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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 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.

We characterize a high-density sample of negatively charged silicon-vacancy (SiV\\(^-\\)) centers in diamond using collinear optical multidimensional coherent spectroscopy. By comparing the results of complementary signal detection schemes, we identify a hidden population of \\ce{SiV^-} 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.

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.

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.

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.

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 tagged with 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 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.

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 WSe2 reveal that these defect-bound excitons exhibit exceptional optical properties including a recombination lifetime approaching 200 ns and a valley lifetime longer than 1 \\(\\mu\\)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.