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Award Detail

Doing Business As Name:University of California-Irvine
  • Vartkess A Apkarian
  • (949) 824-6851
Award Date:08/03/2009
Estimated Total Award Amount: $ 20,000,000
Funds Obligated to Date: $ 20,489,514
  • FY 2013=$3,725,000
  • FY 2010=$4,340,000
  • FY 2011=$4,275,000
  • FY 2012=$4,149,514
  • FY 2009=$4,000,000
Start Date:08/15/2009
End Date:07/31/2014
Transaction Type: Cooperative Agreements
Awarding Agency Code:4900
Funding Agency Code:4900
CFDA Number:47.049
Primary Program Source:040100 NSF RESEARCH & RELATED ACTIVIT
Award Title or Description:The Center for Chemistry at the Space-Time Limit (CaSTL)
Federal Award ID Number:0802913
DUNS ID:046705849
Parent DUNS ID:071549000
Program Officer:
  • Katharine Covert
  • (703) 292-4950

Awardee Location

Street:141 Innovation Drive, Ste 250
Awardee Cong. District:45

Primary Place of Performance

Organization Name:University of California-Irvine
Street:141 Innovation Drive, Ste 250
Cong. District:45

Abstract at Time of Award

The UC Irvine Center for Chemical Innovation - Chemistry at the Space-Time Limit (CaSTL) aims to observe and record chemistry in the act, one event at a time, one molecule at a time. By watching single molecules undergo chemical transformation and creating movies of a molecule's atomic and electronic rearrangements, the Center will uncover the inner workings of important chemical reactions. The vibronic dynamics of a molecule upon reduction, the rearrangement of electron density in a molecule as it adsorbs onto a catalytic site, the transfer of electrons through a molecular wire, and the breaking or making of a bond are among the immediate targets of investigation. The Center achieves its goals by pushing the experimental limits of space and time resolution, using a combination of scanning tunneling microscopy and ultrafast nonlinear spectroscopy to attain simultaneous Ångstrom-femtosecond resolution. On the scale of relevance to macro-molecular chemistry (e.g., nanometer-microsecond), scanning probe microscopies combined with time-resolved nonlinear spectroscopy are used to obtain chemically speciated, time-lapse microscopy. The requisite theory, in particular of plasmon-enhanced spectroscopy and time-dependent density functional methods, are developed in parallel to accurately model these processes, to interpret and to design experiments. The enabling science and tools have a common intellectual base and a toolset that can be tuned in sharpness to provide the precision needed to study a wide range of chemical processes with precise joint space-time resolution, from Ångstrom-femtosecond to micrometer-microsecond. The accessibility of time-lapse images of elementary chemical processes will fundamentally change our modes of inquiry, and manipulation of, molecular science and engineering, and could underlie fundamental breakthroughs in a range of fields relying on sub-molecular understanding and manipulation of our world. CaSTL is committed to education at all levels, directly through graduate research and postdoctoral training in these challenging fields of science, and research opportunities to many California high school and community college students, particularly those from under-represented groups. The development of new scientific instruments and computational chemistry packages will be widely disseminated in partnership with the private sector. The Center will also offer an outreach program to students of all ages through a partnership with the Discovery Science Museum in Santa Ana. The very visual nature of the Center's transformative science makes it particularly accessible to the public at large. CaSTL video clips of fundamental chemical processes will be used in classrooms, podcasts and other web-based formats, and broad public science outreach will be enabled through television broadcasts.

Publications Produced as a Result of this Research

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Lee, J; Perdue, SM; Whitmore, D; Apkariana, VA "Laser-induced scanning tunneling microscopy: Linear excitation of the junction plasmon" JOURNAL OF CHEMICAL PHYSICS, v.133, 2010, p.. doi:10.1063/1.349039  View record at Web of Science

Pozzi, E. A. and Sonntag, M. D. and Jiang, N. and Klingsporn, J. M. and Hersam, M. C. and Van Duyne, R. P. "Tip-Enhanced Raman Imaging: An Emergent Tool for Probing Biology at the Nanoscale" Acs Nano, v.7, 2013, p.885-888. doi:Doi 10.1021/Nn400560t 

D. D. Whitmore (E. Potma, and V. A. Apkarian, as co-advisors) "Design and Use of Nonlinear Optical Parametric Oscillators" MS thesis, University of California, Irvine, v., 2010, p..

Samuel L. Kleinman, Bhavya Sharma, Martin G. Blaber, Anne-Isabelle Henry, Nicholas Valley, R. Griffith Freeman, Michael J. Natan, George C. Schatz, and Richard P. Van Duyne "Structure Enhancement Factor Relationships in Single Gold Nanoantennas by Surface-Enhanced Raman Excitation Spectroscopy" J. Am. Chem. Soc., v.135, 2012, p.301?308. doi:10.1021/ja309300d 

V. R. Khalap, T. Sheps, A. A. Kane, and P. G. Collins "Hydrogen Sensing and Sensitivity of Palladium-Decorated Single-Walled Carbon Nanotubes with Defects" Nano Letters, v.10, 2010, p.896.

Mayukh Banik, Patrick Z. El-Khoury, Amit Nag, Alejandro Rodriguez-Perez, Nekane Guarrottxena, Guillermo C. Bazan, and Vartkess A. Apkarian "Surface-Enhanced Raman Trajectories on a Nano-Dumbbell: Transition from Field to Charge Transfer Plasmons as the Spheres Fuse" ACS Nano, v.X, 2012, p.X. doi:10.1021/nn304277n 

D. Rappoport, F. Furche "Structure of endohedral fullerene Eu@C74" Phys. Chem. Chem. Phys., v.11, 2009, p.6353.

Yong Wang, Xuejun Liu, Aaron R. Halpern, Kyunghee Cho, Robert M. Corn, and Eric O. Potma "Wide-field, surface-sensitive four-wave mixing microscopy of nanostructures" Appl. Opt., v.51, 2012, p.3305.

Guarrotxena, N. and Bazan, G. C. "Antitags: SERS-Encoded Nanoparticle Assemblies that Enable Single-Spot Multiplex Protein Detection" Advanced Materials, v.26, 2014, p.1941-1946. doi:DOI 10.1002/adma.201304107 

Li, S. W. and Yu, A. and Toledo, F. and Han, Z. M. and Wang, H. and He, H. Y. and Wu, R. Q. and Ho, W. "Rotational and Vibrational Excitations of a Hydrogen Molecule Trapped within a Nanocavity of Tunable Dimension" Physical Review Letters, v.111, 2013, p.146102. doi:10.1103/PhysRevLett.111.146102 

Yang Han, Varun Raghunathan, Ran-ran Feng, Hiroaki Maekawa, Chao-Yu Chung, Yuan Feng, Eric O. Potma, and Nien-Hui Ge "Mapping Molecular Orientation with Phase Sensitive Vibrationally Resonant Sum-Frequency Generation Microscopy" J. Phys. Chem. B, v.117, 2013, p.6149?6156. 

Fu, Z. M. and Wang, M. Y. and Zuo, P. J. and Yang, Z. X. and Wu, R. Q. "Importance of oxygen spillover for fuel oxidation on Ni/YSZ anodes in solid oxide fuel cells" Physical Chemistry Chemical Physics, v.16, 2014, p.8536-8540. doi:Doi 10.1039/C3cp55076a 

Samuel L. Kleinman, Renee R. Frontiera, Anne-Isabelle Henry, Jon A. Dieringer and Richard P. Van Duyne "Creating, characterizing, and controlling chemistry with SERS hot spots" Phys. Chem. Chem. Phys., v.15, 2012, p.21--36. doi:10.1039/c2cp42598j 

Maekawa, H; Ballano, G; Toniolo, C; Ge, NH "Linear and Two-Dimensional Infrared Spectroscopic Study of the Amide I and II Modes in Fully Extended Peptide Chains" JOURNAL OF PHYSICAL CHEMISTRY B, v.115, 2011, p.5168. doi:10.1021/jp105527  View record at Web of Science

Sasaki, S. S. and Perdue, S. M. and Perez, A. R. and Tallarida, N. and Majors, J. H. and Apkarian, V. A. and Lee, J. "Note: Automated electrochemical etching and polishing of silver scanning tunneling microscope tips" Review of Scientific Instruments, v.84, 2013, p.. doi:Artn 096109Doi 10.1063/1.4822115 

Alejandro Jara, Rodrigo E. Arias and D. L. Mills "Plasmons and the Electromagnetic Response of Nanowires" Phys. Rev. B, v.81, 2010, p.085422.

Weiss, P. A. and Silverstein, D. W. and Jensen, L. "Non-Condon Effects on the Doubly Resonant Sum Frequency Generation of Rhodamine 6G" Journal of Physical Chemistry Letters, v.5, 2014, p.329-335. doi:Doi 10.1021/Jz402541z 

M. Woznica, P. Kowalska, R. Lysek, M. Masynk, M. Gorecki, M. Kwit, F. Furche, J. Frelek "Stereochemical Assignment of beta-lactam Antibiotics and their Analogues by Electronic Circular Dichroism Spectroscopy" Curr. Org. Chem., v.14, 2010, p.1022.

Jacobsen, O; Maekawa, H; Ge, NH; Gorbitz, CH; Rongved, P; Ottersen, OP; Amiry-Moghaddam, M; Klaveness, J "Stapling of a 3(10)-Helix with Click Chemistry" JOURNAL OF ORGANIC CHEMISTRY, v.76, 2011, p.1228. doi:10.1021/jo101670  View record at Web of Science

Kleinman, SL; Ringe, E; Valley, N; Wustholz, KL; Phillips, E; Scheidt, KA; Schatz, GC; Van Duyne, RP "Single-Molecule Surface-Enhanced Raman Spectroscopy of Crystal Violet Isotopologues: Theory and Experiment" JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.133, 2011, p.4115. doi:10.1021/ja110964  View record at Web of Science

Banik, M; Nag, A; El-Khoury, PZ; Perez, AR; Guarrotxena, N; Bazan, GC; Apkarian, VA "Surface-Enhanced Raman Scattering of a Single Nanodumbbell: Dibenzyldithio-Linked Silver Nanospheres" JOURNAL OF PHYSICAL CHEMISTRY C, v.116, 2012, p.10415. doi:10.1021/jp302013  View record at Web of Science

Sonntag, M. D. and Chulhai, D. and Seideman, T. and Jensen, L. and Van Duyne, R. P. "The Origin of Relative Intensity Fluctuations in Single-Molecule Tip-Enhanced Raman Spectroscopy" Journal of the American Chemical Society, v.135, 2013, p.17187-171. doi:Doi 10.1021/Ja408758j 

Lee, Joonhee and Perdue, Shawn M. and Rodriguez Perez, Alejandro and Apkarian, Vartkess Ara "Vibronic Motion with Joint Angstrom?Femtosecond Resolution Observed through Fano Progressions Recorded within One Molecule" ACS Nano, v.8, 2013, p.54-63. doi:10.1021/nn405335h 

H. Kim, T. Sheps, P. G. Collins, E. O. Potma "Nonlinear Optical Imaging of Individual Carbon Nanotubes with Four-Wave-Mixing Microscopy" Nano Letters, v.9, 2009, p.2991.

Hunt, SR; Wan, D; Khalap, VR; Corso, BL; Collins, PG "Scanning Gate Spectroscopy and Its Application to Carbon Nanotube Defects" NANO LETTERS, v.11, 2011, p.1055. doi:10.1021/nl103935  View record at Web of Science

Frontiera, RR; Henry, AI; Gruenke, NL; Van Duyne, RP "Surface-Enhanced Femtosecond Stimulated Raman Spectroscopy" JOURNAL OF PHYSICAL CHEMISTRY LETTERS, v.2, 2011, p.1199. doi:10.1021/jz200498  View record at Web of Science

Renee R. Frontiera, Natalie L. Gruenke, and Richard P. Van Duyne "Fano-Like Resonances Arising from Long-Lived Molecule-Plasmon Interactions in Colloidal Nanoantennas" Nano Lett., Article ASAP, v.X, 2012, p.X. doi:10.1021/nl303488m 

Zongxian Yang, Yanxing Zhang, Zhaoming Fu, and Ruqian Wu "Unusual Stability and Activity of DI-Pd19 Clusters for O2 Dissociation" J. Phys. Chem. C, v.116, 2012, p.19586?195. 

Yan, Z. J. and Scherer, N. F. "Optical Vortex Induced Rotation of Silver Nanowires" Journal of Physical Chemistry Letters, v.4, 2013, p.2937-2942. doi:Doi 10.1021/Jz401381e 

Eric A. Pozzi, Matthew D. Sonntag, Nan Jiang, Naihao Chiang, Tamar Seideman, Mark C. Hersam, and Richard P. Van Duyne "Ultrahigh Vacuum Tip-Enhanced Raman Spectroscopy with Picosecond Excitation" J. Phys. Chem. Lett., v.5, 2014, p.2657. doi:10.1021/jz501239z 

N. Jiang, E. Foley, J. Klingsporn, M. Sonntag, N. Valley, J. Dieringer, T. Seideman, G.C. Schatz, M.C. Hersam, and R.P Van Duyn "Observation of Multiple Vibrational Modes in Ultrahigh Vacuum Tip-Enhanced Raman Spectroscopy Combined with Molecular-Resolution Scanning Tunneling Microscopy" Nano Lett., ASAP, v., 2012, p.. doi:10.1021 

R. Send, F. Furche "First-order nonadiabatic couplings from time-dependent hybrid density functional response theory: consistent formalism, implementation and performance" J. Chem. Phys., v.132, 2010, p.044107.

Yampolsky, Steven and Fishman, Dmitry A. and Dey, Shirshendu and Hulkko, Eero and Banik, Mayukh and Potma, Eric O. and Apkarian, Vartkess A. "Seeing a single molecule vibrate through time-resolved coherent anti-Stokes Raman scattering" Nat Photon, v.advance, 2014, p.. doi:10.1038/nphoton.2014.143 

Patrick Z. El-Khoury, Dehong Hu, V. A. Apkarian, Wayne P. Hess "Raman Scattering at Plasmonic Junctions Shorted by Conductive Molecular Bridges" Nano Lett., Article ASAP, v.X, 2013, p.X. doi:10.1021/nl400733r 

Shirshendu Dey, Daniel Mirell, Alejandro Rodriguez Perez, Joonhee Lee, and V. Ara Apkarian "Nonlinear femtosecond laser induced scanning tunneling microscopy" J. Chem. Phys., v.138, 2013, p.154202. doi:doi: 10.1063/1.4800965 

Sonntag, M. D. and Klingsporn, J. M. and Zrimsek, A. B. and Sharma, B. and Ruvuna, L. K. and Van Duyne, R. P. "Molecular plasmonics for nanoscale spectroscopy" Chemical Society Reviews, v.43, 2014, p.1230-1247. doi:Doi 10.1039/C3cs60187k 

Jara, A; Arias, RE; Mills, DL "Plasmons and the electromagnetic response of nanowires" PHYSICAL REVIEW B, v.81, 2010, p.. doi:10.1103/PhysRevB.81.08542  View record at Web of Science

Joonhee Lee, Shawn M. Perdue, Alejandro Rodriguez Perez, Patrick Z. El-Khoury, Karoliina Honkala, and V. A. Apkarian "Orbiting Orbitals: Visualization of Vibronic Motion at a Conical Intersection" J. Phys. Chem. A, Article ASAP, v.X, 2013, p.X. doi:10.1021/jp311894n 

Maekawa, H. and Sul, S. and Ge, N. H. "Vibrational correlation between conjugated carbonyl and diazo modes studied by single- and dual-frequency two-dimensional infrared spectroscopy" Chemical Physics, v.422, 2013, p.22-30. doi:DOI 10.1016/j.chemphys.2013.02.010 

P. G. Collins "Defects and disorder in carbon nanotubes" Oxford Handbook of Nanoscience and Technology: Frontiers and Advances, A. V. Narlikar and Y. Y. Fu. Oxford, Oxford Univ. Press, v., 2010, p..

Sonntag, MD; Klingsporn, JM; Garibay, LK; Roberts, JM; Dieringer, JA; Seideman, T; Scheidt, KA; Jensen, L; Schatz, GC; Van Duyne, RP "Single-Molecule Tip-Enhanced Raman Spectroscopy" JOURNAL OF PHYSICAL CHEMISTRY C, v.116, 2012, p.478. doi:10.1021/jp209982  View record at Web of Science

A. A. Kane, T. Sheps, E. T. Branigan, V. A. Apkarian, M. H. Cheng, J. C. Hemminger, S. R. Hunt, and P. G. Collins "Graphitic Electrical Contacts to Metallic Single Walled Carbon Nanotubes using Pt Electrodes" Nano Letters, v.9, 2009, p.3586.

Klingsporn, J. M. and Jiang, N. and Pozzi, E. A. and Sonntag, M. D. and Chulhai, D. and Seideman, T. and Jensen, L. and Hersam, M. C. and Van Duyne, R. P. "Intramolecular Insight into Adsorbate-Substrate Interactions via Low-Temperature, Ultrahigh-Vacuum Tip-Enhanced Raman Spectroscopy" Journal of the American Chemical Society, v.136, 2014, p.3881-3887. doi:Doi 10.1021/Ja411899k 

Sharma, B; Frontiera, RR; Henry, AI; Ringe, E; Van Duyne, RP "SERS: Materials, applications, and the future" MATERIALS TODAY, v.15, 2012, p.16. View record at Web of Science

P. A. Letnes, I. Simonsen, and D. L. Mills "Substrate Influence on the Plasmonic Response of Nanoparticle Clusters" Phys. Rev. B, v.B81, 2010, p.085422.

Liu, XJ; Wang, Y; Potma, EO "Surface-mediated four-wave mixing of nanostructures with counterpropagating surface plasmon polaritons" OPTICS LETTERS, v.36, 2011, p.2348. View record at Web of Science

B. Wild, L. Cao, Y. Sun, B. P. Khanal, E. R. Zubarev, S. K. Gray, N. F. Scherer, M. Pelton "Propagation Lengths and Group Velocities of Plasmons in Chemically Synthesized Gold and Silver Nanowires" ACS Nano, v.6, 2012, p.472.

Chao-Yu Chung, Julie Hsu, Shaul Mukamel, and Eric O. Potma "Controlling stimulated coherent spectroscopy and microscopy by a position-dependent phase" Phys. Rev. A, v.87, 2013, p.033833.

Golschleger, I. U. and van Staveren, M. N. and Apkarian, V. A. "Quantum tomography of a molecular bond in ice" The Journal of Chemical Physics, v.139, 2013, p.034201. doi:10.1063/1.4813437 

Y. Kanai, V. R. Khalap, P. G. Collins, and J. C. Grossman "Atomistic Oxidation of a Carbon Nanotube in Nitric Acid" Physical Review Letters, v.104, 2010, p.066401.

Thomas Spears, Raman Shah, Lina Cao, Norbert F. Scherer "Coherence properties of Ag nanowirebased plasmonic interferometers" ACS Nano, v., 2012, p..

Branigan, ET; Halberstadt, N; Apkarian, VA "Solvation dynamics through Raman spectroscopy: Hydration of Br-2 and Br-3(-), and solvation of Br-2 in liquid bromine" JOURNAL OF CHEMICAL PHYSICS, v.134, 2011, p.. doi:10.1063/1.358347  View record at Web of Science

M. Banik, V. A. Apkarian, T.-H. Park, and M. Galperin "Raman Staircase in Charge Transfer SERS at the Junction of Fusing Nanospheres" J. Phys. Chem. Lett., v.4, 2012, p.88?92. 

Wickramasinghe, H. K. and Chaigneau, M. and Yasukuni, R. and Picardi, G. and Ossikovski, R. "Billion-Fold Increase in Tip-Enhanced Raman Signal" Acs Nano, v.8, 2014, p.3421-3426. doi:Doi 10.1021/Nn406263m 

Chulhai, D. V. and Jensen, L. "Determining Molecular Orientation With Surface-Enhanced Raman Scattering Using Inhomogenous Electric Fields" Journal of Physical Chemistry C, v.117, 2013, p.19622-196. doi:Doi 10.1021/Jp4062626 

Sebek, J. and Knaanie, R. and Albee, B. and Potma, E. O. and Gerber, R. B. "Spectroscopy of the C-H Stretching Vibrational Band in Selected Organic Molecules" Journal of Physical Chemistry A, v.117, 2013, p.7442-7452. doi:10.1021/jp4014674 

van Staveren, MN; Apkarian, VA "Dynamically skewed lines: Rotations in superfluid helium" JOURNAL OF CHEMICAL PHYSICS, v.133, 2010, p.. doi:10.1063/1.346981  View record at Web of Science

E. Vehmanen, V. Ghazarian, C. Sams, I. Khachatryan, J. Eloranta, and V. A. Apkarian "Injection of Atoms and Molecules in a Superfluid Helium Fountain: Cu and Cu2Hen (n = 1, ..., â??)" J. Phys. Chem. A., v.115, 2011, p.7077. doi:10.1021/jp1123986 

Y. Wang, C.-Y. Lin, A. Nikolaenko, V. Raghunathan and E. O. Potma "Four-wave mixing microscopy of nanostructures" Adv. Opt. Photon., v.3, 2011, p.1.

V. A. Apkarian and M. Pettersson "Photodynamics at Low Temperatures, in Real-time" Ch. 6, in Physics and Chemistry at Low Temperatures (Wiley Interscience, v., 2011, p..

Xuejun Liu, Yong Wang, and Eric O. Potma "A dual-color plasmonic focus for surface-selective four-wave mixing" Appl. Phys. Lett., v.101, 2012, p.081116. doi:10.1063/1.4747798 

Sharma, B. and Cardinal, M. Fernanda and Kleinman, S. L. and Greeneltch, N. and Frontiera, R. R. and Van Duyne, R. P. "High Performance SERS Substrates: Advancements and Challenges" MRS Bulletin, v.38, 2013, p.615-634.

Cooper, C. T. and Rodriguez, M. and Blair, S. and Shumaker-Parry, J. S. "Polarization Anisotropy of Multiple Localized Plasmon Resonance Modes in Noble Metal Nanocrescents" Journal of Physical Chemistry C, v.118, 2014, p.1167-1173. doi:Doi 10.1021/Jp4107876 

Brocious, J. and Potma, E. O. "Lighting up micro-structured materials with four-wave mixing microscopy" Materials Today, v.16, 2013, p.344-350. doi:DOI 10.1016/j.mattod.2013.08.001 

Johan Lindgren, Eero Hulkko, Tiina Kiviniemi, Mika Pettersson, V. Ara Apkarian, and Toni Kiljunen "Dynamics Behind the Long-Lived Coherences of I2 in Solid Xe" J. Phys. Chem. A, v.117, 2013, p.4884?4897. doi:10.1021/jp402732b 

Zrimsek, A. B. and Henry, A. I. and Van Duyne, R. P. "Single Molecule Surface-Enhanced Raman Spectroscopy without Nanogaps" Journal of Physical Chemistry Letters, v.4, 2013, p.3206-3210. doi:Doi 10.1021/Jz4017574 

Woznica, M; Butkiewicz, A; Grzywacz, A; Kowalska, P; Masnyk, M; Michalak, K; Luboradzki, R; Furche, F; Kruse, H; Grimme, S; Frelek, J "Ring-Expanded Bicyclic beta-Lactams: A Structure-Chiroptical Properties Relationship Investigation by Experiment and Calculations" JOURNAL OF ORGANIC CHEMISTRY, v.76, 2011, p.3306. doi:10.1021/jo200171  View record at Web of Science

Tatyana Sheps, Jordan Brocious, Brad L. Corso, O. Tolga Gul, Desire Whitmore, Goksel Durkaya, Eric O. Potma, and Philip G. Collins "Four-wave mixing microscopy with electronic contrast of individual carbon nanotubes" Physical Review B, v.86, 2012, p.235412. doi:10.1103/PhysRevB.86.235412 

Rappoport, D; Furche, F "Property-optimized Gaussian basis sets for molecular response calculations" JOURNAL OF CHEMICAL PHYSICS, v.133, 2010, p.. doi:10.1063/1.348428  View record at Web of Science

Y. Wang, X. Liu, D. Whitmore, W. Xing, and Eric O. Potma "Remote multi-color excitation using femtosecond propagating surface plasmon polaritons in gold films" Opt. Express, v.19, 2011, p.13454.

Chulhai, Dhabih V. and Jensen, Lasse "Simulating Surface-Enhanced Raman Optical Activity Using Atomistic Electrodynamics-Quantum Mechanical Models" The Journal of Physical Chemistry A, v., 2014, p.. doi:10.1021/jp502107f 

Kurouski, Dmitry and Zaleski, Stephanie and Casadio, Francesca and Van Duyne, Richard P. and Shah, Nilam C. "Tip-Enhanced Raman Spectroscopy (TERS) for in Situ Identification of Indigo and Iron Gall Ink on Paper" Journal of the American Chemical Society, v.136, 2014, p.8677-8684. doi:10.1021/ja5027612 

Raghunathan, V; Han, Y; Korth, O; Ge, NH; Potma, EO "Rapid vibrational imaging with sum frequency generation microscopy" OPTICS LETTERS, v.36, 2011, p.3891. View record at Web of Science

Chen, C; Chu, P; Bobisch, CA; Mills, DL; Ho, W "Viewing the Interior of a Single Molecule: Vibronically Resolved Photon Imaging at Submolecular Resolution" PHYSICAL REVIEW LETTERS, v.105, 2010, p.. doi:10.1103/PhysRevLett.105.21740  View record at Web of Science

Ying Jiang, Qing Huan, Laura Fabris, Guillermo C. Bazan & Wilson Ho "Submolecular control, spectroscopy and imaging of bond-selective chemistry in single functionalized molecules" Nature Chemistry, v.5, 2012, p.36?41. doi:doi:10.1038/nchem.1488 

I. Warnke, S. Ay, S. Brase, F. Furche "Chiral Cooperativity and Solvent-Induced Tautomerism Effects in Electronic Circular Dichroism Spectra of [2.2]Paracyclophane Ketimines" J. Phys. Chem. A, v.113, 2009, p.6987.

Klingsporn, J. M. and Sonntag, M. D. and Seideman, T. and Van Duyne, R. P. "Tip-Enhanced Raman Spectroscopy with Picosecond Pulses" Journal of Physical Chemistry Letters, v.5, 2014, p.106-110. doi:Doi 10.1021/Jz4024404 

Lee, Joonhee and Tallarida, Nicholas and Rios, Laura and Perdue, Shawn M. and Apkarian, Vartkess Ara "Single Electron Bipolar Conductance Switch Driven by the Molecular Aharonov?Bohm Effect" ACS Nano, v.8, 2014, p.6382-6389. doi:10.1021/nn501875m 

A. A. Kane "Annealing Single-Walled Carbon Nanotube Field Effect Transistors in Ultra High Vacuum" Ph.D. Dissertation, Dept. of Physics and Astronomy, University of California at Irvine, v., 2010, p..

Project Outcomes Report


This Project Outcomes Report for the General Public is displayed verbatim as submitted by the Principal Investigator (PI) for this award. Any opinions, findings, and conclusions or recommendations expressed in this Report are those of the PI and do not necessarily reflect the views of the National Science Foundation; NSF has not approved or endorsed its content.

The Center for Chemistry at the Space-Time Limit (CaSTL) was established in 2009 as an NSF funded Center for Chemical Innovation. The scientific vision of the Center can be summarized as the invention of the Chemiscope – the ability to track individual molecular events in real-time and with atomic resolution. Based at the University of California at Irvine, CaSTL has assembled leading scientists who share the center vision and bring the necessary expertise to realize its goals. In addition to its research mission, CaSTL has spearheaded successful programs of outreach, public education, and efforts to broaden the participation of underrepresented minorities. The Center supports approximately 60 researchers on five different campuses, and prepares a unique brand of scientists trained through multidisciplinary research.

The Chemiscope can be expected to have a similar impact on chemistry and molecular physics as the microscope had on biology. The notable milestones accomplished to date foretell this expectation. Among them are: The observation of the vibration of a single molecule in real-time; seeing the motion of a single electron upon injection into a single molecule; videography of the quantum mechanical motion of a molecular bond; the making and breaking of selected single bonds inside a single molecule; spectroscopy inside a single molecule, with sub-molecular spatial resolution; recording electrical current from a single enzyme molecule as it functions.

The near future will see sharpening of the tools that are already in place, along with developments of equally promising methods, such as ultrafast tunneling microscopy and photo-force microscopy. The implementation of the novel paradigm ushered by CaSTL, to solve outstanding problems in chemistry, is another challenge assumed by the Center. A planned target is the science of direct solar-to-chemical energy conversion. The analytical tools developed in CaSTL are being tuned to have significant technological impact. In this category is the ability to see and track the dynamics of surface states with nanometer spatial resolution, which as a diagnostic tool, should lead to better solar cells, molecular electronics, high performance optoelectronic materials and devices.

As a Center of innovation, in collaboration with its industrial partners, CaSTL is actively pursuing the dissemination of its technologies as they mature. Because of its foreseen demand in nano-engineering, the photo-force microscope is already under commercial co-development as a stand-alone instrument. Targeted to the biomolecular community, and more generally as a surface analytic tool, phase sensitive sum frequency microscopy is an instrument being developed for broad dissemination. And advances toward the Chemiscope are widely emulated.

Beyond the still images of microscopy with atomic resolution that adorn modern textbooks, video clips of CaSTL will bring the dynamic world of molecules to life. A recently published movie of the chemical bond is exemplary. In contrast with classical notions, the quantum reality is a wave motion that can be seen in phase space, and wavefunctions can be directly seen experimentally. The single film clip contains a wealth of lessons to be incorporated in the undergrad curriculum, portending the future of scientific inquiry.

CaSTL has implemented numerous outreach programs aimed at diverse audiences: K-12 education in collaboration with local after-school programs and with local high schools; undergraduate education through targeted laboratory classes; public education by raising awareness through involvement in the science festivals in collaboration with the Optical Society of America, workshops for teachers, and Discovery Science Center; dissemination among the larger scientific community through the organization of symposia and summer schools. CaSTL has already placed over...

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