arXiv subjects

David J. Jones

Publications and source records attributed to David J. Jones.

14 recordsLinked to original sources

arXiv2026

Signatures of rare-earth elements in mineralogical form using laser-ablation dual-comb spectroscopy

Spectroscopy of laser-produced plasmas offers an avenue for real-time, standoff and non-preparatory sensing of rare-earth elements (REEs) within a mineralogical context with applications spanning exploration geology to ore body mapping to ore sorting. Demonstrations of laser-induced breakdown spectroscopy (LIBS) in rock samples have employed both atomic and molecular detection for REE sensors. In this work we evaluate a complementary technique of absorption spectroscopy, realized with dual-frequency combs. This approach provides multi-THz (nm) spectral coverage with simultaneous sub-GHz (pm) resolution. It can improve accuracy and line identification confidence in congested multi-species spectra, which makes it ideal for multi-species evaluations present within mineralogical samples. We analyze REE signatures in calibrated reference materials (CRMs) and a synthesized, REE-containing alloy for atomic, ionic and molecular (oxide) absorptions across three spectral windows. We identify lines from rare-earth and matrix elements, compare absorption line strengths and investigate their temporal evolution. For La I, Sm I and Ce I, preliminary limits of detection from 54-583 ppm are estimated for CRMs, using univariate analysis of selected transitions. Comparing the CRM signatures to those of REEs synthesized in a copper alloy, we observe that all REE lines appear earlier and disappear faster in the CRM samples. We attribute these dynamics to matrix effects: Among other elements, the increased oxygen content in the CRM could favor molecular formation. For rock samples, observations will once again differ due to grain sizes and bonding mechanisms. Compared to LIBS, we can resolve individual REE and matrix lines with minimal spectral overlap. These proof-of-principle results form a foundation for further development of this laser-based method as a mining sensor.

physics.optics↗

arXiv2026

Isolating Exciton Dissociation Pathways in ReSe$_{\text{2}}$

Strongly bound excitons dominate the optical response in many van der Waals semiconductors, yet distinguishing between the different microscopic processes governing exciton dissociation remains challenging. Using time- and angle-resolved photoemission spectroscopy (TR-ARPES), we independently track exciton and band-edge carrier populations in bulk ReSe$_{\text{2}}$ under resonant excitation. By studying the fluence dependence and polarization-controlled exciton density dependence of the exciton dissociation process, we distinguish between competing processes and identify exciton photoionization as the microscopic dissociation mechanism. These results establish a population-resolved strategy for resolving exciton-to-carrier conversion pathways in strongly excitonic materials.

cond-mat.mtrl-sci↗

arXiv2025

Addressing modulational instability in anti-resonant hollow-core fibers for pulse compression

When pulses propagate in gas-filled anti-resonant hollow-core fibers (AR-HCFs) modulational instability (MI) can lead to pulse break-up and loss of coherence. In pulse broadening and compression schemes, MI is a parasitic effect that induces significant shot-to-shot fluctuations of the peak power of compressed pulses and increases rapidly over a narrow range of input pulse energies. In this work we use experimental studies and supporting numerical simulations to compare two AR-HCFs that are chosen to enhance or suppress MI. We demonstrate that judicious selection of the wall thickness of the anti-resonant elements (AREs) can drastically reduce the MI gain, thereby increasing the limit of pulse energy scaling of stable ultrafast pulse compression.

physics.optics↗

arXiv2025

Quenching of excitons at grain boundaries in C60 thin films

Exciton lifetimes play a critical role in the performance of organic optoelectronic devices. In this work, we investigate how the presence of multiple rotational domains, and therefore grain boundaries, impacts exciton dynamics in thin films of C60/Au(111) using time and angle-resolved photoemission spectroscopy (TR-ARPES). We find that films with multiple rotational domains exhibit shorter exciton lifetimes and evidence of exciton-exciton annihilation, even when one domain predominates. Scanning tunneling microscopy (STM) measurements reveal electronic structure changes resulting from a locally reduced dielectric constant at grain boundaries, providing a mechanism for lifetime reduction through exciton funneling and other additional decay channels. These findings highlight the critical role of film quality in determining intrinsic exciton lifetimes, and show that minuscule amounts of disorder that are nearly undetectable by ensemble measurements can significantly impact dynamics. These results imply that precise structural control is essential for optimize the performance of organic optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2024

Two-stage growth for highly ordered epitaxial C$_{60}$ films on Au(111)

As an organic semiconductor and a prototypical acceptor molecule in organic photovoltaics, C$_{60}$ has broad relevance to the world of organic thin film electronics. Although highly uniform C$_{60}$ thin films are necessary to conduct spectroscopic analysis of the electronic structure of these C$_{60}$-based materials, reported C$_{60}$ films show a relatively low degree of order beyond a monolayer. Here, we develop a generalizable two-stage growth technique that consistently produces single-domain C$_{60}$ films of controllable thicknesses, using Au(111) as an epitaxially well-matched substrate. We characterize the films using low-energy electron diffraction, low-energy electron microscopy, scanning tunneling microscopy, and angle-resolved photoemission spectroscopy (ARPES). We report highly oriented epitaxial film growth of C$_{60}$/Au(111) from 1 monolayer (ML) up to 20 ML films. The high-quality of the C$_{60}$ thin films enables the direct observation of the electronic dispersion of the HOMO and HOMO-1 bands via ARPES without need for small spot sizes. Our results indicate a path for the growth of organic films on metallic substrates with long-range ordering.

cond-mat.mtrl-sci↗

arXiv2023

Advancing time- and angle-resolved photoemission spectroscopy: The role of ultrafast laser development

In the last decade, there has been a proliferation of laser sources for time- and angle-resolved photoemission spectroscopy (TR-ARPES), building on the proven capability of this technique to tackle important scientific questions. In this review, we aim to identify the key motivations and technologies that spurred the development of various laser sources, from frequency up-conversion in nonlinear crystals to high-harmonic generation in gases. We begin with a historical overview of the field in Sec.1, framed by advancements in light source and electron spectrometer technology. An introduction to the fundamental aspects of the photoemission process and the observables that can be studied is given in Sec.2, along with its dependencies on the pump and probe pulse parameters. The technical aspects of TR-ARPES are discussed in Sec.3. Here, experimental limitations such as space charge and resultant trade-offs in source parameters are discussed. Details of various systems and their approach to these trade-offs are given in Sec.4. Within this discussion, we present a survey of TR-ARPES laser sources; a meta-analysis of these source parameters showcases the advancements and trends in modern systems. Lastly, we conclude with a brief discussion of future directions for TR-ARPES and its capabilities in elucidating equilibrium and non-equilibrium observables, as well as its integration with micro-ARPES and spin-resolved ARPES (Sec.5).

physics.optics↗

arXiv2023

A versatile laser-based apparatus for time-resolved ARPES with micro-scale spatial resolution

We present the development of a versatile apparatus for a 6.2 eV laser-based time and angle-resolved photoemission spectroscopy with micrometer spatial resolution (time-resolved $μ$-ARPES). With a combination of tunable spatial resolution down to $\sim$11 $μ$m, high energy resolution ($\sim$11 meV), near-transform-limited temporal resolution ($\sim$280 fs), and tunable 1.55 eV pump fluence up to $\sim$3 mJ/cm$^2$, this time-resolved $μ$-ARPES system enables the measurement of ultrafast electron dynamics in exfoliated and inhomogeneous materials. We demonstrate the performance of our system by correlating the spectral broadening of the topological surface state of Bi$_2$Se$_3$ with the spatial dimension of the probe pulse, as well as resolving the spatial inhomogeneity contribution to the observed spectral broadening. Finally, after in-situ exfoliation, we performed time-resolved $μ$-ARPES on a $\sim$30 $μ$m few-layer-thick flake of transition metal dichalcogenide WTe$_2$, thus demonstrating the ability to access ultrafast electron dynamics with momentum resolution on micro-exfoliated and twisted materials.

cond-mat.mtrl-sci↗

arXiv2021

Unveiling the underlying interactions in Ta2NiSe5 from photo-induced lifetime change

We present a generic procedure for quantifying the interplay of electronic and lattice degrees of freedom in photo-doped insulators through a comparative analysis of theoretical many-body simulations and time- and angle-resolved photoemission spectroscopy (TR-ARPES) of the transient response of the candidate excitonic insulator Ta2NiSe5. Our analysis demonstrates that the electron-electron interactions dominate the electron-phonon ones. In particular, a detailed analysis of the TRARPES spectrum enables a clear separation of the dominant broadening (electronic lifetime) effects from the much smaller bandgap renormalization. Theoretical calculations show that the observed strong spectral broadening arises from the electronic scattering of the photo-excited particle-hole pairs and cannot be accounted for in a model in which electron-phonon interactions are dominant. We demonstrate that the magnitude of the weaker subdominant bandgap renormalization sensitively depends on the distance from the semiconductor/semimetal transition in the high-temperature state, which could explain apparent contradictions between various TR-ARPES experiments. The analysis presented here indicates that electron-electron interactions play a vital role (although not necessarily the sole one) in stabilizing the insulating state.

cond-mat.str-el↗

arXiv2021

Fano interference of the Higgs mode in cuprate high-Tc superconductors

Despite decades of search for the pairing boson in cuprate high-Tc superconductors, its identity still remains debated to date. For this reason, spectroscopic signatures of electron-boson interactions in cuprates have always been a center of attention. For example, the kinks in the quasiparticle dispersion observed by angle-resolved photoemission spectroscopy (ARPES) studies have motivated a decade-long investigation of electron-phonon as well as electron-paramagnon interactions in cuprates. On the other hand, the overlap between the charge-order correlations and the pseudogap in the cuprate phase diagram has also generated discussions about the potential link between them. In the present study, we provide a fresh perspective on these intertwined interactions using the novel approach of Higgs spectroscopy, i.e. an investigation of the amplitude oscillations of the superconducting order parameter driven by a terahertz radiation. Uniquely for cuprates, we observe a Fano interference of its dynamically driven Higgs mode with another collective mode, which we reveal to be charge density wave fluctuations from an extensive doping- and magnetic field-dependent study. This finding is further corroborated by a mean field model in which we describe the microscopic mechanism underlying the interaction between the two orders. Our work demonstrates Higgs spectroscopy as a novel and powerful technique for investigating intertwined orders and microscopic processes in unconventional superconductors.

cond-mat.supr-con↗

arXiv2020

Establishing non-thermal regimes in pump-probe electron-relaxation dynamics

Time- and angle-resolved photoemission spectroscopy (TR-ARPES) accesses the electronic structure of solids under optical excitation, and is a powerful technique for studying the coupling between electrons and collective modes. One approach to infer electron-boson coupling is through the relaxation dynamics of optically-excited electrons, and the characteristic timescales of energy redistribution. A common description of electron relaxation dynamics is through the effective electronic temperature. Such a description requires that thermodynamic quantities are well-defined, an assumption that is generally violated at early delays. Additionally, precise estimation of the non-thermal window -- within which effective temperature models may not be applied -- is challenging. We perform TR-ARPES on graphite and show that Boltzmann rate equations can be used to calculate the time-dependent electronic occupation function, and reproduce experimental features given by non-thermal electron occupation. Using this model, we define a quantitative measure of non-thermal electron occupation and use it to define distinct phases of electron relaxation in the fluence-delay phase space. More generally, this approach can be used to inform the non-thermal-to-thermal crossover in pump-probe experiments.

cond-mat.mtrl-sci↗

arXiv2019

Direct determination of mode-projected electron-phonon coupling in the time-domain

Ultrafast spectroscopies have become an important tool for elucidating the microscopic description and dynamical properties of quantum materials. In particular, by tracking the dynamics of non-thermal electrons, a material's dominant scattering processes -- and thus the many-body interactions between electrons and collective excitations -- can be revealed. Here we present a new method for extracting the electron-phonon coupling strength in the time domain, by means of time and angle-resolved photoemission spectroscopy (TR-ARPES). This method is demonstrated in graphite, where we investigate the dynamics of photo-injected electrons at the K point, detecting quantized energy-loss processes that correspond to the emission of strongly-coupled optical phonons. We show that the observed characteristic timescale for spectral-weight-transfer mediated by phonon-scattering processes allows for the direct quantitative extraction of electron-phonon matrix elements, for specific modes, and with unprecedented sensitivity.

cond-mat.str-el↗

arXiv2017

The performance and limitations of FPGA-based digital servos for atomic, molecular, and optical physics experiments

In this work we address the advantages, limitations, and technical subtleties of employing FPGA-based digital servos for high-bandwidth feedback control of lasers in atomic, molecular, and optical (AMO) physics experiments. Specifically, we provide the results of benchmark performance tests in experimental setups including noise, bandwidth, and dynamic range for two digital servos built with low and mid-range priced FPGA development platforms. The digital servo results are compared to results obtained from a commercially available state-of-the-art analog servo using the same plant for control (intensity stabilization). The digital servos have feedback bandwidths of 2.5 MHz, limited by the total signal latency, and we demonstrate improvements beyond the transfer function offered by the analog servo including a three pole filter and a two pole filter with phase compensation to suppress resonances. We also discuss limitations of our FPGA-servo implementation and general considerations when designing and using digital servos.

physics.ins-det↗

arXiv2015

Transforming a 4th year Modern Optics Course Using a Deliberate Practice Framework

We present a study of active learning pedagogies in an upper division physics course. This work was guided by the principle of deliberate practice for the development of expertise, and this principle was used in the design of the materials and the orchestration of the classroom activities of the students. We present our process for efficiently converting a traditional lecture course based on instructor notes into activities for such a course with active learning methods. Ninety percent of the same material was covered and scores on common exam problems showed a 15 % improvement with an effect size greater than 1 after the transformation. We observe that the improvement and the associated effect size is sustained after handing off the materials to a second instructor. Because the improvement on exam questions was independent of specific problem topics and because the material tested was so mathematically advanced and broad (including linear algebra, Fourier Transforms, partial differential equations, vector calculus), we expect the transformation process could be applied to most upper division physics courses having a similar mathematical base.

physics.ed-ph↗

arXiv2013

High resolution photoassociation spectroscopy of the $^{6}$Li$_2$ $1^{3}Σ_{g}^{+}$ state

We present experimental observations of seven vibrational levels $v'=20-26$ of the $1^{3}Σ_{g}^{+}$ excited state of Li$_2$ molecules by the photoassociation (PA) of a degenerate Fermi gas of $^6$Li atoms. For each vibrational level, we resolve the rotational structure using a Feshbach resonance to enhance the PA rates from p-wave collisions. We also, for the first time, determine the spin-spin and spin-rotation interaction constants for this state. The absolute uncertainty of our measurements is $\pm 0.00002$ cm$^{-1}$ ($\pm 600$ kHz). We use these new data to further refine an analytic potential for this state.

physics.atom-ph↗