ACS Physical Chemistry AuPub Date : 2026-09-23Epub Date: 2026-07-30DOI: 10.1021/acsphyschemau.6c00102
Sheikh Jobe, Lamia A. Siddig, Ahmed Elsir, Abbas Khaleel, Fathy Hassan, Nutifafa Y. Doumon
{"title":"Dopant-Induced Photoluminescence Emission in Zero-Dimensional Cesium Zinc Halide Phosphors","authors":"Sheikh Jobe, Lamia A. Siddig, Ahmed Elsir, Abbas Khaleel, Fathy Hassan, Nutifafa Y. Doumon","doi":"10.1021/acsphyschemau.6c00102","DOIUrl":"https://doi.org/10.1021/acsphyschemau.6c00102","url":null,"abstract":"<p>Zero-dimensional(0D) metal halides with isolated polyhedral structureshave attracted attention in optoelectronic applications because oftheir distinctive optical properties, including strong light absorption,large Stokes shift, and tunable emission wavelength. These 0D metalhalides exhibit wide structural diversity, such as Cu<sup>+</sup>,Sn<sup>2+</sup>, Zn<sup>2+</sup>, Mn<sup>2+</sup>, Sb<sup>3+</sup>, Ag<sup>+</sup>, and Ln<sup>3+</sup>-based metal halides. As a branchwithin the 0D metal halides, Zn metal halides exhibit numerous interestingcharacteristics, including simple synthesis, a wide bandgap, and stabilityof Zn<sup>2+</sup> ions. The large separation between [ZnX<sub>4</sub>]<sup>2–</sup> polyhedra provides space that minimizes interactionsbetween polyhedral units and allows wavelength-dependent excitation,making Zn metal halides potential host materials that can accommodatedopant ions to induce a desired emission wavelength. As a newly emergingclass of nonperovskite metal halides, it is necessary to provide areview article to develop a deeper understanding of the impact ofion doping on the optical, electronic, and spectroscopic propertiesof Zn metal halides. Elucidation of these properties is essentialfor tailoring emission wavelengths, optimizing luminescence performance,and elucidating photophysical mechanisms such as self-trapped excitons(STE), energy transfer, and defect states, thereby guiding the rationaldesign of optoelectronics materials and devices.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"6 5","pages":"976–997"},"PeriodicalIF":4.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149022771","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Physical Chemistry AuPub Date : 2026-09-23Epub Date: 2026-06-20DOI: 10.1021/acsphyschemau.6c00036
Maureen M. Kitheka, Yan Jing, Yan Yao, Puja Goyal
{"title":"Efficient Organic Molecular Crystal Structure Prediction Using the Density Functional Tight-Binding Method","authors":"Maureen M. Kitheka, Yan Jing, Yan Yao, Puja Goyal","doi":"10.1021/acsphyschemau.6c00036","DOIUrl":"https://doi.org/10.1021/acsphyschemau.6c00036","url":null,"abstract":"<p>Over the years, computationalcrystal structure prediction (CSP)for organic molecules has thrived as an area of research, spanningvarious scientific disciplines and having significant applicationsin industries such as pharmaceuticals and agrochemicals. Within thefield of batteries, redox-active organic materials (ROMs) such asquinones have received increased attention as promising electrodematerials for rechargeable batteries. However, experimental determinationof the crystal structure of intermediate species formed during thedischarge/charge cycle can often be challenging. Incomplete X-raydiffraction patterns can also lead to difficulties in crystal structuredetermination for ROMs used in batteries. Use of a semiempirical electronicstructure method for CSP helps to avoid force field reparameterizationfor different species, sometimes with complex electronic structure,formed during battery operation. It also helps to significantly lowerthe computational cost compared to the widely used density functionaltheory (DFT). In this study, we report the success of a CSP algorithmbased on a combination of the particle swarm optimization method,as implemented in the CALYPSO software, with third-order density functionaltight-binding, a DFT-based semiempirical method. Accompanied by datapostprocessing using DFT, this method enables the correct identificationof the most stable crystal structures of organic molecules with differentkinds of intermolecular interactions ranging from hydrogen bondingto π-stacking. We also report the experimental crystal structureof pyrene-4,5,9,10-tetrone, a molecule studied intensively for applicationin organic batteries, and predict its crystal structure correctlyusing our method. Our findings emphasize the potential of this approachfor CSP of different classes of organic molecules, including quinones.Additionally, they establish the foundation for future CSP studiesof other organic molecules utilized in rechargeable batteries.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"6 5","pages":"1050–1061"},"PeriodicalIF":4.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149022796","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Physical Chemistry AuPub Date : 2026-09-23Epub Date: 2026-09-09DOI: 10.1021/acsphyschemau.6c00112
Celia Todd, David C. Zeitz, Mariam Khvichia, Jin Zhong Zhang
{"title":"Tracing the Origin of Chiropticity in Lead-Halide Perovskite Nanomaterials","authors":"Celia Todd, David C. Zeitz, Mariam Khvichia, Jin Zhong Zhang","doi":"10.1021/acsphyschemau.6c00112","DOIUrl":"https://doi.org/10.1021/acsphyschemau.6c00112","url":null,"abstract":"<p>Chiral lead-halide perovskite nanomaterials are promisingplatformsfor circularly polarized photonics and spin-selective transport, yetthe origin of their chiroptical response is often difficult to establish.Conventional explanations focus on chiral ligands, lattice distortion,and spin-orbit-coupled electronic structure in the final material.For colloidal nanomaterials in particular, high surface-to-volumeratios and growth through precursor complexes and cluster intermediatesmake formation history and surface chemistry especially important.Circular dichroism (CD), circularly polarized luminescence (CPL),and chirality-induced spin selectivity (CISS) establish asymmetricoptical or spin responses but do not by themselves reveal when asymmetryfirst appears or where it is retained. We compare ligand-induced,structural, electronic, assembly-induced, interfacial, and precursor-mediatedmechanisms by asking when asymmetry is first selected during formationand where it is retained in the final material. We also discuss themeasurements and controls needed to distinguish among these mechanismsin these nanomaterials.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"6 5","pages":"998–1011"},"PeriodicalIF":4.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149027913","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Physical Chemistry AuPub Date : 2026-09-23Epub Date: 2026-09-04DOI: 10.1021/acsphyschemau.6c00114
Sankari Nattuvetty Sunil Kumar, Bignya Rani Dash, Ramesh L. Gardas
{"title":"Hydration Effects in a Guanidine Hydrochloride-Pyruvic Acid Low-Transition-Temperature Mixture: Physicochemical Insights","authors":"Sankari Nattuvetty Sunil Kumar, Bignya Rani Dash, Ramesh L. Gardas","doi":"10.1021/acsphyschemau.6c00114","DOIUrl":"https://doi.org/10.1021/acsphyschemau.6c00114","url":null,"abstract":"<p>A low-transition-temperature mixture (LTTM) composedof guanidinehydrochloride (GUC) and pyruvic acid (PA) in a 1:2 molar ratio wasprepared, and the effect of water on its physicochemical, electrochemical,and structural properties was investigated. To the best of our knowledge,this is the first report of a GUC-PA-based LTTM. Density (ρ),speed of sound (<em>u</em>), and conductivity (κ) weremeasured over the temperature range of 293.15–323.15 K. Theexcess molar volume (<em>V</em><sup>E</sup>) of the pseudo-binaryGUC-PA/water system was calculated and correlated using the third-orderRedlich-Kister equation. Density decreased with increasing temperature,whereas the thermal expansion coefficient (α<sub><em>P</em></sub>) increased. The variation of conductivity with temperatureand water composition was correlated using the VFT and Casteel–Amisequations. Water addition significantly enhanced conductivity, reachinga maximum at an LTTM mole fraction of 0.1170 ± 0.002, indicatingimproved ionic transport upon dilution. Cyclic voltammetry revealedthat the neat GUC-PA LTTM and the system containing an LTTM mole fractionof 0.2314 ± 0.002 exhibited comparable electrochemical behavior.The neat LTTM displayed an electrochemical stability window of −0.45to +1.35 V (vs Ag). Nile Red solvatochromic studies revealed thatthe neat LTTM provides a highly polar microenvironment than water,and water addition induces only a small hypsochromic shift (∼6nm). SAXS measurements showed that water progressively weakens intermolecularcorrelations while preserving the local liquid structure. Densityfunctional theory (DFT) analysis was performed to evaluate the interactionenergies and frontier molecular orbitals (FMOs), providing valuableinsights into the intermolecular interactions within the GUC-PA. Collectively,these results demonstrate that the GUC-PA LTTM retains its characteristichydrogen-bonded structure up to an LTTM mole fraction of 0.2298 ±0.002, beyond which the network progressively weakens. These findingsprovide fundamental insight into the effect of water on the structureand physicochemical properties of LTTM.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"6 5","pages":"1349–1362"},"PeriodicalIF":4.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149027831","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Physical Chemistry AuPub Date : 2026-09-23Epub Date: 2026-09-08DOI: 10.1021/acsphyschemau.6c00122
Imre Bakó, Szilvia Pothoczki
{"title":"Unraveling the Complex Hydrogen-Bonding and Solvation Patterns of Fructose Tautomers via Complementary AIMD and Classical MD Simulations","authors":"Imre Bakó, Szilvia Pothoczki","doi":"10.1021/acsphyschemau.6c00122","DOIUrl":"https://doi.org/10.1021/acsphyschemau.6c00122","url":null,"abstract":"<p>Understanding the molecular-level hydration of fructosetautomersremains a challenge due to their rapid interconversion and structuralcomplexity. A dual-scale approach was employed, combining long-timeclassical molecular dynamics (MD) and ab initio molecular dynamics(AIMD) to elucidate differences in the hydrogen-bonding networks ofboth pyranose and furanose tautomers with statistical and electronicaccuracy. Our simulations highlight the inherent competition betweenintra- and intermolecular hydrogen bonds, driven by the limited numberof hydroxyl donor and acceptor sites. Crucially, the formation ofthese internal bonds is driven by ring puckering in the flexible furanosesalongside the spatial orientation of the hydroxymethyl groups in bothtautomer families. This structural interplay indirectly influencesthe entire intermolecular solvation shell, comprising both hydrophilicand hydrophobic regions. By correlating these competing intra- andintermolecular patterns with Bader charges and water dipole moments,we establish a quantitative electronic-structure basis for carbohydratesolvation. These insights provide a comprehensive atomistic frameworkthat deepens our understanding of biologically relevant processes,such as recognition and docking efficiency within metabolic enzymes.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"6 5","pages":"1372–1386"},"PeriodicalIF":4.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149027954","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Physical Chemistry AuPub Date : 2026-09-23Epub Date: 2026-08-10DOI: 10.1021/acsphyschemau.6c00097
Sindy Julieth Rodríguez-Sotelo, Sebastian Kozuch
{"title":"The Different Levels of Quantum: A Methodological–Philosophical Portrait of Computational Quantum Chemistry§","authors":"Sindy Julieth Rodríguez-Sotelo, Sebastian Kozuch","doi":"10.1021/acsphyschemau.6c00097","DOIUrl":"https://doi.org/10.1021/acsphyschemau.6c00097","url":null,"abstract":"<p><em>In silico</em> and <em>in vitro</em> experimentalchemistry do have many similarities in terms of following the scientificmethod, but they also have epistemological differences. Maybe themost striking difference is that wet chemistry, in terms of physicaleffects, is all-inclusive; it is not possible to remove relativisticeffects or the zero-point energy (to give a couple of examples) fromthe molecules in a real-life flask. On the contrary, computationalchemistry requires a conscious and careful decision on whether thesespecific effects should be included in the virtual experiment. Omitthem, and the chemistry will not be realistic; incorporate unnecessaryeffects, and the job may be intractable. In this perspective, we willdescribe one direction to add quantum effects, depending on the reachand requirements of the studied question. From the electronic to thenuclear wave function and beyond, the addition of deeper and deeperquantum effects must be sequentially and judiciously nested as a matryoshkadoll.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"6 5","pages":"954–975"},"PeriodicalIF":4.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149022646","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Physical Chemistry AuPub Date : 2026-09-23Epub Date: 2026-07-21DOI: 10.1021/acsphyschemau.6c00063
Masoud Keramati, Wei Xie, Mary Jo Ondrechen
{"title":"Molecular Basis of pH-Dependent Activity in T7 RNA Polymerase Revealed by Constant pH Replica Exchange Molecular Dynamics","authors":"Masoud Keramati, Wei Xie, Mary Jo Ondrechen","doi":"10.1021/acsphyschemau.6c00063","DOIUrl":"https://doi.org/10.1021/acsphyschemau.6c00063","url":null,"abstract":"<p>T7 RNA polymerase (T7 RNAP) catalyzes in vitro transcription(IVT)for mRNA vaccines and therapeutics, yet the molecular basis of itspH-dependent activity remains unclear. Here we employ constant pHreplica exchange molecular dynamics (pH-REMD) spanning pH 4.75–9.15(2.88 μs total sampling) to characterize pH-dependent conformationaldynamics of the T7 RNAP initiation complex. Our simulations revealthat His811, adjacent to catalytic Asp812, functions as the primaryactive site pH sensor (p<em>K</em><sub>a</sub> 5.9). Protonationof His811 at acidic pH creates an electrostatic trap that restrictsconformational flexibility required for catalytic turnover, whileits neutral state at optimal pH (∼8.0) permits dynamic motionsessential for nucleotide incorporation. Two critical structural parameters,C-terminal Ala883 to active site distance and specificity loop toβ-hairpin spacing, exhibit opposing pH-dependencies that convergeat optimal pH to establish productive catalytic geometry. The Y639-RNA3′-end distance analysis shows that optimal pH maintains thefunctionally open conformation required for binding by the incomingnucleotide. In contrast, acidic and basic pH conditions have shorterY639-RNA 3′-end distances, promoting collapsed geometries thatsterically occlude binding of the incoming nucleotide. Energy decompositionanalysis reveals that C-terminal repositioning is driven by a pH-dependentswitch in the electrostatic coupling hierarchy from protonated His545and His790 at acidic pH to catalytic metal ions at optimal pH. Glu148(p<em>K</em><sub>a</sub> 5.3) emerges as a structural pH sensorstabilizing the specificity loop–subdomain H interaction criticalfor elongation complex formation. Aggregate charge analysis revealsthat excessive positive charge at acidic pH (+6 at pH 4) impedes promoterescape, while reduced charge at optimal pH (+2 at pH 8) balances bindingand release. These insights establish important electrostatic anddynamic features that promote effective catalysis and can guide optimizationof IVT conditions for the manufacturing of mRNA therapeutics and informengineering of pH-stable T7 RNAP variants.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"6 5","pages":"1220–1234"},"PeriodicalIF":4.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149022717","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Physical Chemistry AuPub Date : 2026-07-22Epub Date: 2026-06-16DOI: 10.1021/acsphyschemau.6c00058
Katharina Konieczny, Tianyin Qiu, Jan Paul Menzel, Jacqueline Maslack, Victor S. Batista, Eszter Baráth
{"title":"Hydrogen Transfer to Internal Alkynes Using Secondary Amines on Carbon-Supported Noble Metals","authors":"Katharina Konieczny, Tianyin Qiu, Jan Paul Menzel, Jacqueline Maslack, Victor S. Batista, Eszter Baráth","doi":"10.1021/acsphyschemau.6c00058","DOIUrl":"10.1021/acsphyschemau.6c00058","url":null,"abstract":"<p>The catalytic hydrogen transfer of internal alkynes usingcarbon-supportednoble metals (Pd/C, Pt/C) was systematically studied with varioussecondary amines, such as indoline (Ind), tetrahydroquinoline (Thq),diisopropylamine ((<sup>i</sup>Pr)<sub>2</sub>NH)), and, for comparison,diisopropylethylamine ((<sup>i</sup>Pr)<sub>2</sub>NEt)) as hydrogendonors. The reactions proceeded sequentially, forming <em>(Z)</em>- and <em>(E)</em>-olefins as interim products, having <em>(Z)</em> as a major olefin product, which were sequentially hydrogenatedto alkanes. The presence of <em>(E)</em>-alkene isomers wasalso observed as minor products. Among the tested systems, Pt/C-Ind,Pd/C-Ind, Pt/C-Thq, and Pd/C-Thq exhibited the highest activity andselectivity. Initial reaction rates and activation parameters (activationenergy, <em>E</em><sub>a</sub>; enthalpy of activation, Δ<em>H</em><sup>‡</sup>; and entropy of activation, Δ<em>S</em><sup>‡</sup>) were determined for these systems.To further elucidate the reaction mechanism, density functional theory(DFT) calculations were performed. The computational results revealedthat the balance between adsorption strength and binding energy ofreactants and intermediates governs the observed selectivity trends.Notably, the strongly negative activation entropies suggest a rigid,highly ordered transition state, independent of the metal catalyst.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"6 4","pages":"887–900"},"PeriodicalIF":4.8,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148585361","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Physical Chemistry AuPub Date : 2026-07-22Epub Date: 2026-06-13DOI: 10.1021/acsphyschemau.6c00066
Panagiotis Mougkogiannis, Andrew Adamatzky
{"title":"Cholinergic Modulation of Proteinoid Microsphere Networks as Prebiotic Depression Models","authors":"Panagiotis Mougkogiannis, Andrew Adamatzky","doi":"10.1021/acsphyschemau.6c00066","DOIUrl":"10.1021/acsphyschemau.6c00066","url":null,"abstract":"<p>The molecular originsof mood disorders remain obscuredby theoverwhelming complexity of biological neural networks. Proteinoidmicrospheres are cell-like structures composed of amino acids, formedthrough heat-driven polymerization. Spontaneous electrical activityis observed in these microspheres and is modulated by nicotine, apotent cholinergic agonist associated with depression. Electrochemicalcharacterization using impedance spectroscopy and cyclic voltammetry,combined with long-duration monitoring (over 75 h), demonstrates thatnicotine induces a “depressive” state in prebiotic networks,defined here as a suppression of coherent, high-amplitude spikingactivity. Crucially, this suppression is not a reduction in totalactivity: nicotine induces hyperactive but low-fidelity dynamics,in which increased firing frequency is accompanied by degraded signalorganization and reduced informational content. This state is notdefined by reduced activity, but rather by degraded signal quality.A 52% increase in firing frequency is accompanied by reduced amplitudeprecision, as deterministic dynamics collapse into stochastic noise.In parallel, phase-space volume expands by 1500-fold, indicating amajor breakdown in homeostatic regulation. Equivalent circuit modelingshows that nicotine decreases membrane charge-transfer resistanceby up to 90%, while capacitance increases 3-fold and exhibits chaoticfluctuations. These effects are consistent with membrane permeabilizationand “shunting inhibition,” which suppress thresholddepolarization. The transition is marked by a shift from self-organizedcriticality (fractal dimension <em>D</em> ≈ 5.0) tolow-dimensional stochasticity (<em>D</em> ≈ 1.5). Shannonentropy increases by 1.67 bits, quantifying the thermodynamic costof the depressed state as information leakage. These results indicatethat cholinergic modulation of excitability is not solely a biologicalphenomenon dependent on evolved receptors, but rather a fundamentalphysicochemical interaction that may have influenced the emergenceof nervous systems. It is proposed that depression reflects a breakdownin thermodynamic self-organization, in which an information-processingsystem shifts from ordered dynamics to chaotic disorder. These resultspoint toward a physicochemical precursor to this principle, potentiallyextending its origins back to the prebiotic era─long beforethe evolutionary emergence of the first synapse.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"6 4","pages":"901–928"},"PeriodicalIF":4.8,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148585166","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Physical Chemistry AuPub Date : 2026-07-22Epub Date: 2026-06-12DOI: 10.1021/acsphyschemau.6c00048
Juan M. Scarpetta, Omar Calderón-Losada, Morten Hjorth-Jensen, John H. Reina
{"title":"Deep Learning Parameter Estimation and Quantum Control of Single Molecules","authors":"Juan M. Scarpetta, Omar Calderón-Losada, Morten Hjorth-Jensen, John H. Reina","doi":"10.1021/acsphyschemau.6c00048","DOIUrl":"10.1021/acsphyschemau.6c00048","url":null,"abstract":"<p>Coherent control, a central concept in physics and chemistry,hassparked significant interest due to its ability to fine-tune interferenceeffects in atoms and individual molecules for applications rangingfrom light-harvesting complexes to molecular qubits. However, precisecharacterization of the system’s dissipative dynamics is requiredfor its implementation, especially at high temperatures. In a quantumcontrol experiment, this means learning system-bath parameters anddriving coupling strengths. Here, we demonstrate how to infer keyphysical parameters of a single molecule driven by spectrally modulatedpulses at room temperature. We develop and compare two computationalapproaches based on two-photon absorption photoluminescence signals:an optimization-based minimization scheme and a feed-forward neuralnetwork. The robustness of our approach highlights the importanceof reliable parameter estimation in designing effective coherent controlprotocols. Our results have direct applications in ultrafast spectroscopy,quantum materials, and technology.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"6 4","pages":"858–868"},"PeriodicalIF":4.8,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148585230","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}