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We demonstrate modulation of the light scattered from a quantum emitter enhanced by surface acoustic wave cavities etched into the surface of GaAs, with the half-wave voltage V π as low as 44 mV.

We demonstrate etched-groove surface acoustic wave cavities on gallium arsenide with finesses reaching 100. These cavities can be used to enhance coupling between phonons and different quantum systems, providing a platform for quantum transduction.

We investigate the exciton exchange interaction of erbium doped GaAs quantum well using MDCS. We observe an energy shift of ~100µeV consistent with the predicted exchange energy and different pulse sequences activate specific excitonic pathways.

We demonstrate focusing cavities of surface acoustic waves on gallium arsenide with quality factors reaching 20,000. These cavities can potentially enhance coupling of surface phonons to a wide variety of quantum systems, possibly enabling efficient quantum transduction.

As optical two-dimensional coherent spectroscopy (2DCS) is extended to a broader range of applications, it is critical to improve the detection sensitivity of optical 2DCS. We developed a fast phase-cycling scheme in a non-collinear optical 2DCS implementation by using liquid crystal phase retarders to modulate the phases of two excitation pulses. The background in the signal can be eliminated by combining either two or four interferograms measured with a proper phase configuration. The effectiveness of this method was validated in optical 2DCS measurements of an atomic vapor. This fast phase-cycling scheme will enable optical 2DCS in novel emerging applications that require enhanced detection sensitivity., 4 pages, 3 figures, 1 table

Multidimensional coherent spectroscopy directly unravels multiply excited states that overlap in a linear spectrum. We report multidimensional coherent optical photocurrent spectroscopy in a semiconductor polariton diode and explore the excitation ladder of cavity polaritons. We measure doubly and triply avoided crossings for pairs and triplets of exciton polaritons, demonstrating the strong coupling between light and dressed doublet and triplet semiconductor excitations. These results demonstrate that multiply excited excitonic states strongly coupled to a microcavity can be described as two coupled quantum-anharmonic ladders.

Improvements in temporal resolution of single-photon detectors enable increased data rates and transmission distances for both classical and quantum optical communication systems, higher spatial resolution in laser ranging, and observation of shorter-lived fluorophores in biomedical imaging. In recent years, superconducting nanowire single-photon detectors (SNSPDs) have emerged as the most efficient time-resolving single-photon-counting detectors available in the near-infrared, but understanding of the fundamental limits of timing resolution in these devices has been limited due to a lack of investigations into the timescales involved in the detection process. We introduce an experimental technique to probe the detection latency in SNSPDs and show that the key to achieving low timing jitter is the use of materials with low latency. By using a specialized niobium nitride SNSPD we demonstrate that the system temporal resolution can be as good as 2.6 ± 0.2 ps for visible wavelengths and 4.3 ± 0.2 ps at 1,550 nm. Knowledge about detection latency provides a guideline to reduce the timing jitter of niobium nitride superconducting nanowire single-photon detectors. A timing jitter of 2.6 ps at visible wavelength and 4.3 ps at 1,550 nm is achieved.

We use two coherent spectroscopy techniques to measure the strain tensor local to an ensemble of silicon-vacancy centers in diamond. Our results provide a possible pathway for using diamond as a tensorial strain gauge.

We demonstrate progress in developing a new microwave-optical quantum transducer. We demonstrate focusing and stable surface acoustic wave cavities at 3.4 GHz and characterize the acoustic performance. This work is a contribution of the National Institute of Standards and Technology; not subject to copyright in the United States of America.

We characterize a high-density sample of negatively charged silicon-vacancy (${\mathrm{SiV}}^{\ensuremath{-}}$) centers in diamond using collinear optical multidimensional coherent spectroscopy. By comparing the results of complementary signal detection schemes, we identify a hidden population of ${\mathrm{SiV}}^{\ensuremath{-}}$ centers that is not typically observed in photoluminescence and which exhibits significant spectral inhomogeneity and extended electronic ${T}_{2}$ times. The phenomenon is likely caused by strain, indicating a potential mechanism for controlling electric coherence in color-center-based quantum devices.

In atomically thin two-dimensional semiconductors such as transition metal dichalcogenides (TMDs), controlling the density and type of defects promises to be an effective approach for engineering light-matter interactions. We demonstrate that electron-beam irradiation is a simple tool for selectively introducing defect-bound exciton states associated with chalcogen vacancies in TMDs. Our first-principles calculations and time-resolved spectroscopy measurements of monolayer ${\mathrm{WSe}}_{2}$ reveal that these defect-bound excitons exhibit exceptional optical properties including a recombination lifetime approaching 200 ns and a valley lifetime longer than $1\text{ }\text{ }\ensuremath{\mu}\mathrm{s}$. The ability to engineer the crystal lattice through electron irradiation provides a new approach for tailoring the optical response of TMDs for photonics, quantum optics, and valleytronics applications.

Multidimensional coherent spectroscopy measurements of SiV− centers in diamond reveal a previously unexamined population of silicon-based defect states, which are not detected in photoluminescence and which exhibit a substantial degree of inhomogeneous broadening.

We present an ultrafast coherent spectroscopy data acquisition scheme that samples slices of the time domain used in multidimensional coherent spectroscopy to achieve faster data collection than full spectra. We derive analytical expressions for resonance lineshapes using this technique that completely separate homogeneous and inhomogeneous broadening contributions into separate projected lineshapes for arbitrary inhomogeneous broadening. These lineshape expressions are also valid for slices taken from full multidimensional spectra and allow direct measurement of the parameters contributing to the lineshapes in those spectra as well as our own.

We demonstrate a new method for multidimensional coherent spectroscopy of nanostructures. We use a heterodyne technique implemented with a confocal microscope to record the amplitude and phase of all degenerate third-order wave-mixing processes.

Multidimensional coherent spectroscopy is a powerful tool for understanding the ultrafast dynamics of complex quantum systems. To fully characterize the nonlinear optical response of a system, multiple pulse sequences must be recorded and quantitatively compared. We present a new single-scan method that enables rapid and parallel acquisition of all unique pulse sequences corresponding to first- and third-order degenerate wave-mixing processes. Signals are recorded with shot-noise limited detection, enabling acquisition times of ∼2 minutes with ∼100 zs phase stability and ∼8 orders of dynamic range, in a collinear geometry, on a single-pixel detector. We demonstrate this method using quantum well excitons, and quantitative analysis reveals new insights into the bosonic nature of excitons. This scheme may enable rapid and scalable analysis of unique chemical signatures, metrology of optical susceptibilities, nonperturbative coherent control, and the implementation of quantum information protocols using multidimensional spectroscopy.

The exciton coherent signal decay rate in GaAs quantum wells, as measured in four-wave mixing experiments, depends on the polarization of the excitation pulses. Using polarization-dependent two-dimensional coherent spectroscopy, we show that this behavior is due to the bosonic character of excitons. Interference between two different quantum mechanical pathways results in a smaller decay rate for cocircular and colinear polarization of the optical excitation pulses. This interference does not exist for cross-linearly polarized excitation pulses resulting in a larger decay rate. Our result shows that the bosonic nature of excitons must be considered when interpreting ultrafast spectroscopic studies of exciton dephasing in semiconductors. This behavior should be considered while interpreting results of ultrafast spectroscopy experiments involving bosonlike excitations.

The emergence of spatially indirect excitons is observed in asymmetric InGaAs/GaAs double quantum well heterostructures via optical multidimensional coherent spectroscopy. Origins of coupling between wells include many-body effects and electron tunneling.

Light-matter coupling in a cavity results in a ladder of states with splittings determined by the coupling strength. We observe the higher ladder rungs in a semiconductor microcavity using multiquantum coherent optical photocurrent spectroscopy.

We have quantified excitonic many-body interaction energies in GaAs quantum wells using two-dimensional coherent spectroscopy. The anharmonic oscillator model for excitons is used to extract the inter- and intra-mode interaction energies from 2D spectra.

We present perturbative analytical solutions to the optical Bloch equations at third order, with finite duration Gaussian pulse envelopes. We find that a given double-sided Feynman diagram in this approximation can be conveniently described in the frequency domain as a product of the expression in the impulsive limit and a finite-pulse factor. Finite-pulse effects are Feynman-diagram-dependent, however, and include nontrivial phase corrections that can occur even in the case of transform-limited pulses. The results constitute a practical framework for modeling phenomena in multidimensional coherent spectroscopy that cannot easily be captured in the impulsive limit, including the roles of bandwidth, resonance, and pulse chirp.

We present a new technique for Multi-Dimensional Coherent spectroscopy of nano-structures. We measure the Four-Wave Mixing (FWM) amplitude and phase via photocurrent detection. The measurement is suitable for any nano-structures that can be electrically contacted.

Our recent work on optical two-dimensional coherent spectroscopy (2DCS) of semiconductor materials is reviewed. We present and compare two approaches that are appropriate for the study of semiconductor nanostructures. The first one is based on a non-collinear geometry, where the Four-Wave-Mixing (FWM) signal is detected in the form of a radiated optical field. This approach works for samples with translational symmetry, such as Quantum Wells (QWs), or large and dense ensembles of Quantum Dots (QDs). The second method is based on a collinear geometry, where the FWM is detected in the form of a photocurrent. This second approach enables 2DCS of samples where translational symmetry is broken, such as single QDs, nanowires, or nanotubes, and small ensembles thereof. For each method, we provide an example of experimental results obtained on semiconductor QWs. In particular, it is shown how 2DCS can reveal coherent excitonic coupling between adjacent QWs.

We study an asymmetric double InGaAs quantum well using optical two-dimensional coherent spectroscopy. The collection of zero-quantum, one-quantum, and two-quantum two-dimensional spectra provides a unique and comprehensive picture of the double well coherent optical response. Coherent and incoherent contributions to the coupling between the two quantum well excitons are clearly separated. An excellent agreement with density matrix calculations reveals that coherent interwell coupling originates from many-body interactions.

The homogeneous and inhomogeneous linewidths of the heavy-hole exciton resonance in a (110)-oriented GaAs multiple-quantum-well sample are measured using optical two-dimensional Fourier transform spectroscopy. By probing the optical nonlinear response for polarization along the in-plane crystal axes [1$\overline{1}$0] and [001], we measure different homogeneous linewidths for the two orthogonal directions. This difference is found to be due to anisotropic excitation-induced dephasing, caused by a crystal-axis-dependent absorption coefficient. The extrapolated zero-excitation density homogeneous linewidth exhibits an activation-like temperature dependence. We find that the homogeneous linewidth extrapolated to zero excitation density and temperature is $\ensuremath{\sim}$34 $\ensuremath{\mu}$eV, while the inhomogeneous linewidth is $\ensuremath{\sim}$1.9 meV for both polarizations.

Multidimensional Coherent Optical Photocurrent Spectroscopy (MD-COPS) is implemented using unstabilized interferometers. Photocurrent from a semiconductor sample is generated using a sequence of four excitation pulses in a collinear geometry. Each pulse is frequency shifted by a unique radio frequency through acousto-optical modulation; the Four-Wave Mixing (FWM) signal is then selected in the frequency domain. The interference of an auxiliary continuous wave laser, which is sent through the same interferometers as the excitation pulses, is used to synthesize reference frequencies for lock-in detection of the photocurrent FWM signal. This scheme enables the partial compensation of mechanical fluctuations in the setup, achieving sufficient phase stability without the need for active stabilization. The method intrinsically provides both the real and imaginary parts of the FWM signal as a function of inter-pulse delays. This signal is subsequently Fourier transformed to create a multi-dimensional spectrum. Measurements made on the excitonic resonance in a double InGaAs quantum well embedded in a p-i-n diode demonstrate the technique.

We study asymmetric double InGaAs quantum well samples, featuring three different barrier widths, using optical two-dimensional Fourier transform spectroscopy. Depending on the barrier width, we observe different coupling mechanisms between the two wells.

Coherent excitonic interactions in an InGaAs asymmetric double quantum well are studied using two-dimensional coherent spectroscopy. Density matrix calculations reveal that an excitation-induced shift is the dominant many-body interaction responsible for the coupling.

We report crystal-axis dependent homogeneous linewidths of the heavy hole exciton resonance in a (110)-oriented GaAs quantum well measured using two-dimensional Fourier transform spectroscopy. The increase in homogeneous linewidth with temperature shows an activation-like behavior.

We review our recent work on multi-dimensional coherent optical spectroscopy (MDCS) of semiconductor nanostructures. Two approaches, appropriate for the study of semiconductor materials, are presented and compared. A first method is based on a non-collinear geometry, where the Four-Wave-Mixing (FWM) signal is detected in the form of a radiated optical field. This approach works for samples with translational symmetry, such as Quantum Wells (QWs) or large and dense ensembles of Quantum Dots (QDs). A second method detects the FWM in the form of a photocurrent in a collinear geometry. This second approach extends the horizon of MDCS to sub-diffraction nanostructures, such as single QDs, nanowires, or nanotubes, and small ensembles thereof. Examples of experimental results obtained on semiconductor QW structures are given for each method. In particular, it is shown how MDCS can assess coupling between excitons confined in separated QWs.