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At least 685 records · Page 38

Twisted Crystalline Organic Semiconductor Photodetectors

Optoelectronic properties of anisotropic crystals vary with direction requiring that the orientation of molecular organic semiconductor crystals is controlled in optoelectronic device active layers to achieve optimal performance. Here, in this work, a generalizable strategy to introduce periodic variations in the out-of-plane orientations of 5,11-bis(triisopropylsilylethynyl)anthradithiophene (TIPS ADT) crystals is presented. TIPS ADT crystallized from the melt in the presence of 16 wt.% polyethylene (PE) forms banded spherulites of crystalline fibrils that twist in concert about the radial growth direction. These spherulites exhibit band-dependent light absorption, photoluminescence, and Raman scattering depending on the local orientation of crystals. Mueller matrix imaging reveals strong circular extinction (CE), with TIPS ADT banded spherulites exhibiting domains of positive or negative CE signal depending on the crystal twisting sense. Furthermore, orientation-dependent enhancement in charge injection and extraction in films of twisted TIPS ADT crystals compared to films of straight crystals is visualized in local conductive atomic force microscopy maps. This enhancement leads to 3.3- and 6.2-times larger photocurrents and external quantum efficiencies, respectively, in photodetectors comprising twisted crystals than those comprising straight crystals.

36 MATERIALS SCIENCE↗

Jarzynski Equality for Conditional Stochastic Work

It has been established that the inclusive work for classical, Hamiltonian dynamics is equivalent to the two-time energy measurement paradigm in isolated quantum systems. However, a plethora of other notions of quantum work has emerged, and thus the natural question arises whether any other quantum notion can provide motivation for purely classical considerations. In the present analysis, we propose the conditional stochastic work for classical, Hamiltonian dynamics, which is inspired by the one-time measurement approach. This novel notion is built upon the change of expectation value of the energy conditioned on the initial energy surface. As main results, we obtain a generalized Jarzynski equality and a sharper maximum work theorem, which account for how non-adiabatic the process is. Our findings are illustrated with the parametric harmonic oscillator.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

H 0 ex machina: Vacuum metamorphosis and beyond H 0

Here, we do not solve tensions with concordance cosmology; we do obtain H 0 ≈ 74 km/s/Mpc from CMB+BAO+SN data in our model, but that is not the point. Discrepancies in Hubble constant values obtained by various astrophysical probes should not be viewed in isolation. While one can resolve at least some of the differences through either an early time transition or late time transition in the expansion rate, these introduce other changes. We advocate a holistic approach, using a wide variety of cosmic data, rather than focusing on one number, H 0 . Vacuum metamorphosis, a late time transition physically motivated by quantum gravitational effects and with the same number of parameters as ΛCDM, can successfully give a high H 0 value from cosmic microwave background data but fails when combined with multiple distance probes. We also explore the influence of spatial curvature, and of a conjoined analysis of cosmic expansion and growth.

79 ASTRONOMY AND ASTROPHYSICS↗

Do atoms age?

Time evolution generically entangles a quantum state with environmental degrees of freedom. The resulting increase in entropy changes the properties of that quantum system leading to “aging”. It is interesting to ask if this familiar property also applies to simple, single particle quantum systems such as the decay of a radioactive particle. We propose a test of such aging in an ion clock setup where we probe for temporal changes to the energies of the electronic state of an ion containing a radioactive nucleus. Such effects are absent in standard quantum mechanics and this test is thus a potent null test for violations of quantum mechanics. As a proof of principle, we show that these effects exist in causal non-linear modifications of quantum mechanics.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Automated Construction of Artificial Lattice Structures with Designer Electronic States

Manipulating matter with a scanning tunneling microscope (STM) enables the creation of atomically defined artificial structures that host designer quantum states. However, the time-consuming nature of the manipulation process, coupled with the sensitivity of the STM tip, constrains the exploration of diverse configurations and limits the size of the designed features. In this study, we present a reinforcement learning (RL)-based framework for creating artificial structures by spatially manipulating carbon monoxide (CO) molecules on a copper substrate by using the STM tip. The automated workflow combines molecule detection and manipulation, employing deep-learning-based object detection to locate CO molecules and linear assignment algorithms to allocate these molecules to designated target sites. We initially perform molecule maneuvering based on randomized parameter sampling for sample bias, tunneling current set point, and manipulation speed. This data set is then structured into an action trajectory used to train an RL agent. The model is subsequently deployed on the STM for real-time fine-tuning of the manipulation parameters during structure construction. Our approach incorporates path-planning protocols coupled with active drift compensation to enable atomically precise fabrication of structures with significantly reduced human input while realizing larger-scale artificial lattices with the desired electronic properties. Furthermore, using our approach, we demonstrate the automated construction of an extended artificial graphene lattice and confirm the existence of a characteristic Dirac point in its electronic structure. Further challenges regarding the RL-based structural assembly scalability are discussed.

Algorithms↗

Enhancing spectroscopy and microscopy with emerging methods in photon correlation and quantum illumination

Quantum optics has led to important advancements in our ability to prepare and detect correlations between individual photons. Its principles are increasingly translated into nanoscale characterization tools, furthering methods in spectroscopy, microscopy and metrology. Here, in this Review, we discuss the rapid progress in this field driven by advanced technologies of single-photon detectors and quantum-light sources, including time-resolved single-photon counting cameras, superconducting nanowire single-photon detectors and entangled photon sources of increasing brightness. We emphasize emerging applications in super-resolution microscopy, measurements below classical noise limits and photon-number-resolved spectroscopy—a powerful paradigm for the characterization of nanoscale electronic materials. We conclude by discussing key technological challenges and future opportunities in materials science and bionanophotonics alike.

Tsao, Chieh [University of California, Berkeley, C↗

Tuning the optical and magnetic properties of lanthanide single-ion magnets using nitro-functionalized trispyrazolylborate ligands

We report the synthesis, crystal structures, photophysical and magnetic properties of 11 novel lanthanide complexes with the asymmetrically functionalized trispyrazolylborate ligand 4-nitrotrispyrazolylborate, 4-NO 2 Tp–: [Ln(4-NO 2 Tp) 3 ] (Ln = La–Dy, except Pm). In-depth photophysical characterization of the ligands via luminescence, reflectance and absorption spectroscopic techniques, decay lifetimes, quantum yields supported by time-dependent density functional theory (TD-DFT) and natural bond order (NBO) analysis reveal that n-NO 2 Tp– ligands are dominated by intra-ligand charge transfer (ILCT) transitions and that second-sphere interactions are critical to the stabilization of the T 1 state of n-NO 2 Tp– ligands and hence their ability to sensitize Ln 3+ emission. The luminescence properties of the complexes indicate that 4-NO 2 Tp– is a poor sensitizer of Ln 3+ emission, unlike 3-NO 2 Tp–. Moreover, [Nd(4-NO 2 Tp) 3 ] (crystallized as a hexane solvate) displays single-molecule magnet (SMM) properties, with longer relaxation times and larger barrier than the non-functionalized [NdTp 3 ], attributed to the addition of the NO 2 -group and subsequent rigidification of the molecular structure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The interplay between chromophore and protein determines the extended excited state dynamics in a single-domain phytochrome

Phytochromes are a diverse family of bilin-binding photoreceptors that regulate a wide range of physiological processes. Their photochemical properties make them attractive for applications in optogenetics and superresolution microscopy. Phytochromes undergo reversible photoconversion triggered by the Z ⇌ E photoisomerization about the double bond in the bilin chromophore. However, it is not fully understood at the molecular level how the protein framework facilitates the complex photoisomerization dynamics. In this work, we have studied a single-domain bilin-binding photoreceptor All2699g1 ( Nostoc sp. PCC 7120) that exhibits photoconversion between the red light-absorbing (P r ) and far red-absorbing (P fr ) states just like canonical phytochromes. We present the crystal structure and examine the photoisomerization mechanism of the P r form as well as the formation of the primary photoproduct Lumi-R using time-resolved spectroscopy and hybrid quantum mechanics/molecular mechanics simulations. We show that the unusually long excited state lifetime (broad lifetime distribution centered at ~300 picoseconds) is due to the interactions between the isomerizing pyrrole ring D and an adjacent conserved Tyr142. The decay kinetics shows a strongly distributed character which is imposed by the nonexponential protein dynamics. Our findings offer a mechanistic insight into how the quantum efficiency of the bilin photoisomerization is tuned by the protein environment, thereby providing a structural framework for engineering bilin-based optical agents for imaging and optogenetics applications.

59 BASIC BIOLOGICAL SCIENCES↗

Ultrafast Events in Electrocyclic Ring-Opening Reactions

Electrocyclic reactions are characterized by the concerted formation and cleavage of multiple σ and π bonds in a molecular system and have been extensively studied since they were introduced by Robert Burns Woodward and Roald Hoffmann in 1965. Recent advances and the integration of time-resolved experiments and nonadiabatic quantum molecular dynamics simulations have transformed the traditional understanding of electrocyclic reactions beyond the Woodward–Hoffmann rules. In this review, we focus on recent studies of 1,3-cyclohexadiene and two of its derivatives, α-phellandrene and α-terpinene, to shed light on the underlying mechanisms of electrocyclic photochemical reactions. We highlight recent progress in ultrafast electron diffraction techniques and the simulation approach of ab initio multiple spawning. Together, these approaches can elucidate molecular structure dynamics from femtosecond to picosecond timescales as well as nuclear and electronic responses at conical intersections.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

F3C++ v0.1

Fast Free Fermion Compiler (F3C) is an application-specific quantum circuit compiler for time-evolution circuits of spin Hamiltonian systems that can be mapped to free fermions.

Van Beeumen, RoelMaria Franciscus↗

F3C v0.1

Fast Free Fermion Compiler (F3C) is an application-specific quantum circuit compiler for time-evolution circuits of spin Hamiltonian systems that can be mapped to free fermions. F3C is the Matlab software version and the related F3C++ is the C++ software version.

Van Beeumen, RoelMaria Franciscus↗

Control and Calibration of GlueX Central Drift Chamber Using Gaussian Process Regression

The Gluonic Excitations (GlueX) experiment is designed to search for exotic hybrid mesons using photoproduction, and to study the hybrid meson spectrum predicted from Lattice Quantum Chromodynamics. For the first time, the GlueX Central Drift Chamber was controlled autonomously using machine learning (ML) to calibrate in real time while recording cosmic ray tracks. We demonstrate the ability of a Gaussian Process to predict the gain correction calibration factor used to determine a high voltage setting that will stabilize the CDC gain in response to changing environmental conditions; this is in contrast to the traditional, computationally expensive method of calibrating raw data after data collection is complete.

McSpadden, Helen↗

Fusing 4D coded thermoacoustic, electromagnetic, and acoustic/seismic wavefields for subsurface characterization and imaging of fluid flow in porous media

This research program aims to address critical challenges in subsurface exploration and monitoring of anthropogenic CO 2 storage by advancing quantitative dynamic sensing and imaging technologies. Two primary applications—petrophysical assessment of hydrocarbon reservoirs (C1) and CO 2 storage monitoring (C2)—require significant innovation to overcome three barriers (B1-B3). These barriers include the need for enhanced understanding of interactions between physical wave fields (thermoacoustic, electromagnetic, acoustic/seismic, and X-ray) with fluid-filled porous media, the development of multi-sensor data fusion for real-time imaging, and upscaling microscopic quantum effects for macroscopic observations. The project’s objective was to establish a unified 4D coded sensing and imaging approach, integrating EM, AC/S, and TA fields for multi-scale and multi-physics material characterization and subsurface imaging.

58 GEOSCIENCES↗

How Quantum Sensing Will Help Solve GPS Denial in Warfare

The U.S. military’s ability to posture, deter, and prevail in future conflicts may rest on the quantum sensing position, navigation, and timing (PNT) capabilities that are currently being developed. Heavy reliance on GPS signals for PNT has become a critical vulnerability for the U.S. military. Meanwhile, the conflict in Ukraine has demonstrated that GPS denial and electronic warfare (EW) is now a key component of modern combat and satellite-guided munitions are reportedly being rendered ineffective. The Department of Defense (DOD) is focusing on upgrading GPS to use stronger, military-specific signals, which will still be vulnerable to EW and anti-satellite capabilities. A more diverse and resilient alternate-PNT strategy is needed to ensure mission success.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

When does a particle arrive?

We compare the proposals that have appeared in the literature to describe a measurement of the time of arrival of a quantum particle at a detector. We show that there are multiple regimes where different proposals give inequivalent, experimentally discriminable, predictions. This analysis paves the way for future experimental tests.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Quantum noise and the threshold of hearing

It is argued that the sensitivity of the ear reaches a limit imposed by the uncertainty principle. This is possible only if the receptor cell holds the detector elements in a special nonequilibrium state which has the same noise characteristics as a ground (T = 0 K) state. To accomplish this 'active cooling' the molecular dynamics of the system must maintain quantum mechanical coherence over the time scale of the measurement.

Bialek, W.↗

Toward astrometric tracking with the infrared spatial interferometer

Infrared interferometric demonstrations with the University of California, Berkeley's infrared spatial interferometer (ISI) on Mt. Wilson explore the potential of infrared and optical astrometry for deep space tracking, reference frame development, and DSN science. Astrometric data taken and analyzed over the last five years from the ISI have shown that instrumental and atmospheric effects limit current demonstrations. The benefits of sensitivity upgrades, which were performed in 1991 and 1992, have been demonstrated by comparing point-to-point phase fluctuations for the fall 1989 and fall 1992 observing epochs. This comparison showed that point-to-point phase fluctuations due to tropospheric and quantum noise, for optimal integration times of 0.2 sec, are approaching the 0.1-cycle level needed to reliably connect the interferometric phase. The increase in sensitivity, coupled with that arising from very recent hardware upgrades, will greatly enhance phase-connection capabilities necessary for astrometry in the presence of atmospheric refractivity fluctuations. The current data set suggests that atmospheric fluctuations on Mt. Wilson during the best seeing are dominated by a low-lying component, approximately 25 m high, which may be minimized with in situ calibration in the future. During poor seeing conditions that currently prohibit the interferometric phase connection necessary for astrometry, fluctuations seem to be generated by atmospheric inhomogeneities at much higher altitudes above Mt. Wilson. Data taken over the last year suggest that the ISI will soon be able to achieve 50- to 100-nrad astrometry in a single observing session, employing current ground-based laser distance interferometer calibrations to minimize atmospheric effects.

Treuhaft, R. N.↗