Probing the real time dynamics of a reacting molecule remains one of the central challenges in chemistry. Here we show how the time-dependent wave function of an excited-state reacting molecule can be completely reconstructed from resonant coherent anti-Stokes Raman spectroscopy. The method assumes knowledge of the ground potential but not of any excited potential. The excited-state potential can in turn be constructed from the wave function. The formulation is general for polyatomics and applies to bound as well as dissociative excited potentials. We demonstrate the method on the Li(2) molecule.
Download full-text PDF |
Source |
|---|---|
| http://dx.doi.org/10.1103/PhysRevLett.106.170405 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Self-consistent Quantum Linear Response with a Polarizable Embedding Environment.
J Phys Chem A
January 2025
Department of Physics, Chemistry and Pharmacy, University of Southern Denmark, Campusvej 55, Odense M DK-5230, Denmark.
Quantum computing presents a promising avenue for solving complex problems, particularly in quantum chemistry, where it could accelerate the computation of molecular properties and excited states. This work focuses on computing excitation energies with hybrid quantum-classical algorithms for near-term quantum devices, combining the quantum linear response (qLR) method with a polarizable embedding (PE) environment. We employ the self-consistent operator manifold of quantum linear response (q-sc-LR) on top of a unitary coupled cluster (UCC) wave function in combination with a Davidson solver.
View Article and Find Full Text PDFNO Oxidation States in Nonheme Iron Nitrosyls: A DMRG-CASSCF Study of {FeNO} Complexes.
Inorg Chem
January 2025
Department of Chemistry, UiT The Arctic University of Norway, N-9037 Tromso̷, Norway.
Building upon an earlier study of heme-nitrosyl complexes (. , , 20496-20505), we examined a wide range of nonheme {FeNO} complexes (the superscript represents the Enemark-Feltham count) and two dinitrosyl iron complexes using DMRG-CASSCF calculations. Analysis of the wave functions in terms of resonance forms with different [π*(NO)] occupancies (where = 0-4 for mononitrosyl complexes) identified the dominant electronic configurations of {FeNO} and {FeNO} complexes as Fe-NO and Fe-NO, respectively, mirroring our previous findings on heme-nitrosyl complexes.
View Article and Find Full Text PDFSkeletal muscle elastic modulus in marathon distance runners.
Eur J Appl Physiol
January 2025
Nike Sport Research Lab, Nike, Inc., One Bowerman Drive, Beaverton, OR, 97005, USA.
Skeletal muscle shear elastic modulus is a non-invasive surrogate for early detection of muscle damage and soreness consequent to unaccustomed eccentric muscle work. We investigated the influence of marathon distance running on skeletal muscle shear elastic modulus. Shear modulus of the rectus femoris was measured via ultrasound shear wave elastography in 80 participants (30 female, 50 male) before and after running a World Marathon Major.
View Article and Find Full Text PDFCardiovascular Performance in Neonates with Hypoxic-Ischemic Encephalopathy Under Therapeutic Hypothermia: Evaluation by Conventional and Advanced Echocardiographic Techniques.
Pediatr Cardiol
January 2025
Echocardiography Laboratory, Instituto Dante Pazzanese de Cardiologia, São Paulo, Brazil.
This study aimed to evaluate the hemodynamic and ventricular performance of neonates with hypoxic-ischemic encephalopathy (HIE) undergoing therapeutic hypothermia using conventional and advanced echocardiographic techniques. This observational, prospective study included 22 neonates with HIE matched with 22 healthy neonates. Echocardiographic studies were performed 24 h after achieving target temperature during hypothermia and 24 h after rewarming.
View Article and Find Full Text PDFThe Best of Both Worlds: ΔDFT Describes Multiresonance TADF Emitters with Wave-Function Accuracy at Density-Functional Cost.
J Phys Chem Lett
January 2025
Mulliken Center for Theoretical Chemistry, Clausius Institute for Physical and Theoretical Chemistry, Rheinische Friedrich-Wilhelms Universität Bonn, Beringstraße 4, 53115 Bonn, Germany.
With their narrow-band emission, high quantum yield, and good chemical stability, multiresonance thermally activated delayed fluorescence (MR-TADF) emitters are promising materials for OLED technology. However, accurately modeling key properties, such as the singlet-triplet (ST) energy gap and fluorescence energy, remains challenging. While time-dependent density functional theory (TD-DFT), the workhorse of computational materials science, suffers from fundamental issues, wave function-based coupled-cluster (CC) approaches, like approximate CC of second-order (CC2), are accurate but suffer from high computational cost and unfavorable scaling with system size.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!