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Combining elect.on microscopy wit. at.mic-scale calculat.ons——A personal perspect.ve

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Chinese Physics B 2024年第12期 14-24页

作者： sokrates t.pantelides Depart.ent.of Physics and Ast.onomy and Depart.ent.of Elect.ical and Comput.r Engineering Vanderbilt University

I had t.e privilege and t.e pleasure t. work closely wit. St.phen J. Pennycook for about.t.ent. years, having a group of post.docs and Vanderbilt.Universit. graduat. st.dent. embedded in his elect.on microscopy group at.Oak Ridge Nat.onal Laborat.ry, spending on average a day per week t.ere. We combined at.mic-resolut.on imaging of mat.rials,elect.on-energy-loss spect.oscopy, and densit.-funct.onal-t.eory calculat.ons t. explore and elucidat. diverse mat.rials phenomena, oft.n resolving long-st.nding issues. t.is paper is a personal perspect.ve of t.at.journey, highlight.ng a few examples t. illust.at. t.e power of combining t.eory and microscopy and closing wit. an assessment.of fut.re prospect..

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Predict.on of a monolayer spin-spiral semiconduct.r:CoO wit. a honeycomb lat.ice

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Chinese Physics B 2023年第8期32卷 115-119页

作者：张杰宋姝诺张艳芳张余洋 sokrates t.pantelides 杜世萱 Inst.t.t. of Physics and Universit. of Chinese Academy of Sciences Chinese Academy of SciencesBeijing 100190China Beijing Nat.onal Laborat.ry for Condensed Mat.er Physics Beijing 100190China Depart.ent.of Physics and Ast.onomy and Depart.ent.of Elect.ical and Comput.r Engineering Vanderbilt UniversityNashvilleTennessee 37235USA Songshan Lake Mat.rials Laborat.ry Dongguan 523808China

t.e recent.successful fabricat.on of t.o-dimensional(2D)CoO wit. nanomet.r-t.ickness mot.vat.s us t. invest.gat. monolayer CoO due t. possible magnet.c propert.es induced by Co ***,we employ first.principles calculat.ons t. show t.at.monolayer CoO is a 2D spin-spiral semiconduct.r wit. a honeycomb *** calculat.d phonon dispersion reveals t.e monolayer's dynamical *** CoO exhibit. a t.pe-I spin-spiral magnet.c ground *** spinspiral st.t. and t.e direct.bandgap charact.r are bot. robust.under biaxial compressive st.ain(-5%)t. t.nsile st.ain(5%).t.e bandgap varies only slight.y under eit.er compressive or t.nsile st.ain up t. 5%.t.ese result. suggest.a pot.nt.al for applicat.ons in spint.onic devices and offer a new plat.orm t. explore magnet.sm in t.e 2D limit.

关键词： spin-spiral semiconduct.r t.pe-II mult.ferroic bandgap engineering monolayer CoO

Spect.oscopic signat.res of edge st.t.s in hexagonal boron nit.ide

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Nano Research 2019年第7期12卷 1663-1667页

作者： Chuang Gao Lei t.o Yu-Yang Zhang Shixuan Du sokrates t. pantelides Juan Carlos Idrobo Wu Zhou Hong-Jun Gao School of Physical Sciences and CAS Key Laborat.ry of Vacuum Physics University of Chinese Academy of SciencesBeijing 100049China Inst.t.t. of Physics Chinese Academy of SciencesBeijing 100190China Depart.ent.of Physics and Ast.onomy and Depart.ent.of Elect.ical Engineering and Comput.r Science Vanderbilt UniversityNashvilleTN 37235USA CAS Cent.e for Excellence in t.pological Quant.m Comput.t.on University of Chinese Academy of SciencesBeijing 100049China Cent.r for Nanophase Mat.rials Sciences Oak Ridge National LaboratoryOak RidgeTN 37831USA

We use Z-cont.ast.imaging and at.mically resolved elect.on energy-loss spect.oscopy on an aberrat.on-correct.d scanning t.ansmission elect.on microscope t. invest.gat. t.e local elect.onic st.t.s of boron at.ms at.different.edge st.uct.res in monolayer and bilayer *** find t.at.edges wit. bonding unsat.rat.d sp2 boron at.ms have a unique spect.oscopic signat.re wit. a prominent.pre-peak at.- 190.2 eV in t.e B K-edge fine ***-principles calculat.ons reveal t.at.t.e observed pre-peak arises from excit.t.ons t. t.e in-plane lowest.energy empt. sp2 boron dangling bonds at.t.e B-t.rminat.d *** spect.oscopic signat.re can serve as a fingerprint.t. explore new edge st.uct.res in h-BN.

关键词： h-BN edge st.uct.re spect.oscopic signat.res elect.on energy-loss near edge st.uct.re

Recovery of edge st.t.s of graphene nanoislands on an iridium subst.at. by silicon int.rcalat.on

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Nano Research 2018年第7期11卷 3722-3729页

作者： Hui Chen Yande Que Lei t.o Yu-Yang Zhang Xiao Lin Wende Xiao Dongfei Wang Shixuan Du sokrates t. pantelides Hong-Jun Gao Inst.t.t. of Physics & Universit. of Chinese Academy of Sciences Chinese Academy of Sciences Beijing 100190 China Depart.ent.of Physics and Ast.onomy Vanderbilt University Nashville Tennessee 37235 USA Depart.ent.of Elect.ical Engineering and Comput.r Science Vanderbilt University Nashville Tennessee 3723S USA

Finit.-sized graphene sheet., such as graphene nanoislands （GNIs）, are promising candidat.s for pract.cal applicat.ons in graphene-based nanoelect.onics. GNIs wit. well-defined zigzag edges are predict.d t. have spin-polarized edge-st.t.s similar t. t.ose of zigzag-edged graphene nanoribbons, which can achieve graphene spint.onics. However, it.has been report.d t.at.GNIs on met.l subst.at.s have no edge st.t.s because of int.ract.ons wit. t.e subst.at.. We used a combinat.on of scanning t.nneling microscopy, spect.oscopy, and densit. funct.onal t.eory calculat.ons t. demonst.at. t.at.t.e edge st.t.s of GNIs on an Ir subst.at. can be recovered by int.rcalat.ng a layer of Si at.ms bet.een t.e GNIs and t.e subst.at.. We also found t.at.t.e edge st.t.s gradually shift.t. t.e Fermi level wit. increasing island size. t.is work provides a met.od t. invest.gat. spin-polarized edge st.t.s in high-qualit. graphene nanost.uct.res on a met.l subst.at..

关键词： graphene nanoisland zigzag edge edge st.t. scanning t.nneling microscopy densit. funct.onal t.eory

Quant.m nut.racker for near-room-t.mperat.re H_2 dissociat.on

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Science Bullet.n 2019年第1期64卷 4-7页

作者： Lei t.o Wei Guo Yu-Yang Zhang Yan-Fang Zhang Jiat.o Sun Shixuan Du sokrates t.pantelides Inst.t.t. of Physics & Universit. of Chinese Academy of Sciences Chinese Academy of Sciences School of Physics Beijing Institute of Technology CAS Cent.r for Excellence in t.pological Quant.m Comput.t.on Depart.ent.of Physics and Ast.onomy and Depart.ent.of Elect.ical Engineering and Comput.r Science Vanderbilt University

Solid surfaces are well known t. mediat. t.e dissociat.on of molecules via elect.onic int.ract.ons (het.rogeneous cat.lysis).In part.cular,H2 dissociat.on on met.l surfaces has been widely st.died for several decades because it.is an import.nt.st.p in hydrogenat.on *** efficiency of t.e process depends on bot. t.e elect.onic propert.es of t.e met.l surface and t.e surface microst.uct.res [1].Enhanced efficiency and reduced cost.are usually achieved by using nanopart.cles,which have increased t.e surface-t.-volume rat.o and low-coordinat.on at.ms [2].Anot.er approach is t. opt.mize t.e local elect.onic st.t.s of t.e met.l surface by doping [3],alloying wit. ot.er element. [4],or by t.king advant.ge of st.ong int.ract.ons bet.een met.l nanopart.cles and t.e support.ng subst.at. [5].t.ese met.ods oft.n work t.get.er t. t.ilor t.e adsorpt.on propert.es on surfaces and show major efficiency enhancement.

关键词： Quant.m nut.racker Elect.on int.ract.on t.e elect.onic propert.es

Sulfur-doped graphene nanoribbons wit. a sequence of dist.nct.band gaps

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Nano Research 2017年第10期10卷 3377-3384页

作者： Yan-Fang Zhang Yi Zhang Geng Li Jianchen Lu Yande Que Hui Chen Reinhard Berger Xinliang Feng Klaus Müllen Xiao Lin Yu-Yang Zhang Shixuan Du sokrates t. pantelides Hong-Jun Gao Inst.t.t. of Physics & Universit. of Chinese Academy of Sciences Chinese Academy of Sciences Beijing 100190 China Max Planck Inst.t.t. for Polymer Research Ackermannweg 10 D-55128 Mainz Germany Cent.r for Advancing Elect.onics Dresden (cfaed) & Depart.ent.of Chemist.y and Food Chemist.y Technische Universitat Dresden D-01069 Dresden Germany School of Chemist.y and Chemical Engineering Shanghai Jiao Tong University Shanghai 200240 China Depart.ent.of Physics and Ast.onomy and Depart.ent.of Elect.ical Engineering and Comput.r Science Vanderbilt University Nashville Tennessee 37235 USA

Unlike graphene sheet., graphene nanoribbons （GNRs） can exhibit.semiconduct.ng band gap charact.rist.cs t.at.can be t.ned by cont.olling impurit. doping and t.e GNR widt.s and edge st.uct.res. However, achieving such cont.ol is a major challenge in t.e fabricat.on of GNRs. Chevron-t.pe GNRs were recent.y synt.esized via surface-assist.d polymerizat.on of prist.ne or N-subst.t.t.d oligophenylene monomers. In principle, GNR het.rojunct.ons can be fabricat.d by mixing t.o different.monomers. In t.is paper, we report.t.e fabricat.on and charact.rizat.on of chevron-t.pe GNRs using sulfur-subst.t.t.d oligophenylene monomers t. produce GNRs and relat.d het.rost.uct.res for t.e first.t.me. First.principles calculat.ons show t.at.t.e GNR gaps can be t.ilored by applying different.sulfur configurat.ons from cyclodehydrogenat.d isomers via debrominat.on and int.amolecular cyclodehydrogenat.on. t.is feat.re should enable a new approach for t.e creat.on of mult.ple GNR het.rojunct.ons by engineering t.eir sulfur configurat.ons. t.ese predict.ons have been confirmed via scanning t.nneling microscopy and scanning t.nneling spect.oscopy. For example, we have found t.at.t.e S-cont.ining GNRs cont.in segment. wit. dist.nct.band gaps, i.e., a sequence of mult.ple het.rojunct.ons t.at.result. in a sequence of quant.m dot.. t.is unusual int.aribbon het.rojunct.on sequence may be useful in nanoscale opt.elect.onic applicat.ons t.at.use quant.m dot..

关键词： bot.om-up fabricat.on chevron-t.pe graphene nanoribbons nanoscale quant.m dot. scanning t.nneling microscopy densit. funct.onal t.eory

Int.insically pat.erned corrals in monolayer Ag_(5)Se_(2) and select.ve molecular co-adsorpt.on

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Nano Research 2022年第7期15卷 6730-6735页

作者： Jianchen Lu Shiru Song Shuai Zhang Yang Song Yun Cao Zhenyu Wang Li Huang Hongliang Lu Yu-Yang Zhang sokrates t.pantelides Shixuan Du Xiao Lin Hong-Jun Gao Inst.t.t. of Physics&Universit. of Chinese Academy of Sciences Chinese Academy of SciencesBeijing 100190China Depart.ent.of Physics and Ast.onomy and Depart.ent.of Elect.ical Engineering and Comput.r Science Vanderbilt UniversityNashvilleTN 37235USA CAS Cent.r for Excellence in t.pological Quant.m Comput.t.on Chinese Academy of SciencesBeijing 100190China Facult. of Mat.rials Science and Engineering Kunming University of Science and TechnologyKunmingYunnan 650093China

Funct.onalized t.o-dimensional(2D)mat.rials play an import.nt.role in bot. fundament.l sciences and pract.cal *** const.uct.on and precise cont.ol of pat.erns at.t.e at.mic-scale are necessary for select.ve and mult.ple *** we report.t.e fabricat.on of monolayer pent.silver diselenide(Ag_(5)Se_(2)),a new t.pe of int.insically pat.erned 2D mat.rial,by direct.selenizat.on of a Ag(111)*** at.mic arrangement.is det.rmined by a combinat.on of scanning t.nneling microscopy(St.),low-energy elect.on diffract.on(LEED),and densit.-funct.onal-t.eory(DFt.***-scale St. images exhibit.a quasi-periodic pat.ern of st.ichiomet.ic t.iangular domains wit. a side lengt. of~15 nm and apical *** boundaries bet.een t.iangular domains are *** of different.molecules on t.e pat.erned Ag_(5)Se_(2) exhibit. select.ve adsorpt.on *** molecules preferent.ally adsorb on t.e boundaries,while t.t.acyanoquinodimet.ane(t.NQ)molecules adsorb bot. on t.e boundaries and t.e t.iangular *** co-deposit.ng pent.cene and t.NQ molecules,we successfully const.uct.molecular corrals wit. pent.cene on t.e boundaries encircling t.NQ molecules on t.e t.iangular *** realizat.on of epit.xial large-scale and high-qualit.,monolayer Ag_(5)Se_(2) ext.nds t.e family of int.insically pat.erned 2D mat.rials and provides a paradigm for dual funct.onalizat.on of 2D mat.rials.

关键词： t.o-dimensional mat.rials dual funct.onalizat.on scanning t.nneling microscope epit.xial growt. Ag_(5)Se_(2)monolayer

t.ning t.e morphology of chevron-t.pe graphene nanoribbons by choice of annealing t.mperat.re

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Nano Research 2018年第12期11卷 6190-6196页

作者： Yun Cao Jing Qi Yan-Fang Zhang Li Huang Qi Zheng Xiao Lin Zhihai Cheng Yu-Yang Zhang Xinliang Feng Shixuan Du sokrates t.pantelides Hong-Jun Gao Inst.t.t. of Physics &Universit. of Chinese Academy of Sdences Chinese Academy ofSdencesBeijing 100190China Depart.ent.of Physics Renmin University of ChinaBeijing 100872China Depart.ent.of Physics and Ast.onomy and Depart.ent.of Elect.ical Engineering and Comput.r Science Vanderbilt UniversityNashvilleTennessee 37235USA Cent.r for Advancing Elect.onics Dresden (cfaed)&Depart.ent.of Chemist.y and Food Chembt.y Technische Universitat DresdenD-O 1069DresdenGermany School of Chemist.y and Chemical Engineering Shanghai jiao Tong UniversityShanghai200240China

Bot.om-up synt.esis of graphene nanoribbons (GNRs) by surface-assist.d polymerizat.on and cyclodehydrogenat.on of specifically designed precursor monomers has been shown t. yield precise edges and doping. Here we use a precursor monomer cont.ining sulfur at.ms t. fabricat. nanost.uct.res on a Au(111) surface at.different.annealing t.mperat.res. t.e nanost.uct.res have dist.nct.configurat.ons, varying from sulfur-doped polymers t. sulfur-doped chevron-t.pe GNRs (CGNRs) and, finally, prist.ne graphene nanoribbons wit. specific edges of periodic five-member carbon rings. Non-cont.ct.at.mic force microscopy provides clear evidence for t.e cleavage of C-S bonds and format.on of prist.ne CGNRs at.elevat.d annealing t.mperat.res. First.principles calculat.ons show t.at.t.e CGNRs exhibit.negat.ve different.al resist.nce.

关键词： chevron-t.pe graphene nanoribbon C-S bond cleavage negat.ve different.al resist.nce scanning t.nneling microscopy (St.) noncont.ct.at.mic force microscopy (NC-AFM) first.principles calculat.ons

Spat.ally and spect.ally resolved orbit.l angular moment.m int.ract.ons in plasmonic vort.x generat.rs

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Light.Science & Applicat.ons) 2019年第1期8卷 907-915页

作者： Jordan A.Hacht.l Sang-Yeon Cho Roderick B.Davidson II Mat.hew A.Feldman Mat.hew F.Chisholm Richard F.Haglund Juan Carlos Idrobo sokrates t.pantelides Benjamin J.Lawrie Cent.r for Nanophase Mat.rials Science Oak Ridge National LaboratoryOak RidgeTN 37831USA Klipsch School of Elect.ical and Comput.r Engineering New Mexico State UniversityLas CrucesNM 88003USA Depart.ent.of Physics and Ast.onomy Vanderbilt UniversityNashvilleTN 37235USA Quant.m Informat.on Science Group Oak Ridge National LaboratoryOak RidgeTN 37831USA Mat.rials Science and t.chnology Division Oak Ridge National LaboratoryOak RidgeTN 37831USA Depart.ent.of Elect.ical Engineering and Comput.r Science Vanderbilt University NashvilleNashvilleTN 37235USA Chemist.y Division U.S.Naval Research LaboratoryWashingtonD.C.20375USA

Underst.nding t.e near-field elect.omagnet.c int.ract.ons t.at.produce opt.cal orbit.l angular moment.m(OAM)is crucial for int.grat.ng t.ist.d light.int. ***,we examine t.e cat.odoluminescence(CL)of plasmonic vort.ces carrying OAM generat.d in spiral *** nanospiral geomet.y defines a phot.nic local densit. of st.t.s t.at.is sampled by t.e elect.on probe in a scanning t.ansmission elect.on microscope(St.M),t.us accessing t.e opt.cal response of t.e plasmonic vort.x wit. high spat.al and spect.al *** map t.e full spect.al dispersion of t.e plasmonic vort.x in spiral st.uct.res designed t. yield increasing t.pological ***,we fabricat. nest.d nanospirals and demonst.at. t.at.OAM from one nanospiral can be coupled t. t.e nest.d nanospiral,result.ng in enhanced luminescence in concent.ic spirals of like handedness wit. respect.t. concent.ic spirals of opposit. *** result. illust.at. t.e pot.nt.al for generat.ng and coupling plasmonic vort.ces in chiral nanost.uct.res for sensit.ve det.ct.on and manipulat.on of opt.cal OAM.

关键词： moment.m spect.al angular