-confined "0-D" diluted magnetic semiconductors (DMS), realized in Mn$^{2+}$-doped ZnSe/CdSe core/shell colloidal nanocrystals. In marked contrast to their 3-D (bulk), 2-D (quantum well), 1-D (quantum wire), and 0-D (self-assembled quantum dot) DMS counterparts, the ubiquitous yellow emission band from internal \emph{d-d} ($^4T_1 \rightarrow ^6A_1$) transitions of the Mn$^{2+}$ ions in these nanocrystals is \emph{not} suppressed in applied magnetic fields and \emph{does} become circularly polarized. This polarization tracks the Mn$^{2+}$ magnetization, and is accompanied by a sizable energy splitting between right- and left-circular emission components that scales with the exciton-Mn \emph{sp-d} coupling strength (which, in turn, is tunable with nanocrystal size). These data highlight the influence of strong quantum confinement on both the excitation and the emission mechanisms of magnetic ions in DMS nano-materials.

cond-mat.mes-hall↗

Revealing the Exciton Fine Structure in PbSe Nanocrystal Quantum Dots

We measure the photoluminescence (PL) lifetime, $τ$, of excitons in colloidal PbSe nanocrystals (NCs) at low temperatures to 270~mK and in high magnetic fields to 15~T. For all NCs (1.3-2.3~nm radii), $τ$ increases sharply below 10~K but saturates by 500~mK. In contrast to the usual picture of well-separated ``bright" and ``dark" exciton states (found, e.g., in CdSe NCs), these dynamics fit remarkably well to a system having two exciton states with comparable - but small - oscillator strengths that are separated by only 300-900 $μ$eV. Importantly, magnetic fields reduce $τ$ below 10~K, consistent with field-induced mixing between the two states. Magnetic circular dichroism studies reveal exciton g-factors from 2-5, and magneto-PL shows $>$10\% circularly polarized emission.

cond-mat.mes-hall↗

"Listening" to the spin noise of conduction electrons in bulk n:GaAs

We report a comprehensive study of stochastic electron spin fluctuations -- spin noise -- in lightly doped ($n$-type) bulk GaAs, which are measured using sensitive optical magnetometry based on off-resonant Faraday rotation. Frequency spectra of electron spin noise are studied as a function of electron density, magnetic field, temperature, probe laser wavelength and intensity, and interaction volume. Electron spin lifetimes $τ_s$ are inferred from the width of the spin noise spectra, and are compared with direct measurements of $τ_s$ using conventional Hanle effect methods. Both methods reveal a strong and similar dependence of $τ_s$ on the wavelength and intensity of the probe laser, highlighting the undesired influence of sub-bandgap absorption effects on the nominally `non-perturbative' spin noise measurements. As a function of temperature, the spin noise power increases approximately linearly from 1.5 K to 30 K, as expected for degenerate electrons obeying Fermi-Dirac statistics, but with an additional zero-temperature offset. Finally, as the cross-sectional area of the probe laser shrinks and fewer electrons are probed, the measured Faraday rotation fluctuations due to electron spin noise are shown to increase, as expected.

cond-mat.mes-hall↗

Spin noise of electrons and holes in self-assembled quantum dots

We measure the frequency spectra of random spin fluctuations, or "spin noise", in ensembles of (In,Ga)As/GaAs quantum dots (QDs) at low temperatures. We employ a spin noise spectrometer based on a sensitive optical Faraday rotation magnetometer that is coupled to a digitizer and field-programmable gate array, to measure and average noise spectra from 0-1 GHz continuously in real time with sub-nanoradian/root-Hz sensitivity. Both electron and hole spin fluctuations generate distinct noise peaks, whose shift and broadening with magnetic field directly reveal their g-factors and dephasing rates within the ensemble. A large, energy-dependent anisotropy of the in-plane hole g-factor is clearly exposed, reflecting systematic variations in the average QD confinement potential.

cond-mat.mes-hall↗

Bias-controlled sensitivity of ferromagnet/semiconductor electrical spin detectors

Using Fe/GaAs Schottky tunnel barriers as electrical spin detectors, we show that the magnitude and sign of their spin-detection sensitivities can be widely tuned with the voltage bias applied across the Fe/GaAs interface. Experiments and theory establish that this tunability derives not just simply from the bias dependence of the tunneling conductances $G_{\uparrow,\downarrow}$ (a property of the interface), but also from the bias dependence of electric fields in the semiconductor which can dramatically enhance or suppress spin-detection sensitivities. Electrons in GaAs with fixed polarization can therefore be made to induce either positive or negative voltage changes at spin detectors, and some detector sensitivities can be enhanced over ten-fold compared to the usual case of zero-bias spin detection.

cond-mat.mtrl-sci↗