Colloidal semiconductor quantum dots(QDs)constitute a perfect material for ink-jet printable large area displays,photovoltaics,light-emitting diode,bio-imaging luminescent markers and many other applications.For this ...Colloidal semiconductor quantum dots(QDs)constitute a perfect material for ink-jet printable large area displays,photovoltaics,light-emitting diode,bio-imaging luminescent markers and many other applications.For this purpose,efficient light emission/absorption and spectral tunability are necessary conditions.These are currently fulfilled by the direct bandgap materials.Si-QDs could offer the solution to major hurdles posed by these materials,namely,toxicity(e.g.,Cd-,Pb-or As-based QDs),scarcity(e.g.,QD with In,Se,Te)and/or instability.Here we show that by combining quantum confinement with dedicated surface engineering,the biggest drawback of Si—the indirect bandgap nature—can be overcome,and a‘direct bandgap’variety of Si-QDs is created.We demonstrate this transformation on chemically synthesized Si-QDs using state-of-the-art optical spectroscopy and theoretical modelling.The carbon surface termination gives rise to drastic modification in electron and hole wavefunctions and radiative transitions between the lowest excited states of electron and hole attain‘direct bandgap-like’(phonon-less)character.This results in efficient fast emission,tunable within the visible spectral range by QD size.These findings are fully justified within a tight-binding theoretical model.When the C surface termination is replaced by oxygen,the emission is converted into the well-known red luminescence,with microsecond decay and limited spectral tunability.In that way,the‘direct bandgap’Si-QDs convert into the‘traditional’indirect bandgap form,thoroughly investigated in the past.展开更多
基金This work was financially supported by Stichting der Fundamenteel Onderzoek der Materie and Stichting voor de Technische Wetenschappen.Part of this work(CPU,JMJP andHZ)was financed by the Dutch Polymer Institute for funding of UCin Functional Polymer Systemsproject no.681,and(ANP andAAP)Russian Foundation for Basic Research and‘Dynasty’-Foundation of International Center for Fundamental Physics in Moscow.
文摘Colloidal semiconductor quantum dots(QDs)constitute a perfect material for ink-jet printable large area displays,photovoltaics,light-emitting diode,bio-imaging luminescent markers and many other applications.For this purpose,efficient light emission/absorption and spectral tunability are necessary conditions.These are currently fulfilled by the direct bandgap materials.Si-QDs could offer the solution to major hurdles posed by these materials,namely,toxicity(e.g.,Cd-,Pb-or As-based QDs),scarcity(e.g.,QD with In,Se,Te)and/or instability.Here we show that by combining quantum confinement with dedicated surface engineering,the biggest drawback of Si—the indirect bandgap nature—can be overcome,and a‘direct bandgap’variety of Si-QDs is created.We demonstrate this transformation on chemically synthesized Si-QDs using state-of-the-art optical spectroscopy and theoretical modelling.The carbon surface termination gives rise to drastic modification in electron and hole wavefunctions and radiative transitions between the lowest excited states of electron and hole attain‘direct bandgap-like’(phonon-less)character.This results in efficient fast emission,tunable within the visible spectral range by QD size.These findings are fully justified within a tight-binding theoretical model.When the C surface termination is replaced by oxygen,the emission is converted into the well-known red luminescence,with microsecond decay and limited spectral tunability.In that way,the‘direct bandgap’Si-QDs convert into the‘traditional’indirect bandgap form,thoroughly investigated in the past.
