Iris Stone, PhD

Latent linear dynamical systems with Bernoulli observations provide a powerful modeling framework for identifying the temporal dynamics underlying binary time series data, which arise in a variety of contexts such as binary decision-making and discrete stochastic processes such as binned neural spike trains. Here, we develop a spectral learning method for fast, efficient fitting of Bernoulli latent linear dynamical system (LDS) models. Our approach extends traditional subspace identification… Show more

Latent linear dynamical systems with Bernoulli observations provide a powerful modeling framework for identifying the temporal dynamics underlying binary time series data, which arise in a variety of contexts such as binary decision-making and discrete stochastic processes such as binned neural spike trains. Here, we develop a spectral learning method for fast, efficient fitting of Bernoulli latent linear dynamical system (LDS) models. Our approach extends traditional subspace identification methods to the Bernoulli setting via a transformation of the first and second sample moments. This results in a robust, fixed-cost estimator that avoids the hazards of local optima and the long computation time of iterative fitting procedures like the expectation-maximization (EM) algorithm. In regimes where data is limited or assumptions about the statistical structure of the data are not met, we demonstrate that the spectral estimate provides a good initialization for Laplace-EM fitting. Finally, we show that the estimator provides substantial benefits to real world settings by analyzing data from mice performing a sensory decision-making task. Show less

Charge transfer (CT) cocrystals, molecular crystals composed of electron donating and accepting species, are being developed for applications in optoelectronics. Here we present optical and electronic characterization of the CT cocrystal phenothiazine–tetracyanoquinodimethane (PTZ–TCNQ). This material has a broad NIR absorption peak with an optical band edge less than 0.6 eV. We used density functional theory calculations to identify the origin of the low energy CT states and changes in the… Show more

Charge transfer (CT) cocrystals, molecular crystals composed of electron donating and accepting species, are being developed for applications in optoelectronics. Here we present optical and electronic characterization of the CT cocrystal phenothiazine–tetracyanoquinodimethane (PTZ–TCNQ). This material has a broad NIR absorption peak with an optical band edge less than 0.6 eV. We used density functional theory calculations to identify the origin of the low energy CT states and changes in the Raman spectra. We also demonstrate the fabrication of long, ribbon-like oriented cocrystals using an evaporative alignment method. Cocrystals grown on Si substrates were fabricated into organic field effect transistors. Despite theoretical predictions of ambipolarity, only electron conduction was observed, with mobilities on the order of 10–4 cm2 V–1 s–1. Measurements of the temperature dependence of the mobility indicated a superexchange mediated hopping mechanism for charge transport, with a characteristic energy scale of 0.19 eV. Show less

A classic view of the striatum holds that activity in direct and indirect pathways oppositely modulates motor output. Whether this involves direct control of movement, or reflects a cognitive process underlying movement, has remained unresolved. Here we find that strong, opponent control of behavior by the two pathways of the dorsomedial striatum (DMS) depends on a task9s cognitive demands. Furthermore, a latent state model (a hidden markov model with generalized linear model observations)… Show more

A classic view of the striatum holds that activity in direct and indirect pathways oppositely modulates motor output. Whether this involves direct control of movement, or reflects a cognitive process underlying movement, has remained unresolved. Here we find that strong, opponent control of behavior by the two pathways of the dorsomedial striatum (DMS) depends on a task9s cognitive demands. Furthermore, a latent state model (a hidden markov model with generalized linear model observations) reveals that - even within a single task - the contribution of the two pathways to behavior is state-dependent. Specifically, the two pathways have large contributions in one of two states associated with a strategy of evidence accumulation, compared to a state associated with a strategy of repeating previous choices. Thus, both the cognitive demands imposed by a task, as well as the strategy that mice pursue within a task, determine whether DMS pathways provide strong and opponent control of behavior. Show less

Classical models of perceptual decision-making assume that animals use a single, consistent strategy to form decisions, or that decision-making strategies evolve slowly over time. Here we present new analyses suggesting that this common view is incorrect. We analyzed data from two mouse decision-making experiments and found that choice behavior relies on an interplay between multiple interleaved strategies. These strategies, characterized by states in a hidden Markov model, persist for tens to… Show more

Classical models of perceptual decision-making assume that animals use a single, consistent strategy to form decisions, or that decision-making strategies evolve slowly over time. Here we present new analyses suggesting that this common view is incorrect. We analyzed data from two mouse decision-making experiments and found that choice behavior relies on an interplay between multiple interleaved strategies. These strategies, characterized by states in a hidden Markov model, persist for tens to hundreds of trials before switching, and may alternate multiple times within a session. The identified strategies were highly consistent across animals, consisting of a single "engaged" state, in which decisions relied heavily on the sensory stimulus, and several biased or disengaged states in which errors frequently occurred. These results provide a powerful alternate explanation for "lapses" often observed in psychophysical experiments, and suggest that standard measures of performance mask the presence of dramatic changes in strategy across trials. Show less

The structural polymorphism in transition metal dichalcogenides (TMDs) provides exciting opportunities for developing advanced electronics. For example, MoTe2 crystallizes in the 2H semiconducting phase at ambient temperature and pressure, but transitions into the 1T' semimetallic phase at high temperatures. Alloying MoTe2 with WTe2 reduces the energy barrier between these two phases, while also allowing access to the T d Weyl semimetal phase. The $\text{M}{{\text{o}}_{1-\text{x}}}$ WxTe2 alloy… Show more

The structural polymorphism in transition metal dichalcogenides (TMDs) provides exciting opportunities for developing advanced electronics. For example, MoTe2 crystallizes in the 2H semiconducting phase at ambient temperature and pressure, but transitions into the 1T' semimetallic phase at high temperatures. Alloying MoTe2 with WTe2 reduces the energy barrier between these two phases, while also allowing access to the T d Weyl semimetal phase. The $\text{M}{{\text{o}}_{1-\text{x}}}$ WxTe2 alloy system is therefore promising for developing phase change memory technology. However, achieving this goal necessitates a detailed understanding of the phase composition in the MoTe2-WTe2 system. We combine polarization-resolved Raman spectroscopy with x-ray diffraction (XRD) and scanning transmission electron microscopy (STEM) to study bulk $\text{M}{{\text{o}}_{1-\text{x}}}$ WxTe2 alloys over the full compositional range x from 0 to 1. We identify Raman and XRD signatures characteristic of the 2H, 1T', and T d structural phases that agree with density-functional theory (DFT) calculations, and use them to identify phase fields in the MoTe2–WTe2 system, including single-phase 2H, 1T', and T d regions, as well as a two-phase 1T'  +  T d region. Disorder arising from compositional fluctuations in $\text{M}{{\text{o}}_{1-\text{x}}}$ WxTe2 alloys breaks inversion and translational symmetry, leading to the activation of an infrared 1T'-MoTe2 mode and the enhancement of a double-resonance Raman process in $\text{2H-M}{{\text{o}}_{1-\text{x}}}$ WxTe2 alloys. Compositional fluctuations limit the phonon correlation length, which we estimate by fitting the observed asymmetric Raman lineshapes with a phonon confinement model. These observations reveal the important role of disorder in $\text{M}{{\text{o}}_{1-\text{x}}}$ WxTe2 alloys, clarify the structural phase boundaries, and provide a foundation for future explorations of phase transitions and electronic phenomena in this system. Show less

We examine anharmonic contributions to the optical phonon modes in bulk Td-MoTe2 through temperature-dependent Raman spectroscopy. At temperatures ranging from 100 K to 200 K, we find that all modes redshift linearly with temperature in agreement with the Grüneisen model. However, below 100 K, we observe nonlinear temperature-dependent frequency shifts in some modes. We demonstrate that this anharmonic behavior is consistent with the decay of an optical phonon into multiple acoustic phonons… Show more

We examine anharmonic contributions to the optical phonon modes in bulk Td-MoTe2 through temperature-dependent Raman spectroscopy. At temperatures ranging from 100 K to 200 K, we find that all modes redshift linearly with temperature in agreement with the Grüneisen model. However, below 100 K, we observe nonlinear temperature-dependent frequency shifts in some modes. We demonstrate that this anharmonic behavior is consistent with the decay of an optical phonon into multiple acoustic phonons. Furthermore, the highest frequency Raman modes show large changes in intensity and linewidth near T ≈ 250 K that correlate well with the Td→1T′ structural phase transition. These results suggest that phonon-phonon interactions can dominate anharmonic contributions at low temperatures in bulk Td-MoTe2, an experimental regime that is currently receiving attention in efforts to understand Weyl semimetals. Show less