arXiv subjects

Steven T. Cundiff

Publications and source records attributed to Steven T. Cundiff.

At least 37 records · Page 2Linked to original sources

arXiv2020

Fast phase cycling in non-collinear optical two-dimensional coherent spectroscopy

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.

physics.optics↗

arXiv2020

Radio frequency polarization modulation based on an optical frequency comb

We propose a method to generate stabilized radio-frequency polarization modulation based on optical frequency combs. Two pulse trains with the same repetition rate and different offset frequencies generate arbitrary polarization states that are modulated at the offset frequency difference. Long-term stability of the polarization modulation is demonstrated with the modulation frequency at frep/2. Modulation at frep/4 is also demonstrated to show the flexibility of the technique. We employ an electrical delay line to fine-tune the polarization states that constitute the time-dependent modulation.

physics.optics↗

arXiv2020

Quantum-Well Laser Diodes for Frequency Comb Spectroscopy

We demonstrate simple optical frequency combs based on semiconductor quantum well laser diodes. The frequency comb spectrum can be tailored by choice of material properties and quantum-well widths, providing spectral flexibility. Finally, we demonstrate the mutual coherence of these devices by using two frequency combs on the same device to generate a radio-frequency dual comb spectrum.

physics.optics↗

arXiv2020

Spectroscopic Signatures of Electron-Phonon Coupling in Silicon-Vacancy Centers in Diamond

Vacancy centers in diamond have proven to be a viable solid-state platform for quantum coherent opto-electronic applications. Among the variety of vacancy centers, silicon-vacancy (SiV) centers have recently attracted much attention as an inversion-symmetric system that is less susceptible to electron-phonon interactions. Nevertheless, phonon-mediated processes still degrade the coherent properties of SiV centers, however characterizing their electron-phonon coupling is extremely challenging due to their weak spectroscopic signatures and remains an open experimental problem. In this paper we theoretically investigate signatures of electron-phonon coupling in simulated linear and nonlinear spectra of SiV centers. We demonstrate how even extremely weak electron-phonon interactions, such as in SiV centers, may be completely characterized via nonlinear spectroscopic techniques and even resolved between different fine-structure transitions.

cond-mat.mtrl-sci↗

arXiv2020

Partially-Bright Triplet Excitons in Perovskite Nanocrystals

Advances in opto-electronics require the development of materials with novel and engineered characteristics. A class of materials that has garnered tremendous interest is metal-halide perovskites, stimulated by meteoric increases in photovoltaic efficiencies of perovskite solar cells. In addition, recent advances have applied perovskite nanocrystals (NCs) in light-emitting devices. It was discovered recently that, for cesium lead-halide perovskite NCs, their unusually efficient light-emission may be due to a unique excitonic fine-structure composed of three bright triplet states that minimally interact with a proximal dark singlet state. To study this fine-structure without isolating single NCs, we use multi-dimensional coherent spectroscopy at cryogenic temperatures to reveal coherences involving triplet states of a CsPbI$_3$ NC ensemble. Picosecond timescale dephasing times are measured for both triplet and inter-triplet coherences, from which we infer a unique exciton fine-structure level-ordering comprised of a dark state energetically positioned within the bright triplet manifold.

cond-mat.mtrl-sci↗

arXiv2019

Effect of Dimensionality on the Optical Absorption Properties of CsPbI$_3$ Perovskite Nanocrystals

The band-gaps of CsPbI$_3$ perovskite nanocrystals are measured by absorption spectroscopy at cryogenic temperatures. Anomalous band-gap shifts are observed in CsPbI$_3$ nanocubes and nanoplatelets, which are modeled accurately by band-gap renormalization due to lattice vibrational modes. We find that decreasing dimensionality of the CsPbI$_3$ lattice in nanoplatelets greatly reduces electron-phonon coupling, and dominant out-of-plane quantum confinement results in a homogeneously broadened absorption lineshape down to cryogenic temperatures. An absorption tail forms at low-temperatures in CsPbI$_3$ nanocubes, which we attribute to shallow defect states positioned near the valence band-edge.

physics.app-ph↗

arXiv2019

Perfect absorption by an atomically thin crystal

Optical absorption is one of fundamental light-matter interactions. In most materials, optical absorption is a weak perturbation to the light. In this regime, absorption and emission are irreversible, incoherent processes due to strong damping. Excitons in monolayer transition metal dichalcogenides, however, interact strongly with light, leading to optical absorption in the non-perturbative regime where coherent re-emission of the light has to be considered. Between the incoherent and coherent limits, we show that a robust critical coupling condition exists, leading to perfect optical absorption. Up to 99.6% absorption is measured in a sub-nanometer thick MoSe2 monolayer placed in front of a mirror. The perfect absorption is controlled by tuning the exciton-phonon, exciton-exciton, and exciton-photon interactions by temperature, pulsed laser excitation, and a movable mirror, respectively. Our work suggests unprecedented opportunities for engineering exciton-light interactions using two-dimensional atomically thin crystals, enabling novel photonic applications including ultrafast light modulators and sensitive optical sensing.

cond-mat.mtrl-sci↗

arXiv2019

Simultaneous Existence of Confined and Delocalized Vibrational Modes in Colloidal Quantum Dots

Coupling to phonon modes is a primary mechanism of excitonic dephasing and energy loss in semiconductors. However, low-energy phonons in colloidal quantum dots and their coupling to excitons are poorly understood, since their experimental signatures are weak and usually obscured by unavoidable inhomogeneous broadening of colloidal dot ensembles. We use multi-dimensional coherent spectroscopy at cryogenic temperatures to extract the homogeneous nonlinear optical response of excitons in a CdSe/CdZnS core/shell colloidal quantum dot ensemble. Comparison to simulation provides evidence that the observed lineshapes arise from the co-existence of confined and delocalized vibrational modes, both of which couple strongly to excitons in CdSe/CdZnS colloidal quantum dots.

cond-mat.mes-hall↗

arXiv2019

Frequency comb generation at 800nm in waveguide array quantum well diode lasers

A traveling wave model for a semiconductor diode laser based on quantum wells is presented as well as a comprehensive theoretical model of the lasing dynamics produced by the intensity discrimination of the nonlinear mode-coupling in a waveguide array. By leveraging a recently developed model for the detailed semiconductor gain dynamics, the temporal shaping effects of the nonlinear mode-coupling induced by the waveguide arrays can be characterized. Specifically, the enhanced nonlinear pulse shaping provided by the waveguides are capable of generating stable frequency combs wavelength of 800 nm in a GaAs device, a parameter regime not feasible for stable combline generation using a single waveguide. Extensive numerical simulations showed that stable waveform generation could be achieved and optimized by an appropriate choice of the linear waveguide coupling coefficient, quantum well depth, and the input currents to the first and second waveguides. The model provides a first demonstration that a compact, efficient and robust on-chip comb source can be produced in GaAs.

physics.optics↗

arXiv2019

Stable Numerical Schemes for Nonlinear Dispersive Equations with Counter-Propagation and Gain Dynamics

We develop a stable and efficient numerical scheme for modeling the optical field evolution in a nonlinear dispersive cavity with counter propagating waves and complex, semiconductor physics gain dynamics that are expensive to evaluate. Our stability analysis is characterized by a von-Neumann analysis which shows that many standard numerical schemes are unstable due to competing physical effects in the propagation equations. We show that the combination of a predictor-corrector scheme with an operator-splitting not only results in a stable scheme, but provides a highly efficient, single-stage evaluation of the gain dynamics. Given that the gain dynamics is the rate-limiting step of the algorithm, our method circumvents the numerical instability induced by the other cavity physics when evaluating the gain in an efficient manner. We demonstrate the stability and efficiency of the algorithm on a diode laser model which includes three waveguides and semiconductor gain dynamics. The laser is able to produce a repeating temporal waveform and stable optical comblines, thus demonstrating that frequency combs generation may be possible in chip scale, diode lasers.

physics.optics↗

arXiv2018

Encapsulation Narrows Excitonic Homogeneous Linewidth of Exfoliated MoSe$_2$ Monolayer

The excitonic homogeneous linewidth of an exfoliated monolayer MoSe$_2$ encapsulated in hexagonal boron nitride is directly measured using multidimensional coherent spectroscopy with micron spatial resolution. The linewidth is 0.26 $\pm$ 0.02 meV, corresponding to a dephasing time $T_2 \approx$ 2.5 ps, which is almost half the narrowest reported values for non-encapsulated MoSe$_2$ flakes. We attribute the narrowed linewidth to Coulomb screening by the encapsulated material and suppression of non-radiative processes. Through direct measurements of encapsulated and non-encapsulated monolayers, we confirm that encapsulation reduces the sample inhomogeneity. However, linewidths measured using photoluminescence and linear absorption remain dominated by inhomogeneity, and these linewidths are roughly 5 times larger than the homogeneous linewidth in even the highest-quality encapsulated materials. The homogeneous linewidth of non-encapsulated monolayers is very sensitive to temperature cycling, whereas encapsulated samples are not modified by temperature cycling. The nonlinear signal intensity of non-encapsulated monolayers is degraded by high-power optical excitation, whereas encapsulated samples are very resilient to optical excitation with optical powers up to the point of completely bleaching the exciton.

cond-mat.mtrl-sci↗

arXiv2018

Tri-comb spectroscopy

Multi-dimensional coherent spectroscopy (MDCS)1,2 is a powerful method for optical spectroscopy that has become an important tool for studying ultrafast dynamics in a wide range of systems. It is an optical analog of multidimensional nuclear magnetic resonance spectroscopy that enables the measurement of homogeneous linewidths in inhomogeneously broadened systems, many-body interactions, and coupling between excited resonances, all of which are not simultaneously accessible by any other linear or non-linear method. Current implementations of MDCS require a bulky apparatus and suffer from resolution and acquisition speed limitations that constrain their applications outside the laboratory3-5. Here we propose and demonstrate an approach to nonlinear coherent spectroscopy that utilizes three frequency combs with slightly different repetition rates. Unlike traditional nonlinear methods, tri-comb spectroscopy uses only a single photodetector and no mechanical moving elements to enable faster acquisition times, while also providing comb resolution. As a proof of concept, a multidimensional coherent spectrum with comb cross-diagonal resolution is generated using only 365 ms of data. These improvements make multidimensional coherent spectroscopy relevant for systems with narrow resonances (especially cold atomic and molecular systems). In addition the method has the potential to be field deployable for chemical sensing applications.

physics.optics↗

arXiv2017

Frequency-comb based double-quantum two-dimensional coherent spectroscopy identifies collective hyperfine resonances in atomic vapor induced by dipole-dipole interactions

Frequency comb based multidimensional coherent spectroscopy is a novel optical method that enables high resolution measurement in a short acquisition time. The method's resolution makes multidimensional coherent spectroscopy relevant for atomic systems that have narrow resonances. We use double-quantum multidimensional coherent spectroscopy to reveal collective hyperfine resonances in rubidium vapor at 100 C induced by dipole-dipole interactions. We observe tilted lineshapes in the double-quantum 2D spectra, which has never been reported for Doppler-broadened systems. The tilted lineshapes suggest that the signal is predominately from the interacting atoms that have near zero relative velocity.

physics.atom-ph↗

arXiv2017

Controlling Coherent Quantum Dot Interactions

We measure many-body interactions in isolated quantum dot states using double-quantum multidimensional coherent spectroscopy. Few states are probed in a diffraction limited spot, which is enabled by a novel collinear scheme in which radiated four-wave-mixing signals are measured with phase resolution. Many-body interactions are enhanced by an additional prepulse tuned to the delocalized quasi-continuum states. We propose this effect as a method for controlling coupling between quantum states.

cond-mat.mes-hall↗

arXiv2017

Traveling Wave Model for Frequency Comb Generation in Single Section Quantum Well Diode Lasers

We present a traveling wave model for a semiconductor diode laser based on quantum wells. The gain model is carefully derived from first principles and implemented with as few phenomeno- logical constants as possible. The transverse energies of the quantum well confined electrons are discretized to automatically capture the effects of spectral and spatial hole burning, gain asym- metry, and the linewidth enhancement factor. We apply this model to semiconductor optical amplifiers and single-section phase-locked lasers. We are able to reproduce the experimental re- sults. The calculated frequency modulated comb shows potential to be a compact, chip-scale comb source without additional external components.

physics.optics↗

arXiv2017

Frequency comb based four-wave-mixing spectroscopy

We experimentally demonstrate four-wave-mixing spectroscopy using frequency combs. The experiment uses a geometry where excitation pulses and four-wave-mixing signals generated by a sample co-propagate. We separate them in the radio frequency domain by heterodyne detection with a local oscillator comb that has a different repetition frequency.

physics.optics↗

arXiv2016

Revealing and Characterizing Dark Excitons Through Coherent Multidimensional Spectroscopy

Dark excitons are of fundamental importance in a broad range of contexts, but are difficult to study using conventional optical spectroscopy due to their weak interaction with light. We show how coherent multidimensional spectroscopy can reveal and characterize dark states. Using this approach, we identify different types of dark excitons in InGaAs/GaAs quantum wells and determine details regarding lifetimes, homogeneous and inhomogeneous linewidths, broadening mechanisms and coupling strengths. The observations of coherent coupling between bright and dark excitons hint at a role for a multi-step process by which excitons in the barrier can relax into the quantum wells.

physics.optics↗

arXiv2014

Mode-Locked Chip Laser using Waveguide Arrays

We demonstrate theoretically that robust mode-locking can be achieved on a semiconductor chip with a waveguide array architecture. The waveguide arrays are used as an ideal saturable absorption mechanism for initial noise start-up as well as pulse shaping and stabilization. The cavity gain is provided by an injection current and forward biasing of the semiconductor material. The technology can be integrated directly with semiconductor architectures and technologies, thus allowing for the potential of an on-chip, broadband device.

physics.optics↗