@article{frick_sridhar_khansari_comstock_norman_o'donnell_maggard_sun_dougherty_2023, title={Spreading resistance effects in tunneling spectroscopy of α-RuCl3 and Ir0.5Ru0.5Cl3}, volume={108}, ISSN={["2469-9969"]}, url={https://doi.org/10.1103/PhysRevB.108.245410}, DOI={10.1103/PhysRevB.108.245410}, abstractNote={The Mott insulating state is the progenitor of many interesting quantum phases of matter including the famous high-temperature superconductors and quantum spin liquids. A recent candidate for novel spin liquid phenomena is $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$, a layered honeycomb Mott insulator whose electronic structure has been a source of mystery. In particular, scanning tunneling spectroscopy has indicated a Mott gap in $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$ that is much lower than the 2-eV value observed in photoemission measurements. Here, we show that the origin of this discrepancy is a spreading resistance artifact associated with tunneling into highly resistive materials by comparing with prior experiments and numerical modeling. A similar phenomenon is also observed in a substitutional alloy, ${\mathrm{Ir}}_{0.5}{\mathrm{Ru}}_{0.5}{\mathrm{Cl}}_{3}$, that has a higher resistivity than the parent compound. While the tunneling measurements cannot be used to accurately measure the sample density of states for these materials, we can take advantage of the spreading resistance sensitivity to quantify the anisotropic resistivity of these layered materials and connect to previous macroscopic transport observations.}, number={24}, journal={PHYSICAL REVIEW B}, author={Frick, Jordan R. and Sridhar, Samanvitha and Khansari, Ario and Comstock, Andrew H. and Norman, Elizabeth and O'Donnell, Shaun and Maggard, Paul A. and Sun, Dali and Dougherty, Daniel B.}, year={2023}, month={Dec} } @article{worku_ben-akacha_sridhar_frick_yin_he_robb_chaaban_liu_winfred_et al._2021, title={Band Edge Control of Quasi-2D Metal Halide Perovskites for Blue Light-Emitting Diodes with Enhanced Performance}, volume={8}, ISSN={["1616-3028"]}, DOI={10.1002/adfm.202103299}, abstractNote={Perovskite light‐emitting diodes (PeLEDs) have received great attention for their potential as next‐generation display technology. While remarkable progress has been achieved in green, red, and near‐infrared PeLEDs with external quantum efficiencies (EQEs) exceeding 20%, obtaining high performance blue PeLEDs remains a challenge. Poor charge balance due to large charge injection barriers in blue PeLEDs has been identified as one of the major roadblocks to achieve high efficiency. Here band edge control of perovskite emitting layers for blue PeLEDs with enhanced charge balance and device performance is reported. By using organic spacer cations with different dipole moments, that is, phenethyl ammonium (PEA), methoxy phenethyl ammonium (MePEA), and 4‐fluoro phenethyl ammonium (4FPEA), the band edges of quasi‐2D perovskites are tuned without affecting their band gaps. Detailed characterization and computational studies have confirmed the effect of dipole moment modification to be mostly electrostatic, resulting in changes in the ionization energies of ≈0.45 eV for MePEA and ≈ −0.65 eV for 4FPEA based thin films relative to PEA‐based thin films. With improved charge balance, blue PeLEDs based on MePEA quasi‐2D perovskites show twofold increase of the EQE as compared to the control PEA based devices.}, journal={ADVANCED FUNCTIONAL MATERIALS}, author={Worku, Michael and Ben-Akacha, Azza and Sridhar, Samanvitha and Frick, Jordan R. and Yin, Shichen and He, Qingquan and Robb, Alex J. and Chaaban, Maya and Liu, He and Winfred, J. S. Raaj Vellore and et al.}, year={2021}, month={Aug} } @article{pazoki_frick_dougherty_2021, title={Dynamics of domain boundaries at metal-organic interfaces}, volume={154}, ISSN={["1089-7690"]}, DOI={10.1063/5.0029313}, abstractNote={Domain boundaries are a determining factor in the performance of organic electronic devices since they can trap mobile charge carriers. We point out the possibility of time-dependent motion of these boundaries and suggest that their thermal fluctuations can be a source of dynamic disorder in organic films. In particular, we study the C8-BTBT monolayer films with several different domain boundaries. After characterizing the crystallography and diversity of structures in the first layer of C8-BTBT on Au(111), we focus on quantifying the domain boundary fluctuations in the saturated monolayer. We find that the mean squared displacement of the boundary position grows linearly with time at early times but tends to saturate after about 7 s. This behavior is ascribed to confined diffusion of the interface position based on fits and numerical integration of a Langevin equation for the interface motion.}, number={12}, journal={JOURNAL OF CHEMICAL PHYSICS}, author={Pazoki, Sara and Frick, Jordan and Dougherty, Daniel B.}, year={2021}, month={Mar} } @article{nevola_bataller_kumar_sridhar_frick_o'donnell_ade_maggard_kemper_gundogdu_et al._2021, title={Timescales of excited state relaxation in alpha-RuCl3 observed by time-resolved two-photon photoemission spectroscopy}, volume={103}, ISSN={["2469-9969"]}, url={https://doi.org/10.1103/PhysRevB.103.245105}, DOI={10.1103/PhysRevB.103.245105}, abstractNote={The nonequilibrium properties of strongly correlated materials present a target in the search for new phases of matter. It is important to observe the types of excitations that exist in these materials and their associated relaxation dynamics. We have studied the photoexcitations in a spin-orbit assisted Mott insulator $\ensuremath{\alpha}\text{\ensuremath{-}}\mathrm{Ru}{\mathrm{Cl}}_{3}$ using time-resolved two-photon photoemission spectroscopy and transient reflection spectroscopy. We find that photoexcited carriers (doublons) in the upper Hubbard band rapidly relax to Mott-Hubbard excitons on a timescale of less than 200 fs. Subsequently, further relaxation of these lower-energy quasiparticles occurs with an energy-dependent time constant of that ranges from 370 to 600 fs due to exciton cooling. The population of Mott-Hubbard excitons persists for timescales up to several microseconds.}, number={24}, journal={PHYSICAL REVIEW B}, author={Nevola, Dan and Bataller, Alexander and Kumar, Ankit and Sridhar, Samanvitha and Frick, Jordan and O'Donnell, Shaun and Ade, Harald and Maggard, Paul A. and Kemper, Alexander F. and Gundogdu, Kenan and et al.}, year={2021}, month={Jun} } @article{frick_sridhar_o'donnell_maggard_dougherty_2020, title={An interface-controlled Mott memristor in α-RuCl3}, volume={116}, ISSN={0003-6951 1077-3118}, url={http://dx.doi.org/10.1063/5.0009670}, DOI={10.1063/5.0009670}, abstractNote={Memristor devices have history-dependent charge transport properties that are ideal for neuromorphic computing applications. We reveal a memristor material and mechanism in the layered Mott insulator α-RuCl3. The pinched hysteresis loops and S-shaped negative differential resistance in bulk crystals verify memristor behavior and are attributed to a nonlinear coupling between charge injection over a Schottky barrier at the electrical contacts and concurrent Joule heating. Direct simulations of this coupling can reproduce the device characteristics.}, number={18}, journal={Applied Physics Letters}, publisher={AIP Publishing}, author={Frick, Jordan R. and Sridhar, Samanvitha and O'Donnell, Shaun and Maggard, Paul A. and Dougherty, Daniel B.}, year={2020}, month={May}, pages={183501} }