{"id":{"repo_id":"uiuc","oai_identifier":"oai:www.ideals.illinois.edu:2142/107864"},"canonical_url":"https://search.dev.ndltd.org/etd/uiuc/oai:www.ideals.illinois.edu:2142/107864","repository":{"repo_id":"uiuc","name":"University of Illinois - Urbana-Champaign","base_url":"https://www.ideals.illinois.edu/oai-pmh"},"display":{"title":"Dynamic imaging of nanoparticles on femtoseconds to minutes time scale at atomic resolution","abstract":"Almost 40 years since its conception, the excellent atomic resolution of the scanning tunneling microscope (STM) continues to be excavated to develop single-molecule techniques. In the last 20 years, our group has developed and improved the single-molecule absorption scanning tunneling microscopy (SMA--STM) technique that enabled high-resolution imaging of nanoparticles' electron probability density. This method has set the stage for the STM to investigate the optical and electronic properties of nanoparticles, on a particle-by-particle basis, with sub-nanometer and 0.1-eV resolutions. Most recent applications of the technique are the imaging and manipulating of energy transfer in PbS quantum dots, the imaging of polarization-dependent plasmons on gold nanoislands, and the unraveling of the carbon dot's fluorescence mechanism. Building on this success, a femtosecond time-resolved optical setup has been implemented to integrate the extra time dimension to provide a complete picture of (space, time, energy) for any given nanoparticle. The combination of improvements in electronics, tip-etching condition, and nanoparticle deposition techniques made this instrumentation project possible. As a result, we were able to image the individual ultrafast energy relaxation and transfer processes in carbon dots as well as quantum dots with characteristic kinetics consistent with bulk scale measurements. Furthermore, in our study of the glassy dynamics of ultra-thin silica films, we achieved exceptional vibrational energy resolution that enabled us to resolve the dynamics and energy levels of 1-nm vibrating silica clusters. In addition, we were able to classify the five characteristic configurational sampling behaviors and the frequencies at which they appear. Our measurements also showed consistency in configurational and vibrational entropies with thermodynamic models of the glass transition and that the entropies are comparable.","abstract_html":"Almost 40 years since its conception, the excellent atomic resolution of the scanning tunneling microscope (STM) continues to be excavated to develop single-molecule techniques. In the last 20 years, our group has developed and improved the single-molecule absorption scanning tunneling microscopy (SMA--STM) technique that enabled high-resolution imaging of nanoparticles' electron probability density. This method has set the stage for the STM to investigate the optical and electronic properties of nanoparticles, on a particle-by-particle basis, with sub-nanometer and 0.1-eV resolutions. Most recent applications of the technique are the imaging and manipulating of energy transfer in PbS quantum dots, the imaging of polarization-dependent plasmons on gold nanoislands, and the unraveling of the carbon dot's fluorescence mechanism. Building on this success, a femtosecond time-resolved optical setup has been implemented to integrate the extra time dimension to provide a complete picture of (space, time, energy) for any given nanoparticle. The combination of improvements in electronics, tip-etching condition, and nanoparticle deposition techniques made this instrumentation project possible. As a result, we were able to image the individual ultrafast energy relaxation and transfer processes in carbon dots as well as quantum dots with characteristic kinetics consistent with bulk scale measurements. Furthermore, in our study of the glassy dynamics of ultra-thin silica films, we achieved exceptional vibrational energy resolution that enabled us to resolve the dynamics and energy levels of 1-nm vibrating silica clusters. In addition, we were able to classify the five characteristic configurational sampling behaviors and the frequencies at which they appear. Our measurements also showed consistency in configurational and vibrational entropies with thermodynamic models of the glass transition and that the entropies are comparable.","abstract_has_math":false,"creators":["Nguyen, Huy Anquoc"],"institution":"University of Illinois at Urbana-Champaign","degree_name":"Ph.D.","degree_level":"Dissertation","degree_discipline":"Chemistry","degree_department":null,"school":null,"contributors":["Gruebele, Martin","Lyding, Joseph","Jain, Prashant","Hirata, So"],"advisors":[],"committee_chairs":[],"committee_members":[],"year":2020,"date_issued":"2020-08-26T21:54:09Z","date_published":"2020-08-26T21:54:09Z","updated_at":"2026-07-22T22:24:47Z","subjects":["STM","pump-probe","carbon dots","quantum dots","glassy dynamics"],"languages":["en"],"rights":["Copyright 2020 Huy Nguyen"],"rights_urls":[],"identifier_entries":[]},"links":{"outbound_url":"http://hdl.handle.net/2142/107864","outbound_label":"Handle","outbound_source":"dc:identifier"},"metadata_groups":[{"id":"people","label":"People","entries":[{"key":"dc:contributor","label":"Contributor","values":["Gruebele, Martin","Lyding, Joseph","Jain, Prashant","Hirata, So"]},{"key":"dc:creator","label":"Author","values":["Nguyen, Huy Anquoc"]}]},{"id":"academic_context","label":"Academic Context","entries":[{"key":"dc:date","label":"Dc Date","values":["2020-08-26T21:54:09Z","2020-05-07","2020-05"]},{"key":"dc:type","label":"Dc Type","values":["text","Thesis"]},{"key":"thesis:degree_discipline","label":"Discipline","values":["Chemistry"]},{"key":"thesis:degree_level","label":"Degree Level","values":["Dissertation"]},{"key":"thesis:degree_name","label":"Degree Name","values":["Ph.D."]},{"key":"thesis:institution_name","label":"Thesis Institution Name","values":["University of Illinois at Urbana-Champaign"]}]},{"id":"subjects_keywords","label":"Subjects and Keywords","entries":[{"key":"dc:subject","label":"Dc Subject","values":["STM","pump-probe","carbon dots","quantum dots","glassy dynamics"]}]},{"id":"language_rights","label":"Language and Rights","entries":[{"key":"dc:language","label":"Dc Language","values":["en"]},{"key":"dc:rights","label":"Dc Rights","values":["Copyright 2020 Huy Nguyen"]}]},{"id":"identifiers","label":"Identifiers","entries":[{"key":"dc:identifier","label":"Identifier","values":["http://hdl.handle.net/2142/107864"]}]},{"id":"additional","label":"Additional Metadata","entries":[{"key":"dc:description","label":"Description","values":["Almost 40 years since its conception, the excellent atomic resolution of the scanning tunneling microscope (STM) continues to be excavated to develop single-molecule techniques. In the last 20 years, our group has developed and improved the single-molecule absorption scanning tunneling microscopy (SMA--STM) technique that enabled high-resolution imaging of nanoparticles' electron probability density. This method has set the stage for the STM to investigate the optical and electronic properties of nanoparticles, on a particle-by-particle basis, with sub-nanometer and 0.1-eV resolutions. Most recent applications of the technique are the imaging and manipulating of energy transfer in PbS quantum dots, the imaging of polarization-dependent plasmons on gold nanoislands, and the unraveling of the carbon dot's fluorescence mechanism. Building on this success, a femtosecond time-resolved optical setup has been implemented to integrate the extra time dimension to provide a complete picture of (space, time, energy) for any given nanoparticle. The combination of improvements in electronics, tip-etching condition, and nanoparticle deposition techniques made this instrumentation project possible. As a result, we were able to image the individual ultrafast energy relaxation and transfer processes in carbon dots as well as quantum dots with characteristic kinetics consistent with bulk scale measurements. Furthermore, in our study of the glassy dynamics of ultra-thin silica films, we achieved exceptional vibrational energy resolution that enabled us to resolve the dynamics and energy levels of 1-nm vibrating silica clusters. In addition, we were able to classify the five characteristic configurational sampling behaviors and the frequencies at which they appear. Our measurements also showed consistency in configurational and vibrational entropies with thermodynamic models of the glass transition and that the entropies are comparable.","Submission original under an indefinite embargo labeled 'Open Access'. The submission was exported from vireo on 2020-08-25 without embargo terms","The student, Huy Nguyen, accepted the attached license on 2020-05-04 at 11:20.","The student, Huy Nguyen, submitted this Dissertation for approval on 2020-05-04 at 11:26.","This Dissertation was approved for publication on 2020-05-07 at 14:37.","DSpace SAF Submission Ingestion Package generated from Vireo submission #14922 on 2020-08-25 at 17:06:00","Made available in DSpace on 2020-08-26T21:54:09Z (GMT). No. of bitstreams: 9 NGUYEN-DISSERTATION-2020.pdf: 69919656 bytes, checksum: 4e2692bfabe27c97ada6384ed1f7c07d (MD5) 10B6.avi: 81862 bytes, checksum: 66f8e1c7e3349e79b10f2167dc0f1503 (MD5) 28Si4.avi: 379512 bytes, checksum: 6fbef4fc9b3aea46116b712e75b5514d (MD5) 5Si4.avi: 416764 bytes, checksum: 7d9acc0f5e814e624a79f6781fbb7547 (MD5) 6Si4.avi: 330232 bytes, checksum: ca6bbba5f72bff448845fa551b15c62f (MD5) Fig 2a cits_dos.mov: 1828958 bytes, checksum: f5f27c552ac7869000cbc924f810f308 (MD5) Fig 2e cits_dos.mov: 1599706 bytes, checksum: c6877b604d4f64c2f1b7db7463f71788 (MD5) LICENSE.txt: 4207 bytes, checksum: 4511754dffbdfa60a29989d2ebde464e (MD5) PROQUEST_LICENSE.txt: 4553 bytes, checksum: 51e772f1ac577dddca1fe603498fd076 (MD5) Previous issue date: 2020-05-07"]},{"key":"dc:format","label":"Dc Format","values":["application/pdf"]},{"key":"dc:title","label":"Title","values":["Dynamic imaging of nanoparticles on femtoseconds to minutes time scale at atomic resolution"]}]}],"canonical_facts":{"dc:contributor":["Gruebele, Martin","Lyding, Joseph","Jain, Prashant","Hirata, So"],"dc:creator":["Nguyen, Huy Anquoc"],"dc:date":["2020-08-26T21:54:09Z","2020-05-07","2020-05"],"dc:description":["Almost 40 years since its conception, the excellent atomic resolution of the scanning tunneling microscope (STM) continues to be excavated to develop single-molecule techniques. In the last 20 years, our group has developed and improved the single-molecule absorption scanning tunneling microscopy (SMA--STM) technique that enabled high-resolution imaging of nanoparticles' electron probability density. This method has set the stage for the STM to investigate the optical and electronic properties of nanoparticles, on a particle-by-particle basis, with sub-nanometer and 0.1-eV resolutions. Most recent applications of the technique are the imaging and manipulating of energy transfer in PbS quantum dots, the imaging of polarization-dependent plasmons on gold nanoislands, and the unraveling of the carbon dot's fluorescence mechanism. Building on this success, a femtosecond time-resolved optical setup has been implemented to integrate the extra time dimension to provide a complete picture of (space, time, energy) for any given nanoparticle. The combination of improvements in electronics, tip-etching condition, and nanoparticle deposition techniques made this instrumentation project possible. As a result, we were able to image the individual ultrafast energy relaxation and transfer processes in carbon dots as well as quantum dots with characteristic kinetics consistent with bulk scale measurements. Furthermore, in our study of the glassy dynamics of ultra-thin silica films, we achieved exceptional vibrational energy resolution that enabled us to resolve the dynamics and energy levels of 1-nm vibrating silica clusters. In addition, we were able to classify the five characteristic configurational sampling behaviors and the frequencies at which they appear. Our measurements also showed consistency in configurational and vibrational entropies with thermodynamic models of the glass transition and that the entropies are comparable.","Submission original under an indefinite embargo labeled 'Open Access'. The submission was exported from vireo on 2020-08-25 without embargo terms","The student, Huy Nguyen, accepted the attached license on 2020-05-04 at 11:20.","The student, Huy Nguyen, submitted this Dissertation for approval on 2020-05-04 at 11:26.","This Dissertation was approved for publication on 2020-05-07 at 14:37.","DSpace SAF Submission Ingestion Package generated from Vireo submission #14922 on 2020-08-25 at 17:06:00","Made available in DSpace on 2020-08-26T21:54:09Z (GMT). No. of bitstreams: 9 NGUYEN-DISSERTATION-2020.pdf: 69919656 bytes, checksum: 4e2692bfabe27c97ada6384ed1f7c07d (MD5) 10B6.avi: 81862 bytes, checksum: 66f8e1c7e3349e79b10f2167dc0f1503 (MD5) 28Si4.avi: 379512 bytes, checksum: 6fbef4fc9b3aea46116b712e75b5514d (MD5) 5Si4.avi: 416764 bytes, checksum: 7d9acc0f5e814e624a79f6781fbb7547 (MD5) 6Si4.avi: 330232 bytes, checksum: ca6bbba5f72bff448845fa551b15c62f (MD5) Fig 2a cits_dos.mov: 1828958 bytes, checksum: f5f27c552ac7869000cbc924f810f308 (MD5) Fig 2e cits_dos.mov: 1599706 bytes, checksum: c6877b604d4f64c2f1b7db7463f71788 (MD5) LICENSE.txt: 4207 bytes, checksum: 4511754dffbdfa60a29989d2ebde464e (MD5) PROQUEST_LICENSE.txt: 4553 bytes, checksum: 51e772f1ac577dddca1fe603498fd076 (MD5) Previous issue date: 2020-05-07"],"dc:format":["application/pdf"],"dc:identifier":["http://hdl.handle.net/2142/107864"],"dc:language":["en"],"dc:rights":["Copyright 2020 Huy Nguyen"],"dc:subject":["STM","pump-probe","carbon dots","quantum dots","glassy dynamics"],"dc:title":["Dynamic imaging of nanoparticles on femtoseconds to minutes time scale at atomic resolution"],"dc:type":["text","Thesis"],"thesis:degree_discipline":["Chemistry"],"thesis:degree_level":["Dissertation"],"thesis:degree_name":["Ph.D."],"thesis:institution_name":["University of Illinois at Urbana-Champaign"]},"updated_at":"2026-07-22T22:24:47Z"}