arXiv subjects

Jeffrey A. Davis

Publications and source records attributed to Jeffrey A. Davis.

At least 19 recordsLinked to original sources

arXiv2026

Multi-dimensional spectroscopy of mobile excitons in two-dimensional semiconductors

Multi-dimensional coherent spectroscopy (MDCS) goes beyond standard linear-response probes and provides a powerful tool for investigating correlations between quasiparticles such as excitons (bound electron-hole pairs). Here we present a microscopic theory of MDCS that accounts for the delocalized nature of excitons in two-dimensional semiconductors. In contrast to the more phenomenological few-level approaches typically employed for modelling MDCS, our theory features mobile excitons with continuous momentum degrees of freedom. We find that the energy continuum associated with exciton momenta is crucial for producing interaction-induced decoherence, as well as capturing the interference between different exciton-polaron quasiparticles in the case of charge-doped semiconductors. Crucially, our calculated MDCS spectra agree well with recent experiments on doped monolayer MoSe$_2$ [Hao et al., Nature Communications 8, 15552 (2017)], and they suggest that the interactions between exciton polarons depend strongly on phase-space filling effects, where exciton polarons compete for electrons. Our results demonstrate that microscopic approaches allow one to gain new insights from the fine structure of MDCS on two-dimensional semiconductors, and they illustrate the utility of microscopic approaches to modelling MDCS experiments more generally.

cond-mat.mes-hall↗

arXiv2026

Ultrafast Two-Dimensional Spectroscopy Uncovers Ubiquitous Electron-Paramagnon Coupling in Cuprate Superconductors

The coupling between electronic excitations and collective bosonic modes is fundamental to the emergence of high-temperature superconductivity in cuprates. Despite extensive effort, conventional equilibrium and pump-probe optical spectroscopies still struggle to disentangle couplings to different bosonic modes when their energy scales overlap. Here we overcome this limitation using ultrafast two-dimensional electronic spectroscopy (2DES), which correlates coherent excitation and detection photon energies with femtosecond time resolution. Applied to optimally doped Bi$_2$Sr$_2$Ca$_{0.92}$Y$_{0.08}$Cu$_2$O$_{8+δ}$, 2DES reveals a pronounced off-diagonal resonance arising from the ultrafast generation of non-thermal bosons with energy $\hbarΩ_\mathbf{q}\simeq200$ meV. By comparing the measured spectra with a theoretical framework that explicitly includes the interaction between charge-transfer and magnetic excitations, we identify these bosons as paramagnons with momenta centered near $(π/2,π/2)$ and extending toward $(0,π)$ and $(π,0)$. The resonance persists across a large range of temperatures and doping concentrations, demonstrating that high-energy paramagnons are ubiquitously and strongly coupled to electronic excitations throughout the cuprate phase diagram. Time-domain analysis constrains the build-up of the paramagnon population to $\lesssim 10$ fs, placing a lower bound $λ\gtrsim 0.7$ on the coupling strength. More broadly, our results establish 2DES as a powerful approach for disentangling mode-selective electron-boson interactions and addressing decoherence dynamics, thereby establishing a new avenue for investigating strongly correlated quantum materials. These findings also provide a direct framework for future time-resolved resonant inelastic X-ray scattering experiments aimed at tracking the ultrafast dynamics of magnetic excitations.

cond-mat.supr-con↗

arXiv2026

Imaging topological polar structures in marginally twisted 2D semiconductors

Moire superlattices formed in van der Waals heterostructures due to twisting, lattice mismatch and strain present an opportunity for creating novel metamaterials with unique properties not present in the individual layers themselves. Ferroelectricity for example, arises due to broken inversion symmetry in twisted and strained bilayers of 2D semiconductors with stacking domains of alternating out-of-plane polarization. However, understanding the individual contributions of twist and strain to the formation of topological polar nanostructures remains to be established and has proven to be experimentally challenging. Inversion symmetry breaking has been predicted to give rise to an in-plane component of polarization along the domain walls, leading to the formation of a network of topologically non-trivial merons (half-skyrmions) that are Bloch-type for twisted and Neel-type for strained systems. Here we utilise angle-resolved, high-resolution vector piezoresponse force microscopy (PFM) to spatially resolve polarization components and topological polar nanostructures in marginally twisted bilayer WSe2, and provide experimental proof for the existence of topologically non-trivial meron/antimeron structures. We observe both Bloch-type and Neel-type merons, allowing us to differentiate between moire superlattices formed due to twist or heterogeneous strain. This first demonstration of non-trivial real-space topology in a twisted van der Waals heterostructure opens pathways for exploring the connection between twist and topology in engineered nano-devices.

cond-mat.mes-hall↗

arXiv2025

Ultrafast dynamics of coherent exciton-polaritons in van der Waals semiconductor metasurfaces

Enabling coherent light-matter interactions is a critical step toward next-generation quantum technologies. However, achieving this under ambient temperature conditions remains challenging due to rapid dephasing in optically excited systems. Optical metasurfaces based on quasi-bound states in the continuum have recently emerged as a powerful platform for reaching the strong light-matter coupling regime in flat, subwavelength thickness devices. Here, we investigate ultrafast exciton-polariton dynamics in self-hybridized WS$_2$ thin-film metasurfaces. Using hyperspectral momentum-resolved imaging, we reconstruct the highly anisotropic exciton-polariton dispersion, with a transition from positive to negative effective mass along orthogonal symmetry axes. Femtosecond pump-probe and multidimensional spectroscopy reveal detuning-dependent polariton dynamics with a coherence time up to ~110 fs, and allow direct observation of the coherent dynamics through ultrafast Rabi oscillations with ~45 fs period. We describe this behaviour with a three-eigenstate model that couples the photonic resonance with both bright and dark excitons, extending the conventional two-state picture of strong coupling. Our results establish van der Waals metasurfaces as a promising platform for next-generation polaritonic devices, enabling coherent quantum transfer of matter excitations at room temperature.

physics.optics↗

arXiv2025

Direct measurement of coherent nodal and antinodal dynamics in underdoped Bi-2212

The physics of strongly correlated materials is deeply rooted in electron interactions and their coupling to low-energy excitations. Unraveling the competing and cooperative nature of these interactions is crucial for connecting microscopic mechanisms to the emergence of exotic macroscopic behavior, such as high-temperature superconductivity. Here we show that polarization-resolved multidimensional coherent spectroscopy (MDCS) is able to selectively drive and measure coherent Raman excitations in different parts of the Fermi surface, where the superconducting gap vanishes or is the largest (respectively called Nodal and Antinodal region) in underdoped Bi-2212. Our evidence reveal that in the superconducting phase, the energy of Raman excitations in the nodal region is anti-correlated with the energy of electronic excitations at $\sim$1.6~eV, and both maintain coherence for over 44~fs. In contrast, excitations in the antinodal region show significantly faster decoherence ($<$18~fs) and no measurable correlations. Importantly, this long-lived coherence is specific to the superconducting phase and vanishes in the pseudogap and normal phases. This anti-correlation reveals a coherent link between the transition energy associated with the many body Cu-O bands and the energy of electronic Raman modes that map to the near-nodal superconducting gap. The different coherent dynamics of the nodal and antinodal excitations in the superconducting phase suggest that nodal fluctuations are protected from dissipation associated with scattering from antiferromagnetic fluctuations and may be relevant to sustaining the quantum coherent behaviour associated with high temperature superconductivity.

cond-mat.supr-con↗

arXiv2025

Efficient light upconversion via resonant exciton-exciton annihilation of dark excitons in few-layer transition metal dichalcogenides

In this work, we report a pronounced light upconversion in few-layer transition metal dichalcogenides. Our joint theory-experiment study attributes the upconversion photoluminescence to a resonant exciton-exciton annihilation involving a pair of dark excitons with opposite momenta, followed by the spontaneous emission of upconverted bright excitons, which can have a high upconversion efficiency. Additionally, the upconversion photoluminescence is generic in MoS2, MoSe2, WS2, and WSe2, showing a high tuneability from green to ultraviolet light.

cond-mat.mtrl-sci↗

arXiv2023

Intrinsic defect engineering of CVD grown monolayer MoS$_2$ for tuneable functional nanodevices

Defects in atomically thin materials can drive new functionalities and expand applications to multifunctional systems that are monolithically integrated. An ability to control formation of defects during the synthesis process is an important capability to create practical deployment opportunities. Molybdenum disulfide (MoS$_2$), a two-dimensional (2D) semiconducting material harbors intrinsic defects that can be harnessed to achieve tuneable electronic, optoelectronic, and electrochemical devices. However, achieving precise control over defect formation within monolayer MoS$_2$, while maintaining the structural integrity of the crystals remains a notable challenge. Here, we present a one-step, in-situ defect engineering approach for monolayer MoS$_2$ using a pressure dependent chemical vapour deposition (CVD) process. Monolayer MoS$_2$ grown in low-pressure CVD conditions (LP-MoS$_2$) produces sulfur vacancy (Vs) induced defect rich crystals primarily attributed to the kinetics of the growth conditions. Conversely, atmospheric pressure CVD grown MoS$_2$ (AP-MoS$_2$) passivates these Vs defects with oxygen. This disparity in defect profiles profoundly impacts crucial functional properties and device performance. AP-MoS$_2$ shows a drastically enhanced photoluminescence, which is significantly quenched in LP-MoS$_2$ attributed to in-gap electron donor states induced by the Vs defects. However, the n-doping induced by the Vs defects in LP-MoS$_2$ generates enhanced photoresponsivity and detectivity in our fabricated photodetectors compared to the AP-MoS$_2$ based devices. Defect-rich LP-MoS$_2$ outperforms AP-MoS$_2$ as channel layers of field-effect transistors (FETs), as well as electrocatalytic material for hydrogen evolution reaction (HER). This work presents a single-step CVD approach for in-situ defect engineering in monolayer MoS$_2$ and presents a pathway to control defects in other monolayer material systems.

physics.app-ph↗

arXiv2023

Floquet engineering in the presence of optically excited carriers

Floquet engineering provides an optical means to manipulate electronic bandstructures, however, carriers excited by the pump field can lead to an effective heating, and can obscure measurement of the band changes. A recent demonstration of the effects of Floquet engineering on a coherent ensemble of excitons in monolayer WS$_2$ proved particularly sensitive to non-adiabatic effects, while still being able to accurately resolve bandstructure changes. Here, we drive an AC-Stark effect in monolayer WS$_2$ using pulses with constant fluence but varying pulse duration (from 25-235~fs). With shorter pump pulses, the corresponding increase in peak intensity introduces additional carriers via two-photon absorption, leading to additional decoherence and peak broadening (which makes it difficult to resolve the AC-Stark shift). We use multidimensional coherent spectroscopy to create a coherent ensemble of excitons in monolayer WS$_2$ and measure the evolution of the coherence throughout the duration of the Floquet pump pulse. Changes to the amplitude of the macroscopic coherence quantifies the additional broadening. At the same time, the evolution of the average phase allows the instantaneous changes to the bandstructure to be quantified, and is not impacted by the additional broadening. This approach to measuring the evolution of Floquet-Bloch states demonstrates a means to quantify effective heating and non-adiabaticity caused by excited carriers, while at the same time resolving the coherent evolution of the bandstructure.

cond-mat.mes-hall↗

arXiv2023

Effects of Floquet Engineering on the Coherent Exciton Dynamics in Monolayer WS$_2$

Coherent optical manipulation of electronic bandstructures via Floquet Engineering is a promising means to control quantum systems on an ultrafast timescale. However, the ultrafast switching on/off of the driving field comes with questions regarding the limits of validity of the Floquet formalism, which is defined for an infinite periodic drive, and to what extent the transient changes can be driven adibatically. Experimentally addressing these questions has been difficult, in large part due to the absence of an established technique to measure coherent dynamics through the duration of the pulse. Here, using multidimensional coherent spectroscopy we explicitly excite, control, and probe a coherent superposition of excitons in the $K$ and $K^\prime$ valleys in monolayer WS$_2$. With a circularly polarized, red-detuned, pump pulse, the degeneracy of the $K$ and $K^\prime$ excitons can be lifted and the phase of the coherence rotated. We demonstrate phase rotations during the 100 fs driving pulse that exceed $π$, and show that this can be described by a combination of the AC-Stark shift of excitons in one valley and Bloch-Siegert shift of excitons in the opposite valley. Despite showing a smooth evolution of the phase that directly follows the intensity envelope of the pump pulse, the process is not perfectly adiabatic. By measuring the magnitude of the macroscopic coherence as it evolves before, during, and after the pump pulse we show that there is additional decoherence caused by power broadening in the presence of the pump. This non-adiabaticity may be a problem for many applications, such as manipulating q-bits in quantum information processing, however these measurements also suggest ways such effects can be minimised or eliminated.

cond-mat.mes-hall↗

arXiv2022

Exciton-polaron interactions in monolayer WS$_2$

Interactions between quasiparticles are of fundamental importance and ultimately determine the macroscopic properties of quantum matter. A famous example is the phenomenon of superconductivity, which arises from attractive electron-electron interactions that are mediated by phonons or even other more exotic fluctuations in the material. Here we introduce mobile exciton impurities into a two-dimensional electron gas and investigate the interactions between the resulting Fermi polaron quasiparticles. We employ multi-dimensional coherent spectroscopy on monolayer WS$_2$, which provides an ideal platform for determining the nature of polaron-polaron interactions due to the underlying trion fine structure and the valley specific optical selection rules. At low electron doping densities, we find that the dominant interactions are between polaron states that are dressed by the same Fermi sea. In the absence of bound polaron pairs (bipolarons), we show using a minimal microscopic model that these interactions originate from a phase-space filling effect, where excitons compete for the same electrons. We furthermore reveal the existence of a bipolaron bound state with remarkably large binding energy, involving excitons in different valleys cooperatively bound to the same electron. Our work lays the foundation for probing and understanding strong electron correlation effects in two-dimensional layered structures such as moiré superlattices.

cond-mat.mes-hall↗

arXiv2020

Multidimensional Analysis of Excitonic Spectra of Monolayers of Tungsten Disulphide: Towards Computer Aided Identification of Structural and Environmental Perturbations of 2D Materials

Despite 2D materials holding great promise for a broad range of applications, the proliferation of devices and their fulfillment of real-life demands are still far from being realized. Experimentally obtainable samples commonly experience a wide range of perturbations (ripples and wrinkles, point and line defects, grain boundaries, strain field, doping, water intercalation, oxidation, edge reconstructions) significantly deviating the properties from idealistic models. These perturbations, in general, can be entangled or occur in groups with each group forming a complex perturbation making the interpretations of observable physical properties and the disentanglement of simultaneously acting effects a highly non-trivial task even for an experienced researcher. Here we generalise statistical correlation analysis of excitonic spectra of monolayer WS2, acquired by hyperspectral absorption and photoluminescence imaging, to a multidimensional case, and examine multidimensional correlations via unsupervised machine learning algorithms. Using principle component analysis we are able to identify 4 dominant components that are correlated with tensile strain, disorder induced by adsorption or intercalation of environmental molecules, multi-layer regions and charge doping, respectively. This approach has the potential to determine the local environment of WS2 monolayers or other 2D materials from simple optical measurements, and paves the way towards advanced, machine-aided, characterisation of monolayer matter.

cond-mat.mes-hall↗

arXiv2019

Disentangling the effects of doping, strain and defects in monolayer WS2 by optical spectroscopy

Monolayers of transition metal dichalcogenides (TMdC) are promising candidates for realization of a new generation of optoelectronic devices. The optical properties of these two-dimensional materials, however, vary from flake to flake, or even across individual flakes, and change over time, all of which makes control of the optoelectronic properties challenging. There are many different perturbations that can alter the optical properties, including charge doping, defects, strain, oxidation, and water intercalation. Identifying which perturbations are present is usually not straightforward and requires multiple measurements using multiple experimental modalities, which presents barriers when attempting to optimise preparation of these materials. Here, we apply highresolution photoluminescence and differential reflectance hyperspectral imaging in situ to CVD-grown WS2 monolayers. By combining these two optical measurements and using a statistical correlation analysis we are able to disentangle three contributions modulating optoelectronic properties of these materials: electron doping, strain and defects. In separating these contributions, we also observe that the B-exciton energy is less sensitive to variations in doping density than A-excitons.

cond-mat.mtrl-sci↗

arXiv2019

Background-free time-resolved coherent Raman spectroscopy (CSRS and CARS): heterodyne detection of low-energy vibrations and recognition of excited-state contributions

Coherent Raman scattering (CRS) spectroscopy techniques have been widely developed and optimized for different applications in biomedicine and fundamental science. The most utilized CRS technique has been coherent anti-Stokes Raman scattering (CARS), and more recently, stimulated Raman scattering (SRS). Coherent Stokes Raman scattering (CSRS) has been largely ignored mainly because it is often strongly affected by fluorescence, particularly for resonance enhanced measurements. However, in the cases of resonant excitation the information contained in the CSRS signal can be different and complementary to that of CARS. Here we combine the approaches of pulse shaping, interferometric heterodyne detection, 8-step phase cycling and Fourier-transform of time-domain measurements, developed in CARS and 2D electronic spectroscopy communities, to measure resonant CSRS and CARS spectra using a Titanium:sapphire oscillator. The signal is essentially background-free (both fluorescent and non-resonant background signals are suppressed) with high spectral resolution and high sensitivity, and can access low-energy modes down to ~30 cm-1. We demonstrate the ability to easily select between CSRS and CARS schemes and show an example in which acquisition of both CSRS and CARS spectra allows vibrational modes on the excited electronic state to be distinguished from those on the ground electronic state.

physics.optics↗

arXiv2019

Persistent coherence of quantum superpositions in an optimally doped cuprate revealed by 2D spectroscopy

Understanding of the precise mechanisms of high-temperature superconductivity is elusive. In particular, in order to solve the puzzle of the pairing mechanism, it is important to understand the detailed nature of the excitations at energies around the superconducting gap. While measurements of the dynamics of excited electronic populations have been able to give some insight, they have largely neglected the intricate dynamics of quantum coherence. Here, we apply multidimensional coherent spectroscopy for the first time to a prototypical cuprate and report unprecedented coherent dynamics persisting for ~500 fs, originating directly from the quantum superposition of optically excited states separated by 20 - 60 meV. These results reveal the correlation between high and low energy excitations, and indicate that the interplay between many-body states on different energy scales conserves phase coherence. In revealing these dynamics we demonstrate that multidimensional coherent spectroscopy can address electronic correlations and interrogate many-body quantum systems in unprecedented ways.

cond-mat.supr-con↗

arXiv2017

Time-domain THz spectroscopy reveals coupled protein-hydration dielectric response in solutions of native and fibrils of human lyso-zyme

Here we reveal details of the interaction between human lysozyme proteins, both native and fibrils, and their water environment by intense terahertz time domain spectroscopy. With the aid of a rigorous dielectric model, we determine the amplitude and phase of the oscillating dipole induced by the THz field in the volume containing the protein and its hydration water. At low concentrations, the amplitude of this induced dipolar response decreases with increasing concentration. Beyond a certain threshold, marking the onset of the interactions between the extended hydration shells, the amplitude remains fixed but the phase of the induced dipolar response, which is initially in phase with the applied THz field, begins to change. The changes observed in the THz response reveal protein-protein interactions me-diated by extended hydration layers, which may control fibril formation and may have an important role in chemical recognition phenomena.

physics.bio-ph↗

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↗

arXiv2016

Two-dimensional double-quantum spectroscopy: peak shapes as a sensitive probe of carrier interactions in quantum wells

We identify carrier scattering at densities below which it has previously been observed in semiconductor quantum wells. These effects are evident in the peakshapes of 2D double-quantum spectra, which change as a function of excitation density. At high excitation densities ($\geq 10^{9}$ carriers/,cm$^{-2}$) we observe untilted peaks similar to those reported in previous experiments. At low excitation densities (<$10^{8}$ carriers cm$^{-2}$) we observe narrower, tilted peaks. Using a simple simulation, we show that tilted peak-shapes are expected in double-quantum spectra when inhomogeneous broadening is much larger than homogeneous broadening, and that fast pure-decoherence of the double-quantum coherence can obscure this peak tilt. These results show that carrier interactions are important at lower densities than previously expected, and that the `natural' double-quantum peakshapes are hidden by carrier interactions at the excitation densities typically used. Furthermore, these results demonstrate that analysis of 2D peak-shapes in double-quantum spectroscopy provides an incisive tool for identifying interactions at low excitation density.

physics.optics↗

arXiv2015

Vibronic resonances facilitate excited state coherence in light harvesting proteins at room temperature

Until recently it was believed that photosynthesis, a fundamental process for life on earth, could be fully understood with semi-classical models. However, puzzling quantum phenomena have been observed in several photosynthetic pigment-protein complexes, prompting questions regarding the nature and role of these effects. Recent attention has focused on discrete vibrational modes that are resonant or quasi-resonant with excitonic energy splittings and strongly coupled to these excitonic states. Here we unambiguously identify excited state coherent superpositions in photosynthetic light-harvesting complexes using a new experimental approach. Decoherence on the timescale of the excited state lifetime allows low energy (56 cm-1) oscillations on the signal intensity to be observed. In conjunction with an appropriate model, these oscillations provide clear and direct experimental evidence that the persistent coherences observed require strong vibronic mixing among excited states.

physics.bio-ph↗