arXiv subjects

Charles J. Sayers

Publications and source records attributed to Charles J. Sayers.

10 recordsLinked to original sources

arXiv2025

Tracking the Catastrophic Collapse of Hybrid Exciton-Phonon Order in a Quantum Material

Revealing the interactions binding electronic and lattice components of cooperative quantum order is central to sculpting new states of matter. This challenge is epitomized by the charge density wave material 1T-TiSe$_2$, where photoexcitation disrupts its presumed hybrid exciton-phonon order. This exposes a paradox: the electronic component collapses within femtoseconds while the periodic lattice distortion persists. If the lattice distortion outlives the excitonic condensate, were they truly intertwined? Here we resolve this by uncovering a low-frequency mode (approx. 0.13 THz) emerging only in the ordered state, signaling exciton-phonon coupling. This mode is consistent with a locked phason -- a collective excitation arising if coupling between the excitonic condensate and lattice reduces continuous phase symmetry to a discrete one, giving the excitonic Goldstone mode finite mass. This is captured by an effective theory describing a shared potential landscape. At a critical threshold, the collapse of excitonic order flattens the potential, triggering an exciton-phonon catastrophe: selective overheating of the charge density wave phonon, disappearance of the locked phason, and sudden loss of electronic coherence. Remarkably, the lattice distortion survives as a dynamically trapped, non-thermal remnant, confirmed by the anomalous temperature dependence of the phononic response. These findings demonstrate that coupled potential energy landscapes can be manipulated to selectively dismantle complex quantum orders, advancing material control through dynamical design.

physics.app-ph↗

arXiv2025

Photoinduced Electronic Band Dynamics and Defect-mediated Surface Potential Evolution in PdSe$_2$

We use time- and angle-resolved photoemission spectroscopy (TR-ARPES) combined with density functional theory to investigate ultrafast carrier dynamics in low-symmetry layered semiconducting PdSe$_2$. The indirect bandgap is determined to be 0.55~eV. Following photoexcitation above this gap, we resolve a valence band shift and broadening, both lasting less than a picosecond, consistent with bandgap renormalization and carrier scattering, indicative of strong many-body interactions. Subsequently, hot carriers populate the conduction band minimum and are captured by defect states. A surface photovoltage (SPV) of $\sim$ 67~meV emerges, persisting for over 50~ps, driven by defect-assisted charge separation. The formation of native vacancies, promoted by the low-symmetry lattice, likely gives rise to the mid-gap states responsible for this long-lived SPV response. Detailed analysis of TR-ARPES spectra disentangles the contributions of bandgap renormalization, carrier scattering, defect states, and SPV. These findings establish PdSe$_2$ as a prototypical layered quantum material exhibiting exotic photoresponses on ultrafast timescales.

cond-mat.mes-hall↗

arXiv2025

Electrically tunable ultrafast dynamics and interactions of hybrid excitons in a 2D semiconductor bilayer

Extended efforts have been devoted to the study of strongly-interacting excitons and their dynamics, towards macroscopic quantum states of matter such as Bose-Einstein condensates of excitons and polaritons. Momentum-direct layer-hybridized excitons in transition metal dichalcogenides have attracted considerable attention due to their high oscillator strength and dipolar nature. However, the tunability of their interactions and dynamics remains unexplored. Here, we achieve an unprecedented control over the nonlinear properties of dipolar layer-hybridized excitons in an electrically gated van der Waals homobilayer monitored by transient optical spectroscopy. By applying a vertical electric field, we reveal strong Coulomb interactions of dipolar hybrid excitons, leading to opposite density-dependent energy shifts of the two main hybrid species based on their dipolar orientation, together with a strongly enhanced optical saturation of their absorption. Furthermore, by electrically tuning the interlayer tunneling between the hybridized carriers, we significantly extend the formation time of hybrid excitons, while simultaneously increasing their decay times. Our findings have implications for the search on quantum blockade and condensation of excitons and dipolaritons in two-dimensional materials.

cond-mat.mes-hall↗

arXiv2024

Anomalous amplitude mode dynamics below the expected charge-density-wave transition in 1$T$-VSe$_2$

A charge-density-wave (CDW) is characterized by a dynamical order parameter consisting of a time-dependent amplitude and phase, which manifest as optically-active collective modes of the CDW phase. Studying the behaviour of such collective modes in the time-domain, and their coupling with electronic and lattice order, provides important insight into the underlying mechanisms behind CDW formation. In this work, we report on femtosecond broadband transient reflectivity experiments on bulk 1$T$-VSe$_2$ using near-infrared excitation. At low temperature, we observe coherent oscillations associated with the CDW amplitude mode and phonons of the distorted lattice. Across the expected transition temperature at 110 K, we confirm signatures of a rearrangement of the electronic structure evident in the quasiparticle dynamics. However, we find that the amplitude mode instead softens to zero frequency at 80 K, possibly indicating an additional phase transition at this temperature. In addition, we demonstrate photoinduced CDW melting, associated with a collapse of the electronic and lattice order, which occurs at moderate excitation densities, consistent with a dominant electron-phonon CDW mechanism.

cond-mat.str-el↗

arXiv2023

Optical response of the bulk stabilized mosaic phase in Se doped TaS$_{2-x}$Se$_{x}$

The layered van der Waals material, TaS$_{2}$ features a meta-stable mosaic phase on the verge of a nearly commensurate to commensurate charge density wave transition. This meta-stable or 'hidden' phase can be reached by laser pumping the low temperature, commensurate charge density wave phase. Here we report the stabilization of a bulk, equilibrium mosaic phase in 1T-TaS$_{1.2}$Se$_{0.8}$ single crystals observed with transport and optical spectroscopy experiments. We identify a bulk pseudogap in the mosaic phase of approximately 200 meV at the lowest temperatures, while the CCDW phase can be obtained by heating and instead has a full optical gap of about 100 meV. Surprisingly, a spectral weight analysis shows that Se doping gives rise to an increased charge density despite the fact that this is formally an isovalent substitution. This finding is consistent with the recent observation that the mosaic phase is stabilized as equilibrium phase through the appearance of charged defects.

cond-mat.str-el↗

arXiv2023

Strong Coupling of Coherent Phonons to Excitons in Semiconducting Monolayer MoTe$_2$

The coupling of the electron system to lattice vibrations and their time-dependent control and detection provides unique insight into the non-equilibrium physics of semiconductors. Here, we investigate the ultrafast transient response of semiconducting monolayer 2$H$-MoTe$_2$ encapsulated with $h$BN using broadband optical pump-probe microscopy. The sub-40-fs pump pulse triggers extremely intense and long-lived coherent oscillations in the spectral region of the A' and B' exciton resonances, up to $\sim$20% of the maximum transient signal, due to the displacive excitation of the out-of-plane $A_{1g}$ phonon. Ab-initio calculations reveal a dramatic rearrangement of the optical absorption of monolayer MoTe$_2$ induced by an out-of-plane stretching and compression of the crystal lattice, consistent with an $A_{1g}$-type oscillation. Our results highlight the extreme sensitivity of the optical properties of monolayer TMDs to small structural modifications and their manipulation with light.

cond-mat.mes-hall↗

arXiv2022

Spectrally resolving the phase and amplitude of coherent phonons in the charge density wave state of 1$T$-TaSe$_2$

The excitation and detection of coherent phonons has given unique insights into condensed matter, in particular for materials with strong electron-phonon coupling. We report a study of coherent phonons in the layered charge density wave (CDW) compound 1$T$-TaSe$_2$ performed using transient broadband reflectivity spectroscopy, in the photon energy range 1.75-2.65 eV. Several intense and long lasting (> 20 ps) oscillations, arising from the CDW superlattice reconstruction, are observed allowing for detailed analysis of the spectral dependence of their amplitude and phase. We find that for energies above 2.4 eV, where transitions involve Ta d-bands, the CDW amplitude mode at 2.19 THz dominates the coherent response. At lower energies, instead, beating arises between additional frequencies, with a particularly intense mode at 2.95 THz. Interestingly, our spectral analysis reveals a $π$ phase shift at 2.4 eV. Results are discussed considering the selective coupling of specific modes to energy bands involved in the optical transitions seen in steady-state reflectivity. The work demonstrates how coherent phonon spectroscopy can distinguish and resolve optical states strongly coupled to the CDW order and provide additional information normally hidden in conventional steady-state experiments.

cond-mat.str-el↗

arXiv2021

Observation of the charge density wave collective mode in the infrared optical response of VSe$_2$

We present a detailed study of the bulk electronic structure of high quality VSe$_{2}$ single crystals using optical spectroscopy. Upon entering the charge density wave phase below the critical temperature of 112 K, the optical conductivity of VSe$_2$ undergoes a significant rearrangement. A Drude response present above the critical temperature is suppressed while a new interband transition appears around 0.07\,eV. From our analysis, we estimate that part of the spectral weight of the Drude response is transferred to a collective mode of the CDW phase. The remaining normal state charge dynamics appears to become strongly damped by interactions with the lattice as evidenced by a mass enhancement factor m$^{*}$/m$\approx$3. In addition to the changes taking place in the electronic structure, we observe the emergence of infrared active phonons below the critical temperature associated with the 4a x 4a lattice reconstruction.

cond-mat.str-el↗

arXiv2020

Investigation of the Non-equilibrium State of Strongly Correlated Materials by Complementary Ultrafast Spectroscopy Techniques

Photoinduced non-thermal phase transitions are new paradigms of exotic non-equilibrium physics of strongly correlated materials. An ultrashort optical pulse can drive the system to a new order through complex microscopic interactions that do not occur in the equilibrium state. Ultrafast spectroscopies are unique tools to reveal the underlying mechanisms of such transitions which lead to transient phases of matter. Yet, their individual specificities often do not provide an exhaustive picture of the physical problem. One effective solution to enhance their performance is the integration of different ultrafast techniques. This provides an opportunity to simultaneously probe physical phenomena from different perspectives whilst maintaining the same experimental conditions. In this context, we performed complementary experiments by combining time-resolved reflectivity and time and angle-resolved photoemission spectroscopy. We demonstrated the advantage of this combined approach by investigating the complex charge density wave (CDW) phase in 1$\it{T}$-TiSe$_{2}$. Specifically, we show the key role of lattice degrees of freedom to establish and stabilize the CDW in this material.

cond-mat.str-el↗

arXiv2019

Excitonic and lattice contributions to the charge density wave in 1T-TiSe$_2$ revealed by a phonon bottleneck

Understanding collective electronic states such as superconductivity and charge density waves is pivotal for fundamental science and applications. The layered transition metal dichalcogenide 1T-TiSe2 hosts a unique charge density wave (CDW) phase transition whose origins are still not fully understood. Here, we present ultrafast time- and angle-resolved photoemission spectroscopy (TR-ARPES) measurements complemented by time-resolved reflectivity (TRR) which allows us to establish the contribution of excitonic and electron-phonon interactions to the CDW. We monitor the energy shift of the valence band (VB) and coupling to coherent phonons as a function of laser fluence. The VB shift, directly related to the CDW gap closure, exhibits a markedly slower recovery dynamics at fluences above Fth = 60 microJ cm-2. This observation coincides with a shift in the relative weight of coherently coupled phonons to higher frequency modes in time-resolved reflectivity (TRR), suggesting a phonon bottleneck. Using a rate equation model, the emergence of a high-fluence bottleneck is attributed to an abrupt reduction in coupled phonon damping and an increase in exciton dissociation rate linked to the loss of CDW superlattice phonons. Thus, our work establishes the important role of both excitonic and phononic interactions in the CDW phase transition and the advantage of combining complementary femtosecond techniques to understand the complex interactions in quantum materials.

cond-mat.str-el↗