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1.
J Phys Chem A ; 128(15): 2971-2981, 2024 Apr 18.
Article in English | MEDLINE | ID: mdl-38579334

ABSTRACT

In our experiment, a trace amount of an organic molecule (M = 1H-phenalen-1-one, 9-fluorenone, pyridine, or acridine) was seeded into a gas mix consisting of 3% O2 with a rare gas buffer (He or Ar) and then supersonically expanded. We excited the resulting molecular beam with ultraviolet light at either 355 nm (1H-phenalen-1-one, 9-fluorenone, or acridine) or 266 nm (pyridine) and used resonance enhanced multiphoton ionization (REMPI) spectroscopy to probe for the formation of O2 in the a-1Δg state, 1O2. For all systems, the REMPI spectra demonstrate that ultraviolet excitation results in the formation of 1O2 and the oxygen product is confirmed to be in the ground vibrational state and with an effective rotational temperature below 80 K. We then recorded the velocity map ion image of the 1O2 product. From the ion images, we determined the center-of-mass translational energy distribution, P(ET), assuming photodissociation of a bimolecular M-O2 complex. We also report results from electronic structure calculations that allow for a determination of the M-O2 ground state binding energy. We use the complex binding energy, the energy to form 1O2, and the adiabatic triplet energy for each organic molecule to determine the available energy following photodissociation. For dissociation of a bimolecular complex, this available energy may be partitioned into either center-of-mass recoil or internal degrees of freedom of the organic moiety. We use the available energy to generate a Prior distribution, which predicts statistical energy partitioning during dissociation. For low available energies, less than 0.2 eV, we find that the statistical prediction is in reasonable agreement with the experimental observations. However, at higher available energies, the experimental distribution is biased to lower center-of-mass kinetic energies compared with the statistical prediction, which suggests the complex undergoes vibrational predissociation.

2.
JMIR Pediatr Parent ; 7: e51570, 2024 Aug 13.
Article in English | MEDLINE | ID: mdl-39137019

ABSTRACT

BACKGROUND: Youth suicide is a pressing public health concern, and transitions in care after a suicidal crisis represent a period of elevated risk. Disruptions in continuity of care and emotional support occur frequently. "Caring contacts" validating messages post discharge have the potential to enhance connections with patients and have been shown to improve outcomes. More recently, positive outcomes have been noted using caring contact text messages (SMS and MMS), which hold promise for engaging patients in a pediatric setting, but there are few studies describing the large-scale implementation of such an approach. OBJECTIVE: This study aims to describe the process of developing and implementing automated caring contacts within a quality improvement framework, using a standardized series of supportive texts and images, for adolescents discharged from high-acuity programs at a large midwestern pediatric hospital. We describe lessons learned, including challenges and factors contributing to success. METHODS: We implemented the caring contacts intervention in 3 phases. Phase 1 entailed developing supportive statements and images designed to promote hope, inclusivity, and connection in order to create 2 sets of 8 text messages and corresponding images. Phase 2 included piloting caring contacts manually in the hospital's Psychiatric Crisis Department and Inpatient Psychiatry Unit and assessing the feasibility of implementation in other services, as well as developing workflows and addressing legal considerations. Phase 3 consisted of implementing an automated process to scale within 4 participating hospital services and integrating enrollment into the hospital's electronic medical records. Process outcome measures included staff compliance with approaching and enrolling eligible patients and results from an optional posttext survey completed by participants. RESULTS: Compliance data are presented for 4062 adolescent patients eligible for caring contacts. Overall, 88.65% (3601/4062) of eligible patients were approached, of whom 52.43% (1888/3601) were enrolled. In total, 94.92% (1792/1888) of enrolled participants completed the program. Comparisons of the patients eligible, approached, enrolled, and completed are presented. Primary reasons for eligible patients declining include not having access to a mobile phone (686/1705, 40.23%) and caregivers preferring to discuss the intervention at a later time (754/1705, 44.22%). The majority of patients responding to the optional posttext survey reported that the texts made them feel moderately to very hopeful (219/264, 83%), supported (232/264, 87.9%), that peers would be helped by these texts (243/264, 92%), and that they would like to keep receiving texts given the option (227/264, 86%). CONCLUSIONS: This study describes the successful implementation of automated postdischarge caring contacts texts to scale with an innovative use of images and demonstrates how a quality improvement methodology resulted in a more effective and efficient process. This paper also highlights the potential for technology to enhance care for at-risk youth and create more accessible, inclusive, and sustainable prevention strategies.

3.
Nat Commun ; 15(1): 3630, 2024 May 01.
Article in English | MEDLINE | ID: mdl-38693113

ABSTRACT

Effective control of magnetic phases in two-dimensional magnets would constitute crucial progress in spintronics, holding great potential for future computing technologies. Here, we report a new approach of leveraging tunneling current as a tool for controlling spin states in CrI3. We reveal that a tunneling current can deterministically switch between spin-parallel and spin-antiparallel states in few-layer CrI3, depending on the polarity and amplitude of the current. We propose a mechanism involving nonequilibrium spin accumulation in the graphene electrodes in contact with the CrI3 layers. We further demonstrate tunneling current-tunable stochastic switching between multiple spin states of the CrI3 tunnel devices, which goes beyond conventional bi-stable stochastic magnetic tunnel junctions and has not been documented in two-dimensional magnets. Our findings not only address the existing knowledge gap concerning the influence of tunneling currents in controlling the magnetism in two-dimensional magnets, but also unlock possibilities for energy-efficient probabilistic and neuromorphic computing.

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