Authors
Anna Rosa ZiefußStephan BarcikowskiKatharine Moore Tibbetts
Topics
Laser-Ablation Synthesis of NanoparticlesNanocluster Synthesis and ApplicationsNonlinear Optical Materials StudiesCite This: J. Phys. Chem. C 2025, 129, 18377−18379 Read OnlineACCESS Metrics & More Article RecommendationsW hen a high-energy laser pulse is focused into a liquid, it creates a local explosion: a transient plasma is ignited, cavitation bubbles grow and collapse, shockwaves ripple through the solvent, and radicals form in the blink of an eye. What may appear as chaos at first glance is, in fact, a playground of transient physical and chemical phenomena that can be harnessed for material design. From this controlled disorder, colloidal nanoparticles emerge�often surfactant-free, compositionally unique, and endowed with properties that are hard to access through conventional chemistry. This observation first emerged in the early 1990s, when Anton Fojtik and Arnim Henglein demonstrated that pulsed laser irradiation of metal targets in liquids could reproducibly yield colloidal nanoparticles, 1 initiating what is now known as laser ablation in liquids (LAL). What began as a physicochemical curiosity has since evolved into a diverse field of laser-based colloid synthesis with growing control, complexity, and application potential. It is an exciting field, both for experts and beginners. 2 This Special Issue celebrates the progress and growth of laser-enabled nanoparticle synthesis in liquid media over the past three decades, and highlights advances reported at the seventh Advanced Nanoparticle Generation and Excitation in Liquids (ANGEL) conference held in Charlottes ville, Virginia, in May 2024. The field of laser-enabled nanoparticle synthesis and processing in liquids 4−8 has grown far beyond its modest origins to now encompass an entire family of related laser synthesis approaches, illustrated in Figure 1: • In LAL, solid targets are ablated into nanoparticles via plasma expansion and cavitation. 9 • In laser fragmentation in liquids (LFL), larger nano- 10 or microparticles 11 are broken down into smaller, often more uniform particles�an approach rooted in optical stress and plasma−particle coupling.• Laser melting in liquids (LML) enables coalescence to submicrometer spheres. 12• In laser reduction in liquids (LRL), reactive chemical species in the plasma initiate nanoparticle nucleation and growth from molecular precursors. 13• Reactive laser ablation in liquids (RLAL) leverages solvents or additives as chemical agents to direct reduction or complexation pathways during ablation of solid targets, 13 including reduction of dissolved gases. 3 • Pulsed Laser Defect Engineering in Liquids (PUDEL) is emerging as a method to introduce point or surface defects, offering yet another lever for tailoring functionality. 14This diversification of laser synthesis techniques has gone hand in hand with a deeper fundamental understanding of laser-material interactions and how they impact the properties of the synthesized nanoparticles. Reaction mechanisms�once inferred solely from ex-situ characterization 15�can now be unraveled through in situ diagnostics as time-resolved spec troscopy 3 and complementary simulations. 3 Tools such as flat jet reactors provide the experimental stability needed to access these ultrafast regimes. 16 This Special Issue highlights work that reveals new insights into a broad array of chemical and physical mechanisms. The fragmentation of metallic micro particles in organic solvents offers insight into radical reaction pathways and the interplay between thermal and nonthermal contributions (DOI: 10.1021/acs.jpcc.4c06653). Work onPublished: October 16, 2025Figure 1. Illustration of methods for laser synthesis and processing in liquid (clockwise, from top): Laser ablation in liquid (LAL), laser fragmentation in liquid (LFL), laser melting in liquid (LML), reactive laser ablation in liquid (RLAL), laser reduction in liquid (LRL), pulsed laser defect engineering in liquid (PUDEL).pubs.acs.org/JPCC Special Issue PrefacePublished 2025 by American Chemical Society https://doi.org/10.1021/acs.jpcc.5c06365J. Phys. Chem. C 2025, 129, 18377−18379 2 .5 6 .2 4 .1 2 o n J u n e4 ,6 a t5 : 7 :5 (UC ) copper and silicon targets in acetone (DOI: 10.1021/ acs.jpcc.4c08231) and organic pigment dispersions in flat jets (DOI: 10.1021/acs.jpcc.4c08643) reveals how precursor composition, laser fluence, and flow affect product selectivity and yield. Solvent decomposition channels and their impact on molecular product distributions have also been dissected (DOI: 10.1021/acs.jpcb.4c05638). The use of frequency resolved photoacoustic response to monitor size changes (DOI: 10.1021/acs.jpcc.4c08334), studies on colloidal caging by graphene oxide (DOI: 10.1021/acs.jpcc.5c00439), defect selective adsorption of gold nanoparticles onto zinc sulfide crystals (DOI: 10.1021/acs.jpcc.4c05728), and mass spec trometry investigations on ligand−nanoparticle interactions (DOI: 10.1021/acs.jpcc.5c03644) further expand our under standing of laser-induced colloid behavior and interfacial chemistry. Building on this foundation, researchers have developed pathways for the synthesis of complex nanomaterials, 17 including new materials presented in this Special Issue. The growing field of laser-based synthesis and processing of carbon and graphene quantum dots in liquids, from fundamental mechanisms to biological applications, has been reviewed with new practical insights for future design of these materials (DOI: 10.1021/acs.jpcc.5c01343). Luminescent erbium-based nanoparticles have been produced via LAL (DOI: 10.1021/ acs.jpcc.4c07101), while femtosecond ablation in liquids has enabled access to high-entropy alloy colloids (DOI: 10.1021/ acs.jpcc.4c04574) and multicomponent ceramics with de signed disorder (DOI: 10.1021/acs.jpcc.4c04851). These systems demonstrate that compositionally complex or metastable materials can emerge from ultrafast nonequilibrium routes, often without surfactants. Laser-induced grafting strategies further bridge colloidal synthesis with macroscopic applications, such as the formation of nanocatalyst−carbon fiber paper composites for electrode fabrication (DOI: 10.1021/acs.jpcc.5c00641), while the crystallization of ionic liquids via scanning pulses (DOI: 10.1021/acs.jpcc.5c00625) expands laser control into the soft-matter domain. The ability to tailor optical properties through laser-based synthesis is another hallmark of this field. Laser-synthesized materials capture ultrafast excitation dynamics, excitonic interactions, and field effects. This is reflected in studies on azobenzene dye dimers (DOI: 10.1021/acs.jpca.4c05237) and in trap-dominated recombination processes in laser-oxidized silicon nanoparticles (DOI: 10.1021/acs.jpcc.4c04410). These examples show how structure−property relations become embedded not just in the material, but in the process that forms it. A major motivation for laser-based nanochemistry remains the pursuit of functional applications. Catalysis, in particular, benefits from the surface cleanliness, defect control, and morphology tuning made possible by pulsed lasers. Enhanced hydrogen evolution was achieved on black TiO2 using real time Raman tracking (DOI: 10.1021/acs.jpcc.4c04174), and UV laser postprocessing significantly improved the activity of Pt/C catalysts (DOI: 10.1021/acs.jpcc.5c00223). These results exemplify the growing use of laser processing not only for synthesis but also for activation and performance tuning. Beyond catalysis, enhanced antimicrobial activity was achieved for Cu/Cu2O/CuO composite particles synthesized by LML that incorporated 5% Ag nanoparticles (DOI: 10.1021/ acs.jpcc.5c00736). Laser-synthesized nanoparticles are also increasingly being explored as functional additives in advanced manufacturing, particularly in additive processes such as laser powder bed fusion. Here, nanoparticle-decorated feedstocks enable new degrees of control over melting behavior, microstructure evolution, and final part functionality 18�a strategy that has shown promise for processing demanding materials such as nanostructured permanent magnets. 19,20 This direction highlights how nanoscale design can extend beyond the particle itself and become integral to macroscale material performance. What connects these works is a common narrative: laser processes once considered uncontrollable are now understood as designable�through time-resolved diagnostics, flow-reactor design, modeling of plasma and solvent dynamics, and deliberate modulation of chemical environments. Nano particles are no longer just the result of interaction�they are the product of orchestration. This Special Issue reflects a maturing field�one that is becoming not only more precise but also more purposeful. We thank all authors and reviewers who contributed to this vision and invite the reader to explore how chaos, when properly harnessed, becomes a tool for nanomaterial design. Anna R. Ziefuss orcid.org/0000-0002-9465-1917 Stephan Barcikowski orcid.org/0000-0002-9739-7272 Katharine Moore Tibbetts orcid.org/0000-0001-8853-5656 ■ AUTHOR INFORMATION Complete contact information is available at: https://pubs.acs.org/10.1021/acs.jpcc.5c06365 Notes Views expressed in this preface are those of the authors and not necessarily the views of the ACS■ REFERENCES (1) Fojtik, A.; Weller, H.; Koch, U.; Henglein, A. Photo-Chemistry of Colloidal Metal Sulfides 8. Photo-Physics of Extremely Small CdS Particles: Q-State CdS and Magic Agglomeration Numbers. Ber. Bunsenges. Phys. Chem. 1984, 88, 969−977. (2) Barcikowski, S.; Amendola, V.; Lau, M.; Marzun, G.; Rehbock, C.; Reichenberger, S.; Zhang, D.; Gökce, B. Handbook of Laser Synthesis & Processing of Colloids, 2nd ed.; 2019; DOI: 10.17185/ duepublico/70584. (3) Plech, A.; Tack, M.; Huang, H.; Arefev, M.; Ziefuss, A. R.; Levantino, M.; Karadas, H.; Chen, C.; Zhigilei, L. V.; Reichenberger, S. Physical Regimes and Mechanisms of Picosecond Laser Fragmentation of Gold Nanoparticles in Water from X-ray Probing and Atomistic Simulations. ACS Nano 2024, 18 (15), 10527−10541. (4) Manshina, A. A.; Tumkin, I. I.; Khairullina, E. M.; Mizoshiri, M.; Ostendorf, A.; Kulinich, S. A.; Makarov, S.; Kuchmizhak, A. A.; Gurevich, E. L. The Second Laser Revolution in Chemistry: Emerging Laser Technologies for Precise Fabrication of Multifunctional Nanomaterials and Nanostructures. Adv. Funct. Mater. 2024, 34 (40), 2405457. (5) Amendola, V.; Amans, D.; Ishikawa, Y.; Koshizaki, N.; Scire, S.; Compagnini, G.; Reichenberger, S.; Barcikowski, S. Room-Temper ature Laser Synthesis in Liquid of Oxide, Metal-Oxide Core-Shells, and Doped Oxide Nanoparticles. Chem. Eur. J. 2020, 26 (42), 9206− 9242. (6) Forsythe, R. C.; Cox, C. P.; Wilsey, M. K.; Muller, A. M. Pulsed Laser in Liquids Made Nanomaterials for Catalysis. Chem. Rev. 2021, 121 (13), 7568−7637. (7) Khairani, I. Y.; Minguez-Vega, G.; Donate-Buendia, C.; Gokce, B. Green nanoparticle synthesis at scale: a perspective on overcomingThe Journal of Physical Chemistry C pubs.acs.org/JPCC Special Issue Prefacehttps://doi.org/10.1021/acs.jpcc.5c06365 J. Phys. Chem. C 2025, 129, 18377−18379 18378the limits of pulsed laser ablation in liquids for high-throughput production. Phys. Chem. Chem. Phys. 2023, 25 (29), 19380−19408. (8) Yogesh, G. K.; Shukla, S.; Sastikumar, D.; Koinkar, P. Progress in pulsed laser ablation in liquid (PLAL) technique for the synthesis of carbon nanomaterials: a review. Appl. Phys. A: Mater. Sci. Process. 2021, 127 (11), 810. (9) Fazio, E.; Gokce, B.; De Giacomo, A.; Meneghetti, M.; Compagnini, G.; Tommasini, M.; Waag, F.; Lucotti, A.; Zanchi, C. G.; Ossi, P. M.; Dell’Aglio, M.; D’Urso, L.; Condorelli, M.; Scardaci, V.; Biscaglia, F.; Litti, L.; Gobbo, M.; Gallo, G.; Santoro, M.; Trusso, S.; Neri, F. Nanoparticles Engineering by Pulsed Laser Ablation in Liquids: Concepts and Applications. Nanomaterials (Basel) 2020, 10 (11), 2317. (10) Pustovalov, V. K. Laser melting, evaporation, and fragmentation of nanoparticles: Experiments, modeling, and applications. Nano technology and Precision Engineering 2025, 8, 025001. (11) Spellauge, M.; Tack, M.; Streubel, R.; Miertz, M.; Exner, K. S.; Reichenberger, S.; Barcikowski, S.; Huber, H. P.; Ziefuss, A. R. Photomechanical Laser Fragmentation of IrO2 Microparticles for the Synthesis of Active and Redox-Sensitive Colloidal Nanoclusters. Small 2023, 19 (10), 2206485. (12) Ishikawa, Y.; Tsuji, T.; Sakaki, S.; Koshizaki, N. Pulsed laser melting in liquid for crystalline spherical submicrometer particle fabrication− Mechanism, process control, and applications. Prog. Mater. Sci. 2023, 131, 101004. (13) Frias Batista, L.; Nag, A.; Meader, V.; Moore Tibbetts, K. Generation of nanomatreials by reactive laser-synthesis in liquids. Sci. China Phys. Mech. Astron. 2022, 65 (7), 274202. (14) Reichenberger, S. Freezing crystallographic defects into nanoparticles: The development of pulsed laser defect engineering in liquid (PUDEL). Science China Physics, Mechanics & Astronomy 2022, 65 (7), 274208. (15) Ziefuß, A. R.; Reichenberger, S.; Rehbock, C.; Chakraborty, I.; Gharib, M.; Parak, W. J.; Barcikowski, S. Laser Fragmentation of Colloidal Gold Nanoparticles with High-Intensity Nanosecond Pulses is Driven by a Single-Step Fragmentation Mechanism with a Defined Educt Particle-Size Threshold. J. Phys. Chem. C 2018, 122 (38), 22125−22136. (16) Zerebecki, S.; Reichenberger, S.; Barcikowski, S. Continuous Flow Flat Jet Setup for Uniform Pulsed Laser Postprocessing of Colloids. J. Phys. Chem. A 2020, 124 (52), 11125−11132. (17) Ziefuss, A. R.; Steenbock, T.; Benner, D.; Plech, A.; Gottlicher, J.; Teubner, M.; Grimm-Lebsanft, B.; Rehbock, C.; Comby-Zerbino, C.; Antoine, R.; Amans, D.; Chakraborty, I.; Bester, G.; Nachev, M.; Sures, B.; Rubhausen, M.; Parak, W. J.; Barcikowski, S. Photo luminescence of Fully Inorganic Colloidal Gold Nanocluster and Their Manipulation Using Surface Charge Effects. Adv. Mater. 2021, 33 (31), No. e2101549. (18) Stratmann, N.; Willeke, M.; Leupold, S.; Schmidt, M.; Barcikowski, S.; Ziefuss, A. R. Near-infrared surface sensitizing of PA12 to enable diode laser-based Powder Bed Fusion. Procedia CIRP 2024, 124, 69−73. (19) Gabriel, P.; Nallathambi, V.; Liu, J.; Staab, F.; Oyedeji, T. D.; Yang, Y.; Hantke, N.; Adabifiroozjaei, E.; Recalde-Benitez, O.; Molina-Luna, L.; Rao, Z.; Gault, B.; Sehrt, J. T.; Scheibel, F.; Skokov, K.; Xu, B. X.; Durst, K.; Gutfleisch, O.; Barcikowski, S.; Ziefuss, A. R. Boosting Coercivity of 3D Printed Hard Magnets through Nano-Modification of the Powder Feedstock. Adv. Sci. (Weinh) 2024, 11 (46), No. e2407972. (20) Nallathambi, V.; Gabriel, P.; Chen, X.; Rao, Z.; Skokov, K.; Gutfleisch, O.; Barcikowski, S.; Ziefuss, A. R.; Gault, B. Effect of Ag nano-additivation on microstructure formation in Nd-Fe-B magnets built by laser powder bed fusion. Acta Mater. 2025, 297, 121353.The Journal of Physical Chemistry C pubs.acs.org/JPCC Special Issue Prefacehttps://doi.org/10.1021/acs.jpcc.5c06365 J. Phys. Chem. C 2025, 129, 18377−18379
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PublishedOct 16, 2025
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