A fundamental challenge in quantum thermodynamics is the exploration of inherent dimensional constraints in thermodynamic machines. In the context of two-level systems, the most compact refrigerator necessitates the involvement of three entities, operating under self-contained conditions that preclude the use of external work sources. Here, we build such a smallest refrigerator using a nuclear spin system, where three distinct two-level carbon-13 nuclei in the same molecule are involved to facilitate the refrigeration process. The self-contained feature enables it to operate without relying on net external work, and the unique mechanism sets this refrigerator apart from its classical counterparts. We evaluate its performance under varying conditions and systematically scrutinize the cooling constraints across a spectrum of scenarios, which sheds light on the interplay between quantum information and thermodynamics.
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http://dx.doi.org/10.1103/PhysRevLett.132.210403 | DOI Listing |
Molecules
December 2024
Department of Organic Chemistry, University of Valencia, Dr. Moliner 50, Burjassot, 46100 Valencia, Spain.
In this study, we investigated the [3+2] cycloaddition reaction of CFCN (TFAN) with nitrilimine (NI) to produce 1,2,4-triazole and compared the resulting isomers. We determined the preferred reaction pathway by examining the electrophilic and nucleophilic properties of the reaction substrates, performing thermodynamic calculations for the individual pathways, and comparing them with the experimental results.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
Department of Chemistry, The University of Hong Kong, Pokfulam Road, Hong Kong SAR 999077, China.
Electrochemical nitrate reduction to ammonia (NORR) is promising to not only tackle environmental issues caused by nitrate but also produce ammonia at room temperatures. However, two critical challenges are the lack of effective electrocatalysts and the understanding of related reaction mechanisms. To overcome these challenges, we employed first-principles calculations to thoroughly study the performance and mechanisms of triple-atom catalysts (TACs) composed of transition metals (including 27 homonuclear TACs and 4 non-noble bimetallic TACs) anchored on N-doped carbon (NC).
View Article and Find Full Text PDFAcc Chem Res
January 2025
Centre for Computational Chemistry, School of Chemistry, University of Bristol, Bristol BS8 1TS, United Kingdom.
ConspectusPhotochemical reactions have always been the source of a great deal of mystery. While classified as a type of chemical reaction, no doubts are allowed that the general tenets of ground-state chemistry do not directly apply to photochemical reactions. For a typical chemical reaction, understanding the critical points of the ground-state potential (free) energy surface and embedding them in a thermodynamics framework is often enough to infer reaction yields or characteristic time scales.
View Article and Find Full Text PDFJ Chem Phys
December 2024
Department of Chemical Sciences, Tata Institute of Fundamental Research, Mumbai 400005, India.
The Marcus semi-classical and quantum theories of electron transfer (ET) have been extensively used to understand and predict tunneling ET reaction rates in the condensed phase. Previously, the traditional Marcus two-state model has been extended to a three-state model, which assumes a harmonic dependence of donor (D), bridge (B), and acceptor (A) free energies on the reaction (e.g.
View Article and Find Full Text PDFNature
January 2025
Department of Physics and Astronomy, Rice University, Houston, TX, USA.
It is commonly believed that there are only two types of particle exchange statistics in quantum mechanics, fermions and bosons, with the exception of anyons in two dimensions. In principle, a second exception known as parastatistics, which extends outside two dimensions, has been considered but was believed to be physically equivalent to fermions and bosons. Here we show that non-trivial parastatistics inequivalent to either fermions or bosons can exist in physical systems.
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